Horizontal and Vertical Distribution of Perfluoroalkyl Acids (PFAAs) in the Water Column of the Atlantic OceanClick to copy article linkArticle link copied!
- Eleni K. Savvidou*Eleni K. Savvidou*Email: [email protected]Department of Environmental Science, Stockholm University, 106 91 Stockholm, SwedenMore by Eleni K. Savvidou
- Bo ShaBo ShaDepartment of Environmental Science, Stockholm University, 106 91 Stockholm, SwedenMore by Bo Sha
- Matthew E. SalterMatthew E. SalterDepartment of Environmental Science, Stockholm University, 106 91 Stockholm, SwedenBolin Centre for Climate Research, Stockholm University, 106 91 Stockholm, SwedenMore by Matthew E. Salter
- Ian T. CousinsIan T. CousinsDepartment of Environmental Science, Stockholm University, 106 91 Stockholm, SwedenMore by Ian T. Cousins
- Jana H. JohanssonJana H. JohanssonDepartment of Thematic Studies − Environmental Change, Linköping University, 581 83 Linköping, SwedenMore by Jana H. Johansson
Abstract
Perfluoroalkyl acids (PFAAs) are widely distributed in the oceans which are their largest global reservoir, but knowledge is limited about their vertical distribution and fate. This study measured the concentrations of PFAAs (perfluoroalkyl carboxylic acids (PFCAs) with 6 to 11 carbons and perfluoroalkanesulfonic acids (PFSAs) with 6 and 8 carbons) in the surface and deep ocean. Seawater depth profiles from the surface to a 5000 m depth at 28 sampling stations were collected in the Atlantic Ocean from ∼50° N to ∼50° S. The results demonstrated PFAA input from the Mediterranean Sea and the English Channel. Elevated PFAA concentrations were observed at the eastern edge of the Northern Atlantic Subtropical Gyre, suggesting that persistent contaminants may accumulate in ocean gyres. The median ΣPFAA surface concentration in the Northern Hemisphere (n = 17) was 105 pg L–1, while for the Southern Hemisphere (n = 11) it was 28 pg L–1. Generally, PFAA concentrations decreased with increasing distance to the coast and increasing depth. The C6–C9 PFCAs and C6 and C8 PFSAs dominated in surface waters, while longer-chain PFAAs (C10–C11 PFCAs) peaked at intermediate depths (500–1500 m). This profile may be explained by stronger sedimentation of longer-chain PFAAs, as they sorb more strongly to particulate organic matter.
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License Summary*
You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below:
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License Summary*
You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below:
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Introduction
Materials and Methods
Figure 1
Figure 1. Map of the sampling stations along the transect and composition pattern of PFAAs (PFAAs below the detection limit are excluded) in the surface water samples (2 and 5 m) at the sampling stations.
Results and Discussion
Trends of PFAA Concentrations in the Surface of the Water Column
Figure 2
Figure 2. Spatial distribution of the sum of PFAAs in the northern and southern hemisphere of the Atlantic Ocean. Black dots represent sample points where ΣPFAAs could be detected; gray triangles represent nondetects.
Trends of PFAA Concentrations with Depth and Their Vertical Distribution
Figure 3
Figure 3. Distribution of PFNA in the vertical water column in the Northern Hemisphere. Black dots represent the sampling stations; gray triangles are nondetects (<MDL).
Supporting Information
The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.estlett.3c00119.
Additional information on materials and methods including additional tables and graphs (PDF)
All CTD data and concentrations (XLSX)
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Acknowledgments
The Atlantic Meridional Transect is funded by the UK Natural Environment Research Council through its National Capability Long-term Single Centre Science Programme, Climate Linked Atlantic Sector Science (Grant Number NE/R015953/1). This study contributes to the international IMBeR project and is contribution number 390 of the AMT programme. The study received funding from the Swedish Research Council (2016-04131) and FORMAS (2016-00644 and 2020-01978).
References
This article references 51 other publications.
- 1Prevedouros, K.; Cousins, I. T.; Buck, R. C.; Korzeniowski, S. H. Sources, Fate and Transport of Perfluorocarboxylates. Environ. Sci. Technol. 2006, 40 (1), 32– 44, DOI: 10.1021/es0512475Google Scholar1https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXht1Gru7zK&md5=39fe4ec81ae1fa6d9b5fa387ff0e74b7Sources, Fate and Transport of PerfluorocarboxylatesPrevedouros, Konstantinos; Cousins, Ian T.; Buck, Robert C.; Korzeniowski, Stephen H.Environmental Science and Technology (2006), 40 (1), 32-44CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A review describes the sources, fate, and transport of perfluorocarboxylates (PFCAs) in the environment, with a specific focus on perfluorooctanoate (PFO). The global historical industry-wide emissions of total PFCAs from direct (manuf., use, consumer products) and indirect (PFCA impurities and/or precursors) sources were estd. to be 3200-7300 tons. It was estd. that the majority (∼80%) of PFCAs have been released to the environment from fluoropolymer manuf. and use. Although indirect sources were estd. to be much less important than direct sources, there were larger uncertainties assocd. with the calcns. for indirect sources. The phys.-chem. properties of PFO (negligible vapor pressure, high soly. in water, and moderate sorption to solids) suggested that PFO would accumulate in surface waters. Estd. mass inventories of PFO in various environmental compartments confirmed that surface waters, esp. oceans, contain the majority of PFO. The only environmental sinks for PFO were identified to be sediment burial and transport to the deep oceans, implying a long environmental residence time. Transport pathways for PFCAs in the environment were reviewed, and it was concluded that, in addn. to atm. transport/degrdn. of precursors, atm. and ocean water transport of the PFCAs themselves could significantly contribute to their long-range transport. It was estd. that 2-12 tons/yr of PFO are transported to the Arctic by oceanic transport, which is greater than the amt. estd. to result from atm. transport/degrdn. of precursors.
- 2Paul, A. G.; Jones, K. C.; Sweetman, A. J. A First Global Production, Emission, And Environmental Inventory For Perfluorooctane Sulfonate. Environ. Sci. Technol. 2009, 43 (2), 386– 392, DOI: 10.1021/es802216nGoogle Scholar2https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhsVyks7%252FJ&md5=a56b37805ef14fb968abcb1a528cd55dA First Global Production, Emission, And Environmental Inventory For Perfluorooctane SulfonatePaul, Alexander G.; Jones, Kevin C.; Sweetman, Andrew J.Environmental Science & Technology (2009), 43 (2), 386-392CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)This study makes a new est. of the global historical prodn. for perfluorooctane sulfonyl fluoride (POSF), and then focuses on producing a first est. of the global historical environmental releases of perfluorooctane sulfonate (PFOS). The total historical worldwide prodn. of POSF was estd. to be 96,000 t (or 122 500 t, including unusable wastes) between 1970-2002, with an estd. global release of 45,250 t to air and water between 1970-2012 from direct (manuf., use, and consumer products) and indirect (PFOS precursors and/or impurities) sources. Ests. indicate that direct emissions from POSF-derived products are the major source to the environment resulting in releases of 450-2700 t PFOS into wastewater streams, primarily through losses from stain repellent treated carpets, waterproof apparel, and aq. fire fighting foams. Large uncertainties surround indirect sources and have not yet been estd. due to limited information on environmental degrdn., although it can be assumed that some POSF-derived chems. will degrade to PFOS over time. The properties of PFOS (high water soly., negligible vapor pressure, and limited sorption to particles) imply it will reside in surface waters, predominantly in oceans. Measured oceanic data suggests ∼235-1770 t of PFOS currently reside in ocean surface waters, similar to the estd. PFOS releases. Environmental monitoring from the 1970s onward shows strong upward trends in biota, in broad agreement with the ests. of use and emissions made here. Since cessation of POSF prodn. by 3M in 2002, a redn. in some compartments has been obsd., although current and future exposure is dependent on emission routes, subsequent transport and degrdn.
- 3Wania, F. A Global Mass Balance Analysis of the Source of Perfluorocarboxylic Acids in the Arctic Ocean. Environ. Sci. Technol. 2007, 41 (13), 4529– 4535, DOI: 10.1021/es070124cGoogle Scholar3https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXlsFenu7k%253D&md5=04c24935ebd5aa30fdd38996b2533bd6A Global Mass Balance Analysis of the Source of Perfluorocarboxylic Acids in the Arctic OceanWania, FrankEnvironmental Science & Technology (2007), 41 (13), 4529-4535CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Whereas the pervasive and abundant presence of perfluorinated carboxylic acids (PFCAs) in the Arctic marine food chain is clearly established, their origin and transport pathway into the Arctic Ocean are not. Either the atm. oxidn. of volatile precursor compds., such as the fluorotelomer alcs. (FTOHs), or the long-range oceanic transport of directly emitted PFCAs is seen as contributing the bulk of the PFCA input to the Arctic. Here simulations with the zonally averaged global fate and transport model Globo-POP, in combination with historical emission ests. for FTOHs and perfluorooctanoic acid (PFOA), are used to evaluate the relative efficiency and importance of the two transport pathways. Ests. of the emission-independent Arctic Contamination Potential reveal that the oceanic transport of directly emitted PFCAs is more than 10-fold more efficient than the atm. degrdn. of FTOHs in delivering PFCAs to the Arctic, mostly because of the low yield of the reaction. The cumulative historic emissions of FTOHs are lower than those estd. for PFOA alone by a factor of 2-3, further limiting the contribution that precursor oxidn. makes to the total PFCAs load in the Arctic Ocean. Accordingly, when fed only with FTOH emissions, the model predicts FTOH air concns. in agreement with the reported measurements, but yields Arctic seawater concns. for the PFOA that are 2 orders of magnitude too low. Whereas ocean transport is thus very likely the dominant pathway of PFOA into the Arctic Ocean, the major transport route of longer chain PFCAs depends on the size of their direct emissions relative to those of 10:2 FTOH. The predicted time course of Arctic seawater concns. is very similar for directly emitted and atmospherically generated PFCAs, implying that neither past doubling times of PFCA concns. in Arctic marine mammals nor any future time trends are likely to resolve the question of the dominant source of PFCAs.
- 4Armitage, J. M.; MacLeod, M.; Cousins, I. T. Comparative Assessment of the Global Fate and Transport Pathways of Long-Chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct Sources. Environ. Sci. Technol. 2009, 43 (15), 5830– 5836, DOI: 10.1021/es900753yGoogle Scholar4https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXnsVWhtL0%253D&md5=656ebab43c645ea97cb3f4f39e295ad8Comparative Assessment of the Global Fate and Transport Pathways of Long-Chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct SourcesArmitage, James M.; MacLeod, Matthew; Cousins, Ian T.Environmental Science & Technology (2009), 43 (15), 5830-5836CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A global-scale, multispecies mass balance model simulated the long-term fate and transport of perfluorocarboxylic acids (PFCA) with 8-13 (C8-13) and their conjugate bases, perfluorocarboxylates (PFC), to assess the relative long-range transport (LRT) potential of each conjugate pair, collectively termed PFC(A), considering only direct source emissions (i.e., manufg. and use). Overall LRT potential (atm. + oceanic) varied as a function of chain length and depended on assumptions regarding pKa and mode of entry. Atm. transport had a relatively higher contribution to overall LRT potential for PFC(A) with longer chain length, reflecting the increasing trend in air/water partition coeff. (KAW) of neutral PFCA species with chain length. Model scenarios using estd. direct emissions of C8, C9, and C11 PFC(A) indicated mass fluxes to the Arctic marine environment assocd. with oceanic transport were greater than mass fluxes from indirect sources (i.e., atm. transport of precursor substances [fluoro-telomer alcs.] and subsequent degrdn. to PFCA). Modeled C8-9 concns. in the abiotic environment were broadly consistent with available surface ocean water monitoring data; modeled C8:C9 concn. ratios were reconcilable with the homolog pattern frequently obsd. in biota, assuming a pos. correlation between bioaccumulation potential and chain length. Modeled C11:C10 concn. ratios were more difficult to reconcile with monitoring data for sources and remote regions. Thus, C11 and C10 model results implied either indirect sources were dominant; or estd. direct emission were not accurate for these homologs.
- 5Armitage, J. M.; Schenker, U.; Scheringer, M.; Martin, J. W.; MacLeod, M.; Cousins, I. T. Modeling the Global Fate and Transport of Perfluorooctane Sulfonate (PFOS) and Precursor Compounds in Relation to Temporal Trends in Wildlife Exposure. Environ. Sci. Technol. 2009, 43 (24), 9274– 9280, DOI: 10.1021/es901448pGoogle Scholar5https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXhsVSgtbrF&md5=1752a410810a52feaba0ea4f460a51b9Modeling the Global Fate and Transport of Perfluorooctane Sulfonate (PFOS) and Precursor Compounds in Relation to Temporal Trends in Wildlife ExposureArmitage, James M.; Schenker, Urs; Scheringer, Martin; Martin, Jonathan W.; MacLeod, Matthew; Cousins, Ian T.Environmental Science & Technology (2009), 43 (24), 9274-9280CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A global-scale fate and transport model was applied to study the historic and future trends in ambient concns. of perfluorooctane sulfonate (PFOS) and volatile perfluorooctane sulfonyl fluoride (POSF)-based precursor compds. in the environment. A global emission inventory for PFOS and its precursor compds. was estd. for 1957-2010. We used this inventory as input to a global-scale contaminant fate model and compared modeled concns. with field data. The main focus of the simulations was to examine how modeled concns. of PFOS and volatile precursor compds. respond to the major prodn. phase-out that occurred in 2000-2002. Modeled concns. of PFOS in surface ocean waters are generally within a factor of 5 of field data and are dominated by direct emissions of this substance. In contrast, modeled concns. of the precursor compds. considered in this study are lower than measured concns. both before and after the prodn. phase-out. Modeled surface ocean water concns. of PFOS in source regions decline slowly in response to the prodn. phase-out while concns. in remote regions continue to increase until 2030. In contrast, modeled concns. of precursor compds. in both the atm. and surface ocean water compartment in all regions respond rapidly to the prodn. phase-out (i.e., decline quickly to much lower levels). With respect to wildlife biomonitoring data, since precursor compds. are bioavailable and degrade to PFOS in vivo, it is at least plausible that declining trends in PFOS body burdens obsd. in some marine organisms are attributable to this exposure pathway. The continued increases in PFOS body burdens obsd. in marine organisms inhabiting other regions may reflect exposure primarily to PFOS itself, present in the environment due to prodn. and use of this compd. as well as degrdn. of precursor compds.
- 6Armitage, J. M.; MacLeod, M.; Cousins, I. T. Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance Model. Environ. Sci. Technol. 2009, 43 (4), 1134– 1140, DOI: 10.1021/es802900nGoogle Scholar6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXotlKmtw%253D%253D&md5=d24d3aa685ebbcd74fb2bf3626e866a5Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance ModelArmitage, James M.; MacLeod, Matthew; Cousins, Ian T.Environmental Science & Technology (2009), 43 (4), 1134-1140CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Global-scale fate and transport processes for perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted by direct sources were simulated using a multi-species mass balance model for 1950-2010. This work assessed the atm. and oceanic long-range transport potential of direct source emissions and implications for pollution of terrestrial and marine systems worldwide. Consistent with previous modeling studies, ocean transport was the dominant pathway for delivering direct source-released PFOA to the Arctic marine environment, regardless of model assumptions. Modeled surface seawater concns. were insensitive to assumptions regarding physicochem. properties and entry emission modes reasonably agreed with available Northern Hemisphere monitoring data. Model outputs characterizing atm. transport potential were highly sensitive to model assumptions, esp. assumed acid dissocn. const. (pKa) values; however, the complete range of model results for scenarios with different assumptions about partitioning and emissions provide evidence that atm. transport of directly emitted PFOA can deliver this compd. to terrestrial environments distant from sources. Addnl. studies in remote or isolated terrestrial systems may provide further insight into the scale of pollution actually attributable to direct sources.
- 7Wang, P.; Lu, Y.; Wang, T.; Fu, Y.; Zhu, Z.; Liu, S.; Xie, S.; Xiao, Y.; Giesy, J. P. Occurrence and Transport of 17 Perfluoroalkyl Acids in 12 Coastal Rivers in South Bohai Coastal Region of China with Concentrated Fluoropolymer Facilities. Environ. Pollut. 2014, 190, 115– 122, DOI: 10.1016/j.envpol.2014.03.030Google Scholar7https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXntFyhsLk%253D&md5=8951e1b78452610b281ce2a235cce861Occurrence and transport of 17 perfluoroalkyl acids in 12 coastal rivers in south Bohai coastal region of China with concentrated fluoropolymer facilitiesWang, Pei; Lu, Yonglong; Wang, Tieyu; Fu, Yaning; Zhu, Zhaoyun; Liu, Shijie; Xie, Shuangwei; Xiao, Yang; Giesy, John P.Environmental Pollution (Oxford, United Kingdom) (2014), 190 (), 115-122CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)Perfluoroalkyl acids (PFAAs) are emerging contaminants that have raised great concern in recent years. While PFAAs manufg. becomes regulated in developed countries, prodn. has been partly shifted to China. Eight fluoropolymer manufg. facilities located in the South Bohai coastal region, one of the most populated areas of China, have been used to manuf. PFAA-related substances since 2001. The environmental consequence of the intensive prodn. of PFAAs in this region remains largely unknown. We analyzed 17 PFAAs in twelve coastal rivers of this region, and found staggeringly high concns. of perfluorooctanoic acid (PFOA) ranging from 0.96 to 4534.41 ng/L. The highest concn. was obsd. in the Xiaoqing River which received effluents from certain fluoropolymer facilities. Principal component anal. indicated similar sources of several perfluoroalkyl carboxylic acids (PFCAs) in all rivers, which indicated that atm. transport, wastewater treatment and surface runoff also acted as important supplements to direct discharge to surface water.
- 8Wang, Z.; Boucher, J. M.; Scheringer, M.; Cousins, I. T.; Hungerbühler, K. Toward a Comprehensive Global Emission Inventory of C4–C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C8-Based Products and Ongoing Industrial Transition. Environ. Sci. Technol. 2017, 51 (8), 4482– 4493, DOI: 10.1021/acs.est.6b06191Google Scholar8https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXks12iurg%253D&md5=34dbfa59b48a23b421b977bf922262beToward a Comprehensive Global Emission Inventory of C4-C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C8-Based Products and Ongoing Industrial TransitionWang, Zhanyun; Boucher, Justin M.; Scheringer, Martin; Cousins, Ian T.; Hungerbuhler, KonradEnvironmental Science & Technology (2017), 51 (8), 4482-4493CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A global emission inventory of C4-10 perfluoroalkanesulfonic acids (PFSA) from the life cycle of perfluorooctanesulfonyl fluoride (POSF)-based products in 1958-2030 is presented. It substantially improves and expands previous frameworks by incorporating missing pieces (e.g., emissions to soil by land treatment, overlooked precursors) and updating parameters (e.g., emission factors, degrdn. half-lives). In 1958-2015, total direct and indirect emissions of perfluorooctanesulfonic acid (PFOS) were estd. to be 1228-4930 tonnes; emissions of PFOS precursors were estd. to be 1230-8738 tonnes, ∼670 tonnes for x-perfluorooctanesulfonamides/sulfonamido ethanols (xFOSA/E) and POSF, resp. Most emissions occurred between 1958 and 2002, followed by a substantial decrease. This confirmed the pos. effect of the ongoing transition to phase-out POSF-based products, although this transition may still require substantial time and cause substantial addnl. releases of PFOS (8-153 tonnes) and xFOSA/Es (4-698 tonnes) in 2016 to 2030. Modeled environmental concns. obtained by coupling the emission inventory and a global multi-media mass balance model generally agree well with reported field measurements, suggesting the inventory captures, for the first time, actual emissions of PFOS and xFOSA/E despite remaining uncertainties. An anal. of key uncertainties and open questions of and beyond the inventory showed that, among others, degrdn. of side-chain fluorinated polymers in the environment and landfills can be a long-term, (potentially) substantial source of PFOS.
- 9Zhang, X.; Zhang, Y.; Dassuncao, C.; Lohmann, R.; Sunderland, E. M. North Atlantic Deep Water Formation Inhibits High Arctic Contamination by Continental Perfluorooctane Sulfonate Discharges. Global Biogeochemical Cycles 2017, 31 (8), 1332– 1343, DOI: 10.1002/2017GB005624Google Scholar9https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhsVektrzJ&md5=77a7a365d3a0beeee35a05e839073a7aNorth Atlantic Deep Water formation inhibits high Arctic contamination by continental perfluorooctane sulfonate dischargesZhang, Xianming; Zhang, Yanxu; Dassuncao, Clifton; Lohmann, Rainer; Sunderland, Elsie M.Global Biogeochemical Cycles (2017), 31 (8), 1332-1343CODEN: GBCYEP; ISSN:1944-9224. (Wiley-Blackwell)Perfluorooctane sulfonate (PFOS) is an aliph. fluorinated compd. with eight carbon atoms that is extremely persistent in the environment and can adversely affect human and ecol. health. The stability, low reactivity, and high water soly. of PFOS combined with the North American phaseout in prodn. around the year 2000 make it a potentially useful new tracer for ocean circulation. Here we characterize processes affecting the lifetime and accumulation of PFOS in the North Atlantic Ocean and transport to sensitive Arctic regions by developing a 3-D simulation within the MITgcm. The model captures variability in measurements across biogeog. provinces (R2 = 0.90, p = 0.01). In 2015, the North Atlantic PFOS reservoir was equiv. to 60% of cumulative inputs from the North American and European continents (1400 Mg). Cumulative inputs to the Arctic accounted for 30% of continental discharges, while the remaining 10% was transported to the tropical Atlantic and other regions. PFOS concns. declined rapidly after 2002 in the surface mixed layer (half-life: 1-2 years) but are still increasing below 1000 m depth. During peak prodn. years (1980-2000), plumes of PFOS-enriched seawater were transported to the sub-Arctic in energetic surface ocean currents. However, Atlantic Meridional Overturning Circulation (AMOC) and deep ocean transport returned a substantial fraction of this northward transport (20%, 530 Mg) to southern latitudes and reduced cumulative inputs to the Arctic (730 Mg) by 70%. Weakened AMOC due to climate change is thus likely to increase the magnitude of persistent bioaccumulative pollutants entering the Arctic Ocean.
- 10Boucher, J. M.; Cousins, I. T.; Scheringer, M.; Hungerbühler, K.; Wang, Z. Toward a Comprehensive Global Emission Inventory of C4–C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C6- and C10-Based Products. Environ. Sci. Technol. Lett. 2019, 6 (1), 1– 7, DOI: 10.1021/acs.estlett.8b00531Google Scholar10https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXitFyrt7fE&md5=b3bb61ecf244f2734cd487bb5127c8abToward a Comprehensive Global Emission Inventory of C4-C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C6- and C10-Based ProductsBoucher, Justin M.; Cousins, Ian T.; Scheringer, Martin; Hungerbuhler, Konrad; Wang, ZhanyunEnvironmental Science & Technology Letters (2019), 6 (1), 1-7CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)A first global emission inventory of C4-C10 perfluoroalkanesulfonic acids (PFSAs) released during the life cycle of perfluorohexanesulfonyl fluoride (PHxSF)- and perfluorodecanesulfonyl fluoride (PDSF)-based products is presented. This study complements previous research on emissions of PFSAs that focused largely on the life cycle of perfluorooctanesulfonyl fluoride (POSF) and its derivs. It reviews and integrates existing information about the life cycle of PHxSF, PDSF, and their derivs.; the limited data available in the public domain point to potentially significant global prodn., uses, and releases of these substances. Between 1958 and 2015, ranges of total emissions of perfluorohexanesulfonic acid (PFHxS) and perfluorodecanesulfonic acid (PFDS) are estd. to be 120-1022 and 38-378 metric tons, resp. With the new emission ests. as inputs in a global multimedia environmental fate model (CliMoChem), the model-derived environmental concns. well capture the reported field concns., providing strong support for the plausibility of the developed emission inventories. The results highlight the ongoing environmental exposure to these substances and the need for more detailed data in the public domain about their prodn. levels and uses.
- 11Johansson, J. H.; Salter, M. E.; Acosta Navarro, J. C.; Leck, C.; Nilsson, E. D.; Cousins, I. T. Global Transport of Perfluoroalkyl Acids via Sea Spray Aerosol. Environmental Science: Processes & Impacts 2019, 21 (4), 635– 649, DOI: 10.1039/C8EM00525GGoogle Scholar11https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXltFGlu78%253D&md5=abfed0e0165a4a299919ccbe6d8a5b84Global transport of perfluoroalkyl acids via sea spray aerosolJohansson, J. H.; Salter, M. E.; Acosta Navarro, J. C.; Leck, C.; Nilsson, E. D.; Cousins, I. T.Environmental Science: Processes & Impacts (2019), 21 (4), 635-649CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)Perfluoroalkyl acids (PFAAs) are persistent org. pollutants found throughout the world's oceans. Previous research suggests that long-range atm. transport of these substances may be substantial. However, it remains unclear what the main sources of PFAAs to the atm. are. We have used a lab. sea spray chamber to study water-to-air transfer of 11 PFAAs via sea spray aerosol (SSA). We obsd. significant enrichment of all PFAAs relative to sodium in the SSA generated. The highest enrichment was obsd. in aerosols with aerodynamic diam. < 1.6μm, which had aerosol PFAA concns. up to ∼62 000 times higher than the PFAA water concns. in the chamber. In surface microlayer samples collected from the sea spray chamber, the enrichment of the substances investigated was orders of magnitude smaller than the enrichment obsd. in the aerosols. In expts. with mixts. of structural isomers, a lower contribution of branched PFAA isomers was obsd. in the surface microlayer compared to the bulk water. However, no clear trend was obsd. in the comparison of structural isomers in SSA and bulk water. Using the measured enrichment factors of perfluorooctanoic acid and perfluorooctane sulfonic acid vs. sodium we have estd. global annual emissions of these substances to the atm. via SSA as well as their global annual deposition to land areas. Our expts. suggest that SSA may currently be an important source of these substances to the atm. and, over certain areas, to terrestrial environments.
- 12Sha, B.; Johansson, J. H.; Benskin, J. P.; Cousins, I. T.; Salter, M. E. Influence of Water Concentrations of Perfluoroalkyl Acids (PFAAs) on Their Size-Resolved Enrichment in Nascent Sea Spray Aerosols. Environ. Sci. Technol. 2021, 55 (14), 9489– 9497, DOI: 10.1021/acs.est.0c03804Google Scholar12https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXhslSmt7%252FO&md5=84d2352cc7618aa9511012cce58a94f5Influence of water concentrations of perfluoroalkyl acids (PFAAs) on their size-resolved enrichment in nascent sea spray aerosolsSha, Bo; Johansson, Jana H.; Benskin, Jonathan P.; Cousins, Ian T.; Salter, Matthew E.Environmental Science & Technology (2021), 55 (14), 9489-9497CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Perfluoroalkyl acids (PFAAs) are persistent org. substances that have been widely detected in the global oceans. Previous lab. expts. have demonstrated effective enrichment of PFAAs in nascent sea spray aerosols (SSA), suggesting that SSA are an important source of PFAAs to the atm. In the present study, the effects of the water concn. of PFAAs on their size-resolved enrichment in SSA were examd. using a sea spray simulation chamber. Aerosolization of the target compds. in almost all sizes of SSA revealed a strong linear relationship with their water concns. (p < 0.05, r2 > 0.9). The enrichment factors (EF) of the target compds. showed no correlation with their concns. in the chamber water, despite the concns. varying by a factor of 500 (~ 0.3 to ~ 150 ng L-1). The particle surface-area-to-vol. ratio appeared to be a key predictor of the enrichment of perfluoroalkyl carboxylic acids (PFCAs) with ≥7 perfluorinated carbons and perfluoroalkanesulfonic acids (PFSAs) with ≥6 perfluorinated carbons in supermicron particles (p < 0.05, r2 > 0.8), but not in submicron particles. The different enrichment behaviors of PFAAs in submicron and supermicron particles might be a result of the different prodn. mechanisms of film droplets and jet droplets. The results suggest that the variability in seawater concns. of PFAAs has little influence on EFs and that modeling studies designed to quantify the source of PFAAs via SSA emissions do not need to consider this factor.
- 13Sha, B.; Johansson, J. H.; Tunved, P.; Bohlin-Nizzetto, P.; Cousins, I. T.; Salter, M. E. Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere: Field Evidence from Long-Term Air Monitoring. Environ. Sci. Technol. 2022, 56 (1), 228– 238, DOI: 10.1021/acs.est.1c04277Google Scholar13https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXislartLrJ&md5=83653024bf4fb4df09fb0ee1ce47c503Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere: Field Evidence from Long-Term Air MonitoringSha, Bo; Johansson, Jana H.; Tunved, Peter; Bohlin-Nizzetto, Pernilla; Cousins, Ian T.; Salter, Matthew E.Environmental Science & Technology (2022), 56 (1), 228-238CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)The effective enrichment of perfluoroalkyl acids (PFAAs) in sea spray aerosols (SSA) demonstrated in previous lab. studies suggests that SSA is a potential source of PFAAs to the atm. In order to investigate the influence of SSA on atm. PFAAs in the field, 48 h aerosol samples were collected regularly between 2018 and 2020 at two Norwegian coastal locations, Andoya and Birkenes. Significant correlations (p < 0.05) between the SSA tracer ion, Na+, and PFAA concns. were obsd. in the samples from both locations, with Pearson's correlation coeffs. (r) between 0.4-0.8. Such significant correlations indicate SSA to be an important source of atm. PFAAs to coastal areas. The correlations in the samples from Andoya were obsd. for more PFAA species and were generally stronger than in the samples from Birkenes, which is located further away from the coast and closer to urban areas than Andoya. Factors such as the origin of the SSA, the distance of the sampling site to open water, and the presence of other PFAA sources (e.g., volatile precursor compds.) can have influence on the contribution of SSA to PFAA in air at the sampling sites and therefore affect the obsd. correlations between PFAAs and Na+.
- 14Wei, S.; Chen, L. Q.; Taniyasu, S.; So, M. K.; Murphy, M. B.; Yamashita, N.; Yeung, L. W. Y.; Lam, P. K. S. Distribution of Perfluorinated Compounds in Surface Seawaters between Asia and Antarctica. Mar. Pollut. Bull. 2007, 54 (11), 1813– 1818, DOI: 10.1016/j.marpolbul.2007.08.002Google Scholar14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXhtlaqtLjI&md5=35aa6da53feb11c3cc2be230c537701cDistribution of perfluorinated compounds in surface seawaters between Asia and AntarcticaWei, S.; Chen, L. Q.; Taniyasu, S.; So, M. K.; Murphy, M. B.; Yamashita, N.; Yeung, L. W. Y.; Lam, P. K. S.Marine Pollution Bulletin (2007), 54 (11), 1813-1818CODEN: MPNBAZ; ISSN:0025-326X. (Elsevier B.V.)There is no expanded citation for this reference.
- 15Yamashita, N.; Taniyasu, S.; Petrick, G.; Wei, S.; Gamo, T.; Lam, P. K. S.; Kannan, K. Perfluorinated Acids as Novel Chemical Tracers of Global Circulation of Ocean Waters. Chemosphere 2008, 70 (7), 1247– 1255, DOI: 10.1016/j.chemosphere.2007.07.079Google Scholar15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXivVyjsw%253D%253D&md5=276d7ee4ebdaef9d76ac1a3cc879991fPerfluorinated acids as novel chemical tracers of global circulation of ocean watersYamashita, Nobuyoshi; Taniyasu, Sachi; Petrick, Gert; Wei, Si; Gamo, Toshitaka; Lam, Paul K. S.; Kannan, KurunthachalamChemosphere (2008), 70 (7), 1247-1255CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Perfluorinated acids (PFAs) such as perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) are global environmental contaminants. The physicochem. properties of PFAs are unique in that they have high water solubilities despite the low reactivity of C-F bond, which also imparts high stability in the environment. Because of the high water solubilities, the open-ocean water column is suggested to be the final sink for PFOS and PFOA. However, little is known on the distribution of PFAs in the oceans around the world. We describe the horizontal (spatial) and vertical distribution of PFAs in ocean waters worldwide. PFOS and PFOA concns. in the North Atlantic Ocean ranged from 8.6 to 36 pg/L and from 52 to 338 pg/L, resp., whereas the corresponding concns. in the Mid Atlantic Ocean were 13-73 and 67-439 pg/L. These were completely different from the surface waters of the South Pacific Ocean and the Indian Ocean (overall range of <5-11 pg/L for PFOS and PFOA). Vertical profiles of PFAs in the marine water column were assocd. with the global ocean circulation theory. Vertical profiles of PFAs in water columns from the Labrador Sea reflected the influx of the North Atlantic Current in surface waters, the Labrador Current in subsurface waters, and the Denmark Strait Overflow Water in deep layers below 2000 m. Striking differences in the vertical and spatial distribution of PFAs, depending on the oceans, suggest that these persistent acids can serve as useful chem. tracers to allow us to study oceanic transport by major water currents. The results provide evidence that PFA concns. and profiles in the oceans adhere to a pattern consistent with the global Broecker's Conveyor Belt theory of open ocean water circulation.
- 16Ahrens, L.; Barber, J. L.; Xie, Z.; Ebinghaus, R. Longitudinal and Latitudinal Distribution of Perfluoroalkyl Compounds in the Surface Water of the Atlantic Ocean. Environ. Sci. Technol. 2009, 43 (9), 3122– 3127, DOI: 10.1021/es803507pGoogle Scholar16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXjvFalsb0%253D&md5=bdee241499275203506b1132065db770Longitudinal and Latitudinal Distribution of Perfluoroalkyl Compounds in the Surface Water of the Atlantic OceanAhrens, Lutz; Barber, Jonathan L.; Xie, Zhiyong; Ebinghaus, RalfEnvironmental Science & Technology (2009), 43 (9), 3122-3127CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Perfluoroalkyl compds. (PFCs) were detd. in 2 L surface water samples collected in the Atlantic Ocean onboard the research vessels Maria S. Merian along the longitudinal gradient from Las Palmas (Spain) to St. Johns (Canada) (15° W to 52° W) and Polarstern along the latitudinal gradient from the Bay of Biscay to the South Atlantic Ocean (46° N to 26° S) in spring and fall 2007, resp. After filtration the dissolved and particulate phases were extd. sep., and PFC concns. were detd. using HPLC interfaced to tandem mass spectrometry. No PFCs were detected in the particulate phase. This study provides the 1st concn. data of perfluorooctanesulfonamide (FOSA), perfluorohexanoic acid, and perfluoroheptanoic acid from the Atlantic Ocean. Results indicate that trans-Atlantic Ocean currents caused the decreasing concn. gradient from the Bay of Biscay to the South Atlantic Ocean and the concn. drop-off close to the Labrador Sea. Maximum concns. were found for FOSA, perfluorooctanesulfonate, and perfluorooctanoic acid at 302, 291, and 229 pg/L, resp. However, the concn. of each single compd. was usually in the tens of pg/L range. South of the equator only FOSA and below 4° S no PFCs could be detected.
- 17Ahrens, L.; Xie, Z.; Ebinghaus, R. Distribution of Perfluoroalkyl Compounds in Seawater from Northern Europe, Atlantic Ocean, and Southern Ocean. Chemosphere 2010, 78 (8), 1011– 1016, DOI: 10.1016/j.chemosphere.2009.11.038Google Scholar17https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXhtlWkurw%253D&md5=f76cffde333395dabc06cebddc6a9e72Distribution of perfluoroalkyl compounds in seawater from Northern Europe, Atlantic Ocean, and Southern OceanAhrens, Lutz; Xie, Zhiyong; Ebinghaus, RalfChemosphere (2010), 78 (8), 1011-1016CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)The global distribution of perfluoroalkyl compds. (PFCs) were investigated in surface water samples collected onboard the Polarstern in Northern Europe, Atlantic and Southern Ocean (52°N-69°S) in 2008. The water samples were solid-phase extd. with Oasis WAX cartridges and analyzed using the high-performance liq. chromatog. interfaced to tandem mass spectrometry. Concns. of various PFCs, including C4, C6, C8 perfluoroalkyl sulfonates (PFSAs), perfluorooctane sulfinate (PFOSi), C5-C12 perfluoroalkyl carboxylic acids (PFCA) and perfluorooctane sulfonamide (FOSA) were quantified. Perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) were the predominant compds. with a max. concn. of 232 and 223 pg L-1, resp. Results indicate that industrial areas like the European Continent act as source of PFCs, while ocean water is an important as a sink as well as the transport medium of these compds. Interestingly, in the equator area the .sum.PFC concn. increased, which indicates that there exists an atm. or other unknown input source of PFCs. In the Southern Ocean only PFOS was detected which could be caused by atm. transport of its precursors.
- 18Zhao, Z.; Xie, Z.; Möller, A.; Sturm, R.; Tang, J.; Zhang, G.; Ebinghaus, R. Distribution and Long-Range Transport of Polyfluoroalkyl Substances in the Arctic, Atlantic Ocean and Antarctic Coast. Environ. Pollut. 2012, 170, 71– 77, DOI: 10.1016/j.envpol.2012.06.004Google Scholar18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC38XhtF2rsr%252FN&md5=a783ed6e2adc4a4b7b1a3c973107d3d1Distribution and long-range transport of polyfluoroalkyl substances in the Arctic, Atlantic Ocean and Antarctic coastZhao, Zhen; Xie, Zhiyong; Moeller, Axel; Sturm, Renate; Tang, Jianhui; Zhang, Gan; Ebinghaus, RalfEnvironmental Pollution (Oxford, United Kingdom) (2012), 170 (), 71-77CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)The global distribution and long-range transport of polyfluoroalkyl substances (PFASs) were investigated using seawater samples collected from the Greenland Sea, East Atlantic Ocean, and the Southern Ocean in 2009-2010. Elevated levels of ΣPFASs were detected in the North Atlantic Ocean with the concns. ranging from 130-650 pg/L. In the Greenland Sea, the ΣPFASs concns. ranged from 45-280 pg/L, and 5 most frequently detected compds. were perfluorooctanoic acid (PFOA), perfluorohexanesulfonate (PFHxS), perfluorohexanoic acid (PFHxA), perfluorooctane sulfonate (PFOS), and perfluorobutane sulfonate (PFBS). PFOA (15 pg/L) and PFOS (25-45 pg/L) were occasionally found in the Southern Ocean. In the Atlantic Ocean, the ΣPFASs concn. decreased from 2007-2010. The elevated PFOA level that resulted from melting snow and ice in Greenland Sea implies that the Arctic may were driven by climate change and turned to be a source of PFASs for the marine ecosystem. Polyfluoroalkyl substances (PFASs) were reported for the Arctic, Atlantic, and the Southern Ocean, which improves understanding the fate of PFASs in the global oceans.
- 19Benskin, J. P.; Muir, D. C. G.; Scott, B. F.; Spencer, C.; De Silva, A. O.; Kylin, H.; Martin, J. W.; Morris, A.; Lohmann, R.; Tomy, G.; Rosenberg, B.; Taniyasu, S.; Yamashita, N. Perfluoroalkyl Acids in the Atlantic and Canadian Arctic Oceans. Environ. Sci. Technol. 2012, 46 (11), 5815– 5823, DOI: 10.1021/es300578xGoogle Scholar19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC38XmtlOlt7Y%253D&md5=7921afb5ff8600731268538bb0fc969fPerfluoroalkyl Acids in the Atlantic and Canadian Arctic OceansBenskin, Jonathan P.; Muir, Derek C. G.; Scott, Brian F.; Spencer, Christine; De Silva, Amila O.; Kylin, Henrik; Martin, Jonathan W.; Morris, Adam; Lohmann, Rainer; Tomy, Gregg; Rosenberg, Bruno; Taniyasu, Sachi; Yamashita, NobuyoshiEnvironmental Science & Technology (2012), 46 (11), 5815-5823CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The spatial distribution of C4, C6, and C8 perfluoroalkyl sulfonates; C6-C14 perfluoroalkyl carboxylates; and perfluorooctanesulfonamide in Atlantic and Arctic oceans, including previously unstudied coastal water of North and South America,and the Canadian Arctic Archipelago, is reported. Perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) were typically the dominant perfluoroalkyl acids (PFAA) in Atlantic water. In the mid-northwest Atlantic/Gulf Stream, sum PFAA concns. (.sum.PFAA) were low (77-190 pg/L) but increased rapidly upon crossing into US coastal water (≤5800 pg/L near Rhode Island). .sum.PFAA in the northeast Atlantic were highest north of the Canary Islands (280-980 pg/L) and decreased with latitude. In the South Atlantic, concns. increased near Rio de la Plata (Argentina/Uruguay; 350-540 pg/L .sum.PFAA), possibly due to insecticides contg. N-Et perfluorooctanesulfonamide or proximity to Montevideo and Buenos Aires. In all other southern hemisphere locations, .sum.PFAA were <210 pg/L. PFOA:PFOS ratios were typically ≥1 in the northern hemisphere, ∼1 near the equator, and ≤1 in the southern hemisphere. In the Canadian Arctic, .sum.PFAA occurred at 40-250 pg/; perfluoroheptanoate, PFOA, and PFOS were among PFAA detected in highest concns. PFOA:PFOS ratios (typically »1) decreased from Baffin Bay to Amundsen Gulf, possibly due to increased atm. inputs. These data help validate global emission models and contribute to understanding PFAA long-range transport pathways and sources in remote regions.
- 20González-Gaya, B.; Dachs, J.; Roscales, J. L.; Caballero, G.; Jiménez, B. Perfluoroalkylated Substances in the Global Tropical and Subtropical Surface Oceans. Environ. Sci. Technol. 2014, 48 (22), 13076– 13084, DOI: 10.1021/es503490zGoogle Scholar20https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhslKgtLzL&md5=b41a06cc3867126d167223c52368810dPerfluoroalkylated Substances in the Global Tropical and Subtropical Surface OceansGonzalez-Gaya, Belen; Dachs, Jordi; Roscales, Jose L.; Caballero, Gemma; Jimenez, BegonaEnvironmental Science & Technology (2014), 48 (22), 13076-13084CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Perfluoroalkylated substances (PFASs) were analyzed in 92 surface seawater samples taken during the Malaspina 2010 expedition which covered all the tropical and subtropical Atlantic, Pacific and Indian oceans. Nine ionic PFASs including C6-C10 perfluoroalkyl carboxylic acids (PFCAs), C4 and C6-C8 perfluoroalkyl sulfonic acids (PFSAs) and 2 neutral precursors perfluoroalkyl sulfonamides (PFASAs), were identified and quantified. The Atlantic Ocean presented the broader range in concns. of total PFASs (131-10900 pg/L, median 645 pg/L, n =45) compared to the other oceanic basins, probably due to a better spatial coverage. Total concns. in the Pacific were 344-2500 pg/L (median =527 pg/L, n =27) and in the Indian Ocean 176-1976 pg/L (median =329, n =18). Perfluorooctanesulfonic acid (PFOS) was the most abundant compd., accounting for 33% of the total PFASs globally, followed by perfluorodecanoic acid (PFDA, 22%) and perfluorohexanoic acid (PFHxA, 12%), being the rest of the individual congeners under 10% of total PFASs, even for perfluorooctane carboxylic acid (PFOA, 6%). PFASAs accounted for <1% of the total PFASs concn. This study reports the ubiquitous occurrence of PFCAs, PFSAs, and PFASAs in the global ocean, being the first attempt, to our knowledge, to show a comprehensive assessment in surface water samples collected in a single oceanic expedition covering tropical and subtropical oceans. The potential factors affecting their distribution patterns were assessed including the distance to coastal regions, oceanic subtropical gyres, currents and biogeochem. processes. Field evidence of biogeochem. controls on the occurrence of PFASs was tentatively assessed considering environmental variables (solar radiation, temp., chlorophyll a concns. among others), and these showed significant correlations with some PFASs, but explaining small to moderate percentages of variability. This suggests that a no. of phys. and biogeochem. processes collectively drive the oceanic occurrence and fate of PFASs in a complex manner.
- 21Yeung, L. W. Y.; Dassuncao, C.; Mabury, S.; Sunderland, E. M.; Zhang, X.; Lohmann, R. Vertical Profiles, Sources, and Transport of PFASs in the Arctic Ocean. Environ. Sci. Technol. 2017, 51 (12), 6735– 6744, DOI: 10.1021/acs.est.7b00788Google Scholar21https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXnvVyjsb0%253D&md5=22400217c247069fd43980eb8a1a5953Vertical Profiles, Sources, and Transport of PFASs in the Arctic OceanYeung, Leo W. Y.; Dassuncao, Clifton; Mabury, Scott; Sunderland, Elsie M.; Zhang, Xianming; Lohmann, RainerEnvironmental Science & Technology (2017), 51 (12), 6735-6744CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The relative importance of atm. vs. oceanic transport for poly- and perfluorinated alkyl substances (PFASs) reaching the Arctic Ocean is not well understood. Vertical profiles from the Central Arctic Ocean and shelf water, snow and meltwater samples were collected in 2012; 13 PFASs (C6-C12 PFCAs; C6, 8, 10 PFSAs; MeFOSAA and EtFOSAA; and FOSA) were routinely detected (range: <5-343 pg/L). PFASs were only detectable above 150 m depth in the polar mixed layer (PML) and halocline. Enhanced concns. were obsd. in snow and melt pond samples, implying atm. deposition as an important source of PFASs. Model results suggested atm. inputs to account for 34-59% (∼11-19 pg/L) of measured PFOA concns. in the PML (mean 32 ± 15 pg/L). Modeled surface and halocline measurements for PFOS based on North Atlantic inflow (11-36 pg/L) agreed with measurements (mean, 17, range <5-41 pg/L). Modeled deep water concns. below 200 m (5-15 pg/L) were slightly higher than measurements (<5 pg/L), suggesting the lower bound of PFAS emissions ests. from wastewater and rivers may provide the best est. of inputs to the Arctic. Despite low concns. in deep water, this reservoir is expected to contain most of the PFOS mass in the Arctic (63-180 Mg) and is projected to continue increasing to 2038.
- 22Zhang, X.; Lohmann, R.; Sunderland, E. M. Poly- and Perfluoroalkyl Substances in Seawater and Plankton from the Northwestern Atlantic Margin. Environ. Sci. Technol. 2019, 53 (21), 12348– 12356, DOI: 10.1021/acs.est.9b03230Google Scholar22https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhvVOisbnL&md5=b35412e79f05eba5e1dc04de532c1d4bPoly- and Perfluoroalkyl Substances in Seawater and Plankton from the Northwestern Atlantic MarginZhang, Xianming; Lohmann, Rainer; Sunderland, Elsie M.Environmental Science & Technology (2019), 53 (21), 12348-12356CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The ocean probably is the terminal sink for poly- and perfluoroalkyl substances (PFAS) that have been produced and released in large quantities for >60 years. Regulatory actions have curbed prodn. of legacy compds. such as perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) but impacts on releases to the marine environment are poorly understood. Here we report new data for 21 targeted PFASs in marine seawater and plankton from the coast, shelf and slope of the Northwestern Atlantic Ocean. We find strong inverse correlations between salinity and concns. of most PFASs, indicating ongoing continental discharges are the major source to the marine environment. For legacy PFASs such as PFOS and PFOA, a comparison of inland and offshore measurements from the same year suggests there are ongoing releases to the marine environment from sources such as submarine groundwater discharges. Vertical transport of most PFASs assocd. with settling particles from the surface 10 m to deeper waters is small compared to advective transport except for perfluorodecanoic acid: PFDA (35% of vertical flux) and precursor compds. to PFOS (up to 86%). We find higher than expected bioaccumulation factors (BAFs = Cplankton/Cwater) for perfluorinated carboxylic acids (PFCAs) with 5 and 6 carbons (log BAFs = 2.9-3.4) and linear PFOS (log BAF = 2.6-4.3) in marine plankton compared to PFCAs with 7-11 carbons. We postulate that this reflects addnl. contributions from precursor compds. Known precursor compds. detected in this study have among the highest BAFs (log BAFs > 3.0) for all PFASs suggesting addnl. research on the bioaccumulation potential of unknown organoflourine compds. is urgently needed.
- 23Miranda, D. de A.; Leonel, J.; Benskin, J. P.; Johansson, J.; Hatje, V. Perfluoroalkyl Substances in the Western Tropical Atlantic Ocean. Environ. Sci. Technol. 2021, 55 (20), 13749– 13758, DOI: 10.1021/acs.est.1c01794Google Scholar23https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXitFymsbnP&md5=9f6acc5b10a719a49972daa723e811b2Perfluoroalkyl Substances in the Western Tropical Atlantic OceanMiranda, Daniele de A.; Leonel, Juliana; Benskin, Jonathan P.; Johansson, Jana; Hatje, VanessaEnvironmental Science & Technology (2021), 55 (20), 13749-13758CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)The dispersion of perfluoroalkyl substances (PFAS) in surface and deep-water profiles (down to 5845 m deep) was evaluated through the Western Tropical Atlantic Ocean (TAO) between 15°N and 23°S. The sum concns. for eight quantifiable PFAS (.sum.8PFAS) in surface waters ranged from 11 to 69 pg/L, which is lower than previously reported in the same area as well as in higher latitudes. Perfluoroalkyl carboxylic acids (PFCAs) were the predominant PFASs present in the Western TAO. The 16 surface samples showed variable PFAS distributions, with the predominance of perfluorooctanoic acid (PFOA) along the transect (67%; 11 ± 8 pg/L) and detection of perfluoroalkyl sulfonic acids (PFSAs) only in the Southern TAO. Perfluoroheptanoic acid (PFHpA) was often detected in the vertical profiles. PFAS distribution patterns (i.e., profiles and concns.) varied with depth throughout the TAO latitudinal sectors (North, Equator, South Atlantic, and in the Brazilian coastal zone). Vertical profiles in coastal samples displayed decreasing PFAS concns. with increasing depth, whereas offshore samples displayed higher PFAS detection frequencies in the intermediate water masses. Together with the surface currents and coastal upwelling, the origin of the water masses was an important factor in explaining PFAS concns. and profiles in the TAO.
- 24Yamazaki, E.; Taniyasu, S.; Wang, X.; Yamashita, N. Per- and Polyfluoroalkyl Substances in Surface Water, Gas and Particle in Open Ocean and Coastal Environment. Chemosphere 2021, 272, 129869, DOI: 10.1016/j.chemosphere.2021.129869Google Scholar24https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXks1Krs7g%253D&md5=63c6f8515ff39275df6c045eb5f8797ePer- and polyfluoroalkyl substances in surface water, gas and particle in open ocean and coastal environmentYamazaki, Eriko; Taniyasu, Sachi; Wang, Xinhong; Yamashita, NobuyoshiChemosphere (2021), 272 (), 129869CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)A simultaneous sampling of atm. and seawater samples was performed in the Taiwan Western Strait, western Arctic Ocean, and the Antarctic Ocean. Anal. of both particle and gas phase PFAS in oceanic air was conducted using cascade impactor particle fractionator, cryogenic air sampler and activated charcoal fiber sorbent for the first time with application in the Taiwan Western Strait. Mean concn. of Σ12PFAS in surface seawater and atm. samples were 1178 pg/L and 24 pg/m3 in the Taiwan Western Strait, 430 pg/L and 6 pg/m3 in the western Arctic Ocean, and 456 pg/L and 3 pg/m3 in the Antarctic Ocean. In oceanic air from the Taiwan Western Strait, fluorotelomer alc. (FTOH) and the ionic PFAS [perfluoroalkyl sulfonic acid (PFSA) and perfluoroalkyl carboxylic acid (PFCA)] were found in 76% and 7% resp. Regional comparison of air/water exchange (KAW) and gas-particle (Kp) partition coeffs. of PFAS in the oceanic environment indicated potential partitioning of ionic PFAS between surface seawater and oceanic air. These findings highlight the advancement in atm. PFAS measurements through combined novel technologies, namely size-fractionated particle sampling with cryogenic air trapping and/or activated charcoal sorption. Correlation between Kp and carbon chain length of PFAS was obsd. using both hyphenated techniques.
- 25Han, T.; Chen, J.; Lin, K.; He, X.; Li, S.; Xu, T.; Xin, M.; Wang, B.; Liu, C.; Wang, J. Spatial Distribution, Vertical Profiles and Transport of Legacy and Emerging per- and Polyfluoroalkyl Substances in the Indian Ocean. Journal of Hazardous Materials 2022, 437, 129264, DOI: 10.1016/j.jhazmat.2022.129264Google Scholar25https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XhsFertL%252FP&md5=d0502df999a50c61e63dd9a25cb156aaSpatial distribution, vertical profiles and transport of legacy and emerging per- and polyfluoroalkyl substances in the Indian OceanHan, Tongzhu; Chen, Junhui; Lin, Kun; He, Xiuping; Li, Shujiang; Xu, Tengfei; Xin, Ming; Wang, Baodong; Liu, Chenguang; Wang, JiangtaoJournal of Hazardous Materials (2022), 437 (), 129264CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)The contamination status and transport of per- and polyfluoroalkyl substances (PFASs) in the seawater of the Indian Ocean (IO) and an adjacent subregion of the Northwest Pacific Ocean (NWPO) were investigated. Eight legacy PFASs were widely distributed in the surface seawater, and perfluoroheptanoic acid (PFHpA) and perfluorooctanoic acid (PFOA) were the two predominant PFASs. ΣPFAS concn. decreased in the following order: NWPO>Joining area of Asia and Indian-Pacific Oceans (JAIPO)>Northeast Indian Ocean>Southwest Indian Ocean. Hexafluoropropylene oxide-dimer acid, a replacement surfactant for PFOA was extensively detected in the IO (∼34.8 pg/L) for the first time, showing an early sign of emerging PFAS spread in global open oceans. Eight depth profiles across the JAIPO (down to 5433 m depth) revealed a 'surface-enrichment' and 'depth-depletion' pattern for PFASs in the water column, and two noticeable fluctuations were mainly located at depths of 150-200 and 200-500 m. Phys. processes, including eddy diffusion, and the origin and trajectory of water mass were crucial factors for structuring PFAS vertical profiles. Mass transport ests. revealed a remarkable PFOA contribution through the JAIPO to IO carried by the Indonesian Throughflow, and a nonnegligible PFHpA contribution from Antarctic Immediate Water to deep water of the JAIPO driven by thermohaline circulation.
- 26Muir, D.; Miaz, L. T. Spatial and Temporal Trends of Perfluoroalkyl Substances in Global Ocean and Coastal Waters. Environ. Sci. Technol. 2021, 55 (14), 9527– 9537, DOI: 10.1021/acs.est.0c08035Google Scholar26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXlt1Kks7k%253D&md5=7688dc2dc3986cf4a03b1632185fca7eSpatial and temporal trends of perfluoroalkyl substances in global ocean and coastal watersMuir, Derek; Miaz, Luc T.Environmental Science & Technology (2021), 55 (14), 9527-9537CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Per- and polyfluoroalkyl substances (PFAS) have been widely detected in global surface waters since the early 2000s. Here, we have compiled and analyzed the published data for perfluorocarboxylates (PFCAs) and perfluorosulfonates (PFSAs) in surface waters of coastal seas, the Great Lakes, and open oceans to examine temporal and geospatial trends. Mass discharges from major rivers were also estd. A large no. of measurements of individual PFAS have been made in these surface waters (29 500 values), with seven C4-C10 PFSAs and nine C4-C12 PFCAs accounting for 83% of all data. However, most results (85% for PFSAs; 80% for PFCAs) were for the coastal seas of Western Europe, China, Korea, and Japan, while results were limited for coastal North America and lacking for South America and Africa. Highest median concns. of PFCAs and PFSAs were reported in the Bohai and Yellow Seas region of China as well as in the North and Baltic seas in Europe. Significant declines in median PFSAs and C7-C12 PFCAs were also obsd. for the period 2012-2018 in these same regions, and for 2004-2017 in the Great Lakes. Mass discharge ests. indicated continued substantial riverine emissions of long chain (C7-C12) PFCAs in the period 2015-2019 for the coastal seas of China and redns. in emissions for Western European rivers compared to earlier time periods.
- 27Al Amin, Md.; Sobhani, Z.; Liu, Y.; Dharmaraja, R.; Chadalavada, S.; Naidu, R.; Chalker, J. M.; Fang, C. Recent Advances in the Analysis of Per- and Polyfluoroalkyl Substances (PFAS)─A Review. Environmental Technology & Innovation 2020, 19, 100879, DOI: 10.1016/j.eti.2020.100879Google ScholarThere is no corresponding record for this reference.
- 28Yamazaki, E.; Taniyasu, S.; Ruan, Y.; Wang, Q.; Petrick, G.; Tanhua, T.; Gamo, T.; Wang, X.; Lam, P. K. S.; Yamashita, N. Vertical Distribution of Perfluoroalkyl Substances in Water Columns around the Japan Sea and the Mediterranean Sea. Chemosphere 2019, 231, 487– 494, DOI: 10.1016/j.chemosphere.2019.05.132Google Scholar28https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhtVGgsLvM&md5=c34f6b4539684fd7460f8a08c3228ed1Vertical distribution of perfluoroalkyl substances in water columns around the Japan sea and the Mediterranean SeaYamazaki, Eriko; Taniyasu, Sachi; Ruan, Yuefei; Wang, Qi; Petrick, Gert; Tanhua, Toste; Gamo, Toshitaka; Wang, Xinhong; Lam, Paul K. S.; Yamashita, NobuyoshiChemosphere (2019), 231 (), 487-494CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Perfluoroalkyl substances (PFASs) have become an important class of global environmental contaminants, yet their vertical profile in the marine water column is still less understood, esp. for the semi-closed seas. In this study, the contamination level and spatial distribution of 8 PFASs were investigated in both surface and vertical water samples from two semi-closed seas, the Japan Sea and the Mediterranean Sea. Similar levels and compns. of PFASs were found between these two seas. The vertical profile of PFASs in the Mediterranean Sea was variable while that was relatively steady in the Japan Sea, probably due to their different pollution sources. The accumulation rate of PFASs from the East China Sea to the Japan Sea was calcd., for which perfluorooctanesulfonic acid and perfluorooctanoic acid were found to have high accumulation potency in both surface and deep water; most of the investigated PFASs were accumulated in the deep water due to the long residence time while they were more likely to escape to the Pacific Ocean in the surface water. This work aimed (i) to study the distribution of PFASs in both surface and vertical water samples in two semi-closed seas, namely the Japan Sea and for the first time the Mediterranean Sea, (ii) to assess the temporal trend in the Japan Sea, and (iii) to firstly investigate the potential transport of PFASs from the East China Sea and Taiwan Strait in order to est. the inventory of PFASs in whole water mass in the Japan Sea.
- 29Joerss, H.; Xie, Z.; Wagner, C. C.; von Appen, W.-J.; Sunderland, E. M.; Ebinghaus, R. Transport of Legacy Perfluoroalkyl Substances and the Replacement Compound HFPO-DA through the Atlantic Gateway to the Arctic Ocean─Is the Arctic a Sink or a Source?. Environ. Sci. Technol. 2020, 54 (16), 9958– 9967, DOI: 10.1021/acs.est.0c00228Google Scholar29https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXhsVGrtrfI&md5=89a245af5de56bd32490b61b466c6418Transport of legacy perfluoroalkyl substances and the replacement compound HFPO-DA through the Atlantic gateway to the Arctic Ocean: Is the Arctic a sink or a source?Joerss, Hanna; Xie, Zhiyong; Wagner, Charlotte C.; von Appen, Wilken-Jon; Sunderland, Elsie M.; Ebinghaus, RalfEnvironmental Science & Technology (2020), 54 (16), 9958-9967CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The spatial distribution of 29 per- and polyfluoroalkyl substances (PFASs) in seawater was investigated along a sampling transect from Europe to the Arctic and two transects within Fram Strait, located between Greenland and Svalbard, in the summer of 2018. Hexafluoropropylene oxide-dimer acid (HFPO-DA), a replacement compd. for perfluorooctanoic acid (PFOA), was detected in Arctic seawater for the first time. This provides evidence for its long-range transport to remote areas. The total PFAS concn. was significantly enriched in the cold, low-salinity surface water exiting the Arctic compared to warmer, higher-salinity water from the North Atlantic entering the Arctic (260 ± 20 pg/L vs. 190 ± 10 pg/L). The higher ratio of perfluoroheptanoic acid (PFHpA) to perfluorononanoic acid (PFNA) in outflowing water from the Arctic suggests a higher contribution of atm. sources compared to ocean circulation. An east-west cross section of the Fram Strait, which included seven depth profiles, revealed higher PFAS concns. in the surface water layer than in intermediate waters and a negligible intrusion into deep waters (>1000 m). Mass transport ests. indicated a net inflow of PFASs with ≥8 perfluorinated carbons via the boundary currents and a net outflow of shorter-chain homologues. We hypothesize that this reflects higher contributions from atm. sources to the Arctic outflow and a higher retention of the long-chain compds. in melting snow and ice.
- 30Sanchez-Vidal, A.; Llorca, M.; Farré, M.; Canals, M.; Barceló, D.; Puig, P.; Calafat, A. Delivery of Unprecedented Amounts of Perfluoroalkyl Substances towards the Deep-Sea. Science of The Total Environment 2015, 526, 41– 48, DOI: 10.1016/j.scitotenv.2015.04.080Google Scholar30https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXnt1entbY%253D&md5=c6a75618587f5274fae092a0580ac47aDelivery of unprecedented amounts of perfluoroalkyl substances towards the deep-seaSanchez-Vidal, Anna; Llorca, Marta; Farre, Marinella; Canals, Miquel; Barcelo, Damia; Puig, Pere; Calafat, AntoniScience of the Total Environment (2015), 526 (), 41-48CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)The finding of perfluoroalkyl substances (PFASs) in particles sinking to the deep northwestern Mediterranean Sea confirms the role of the latter as ballast for the transfer of pollutants to the deep sea. The transfer of particulate matter down to the deep is enhanced during atm.-driven, high-energy phys. oceanog. processes like dense shelf water cascading (DSWC), which is caused by winter surface heat losses and evapn. We present data from samples collected during winter 2012, when dense shelf water formation and subsequent cascading triggered the flushing of large amts. of PFASs through a submarine canyon to depths in excess of 1000 m. The finding of quantifiable concns. of long-chain PFOA, PFOS and PFNA substances and significantly high concns. of the short-chain substances PFHxA and PFBA indicates that these compds., sorbed onto particulate matter, are quickly and directly transferred to the ocean's interior, thus highlighting the role of DSWC in removing those pollutants from the coastal ocean. Eventually, uncertainties about our results arising from the limited no. of samples available are counterbalanced by their intrinsic value as intense DSWC events, like the one in 2012, occur only every 5-7 yr in the study area, which seriously restricts sampling opportunities. Our results add PFASs to the list of persistent org. pollutants like polychlorinated biphenyls, chlorobenzenes or polycyclic arom. hydrocarbons known to be conveyed to the deep marine environment.
- 31Casal, P.; González-Gaya, B.; Zhang, Y.; Reardon, A. J. F.; Martin, J. W.; Jiménez, B.; Dachs, J. Accumulation of Perfluoroalkylated Substances in Oceanic Plankton. Environ. Sci. Technol. 2017, 51 (5), 2766– 2775, DOI: 10.1021/acs.est.6b05821Google Scholar31https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXis1Sqs7s%253D&md5=76d98670f30edc056c5155f5e73bd905Accumulation of Perfluoroalkylated Substances in Oceanic PlanktonCasal, Paulo; Gonzalez-Gaya, Belen; Zhang, Yifeng; Reardon, Anthony J. F.; Martin, Jonathan W.; Jimenez, Begona; Dachs, JordiEnvironmental Science & Technology (2017), 51 (5), 2766-2775CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The bioaccumulation of perfluoroalkylated substances (PFASs) in plankton has previously been evaluated only in freshwater and regional seas, but not for the large oligotrophic global oceans. Plankton samples from the tropical and subtropical Pacific, Atlantic and Indian Oceans were collected during the Malaspina 2010 circumnavigation expedition, and analyzed for 14 ionizable PFASs, including perfluorooctanoate (PFOA), perfluorooctanesulfonate (PFOS) and their resp. linear and branched isomers. PFOA and PFOS concns. in plankton ranged from 0.1 to 43 ng gdw-1 and from 0.5 to 6.7 ng gdw-1, resp. The relative abundance of branched PFOA in the northern hemisphere was correlated with distance to North America, consistent with the historical prodn. and coherent with previously reported patterns in seawater. The plankton samples showing the highest PFOS concns. also presented the largest relative abundances of branched PFOS, suggesting a selective cycling/fractionation of branched PFOS in the surface ocean mediated by plankton. Bioaccumulation factors (BAFs) for plankton were calcd. for six PFASs, including short chain PFASs. PFASs Log BAFs (wet wt.) ranged from 2.6±0.8 for perfluorohexanesulfonic acid (PFHxS), to 4.4±0.6 for perfluoroheptanoic acid (PFHpA). The vertical transport of PFASs due to the settling of org. matter bound PFAS (biol. pump) was estd. from an org. matter settling fluxes climatol. and the PFAS concns. in plankton. The global av. sinking fluxes were 0.8±1.3 ng m-2d-1 for PFOA, and 1.1±2.1 ng m-2d-1 for PFOS. The residence times of PFAS in the surface ocean, assuming the biol. pump as the unique sink, showed a wide range of variability, from few years to millennia, depending on the sampling site and individual compd. Further process-based studies are needed to constrain the oceanic sink of PFAS.
- 32González-Gaya, B.; Casal, P.; Jurado, E.; Dachs, J.; Jiménez, B. Vertical Transport and Sinks of Perfluoroalkyl Substances in the Global Open Ocean. Environmental Science: Processes & Impacts 2019, 21 (11), 1957– 1969, DOI: 10.1039/C9EM00266AGoogle Scholar32https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhsV2is7bN&md5=a45cbb2a3e67600204da56a10311a1d1Vertical transport and sinks of perfluoroalkyl substances in the global open oceanGonzalez-Gaya, Belen; Casal, Paulo; Jurado, Elena; Dachs, Jordi; Jimenez, BegonaEnvironmental Science: Processes & Impacts (2019), 21 (11), 1957-1969CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)The ubiquitous occurrence of perfluoroalkyl substances (PFAS) in the open ocean has been previously documented, but their vertical transport and oceanic sinks have not been comprehensively characterized and quantified at the oceanic scale. During the Malaspina 2010 circumnavigation expedition, 21 PFAS were measured at the surface and at the deep chlorophyll max. (DCM) in the Atlantic, Indian and Pacific oceans. In this work, we report an extended data set of PFAS dissolved phase concns. at the DCM. .sum.PFAS at the DCM varied from 130 to 11 000 pg L-1, with a global av. value of 500 pg L-1. Perfluorooctanesulfonate (PFOS) abundance contributed 39% of .sum.PFAS, followed by perfluorodecanoate (PFDA, 17%), and perfluorohexanoate (PFHxA, 12%). The relative contribution of the remaining compds. was below 10%, with perfluorooctanoate (PFOA) contributing only 5% to PFAS measured at the DCM. Ests. of vertical diffusivity, derived from microstructure turbulence observations in the upper (<300 m) water column, allowed the derivation of PFAS eddy diffusive fluxes from concurrent field measurements of eddy diffusivity and PFAS concns. The PFAS concns. at the DCM predicted from an eddy diffusivity model were lower than field-measured concns., suggesting a relevant role of other vertical transport mechanisms. Settling fluxes of org. matter bound PFAS (biol. pump), oceanic circulation and potential, yet un-reported, biol. transformations are discussed.
- 33Löfstedt Gilljam, J.; Leonel, J.; Cousins, I. T.; Benskin, J. P. Is Ongoing Sulfluramid Use in South America a Significant Source of Perfluorooctanesulfonate (PFOS)? Production Inventories, Environmental Fate, and Local Occurrence. Environ. Sci. Technol. 2016, 50 (2), 653– 659, DOI: 10.1021/acs.est.5b04544Google Scholar33https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC28vptFGksg%253D%253D&md5=830a5494e7b8cf5b3ef92ffa46b9fad1Is Ongoing Sulfluramid Use in South America a Significant Source of Perfluorooctanesulfonate (PFOS)? Production Inventories, Environmental Fate, and Local OccurrenceLofstedt Gilljam John; Cousins Ian T; Benskin Jonathan P; Leonel JulianaEnvironmental science & technology (2016), 50 (2), 653-9 ISSN:.Despite international phase-out initiatives, production and use of perfluorooctanesulfonate (PFOS) and related substances continues in some countries. In Brazil, the PFOS-precursor N-ethyl perfluorooctane sulfonamide (EtFOSA) is used in Sulfluramid, a pesticide for controlling leaf-cutting ants. New data on production, environmental fate, and occurrence of Brazilian Sulfluramid are reported herein. From 2003 to 2013, Brazilian Sulfluramid manufacturing increased from 30 to 60 tonnes yr(-1) EtFOSA. During this time <1.3 tonnes yr(-1) were imported, while exports increased from ∼0.3 to 2 tonnes yr(-1). From 2004 to 2015, most EtFOSA was exported to Argentina (7.2 tonnes), Colombia (2.07 tonnes), Costa Rica (1.13 tonnes), Equador (2.16 tonnes), and Venezuela (2.4 tonnes). Within Brazil, sales occurred primarily in the states of Minas Gerais, Sao Paulo, Mato Grosso do Sul, Espirito Santo, and Bahia. Model simulations predict EtFOSA will partition to soils, while transformation products perfluorooctane sulfonamide (FOSA) and PFOS are sufficiently mobile to leach into surface waters. In support of these predictions, up to 3400 pg L(-1) of FOSA and up to 1100 pg L(-1) of PFOS were measured in Brazilian surface water, while EtFOSA was not detected. The high FOSA/PFOS ratio observed here (up to 14:1) is unprecedented in the scientific literature to our knowledge. Depending on the extent of conversion of EtFOSA, cumulative Brazilian Sulfluramid production and import from 2004 to 2015 may contribute between 167 and 487 tonnes of PFOS/FOSA to the environment. These levels are clearly nontrivial and of concern since production is continuing unabated.
- 34Catherine, M.; Nadège, B.; Charles, P.; Yann, A. Perfluoroalkyl Substances (PFASs) in the Marine Environment: Spatial Distribution and Temporal Profile Shifts in Shellfish from French Coasts. Chemosphere 2019, 228, 640– 648, DOI: 10.1016/j.chemosphere.2019.04.205Google Scholar34https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXovFentLY%253D&md5=b83d174035f7bdbc7fe5d83d9f435e1bPerfluoroalkyl substances (PFASs) in the marine environment: Spatial distribution and temporal profile shifts in shellfish from French coastsCatherine, Munschy; Nadege, Bely; Charles, Pollono; Yann, AminotChemosphere (2019), 228 (), 640-648CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Perfluoroalkyl substances (PFASs) were investigated in filter-feeding shellfish collected from 2013-2017 along the English Channel, Atlantic and Mediterranean coasts of France. PFOS (perfluorooctane sulfonate), PFTrDA (perfluorotridecanoic acid), PFTeDA (perfluorotetradecanoic acid), PFDoDA (perfluorododecanoic acid) and PFUnDA (perfluoroundecanoic acid) were detected in more than 80% of samples, thus indicating widespread contamination of the French coastal environment by these chems. The distribution of PFAS concns. showed differences according to sampling locations and years. PFOS was the predominant PFAS in most samples collected from English Channel and Atlantic coasts until 2014, but the opposite was obsd. in 2015, 2016 and 2017, while perfluoroalkyl carboxylic acids (PFCAs) prevailed in Mediterranean samples in all study years. Among PFCAs, PFTrDA showed the highest max. (1.36 ng g-1 ww) and median (0.077 ng g-1 ww) concns. in 2016-2017. Other PFAS median concns. were within the 0.014 (PFNA) - 0.055 (PFTeDA) ng g-1 ww range. The profiles detd. each year in most Mediterranean samples suggest distinctive sources. PFOS median concns. showed a significant decrease over the study years, from 0.118 to 0.126 ng g-1 ww in 2013-2015 to 0.066 ng g-1 ww in 2016 and 2017. .sum.PFCAs showed no trends in concn. ranges over the same years. The shift in PFAS profiles from PFOS to long-chain PFCAs over the study period reflects PFOS prodn. phase-out, combined with continuous inputs of PFCAs into the marine environment. These results provide ref. data for future studies of the occurrence of contaminants of emerging concern on European coasts.
- 35Santucci, L.; Carol, E.; Tanjal, C. Industrial Waste as a Source of Surface and Groundwater Pollution for More than Half a Century in a Sector of the Río de La Plata Coastal Plain (Argentina). Chemosphere 2018, 206, 727– 735, DOI: 10.1016/j.chemosphere.2018.05.084Google Scholar35https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXpvVOjsr0%253D&md5=01ff6e05a13954ac1c91198ff8fedcf7Industrial waste as a source of surface and groundwater pollution for more than half a century in a sector of the Rio de la Plata coastal plain (Argentina)Santucci, Lucia; Carol, Eleonora; Tanjal, CarolinaChemosphere (2018), 206 (), 727-735CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Environmental liabilities have become one of the most important problems of the last years, esp. those of contaminated sites located in urban areas which have been abandoned by pollution intensive industries. Such sites may contain hazardous materials that pose risks to human health and the environment. Industrial waste from the ancient sulfuric acid industry is scattered in a local area at the petrochem. pole in a sector of the Rio de la Plata coastal plain. A survey of soil and waste deposit was carried out and samples were examd. by X-ray diffraction, under a scanning electron microscope and a polarizing microscope. Surface water and groundwater samples, both to the unconfined and semi-confined aquifers, were collected to det. elec. cond., pH and major elements. The results show the presence of minerals composed of sulfur assocd. with jarosite and iron oxides on superficial sediments. The detailed study of soil sediments together with that of the water physicochem. characteristics make it possible to understand the geochem. processes developed in soil that cause the high concns. of sulfates in groundwater. Furthermore, high SO-24 concn. registered in the semi-confined aquifer due to its infiltration from the unconfined aquifer shows that the industrial pollution has an important impact at local level. These results may contribute to the understanding of chem. processes and pollutants distribution in highly industrialized coastal plain areas.
- 36Bentancur, S.; López-Vázquez, C. M.; García, H. A.; Duarte, M.; Travers, D.; Brdjanovic, D. Resource Recovery Assessment at a Pulp Mill Wastewater Treatment Plant in Uruguay. Journal of Environmental Management 2020, 255, 109718, DOI: 10.1016/j.jenvman.2019.109718Google Scholar36https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXit12ksbvJ&md5=8870c6739def37c59cd8e21a66878664Resource recovery assessment at a pulp mill wastewater treatment plant in UruguayBentancur, S.; Lopez-Vazquez, C. M.; Garcia, H. A.; Duarte, M.; Travers, D.; Brdjanovic, D.Journal of Environmental Management (2020), 255 (), 109718CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)Using a math. model, a resource recovery assessment was carried out at a pulp mill activated sludge wastewater treatment plant (WWTP) located in Uruguay. Through the evaluation of different scenarios, the potential prodn. of methane from secondary sludge, with its inherent energy savings, and the recovery of phosphorus (P) as struvite were estd. Considering the current WWTP configuration with a sludge retention time (SRT) of 32 days, and according to the model, which is a simplification of reality, the assessment indicates that the implementation of an anaerobic digester (AD) to treat the excess sludge can lead to a methane prodn. of approx. 1736 m3 CH4 d-1, being a promising alternative to increase the WWTP treatment performance. Furthermore, the model predictions suggest that by shortening the SRT from 32 to 5 days, the methane prodn. could increase by up to 5568 m3 CH4 d-1. If the methane produced is used to generate elec. energy to operate the WWTP, energy savings of about 88% can be achieved. Regarding the potential recovery of P as struvite, the addn. of a struvite reactor could be an efficient option to recover approx. 1611 mg L-1 of struvite (corresponding to a load of about 433 kg d-1). By optimizing the process performance, these findings highlight the potential recovery of resources in pulp mill WWTP, while complying with stringent effluent discharge stds. In addn., further research activities such as pilot-test or detailed lab. studies may be needed to validate the previous recommendations for industrial scale application.
- 37Langberg, H. A.; Arp, H. P. H.; Breedveld, G. D.; Slinde, G. A.; Høiseter, Å.; Grønning, H. M.; Jartun, M.; Rundberget, T.; Jenssen, B. M.; Hale, S. E. Paper Product Production Identified as the Main Source of Per- and Polyfluoroalkyl Substances (PFAS) in a Norwegian Lake: Source and Historic Emission Tracking. Environ. Pollut. 2021, 273, 116259, DOI: 10.1016/j.envpol.2020.116259Google Scholar37https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhsVersL8%253D&md5=b0d9b392894c9a2b7663141b945556eaPaper product production identified as the main source of per- and polyfluoroalkyl substances (PFAS) in a Norwegian lake: Source and historic emission trackingLangberg, Haakon A.; Arp, Hans Peter H.; Breedveld, Gijs D.; Slinde, Goeril A.; Hoeiseter, Aase; Groenning, Hege M.; Jartun, Morten; Rundberget, Thomas; Jenssen, Bjoern M.; Hale, Sarah E.Environmental Pollution (Oxford, United Kingdom) (2021), 273 (), 116259CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)The entirety of the sediment bed in lake Tyrifjorden, Norway, is contaminated by per- and polyfluoroalkyl substances (PFAS). A factory producing paper products and a fire station were investigated as possible sources. Fire station emissions were dominated by the eight carbon perfluoroalkyl sulfonic acid (PFSA), perfluorooctanesulfonic acid (PFOS), from aq. film forming foams. Factory emissions contained PFOS, PFOS precursors (preFOS and SAmPAP), long chained fluorotelomer sulfonates (FTS), and perfluoroalkyl carboxylic acids (PFCA). Concns. and profiles in sediments and biota indicated that emissions originating from the factory were the main source of pollution in the lake, while no clear indication of fire station emissions was found. Ratios of linear-to branched-PFOS increased with distance from the factory, indicating that isomer profiles can be used to trace a point source. A dated sediment core contained higher concns. in older sediments and indicated that two different PFAS products have been used at the factory, referred to here as Scotchban and FTS mixt. Modeling, based on the sediment concns., indicated that 42-189 tons Scotchban, and 2.4-15.6 tons FTS mixt., were emitted. Prodn. of paper products may be a major PFAS point source, that has generally been overlooked. It is hypothesized that paper fibers released from such facilities are important vectors for PFAS transport in the aquatic environment.
- 38No a La Sulfluramida: Razones para la Prohibición Mundial de este Agrótoxico. IPEN. https://ipen.org/documents/no-la-sulfluramida (accessed 2022–11–28).Google ScholarThere is no corresponding record for this reference.
- 39Rogerson, M.; Rohling, E. J.; Weaver, P. P. E.; Murray, J. W. The Azores Front since the Last Glacial Maximum. Earth and Planetary Science Letters 2004, 222 (3), 779– 789, DOI: 10.1016/j.epsl.2004.03.039Google Scholar39https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2cXkvVSnsL8%253D&md5=5b1235dfc274873e0f1a9247b6c4b19dThe Azores Front since the Last Glacial MaximumRogerson, M.; Rohling, E. J.; Weaver, P. P. E.; Murray, J. W.Earth and Planetary Science Letters (2004), 222 (3-4), 779-789CODEN: EPSLA2; ISSN:0012-821X. (Elsevier Science B.V.)The spatial distribution of warm surface water in the Atlantic Ocean reflects the state of the thermohaline circulation. The Azores Current/Front, which is a recirculation of the Gulf Stream, marks the northeastern boundary of the North Atlantic subtropical gyre. Its position is therefore diagnostic of the width of the Atlantic warm water sphere. Here we report high resoln. stable isotope and faunal abundance records of planktonic foraminifera in a sediment core from the Gulf of Cadiz (southwest Spain) which reflects shifting of the Azores Front since the Last Glacial Maximum (LGM). Today, the Azores Front does not penetrate into the Gulf of Cadiz, even though the front resides at the same latitude as the Gulf of Cadiz in the Atlantic. Our results indicate that the Azores Front is a robust feature of the Atlantic surface circulation, and that is present both in interglacial times and during the LGM at roughly the same latitude. However, during the LGM prior to 16 ka BP and during the Younger Dryas, the Azores Front did penetrate eastward into the Gulf of Cadiz.
- 40Neuer, S.; Cianca, A.; Helmke, P.; Freudenthal, T.; Davenport, R.; Meggers, H.; Knoll, M.; Santana-Casiano, J. M.; González-Davila, M.; Rueda, M.-J.; Llinás, O. Biogeochemistry and Hydrography in the Eastern Subtropical North Atlantic Gyre. Results from the European Time-Series Station ESTOC. Progress in Oceanography 2007, 72 (1), 1– 29, DOI: 10.1016/j.pocean.2006.08.001Google ScholarThere is no corresponding record for this reference.
- 41Law, K. L.; Morét-Ferguson, S.; Maximenko, N. A.; Proskurowski, G.; Peacock, E. E.; Hafner, J.; Reddy, C. M. Plastic Accumulation in the North Atlantic Subtropical Gyre. Science 2010, 329 (5996), 1185– 1188, DOI: 10.1126/science.1192321Google Scholar41https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXhtV2hsr7J&md5=13b19b8068ceb9d2217fcac9e833a4d7Plastic Accumulation in the North Atlantic Subtropical GyreLaw, Kara Lavender; Moret-Ferguson, Skye; Maximenko, Nikolai A.; Proskurowski, Giora; Peacock, Emily E.; Hafner, Jan; Reddy, Christopher M.Science (Washington, DC, United States) (2010), 329 (5996), 1185-1188CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Plastic marine pollution is a major environmental concern, yet a quant. description of the scope of this problem in the open ocean is lacking. Here, we present a time series of plastic content at the surface of the western North Atlantic Ocean and Caribbean Sea from 1986 to 2008. More than 60% of 6136 surface plankton net tows collected buoyant plastic pieces, typically millimeters in size. The highest concn. of plastic debris was obsd. in subtropical latitudes and assocd. with the obsd. large-scale convergence in surface currents predicted by Ekman dynamics. Despite a rapid increase in plastic prodn. and disposal during this time period, no trend in plastic concn. was obsd. in the region of highest accumulation.
- 42Reißig, S.; Nürnberg, D.; Bahr, A.; Poggemann, D.-W.; Hoffmann, J. Southward Displacement of the North Atlantic Subtropical Gyre Circulation System During North Atlantic Cold Spells. Paleoceanography and Paleoclimatology 2019, 34 (5), 866– 885, DOI: 10.1029/2018PA003376Google ScholarThere is no corresponding record for this reference.
- 43Ter Halle, A.; Jeanneau, L.; Martignac, M.; Jardé, E.; Pedrono, B.; Brach, L.; Gigault, J. Nanoplastic in the North Atlantic Subtropical Gyre. Environ. Sci. Technol. 2017, 51 (23), 13689– 13697, DOI: 10.1021/acs.est.7b03667Google Scholar43https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhvVaqtrfK&md5=7480dbf6584ac7d3d0ed2ecda43d3499Nanoplastic in the North Atlantic Subtropical GyreTer Halle, Alexandra; Jeanneau, Laurent; Martignac, Marion; Jarde, Emilie; Pedrono, Boris; Brach, Laurent; Gigault, JulienEnvironmental Science & Technology (2017), 51 (23), 13689-13697CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Plastics can be found in all ecosystems across the globe. This type of environmental pollution is important, even if its impact is not fully understood. The presence of small plastic particles at the micro- and nanoscales is of growing concern, but nanoplastic has not yet been obsd. in natural samples. We examd. 4 size fractions (meso-, large micro-, small micro-, and nanoplastics) of debris collected in the North Atlantic subtropical gyre. To obtain the nanoplastic portion, we isolated the colloidal fraction of seawater. After ultrafiltration, the occurrence of nanoscale particles was demonstrated using dynamic light scattering expts. The chem. fingerprint of the colloids was obtained by pyrolysis coupled with gas chromatog.-mass spectrometry. We demonstrated that the signal was anthropogenic and attributed to a combination of plastics. The polymer compn. varied among the size classes. At the micro- and nanoscales, polyvinyl chloride, polyethylene terephthalate, polystyrene and polyethylene were obsd. We also obsd. changes in the pyrolytic signals of polyethylene with decreasing debris size, which could be related to the structural modification of this plastic as a consequence of weathering.
- 44Egger, M.; Sulu-Gambari, F.; Lebreton, L. First Evidence of Plastic Fallout from the North Pacific Garbage Patch. Sci. Rep 2020, 10 (1), 7495, DOI: 10.1038/s41598-020-64465-8Google Scholar44https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXptVeiu7Y%253D&md5=88ca6178113431518b16e98b9a20e5ccFirst evidence of plastic fallout from the North Pacific Garbage PatchEgger, Matthias; Sulu-Gambari, Fatimah; Lebreton, LaurentScientific Reports (2020), 10 (1), 7495CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)He infamous garbage patches on the surface of subtropical oceanic gyres are proof that plastic is polluting the ocean on an unprecedented scale. The fate of floating plastic debris 'trapped' in these gyres, however, remains largely unknown. Here, we provide the first evidence for the vertical transfer of plastic debris from the North Pacific Garbage Patch (NPGP) into the underlying deep sea. The numerical and mass concns. of plastic fragments (500μm to 5 cm in size) suspended in the water column below the NPGP follow a power law decline with water depth, reaching values <0.001 pieces/m3 and <0.1μg/m3 in the deep sea. The plastic particles in the NPGP water column are mostly in the size range of particles that are apparently missing from the ocean surface and the polymer compn. of plastic in the NPGP water column is similar to that of floating debris circulating in its surface waters (i.e. dominated by polyethylene and polypropylene). Our results further reveal a pos. correlation between the amt. of plastic debris at the sea surface and the depth-integrated concns. of plastic fragments in the water column. We therefore conclude that the presence of plastics in the water column below the NPGP is the result of 'fallout' of small plastic fragments from its surface waters.
- 45Mato, Y.; Isobe, T.; Takada, H.; Kanehiro, H.; Ohtake, C.; Kaminuma, T. Plastic Resin Pellets as a Transport Medium for Toxic Chemicals in the Marine Environment. Environ. Sci. Technol. 2001, 35 (2), 318– 324, DOI: 10.1021/es0010498Google Scholar45https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXosFyqt70%253D&md5=751d40a75427a1cea06bd8555aca2d0aPlastic Resin Pellets as a Transport Medium for Toxic Chemicals in the Marine EnvironmentMato, Yukie; Isobe, Tomohiko; Takada, Hideshige; Kanehiro, Haruyuki; Ohtake, Chiyoko; Kaminuma, TsuguchikaEnvironmental Science and Technology (2001), 35 (2), 318-324CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Plastic resin pellets (small granules 0.1-0.5 cm diam.) are widely distributed in the ocean worldwide. They are an industrial raw material for the plastic industry and are unintentionally released to the environment during manufg. and transport. They are sometimes ingested by seabirds and other marine organisms; their adverse effects on organisms are a concern. In this, polychlorinated biphenyls (PCB), DDE, and nonylphenols (NP) were detected in polypropylene (PP) resin pellets collected from 4 Japanese coasts. Concns. of PCB (4-117 ng/g), DDE (0.16-3.1 ng/g), and NP (0.13-16 μg/g) varied among sample site. Concns. were comparable to those for suspended particles and bottom sediment collected from the same area as the pellets. Field adsorption expts. using PP virgin pellets demonstrated a significant, steady increase in PCB and DDE concns. throughout a 6-day expt., indicating the source of PCB and DDE is ambient seawater and that adsorption to pellet surfaces is the mechanism of enrichment. The major source of NP in the marine PP resin pellets was thought to be plastic additives and/or their degrdn. products. Comparison of PCB and DDE concns. in marine PP resin pellets with those in seawater suggested their high degree of accumulation (apparent adsorption coeff.: 105-106). The high accumulation potential suggested that plastic resin pellets serve as a transport medium and a potential source of toxic chems. in the marine environment.
- 46Rios, L. M.; Moore, C.; Jones, P. R. Persistent Organic Pollutants Carried by Synthetic Polymers in the Ocean Environment. Mar. Pollut. Bull. 2007, 54 (8), 1230– 1237, DOI: 10.1016/j.marpolbul.2007.03.022Google Scholar46https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXotlKju7w%253D&md5=5d8f8b494e8d2390bc96fb0b9a0da4e3Persistent organic pollutants carried by synthetic polymers in the ocean environmentRios, Lorena M.; Moore, Charles; Jones, Patrick R.Marine Pollution Bulletin (2007), 54 (8), 1230-1237CODEN: MPNBAZ; ISSN:0025-326X. (Elsevier B.V.)Thermoplastic resin pellets are melted and formed into an enormous no. of inexpensive consumer goods, many of which are discarded after a relatively short period of use, dropped haphazardly onto watersheds and then make their way to the ocean where some get ingested by marine life. In 2003 and 2004 pre-prodn. thermoplastic resin pellets and post-consumer plastic fragments were collected and analyzed for contamination for persistent org. pollutants (POPs). Samples were taken from the North Pacific Gyre, and selected sites in California, Hawaii, and from Guadalupe Island, Mexico. The total concn. of PCBs was 27-980 ng/g, DDTs 22-7100 ng/g and PAHs 39-1200 ng/g, and aliph. hydrocarbons 1.1-8600 μg/g. Anal. methods were developed to ext., conc. and identify POPs that may have accumulated on plastic fragments and plastic pellets. The results confirm that plastic debris is a trap for POPs.
- 47Wang, F.; Shih, K. M.; Li, X. Y. The Partition Behavior of Perfluorooctanesulfonate (PFOS) and Perfluorooctanesulfonamide (FOSA) on Microplastics. Chemosphere 2015, 119, 841– 847, DOI: 10.1016/j.chemosphere.2014.08.047Google Scholar47https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhsVOmsb%252FM&md5=597ed4f5bad0f7c51ce06918be93b60fThe partition behavior of perfluorooctanesulfonate (PFOS) and perfluorooctanesulfonamide (FOSA) on microplasticsWang, Fei; Shih, Kai Min; Li, Xiao YanChemosphere (2015), 119 (), 841-847CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Microplastics have been recognized as transport vectors for heavy metals and org. pollutants to marine animals. Thus, the sorption behavior of contaminant on microplastic is crucial to their transport in marine system. In this study, the sorption behavior of PFOS and FOSA (two perfluorochems.) on three kinds of microplastics (PE, PS, and PVC) are reported. The isotherm study showed that the sorption of PFOS and FOSA on microplastics is highly linear, and it indicated that partition by hydrophobic interaction is the predominant sorption mechanism. The Kd values of FOSA on three kinds of microplastics are all higher than those of PFOS, and the reason is attributed to their different functional groups. The Kd value of FOSA on three types of microplastics followed the order as: PE > PVC > PS. Such finding may indicate that the mol. compn. and structure of microplastics play important roles in their sorption processes of org. pollutants. The PFOS sorption levels on PE and PS particles were increased with the increase of NaCl and CaCl2 concns., while the ion concns. have no effect on FOSA sorption. The study on the pH effects on PFOS and FOSA sorption indicated FOSA could partition under various pH conditions on three types of microplastics while PFOS sorption on PE and PS were favored with lower pH.
- 48Islam, N.; Garcia da Fonseca, T.; Vilke, J.; Gonçalves, J. M.; Pedro, P.; Keiter, S.; Cunha, S. C.; Fernandes, J. O.; Bebianno, M. J. Perfluorooctane Sulfonic Acid (PFOS) Adsorbed to Polyethylene Microplastics: Accumulation and Ecotoxicological Effects in the Clam Scrobicularia Plana. Marine Environmental Research 2021, 164, 105249, DOI: 10.1016/j.marenvres.2020.105249Google Scholar48https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhs1yhs74%253D&md5=64ca3fd9a72e84d1dd0e6bc3dd8476b1Perfluorooctane sulfonic acid (PFOS) adsorbed to polyethylene microplastics: Accumulation and ecotoxicological effects in the clam Scrobicularia planaIslam, Naimul; Garcia da Fonseca, Taina; Vilke, Juliano; Goncalves, Joanna M.; Pedro, Paulo; Keiter, Steffen; Cunha, Sara C.; Fernandes, Jose O.; Bebianno, M. J.Marine Environmental Research (2021), 164 (), 105249CODEN: MERSDW; ISSN:0141-1136. (Elsevier Ltd.)Microplastics are widespread in the marine environment, whereby the uptake of these tiny particles by organisms, can cause adverse biol. responses. Plastic debris also act as a vector of many contaminants, herein depending on type, size, shape and chem. properties, possibly intensifying their effects on marine organisms. This study aimed to assess the accumulation and potential toxicity of different sizes of microplastics with and without adsorbed perfluorooctane sulfonic acid (PFOS) in the clam Scrobicularia plana. Clams were exposed to low-d. polyethylene microplastics (1 mg L-1) of two different sizes (4-6 and 20-25μm) virgin and contaminated with PFOS (55.7 ± 5.3 and 46.1 ± 2.9μg g-1 resp.) over 14 days. Microplastic ingestion, PFOS accumulation and filtration rate were detd. along with a multi biomarker approach to assess the biol. effects of microplastics ingestion. Biomarkers include oxidative stress (superoxide dismutase, catalase, glutathione peroxidases), biotransformation enzymes (glutathione-S-transferases activity), neurotoxicity (acetylcholinesterase activity), oxidative damage and apoptosis. Microplastics ingestion and PFOS accumulation was microplastic size dependent but not PFOS dependent and filtration rate was reduced at the end of the exposure. Reactive oxygen species in gills and digestive gland were generated as a result of exposure to both types of microplastics, confirming the disturbance of the antioxidant system. Larger virgin microparticles lead to stronger impacts, when compared to smaller ones which was also supported by the Integrated Biomarker Responses index calcd. for both tissues. An anti-apoptotic response was detected in digestive glands under exposure to any of the MPs treatments.
- 49Brumovský, M.; Karásková, P.; Borghini, M.; Nizzetto, L. Per- and Polyfluoroalkyl Substances in the Western Mediterranean Sea Waters. Chemosphere 2016, 159, 308– 316, DOI: 10.1016/j.chemosphere.2016.06.015Google Scholar49https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XpvFaktbk%253D&md5=5b326d75056b5680640376ac78643802Per- and polyfluoroalkyl substances in the Western Mediterranean Sea watersBrumovsky, Miroslav; Karaskova, Pavlina; Borghini, Mireno; Nizzetto, LucaChemosphere (2016), 159 (), 308-316CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)The spatial and temporal distribution of per- and polyfluoroalkyl substances (PFASs) in the open Western Mediterranean Sea waters was investigated in this study for the first time. In addn. to surface water samples, a deep water sample (1390 m depth) collected in the center of the western basin was analyzed. Perfluorohexanoic acid (PFHxA), perfluoroheptanoic acid (PFHpA), perfluorooctanoic acid (PFOA), perfluorohexanesulfonate (PFHxS) and perfluorooctanesulfonate (PFOS) were detected in all samples and were the dominant PFASs found. The sum of PFAS concns. (ΣPFASs) ranged 246-515 pg/L for surface water samples. PFASs in surface water had a relatively homogeneous distribution with levels similar to those previously measured in the Atlantic near the Strait of Gibraltar, in water masses feeding the inflow to the Mediterranean Sea. Higher concns. of PFHxA, PFHpA and PFHxS were, however, found in the present study. Inflowing Atlantic water and river/coastal discharges are likely the major sources of PFASs to the Western Mediterranean basin. Slightly lower (factor of 2) ΣPFASs was found in the deep water sample (141 pg/L). Such a relatively high contamination of deep water is likely to be linked to recurring deep water renewal fed by downwelling events in the Gulf of Lion and/or Ligurian Sea.
- 50García-Gallardo, Á.; Grunert, P.; Piller, W. E. Variations in Mediterranean–Atlantic Exchange across the Late Pliocene Climate Transition. Climate of the Past 2018, 14 (3), 339– 350, DOI: 10.5194/cp-14-339-2018Google ScholarThere is no corresponding record for this reference.
- 51Lyu, X.; Xiao, F.; Shen, C.; Chen, J.; Park, C. M.; Sun, Y.; Flury, M.; Wang, D. Per- and Polyfluoroalkyl Substances (PFAS) in Subsurface Environments: Occurrence, Fate, Transport, and Research Prospect. Reviews of Geophysics 2022, 60 (3), e2021RG000765 DOI: 10.1029/2021RG000765Google ScholarThere is no corresponding record for this reference.
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Abstract
Figure 1
Figure 1. Map of the sampling stations along the transect and composition pattern of PFAAs (PFAAs below the detection limit are excluded) in the surface water samples (2 and 5 m) at the sampling stations.
Figure 2
Figure 2. Spatial distribution of the sum of PFAAs in the northern and southern hemisphere of the Atlantic Ocean. Black dots represent sample points where ΣPFAAs could be detected; gray triangles represent nondetects.
Figure 3
Figure 3. Distribution of PFNA in the vertical water column in the Northern Hemisphere. Black dots represent the sampling stations; gray triangles are nondetects (<MDL).
References
This article references 51 other publications.
- 1Prevedouros, K.; Cousins, I. T.; Buck, R. C.; Korzeniowski, S. H. Sources, Fate and Transport of Perfluorocarboxylates. Environ. Sci. Technol. 2006, 40 (1), 32– 44, DOI: 10.1021/es05124751https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXht1Gru7zK&md5=39fe4ec81ae1fa6d9b5fa387ff0e74b7Sources, Fate and Transport of PerfluorocarboxylatesPrevedouros, Konstantinos; Cousins, Ian T.; Buck, Robert C.; Korzeniowski, Stephen H.Environmental Science and Technology (2006), 40 (1), 32-44CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A review describes the sources, fate, and transport of perfluorocarboxylates (PFCAs) in the environment, with a specific focus on perfluorooctanoate (PFO). The global historical industry-wide emissions of total PFCAs from direct (manuf., use, consumer products) and indirect (PFCA impurities and/or precursors) sources were estd. to be 3200-7300 tons. It was estd. that the majority (∼80%) of PFCAs have been released to the environment from fluoropolymer manuf. and use. Although indirect sources were estd. to be much less important than direct sources, there were larger uncertainties assocd. with the calcns. for indirect sources. The phys.-chem. properties of PFO (negligible vapor pressure, high soly. in water, and moderate sorption to solids) suggested that PFO would accumulate in surface waters. Estd. mass inventories of PFO in various environmental compartments confirmed that surface waters, esp. oceans, contain the majority of PFO. The only environmental sinks for PFO were identified to be sediment burial and transport to the deep oceans, implying a long environmental residence time. Transport pathways for PFCAs in the environment were reviewed, and it was concluded that, in addn. to atm. transport/degrdn. of precursors, atm. and ocean water transport of the PFCAs themselves could significantly contribute to their long-range transport. It was estd. that 2-12 tons/yr of PFO are transported to the Arctic by oceanic transport, which is greater than the amt. estd. to result from atm. transport/degrdn. of precursors.
- 2Paul, A. G.; Jones, K. C.; Sweetman, A. J. A First Global Production, Emission, And Environmental Inventory For Perfluorooctane Sulfonate. Environ. Sci. Technol. 2009, 43 (2), 386– 392, DOI: 10.1021/es802216n2https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhsVyks7%252FJ&md5=a56b37805ef14fb968abcb1a528cd55dA First Global Production, Emission, And Environmental Inventory For Perfluorooctane SulfonatePaul, Alexander G.; Jones, Kevin C.; Sweetman, Andrew J.Environmental Science & Technology (2009), 43 (2), 386-392CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)This study makes a new est. of the global historical prodn. for perfluorooctane sulfonyl fluoride (POSF), and then focuses on producing a first est. of the global historical environmental releases of perfluorooctane sulfonate (PFOS). The total historical worldwide prodn. of POSF was estd. to be 96,000 t (or 122 500 t, including unusable wastes) between 1970-2002, with an estd. global release of 45,250 t to air and water between 1970-2012 from direct (manuf., use, and consumer products) and indirect (PFOS precursors and/or impurities) sources. Ests. indicate that direct emissions from POSF-derived products are the major source to the environment resulting in releases of 450-2700 t PFOS into wastewater streams, primarily through losses from stain repellent treated carpets, waterproof apparel, and aq. fire fighting foams. Large uncertainties surround indirect sources and have not yet been estd. due to limited information on environmental degrdn., although it can be assumed that some POSF-derived chems. will degrade to PFOS over time. The properties of PFOS (high water soly., negligible vapor pressure, and limited sorption to particles) imply it will reside in surface waters, predominantly in oceans. Measured oceanic data suggests ∼235-1770 t of PFOS currently reside in ocean surface waters, similar to the estd. PFOS releases. Environmental monitoring from the 1970s onward shows strong upward trends in biota, in broad agreement with the ests. of use and emissions made here. Since cessation of POSF prodn. by 3M in 2002, a redn. in some compartments has been obsd., although current and future exposure is dependent on emission routes, subsequent transport and degrdn.
- 3Wania, F. A Global Mass Balance Analysis of the Source of Perfluorocarboxylic Acids in the Arctic Ocean. Environ. Sci. Technol. 2007, 41 (13), 4529– 4535, DOI: 10.1021/es070124c3https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXlsFenu7k%253D&md5=04c24935ebd5aa30fdd38996b2533bd6A Global Mass Balance Analysis of the Source of Perfluorocarboxylic Acids in the Arctic OceanWania, FrankEnvironmental Science & Technology (2007), 41 (13), 4529-4535CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Whereas the pervasive and abundant presence of perfluorinated carboxylic acids (PFCAs) in the Arctic marine food chain is clearly established, their origin and transport pathway into the Arctic Ocean are not. Either the atm. oxidn. of volatile precursor compds., such as the fluorotelomer alcs. (FTOHs), or the long-range oceanic transport of directly emitted PFCAs is seen as contributing the bulk of the PFCA input to the Arctic. Here simulations with the zonally averaged global fate and transport model Globo-POP, in combination with historical emission ests. for FTOHs and perfluorooctanoic acid (PFOA), are used to evaluate the relative efficiency and importance of the two transport pathways. Ests. of the emission-independent Arctic Contamination Potential reveal that the oceanic transport of directly emitted PFCAs is more than 10-fold more efficient than the atm. degrdn. of FTOHs in delivering PFCAs to the Arctic, mostly because of the low yield of the reaction. The cumulative historic emissions of FTOHs are lower than those estd. for PFOA alone by a factor of 2-3, further limiting the contribution that precursor oxidn. makes to the total PFCAs load in the Arctic Ocean. Accordingly, when fed only with FTOH emissions, the model predicts FTOH air concns. in agreement with the reported measurements, but yields Arctic seawater concns. for the PFOA that are 2 orders of magnitude too low. Whereas ocean transport is thus very likely the dominant pathway of PFOA into the Arctic Ocean, the major transport route of longer chain PFCAs depends on the size of their direct emissions relative to those of 10:2 FTOH. The predicted time course of Arctic seawater concns. is very similar for directly emitted and atmospherically generated PFCAs, implying that neither past doubling times of PFCA concns. in Arctic marine mammals nor any future time trends are likely to resolve the question of the dominant source of PFCAs.
- 4Armitage, J. M.; MacLeod, M.; Cousins, I. T. Comparative Assessment of the Global Fate and Transport Pathways of Long-Chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct Sources. Environ. Sci. Technol. 2009, 43 (15), 5830– 5836, DOI: 10.1021/es900753y4https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXnsVWhtL0%253D&md5=656ebab43c645ea97cb3f4f39e295ad8Comparative Assessment of the Global Fate and Transport Pathways of Long-Chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct SourcesArmitage, James M.; MacLeod, Matthew; Cousins, Ian T.Environmental Science & Technology (2009), 43 (15), 5830-5836CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A global-scale, multispecies mass balance model simulated the long-term fate and transport of perfluorocarboxylic acids (PFCA) with 8-13 (C8-13) and their conjugate bases, perfluorocarboxylates (PFC), to assess the relative long-range transport (LRT) potential of each conjugate pair, collectively termed PFC(A), considering only direct source emissions (i.e., manufg. and use). Overall LRT potential (atm. + oceanic) varied as a function of chain length and depended on assumptions regarding pKa and mode of entry. Atm. transport had a relatively higher contribution to overall LRT potential for PFC(A) with longer chain length, reflecting the increasing trend in air/water partition coeff. (KAW) of neutral PFCA species with chain length. Model scenarios using estd. direct emissions of C8, C9, and C11 PFC(A) indicated mass fluxes to the Arctic marine environment assocd. with oceanic transport were greater than mass fluxes from indirect sources (i.e., atm. transport of precursor substances [fluoro-telomer alcs.] and subsequent degrdn. to PFCA). Modeled C8-9 concns. in the abiotic environment were broadly consistent with available surface ocean water monitoring data; modeled C8:C9 concn. ratios were reconcilable with the homolog pattern frequently obsd. in biota, assuming a pos. correlation between bioaccumulation potential and chain length. Modeled C11:C10 concn. ratios were more difficult to reconcile with monitoring data for sources and remote regions. Thus, C11 and C10 model results implied either indirect sources were dominant; or estd. direct emission were not accurate for these homologs.
- 5Armitage, J. M.; Schenker, U.; Scheringer, M.; Martin, J. W.; MacLeod, M.; Cousins, I. T. Modeling the Global Fate and Transport of Perfluorooctane Sulfonate (PFOS) and Precursor Compounds in Relation to Temporal Trends in Wildlife Exposure. Environ. Sci. Technol. 2009, 43 (24), 9274– 9280, DOI: 10.1021/es901448p5https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXhsVSgtbrF&md5=1752a410810a52feaba0ea4f460a51b9Modeling the Global Fate and Transport of Perfluorooctane Sulfonate (PFOS) and Precursor Compounds in Relation to Temporal Trends in Wildlife ExposureArmitage, James M.; Schenker, Urs; Scheringer, Martin; Martin, Jonathan W.; MacLeod, Matthew; Cousins, Ian T.Environmental Science & Technology (2009), 43 (24), 9274-9280CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A global-scale fate and transport model was applied to study the historic and future trends in ambient concns. of perfluorooctane sulfonate (PFOS) and volatile perfluorooctane sulfonyl fluoride (POSF)-based precursor compds. in the environment. A global emission inventory for PFOS and its precursor compds. was estd. for 1957-2010. We used this inventory as input to a global-scale contaminant fate model and compared modeled concns. with field data. The main focus of the simulations was to examine how modeled concns. of PFOS and volatile precursor compds. respond to the major prodn. phase-out that occurred in 2000-2002. Modeled concns. of PFOS in surface ocean waters are generally within a factor of 5 of field data and are dominated by direct emissions of this substance. In contrast, modeled concns. of the precursor compds. considered in this study are lower than measured concns. both before and after the prodn. phase-out. Modeled surface ocean water concns. of PFOS in source regions decline slowly in response to the prodn. phase-out while concns. in remote regions continue to increase until 2030. In contrast, modeled concns. of precursor compds. in both the atm. and surface ocean water compartment in all regions respond rapidly to the prodn. phase-out (i.e., decline quickly to much lower levels). With respect to wildlife biomonitoring data, since precursor compds. are bioavailable and degrade to PFOS in vivo, it is at least plausible that declining trends in PFOS body burdens obsd. in some marine organisms are attributable to this exposure pathway. The continued increases in PFOS body burdens obsd. in marine organisms inhabiting other regions may reflect exposure primarily to PFOS itself, present in the environment due to prodn. and use of this compd. as well as degrdn. of precursor compds.
- 6Armitage, J. M.; MacLeod, M.; Cousins, I. T. Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance Model. Environ. Sci. Technol. 2009, 43 (4), 1134– 1140, DOI: 10.1021/es802900n6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXotlKmtw%253D%253D&md5=d24d3aa685ebbcd74fb2bf3626e866a5Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance ModelArmitage, James M.; MacLeod, Matthew; Cousins, Ian T.Environmental Science & Technology (2009), 43 (4), 1134-1140CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Global-scale fate and transport processes for perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted by direct sources were simulated using a multi-species mass balance model for 1950-2010. This work assessed the atm. and oceanic long-range transport potential of direct source emissions and implications for pollution of terrestrial and marine systems worldwide. Consistent with previous modeling studies, ocean transport was the dominant pathway for delivering direct source-released PFOA to the Arctic marine environment, regardless of model assumptions. Modeled surface seawater concns. were insensitive to assumptions regarding physicochem. properties and entry emission modes reasonably agreed with available Northern Hemisphere monitoring data. Model outputs characterizing atm. transport potential were highly sensitive to model assumptions, esp. assumed acid dissocn. const. (pKa) values; however, the complete range of model results for scenarios with different assumptions about partitioning and emissions provide evidence that atm. transport of directly emitted PFOA can deliver this compd. to terrestrial environments distant from sources. Addnl. studies in remote or isolated terrestrial systems may provide further insight into the scale of pollution actually attributable to direct sources.
- 7Wang, P.; Lu, Y.; Wang, T.; Fu, Y.; Zhu, Z.; Liu, S.; Xie, S.; Xiao, Y.; Giesy, J. P. Occurrence and Transport of 17 Perfluoroalkyl Acids in 12 Coastal Rivers in South Bohai Coastal Region of China with Concentrated Fluoropolymer Facilities. Environ. Pollut. 2014, 190, 115– 122, DOI: 10.1016/j.envpol.2014.03.0307https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXntFyhsLk%253D&md5=8951e1b78452610b281ce2a235cce861Occurrence and transport of 17 perfluoroalkyl acids in 12 coastal rivers in south Bohai coastal region of China with concentrated fluoropolymer facilitiesWang, Pei; Lu, Yonglong; Wang, Tieyu; Fu, Yaning; Zhu, Zhaoyun; Liu, Shijie; Xie, Shuangwei; Xiao, Yang; Giesy, John P.Environmental Pollution (Oxford, United Kingdom) (2014), 190 (), 115-122CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)Perfluoroalkyl acids (PFAAs) are emerging contaminants that have raised great concern in recent years. While PFAAs manufg. becomes regulated in developed countries, prodn. has been partly shifted to China. Eight fluoropolymer manufg. facilities located in the South Bohai coastal region, one of the most populated areas of China, have been used to manuf. PFAA-related substances since 2001. The environmental consequence of the intensive prodn. of PFAAs in this region remains largely unknown. We analyzed 17 PFAAs in twelve coastal rivers of this region, and found staggeringly high concns. of perfluorooctanoic acid (PFOA) ranging from 0.96 to 4534.41 ng/L. The highest concn. was obsd. in the Xiaoqing River which received effluents from certain fluoropolymer facilities. Principal component anal. indicated similar sources of several perfluoroalkyl carboxylic acids (PFCAs) in all rivers, which indicated that atm. transport, wastewater treatment and surface runoff also acted as important supplements to direct discharge to surface water.
- 8Wang, Z.; Boucher, J. M.; Scheringer, M.; Cousins, I. T.; Hungerbühler, K. Toward a Comprehensive Global Emission Inventory of C4–C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C8-Based Products and Ongoing Industrial Transition. Environ. Sci. Technol. 2017, 51 (8), 4482– 4493, DOI: 10.1021/acs.est.6b061918https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXks12iurg%253D&md5=34dbfa59b48a23b421b977bf922262beToward a Comprehensive Global Emission Inventory of C4-C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C8-Based Products and Ongoing Industrial TransitionWang, Zhanyun; Boucher, Justin M.; Scheringer, Martin; Cousins, Ian T.; Hungerbuhler, KonradEnvironmental Science & Technology (2017), 51 (8), 4482-4493CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)A global emission inventory of C4-10 perfluoroalkanesulfonic acids (PFSA) from the life cycle of perfluorooctanesulfonyl fluoride (POSF)-based products in 1958-2030 is presented. It substantially improves and expands previous frameworks by incorporating missing pieces (e.g., emissions to soil by land treatment, overlooked precursors) and updating parameters (e.g., emission factors, degrdn. half-lives). In 1958-2015, total direct and indirect emissions of perfluorooctanesulfonic acid (PFOS) were estd. to be 1228-4930 tonnes; emissions of PFOS precursors were estd. to be 1230-8738 tonnes, ∼670 tonnes for x-perfluorooctanesulfonamides/sulfonamido ethanols (xFOSA/E) and POSF, resp. Most emissions occurred between 1958 and 2002, followed by a substantial decrease. This confirmed the pos. effect of the ongoing transition to phase-out POSF-based products, although this transition may still require substantial time and cause substantial addnl. releases of PFOS (8-153 tonnes) and xFOSA/Es (4-698 tonnes) in 2016 to 2030. Modeled environmental concns. obtained by coupling the emission inventory and a global multi-media mass balance model generally agree well with reported field measurements, suggesting the inventory captures, for the first time, actual emissions of PFOS and xFOSA/E despite remaining uncertainties. An anal. of key uncertainties and open questions of and beyond the inventory showed that, among others, degrdn. of side-chain fluorinated polymers in the environment and landfills can be a long-term, (potentially) substantial source of PFOS.
- 9Zhang, X.; Zhang, Y.; Dassuncao, C.; Lohmann, R.; Sunderland, E. M. North Atlantic Deep Water Formation Inhibits High Arctic Contamination by Continental Perfluorooctane Sulfonate Discharges. Global Biogeochemical Cycles 2017, 31 (8), 1332– 1343, DOI: 10.1002/2017GB0056249https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhsVektrzJ&md5=77a7a365d3a0beeee35a05e839073a7aNorth Atlantic Deep Water formation inhibits high Arctic contamination by continental perfluorooctane sulfonate dischargesZhang, Xianming; Zhang, Yanxu; Dassuncao, Clifton; Lohmann, Rainer; Sunderland, Elsie M.Global Biogeochemical Cycles (2017), 31 (8), 1332-1343CODEN: GBCYEP; ISSN:1944-9224. (Wiley-Blackwell)Perfluorooctane sulfonate (PFOS) is an aliph. fluorinated compd. with eight carbon atoms that is extremely persistent in the environment and can adversely affect human and ecol. health. The stability, low reactivity, and high water soly. of PFOS combined with the North American phaseout in prodn. around the year 2000 make it a potentially useful new tracer for ocean circulation. Here we characterize processes affecting the lifetime and accumulation of PFOS in the North Atlantic Ocean and transport to sensitive Arctic regions by developing a 3-D simulation within the MITgcm. The model captures variability in measurements across biogeog. provinces (R2 = 0.90, p = 0.01). In 2015, the North Atlantic PFOS reservoir was equiv. to 60% of cumulative inputs from the North American and European continents (1400 Mg). Cumulative inputs to the Arctic accounted for 30% of continental discharges, while the remaining 10% was transported to the tropical Atlantic and other regions. PFOS concns. declined rapidly after 2002 in the surface mixed layer (half-life: 1-2 years) but are still increasing below 1000 m depth. During peak prodn. years (1980-2000), plumes of PFOS-enriched seawater were transported to the sub-Arctic in energetic surface ocean currents. However, Atlantic Meridional Overturning Circulation (AMOC) and deep ocean transport returned a substantial fraction of this northward transport (20%, 530 Mg) to southern latitudes and reduced cumulative inputs to the Arctic (730 Mg) by 70%. Weakened AMOC due to climate change is thus likely to increase the magnitude of persistent bioaccumulative pollutants entering the Arctic Ocean.
- 10Boucher, J. M.; Cousins, I. T.; Scheringer, M.; Hungerbühler, K.; Wang, Z. Toward a Comprehensive Global Emission Inventory of C4–C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C6- and C10-Based Products. Environ. Sci. Technol. Lett. 2019, 6 (1), 1– 7, DOI: 10.1021/acs.estlett.8b0053110https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXitFyrt7fE&md5=b3bb61ecf244f2734cd487bb5127c8abToward a Comprehensive Global Emission Inventory of C4-C10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C6- and C10-Based ProductsBoucher, Justin M.; Cousins, Ian T.; Scheringer, Martin; Hungerbuhler, Konrad; Wang, ZhanyunEnvironmental Science & Technology Letters (2019), 6 (1), 1-7CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)A first global emission inventory of C4-C10 perfluoroalkanesulfonic acids (PFSAs) released during the life cycle of perfluorohexanesulfonyl fluoride (PHxSF)- and perfluorodecanesulfonyl fluoride (PDSF)-based products is presented. This study complements previous research on emissions of PFSAs that focused largely on the life cycle of perfluorooctanesulfonyl fluoride (POSF) and its derivs. It reviews and integrates existing information about the life cycle of PHxSF, PDSF, and their derivs.; the limited data available in the public domain point to potentially significant global prodn., uses, and releases of these substances. Between 1958 and 2015, ranges of total emissions of perfluorohexanesulfonic acid (PFHxS) and perfluorodecanesulfonic acid (PFDS) are estd. to be 120-1022 and 38-378 metric tons, resp. With the new emission ests. as inputs in a global multimedia environmental fate model (CliMoChem), the model-derived environmental concns. well capture the reported field concns., providing strong support for the plausibility of the developed emission inventories. The results highlight the ongoing environmental exposure to these substances and the need for more detailed data in the public domain about their prodn. levels and uses.
- 11Johansson, J. H.; Salter, M. E.; Acosta Navarro, J. C.; Leck, C.; Nilsson, E. D.; Cousins, I. T. Global Transport of Perfluoroalkyl Acids via Sea Spray Aerosol. Environmental Science: Processes & Impacts 2019, 21 (4), 635– 649, DOI: 10.1039/C8EM00525G11https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXltFGlu78%253D&md5=abfed0e0165a4a299919ccbe6d8a5b84Global transport of perfluoroalkyl acids via sea spray aerosolJohansson, J. H.; Salter, M. E.; Acosta Navarro, J. C.; Leck, C.; Nilsson, E. D.; Cousins, I. T.Environmental Science: Processes & Impacts (2019), 21 (4), 635-649CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)Perfluoroalkyl acids (PFAAs) are persistent org. pollutants found throughout the world's oceans. Previous research suggests that long-range atm. transport of these substances may be substantial. However, it remains unclear what the main sources of PFAAs to the atm. are. We have used a lab. sea spray chamber to study water-to-air transfer of 11 PFAAs via sea spray aerosol (SSA). We obsd. significant enrichment of all PFAAs relative to sodium in the SSA generated. The highest enrichment was obsd. in aerosols with aerodynamic diam. < 1.6μm, which had aerosol PFAA concns. up to ∼62 000 times higher than the PFAA water concns. in the chamber. In surface microlayer samples collected from the sea spray chamber, the enrichment of the substances investigated was orders of magnitude smaller than the enrichment obsd. in the aerosols. In expts. with mixts. of structural isomers, a lower contribution of branched PFAA isomers was obsd. in the surface microlayer compared to the bulk water. However, no clear trend was obsd. in the comparison of structural isomers in SSA and bulk water. Using the measured enrichment factors of perfluorooctanoic acid and perfluorooctane sulfonic acid vs. sodium we have estd. global annual emissions of these substances to the atm. via SSA as well as their global annual deposition to land areas. Our expts. suggest that SSA may currently be an important source of these substances to the atm. and, over certain areas, to terrestrial environments.
- 12Sha, B.; Johansson, J. H.; Benskin, J. P.; Cousins, I. T.; Salter, M. E. Influence of Water Concentrations of Perfluoroalkyl Acids (PFAAs) on Their Size-Resolved Enrichment in Nascent Sea Spray Aerosols. Environ. Sci. Technol. 2021, 55 (14), 9489– 9497, DOI: 10.1021/acs.est.0c0380412https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXhslSmt7%252FO&md5=84d2352cc7618aa9511012cce58a94f5Influence of water concentrations of perfluoroalkyl acids (PFAAs) on their size-resolved enrichment in nascent sea spray aerosolsSha, Bo; Johansson, Jana H.; Benskin, Jonathan P.; Cousins, Ian T.; Salter, Matthew E.Environmental Science & Technology (2021), 55 (14), 9489-9497CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Perfluoroalkyl acids (PFAAs) are persistent org. substances that have been widely detected in the global oceans. Previous lab. expts. have demonstrated effective enrichment of PFAAs in nascent sea spray aerosols (SSA), suggesting that SSA are an important source of PFAAs to the atm. In the present study, the effects of the water concn. of PFAAs on their size-resolved enrichment in SSA were examd. using a sea spray simulation chamber. Aerosolization of the target compds. in almost all sizes of SSA revealed a strong linear relationship with their water concns. (p < 0.05, r2 > 0.9). The enrichment factors (EF) of the target compds. showed no correlation with their concns. in the chamber water, despite the concns. varying by a factor of 500 (~ 0.3 to ~ 150 ng L-1). The particle surface-area-to-vol. ratio appeared to be a key predictor of the enrichment of perfluoroalkyl carboxylic acids (PFCAs) with ≥7 perfluorinated carbons and perfluoroalkanesulfonic acids (PFSAs) with ≥6 perfluorinated carbons in supermicron particles (p < 0.05, r2 > 0.8), but not in submicron particles. The different enrichment behaviors of PFAAs in submicron and supermicron particles might be a result of the different prodn. mechanisms of film droplets and jet droplets. The results suggest that the variability in seawater concns. of PFAAs has little influence on EFs and that modeling studies designed to quantify the source of PFAAs via SSA emissions do not need to consider this factor.
- 13Sha, B.; Johansson, J. H.; Tunved, P.; Bohlin-Nizzetto, P.; Cousins, I. T.; Salter, M. E. Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere: Field Evidence from Long-Term Air Monitoring. Environ. Sci. Technol. 2022, 56 (1), 228– 238, DOI: 10.1021/acs.est.1c0427713https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXislartLrJ&md5=83653024bf4fb4df09fb0ee1ce47c503Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere: Field Evidence from Long-Term Air MonitoringSha, Bo; Johansson, Jana H.; Tunved, Peter; Bohlin-Nizzetto, Pernilla; Cousins, Ian T.; Salter, Matthew E.Environmental Science & Technology (2022), 56 (1), 228-238CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)The effective enrichment of perfluoroalkyl acids (PFAAs) in sea spray aerosols (SSA) demonstrated in previous lab. studies suggests that SSA is a potential source of PFAAs to the atm. In order to investigate the influence of SSA on atm. PFAAs in the field, 48 h aerosol samples were collected regularly between 2018 and 2020 at two Norwegian coastal locations, Andoya and Birkenes. Significant correlations (p < 0.05) between the SSA tracer ion, Na+, and PFAA concns. were obsd. in the samples from both locations, with Pearson's correlation coeffs. (r) between 0.4-0.8. Such significant correlations indicate SSA to be an important source of atm. PFAAs to coastal areas. The correlations in the samples from Andoya were obsd. for more PFAA species and were generally stronger than in the samples from Birkenes, which is located further away from the coast and closer to urban areas than Andoya. Factors such as the origin of the SSA, the distance of the sampling site to open water, and the presence of other PFAA sources (e.g., volatile precursor compds.) can have influence on the contribution of SSA to PFAA in air at the sampling sites and therefore affect the obsd. correlations between PFAAs and Na+.
- 14Wei, S.; Chen, L. Q.; Taniyasu, S.; So, M. K.; Murphy, M. B.; Yamashita, N.; Yeung, L. W. Y.; Lam, P. K. S. Distribution of Perfluorinated Compounds in Surface Seawaters between Asia and Antarctica. Mar. Pollut. Bull. 2007, 54 (11), 1813– 1818, DOI: 10.1016/j.marpolbul.2007.08.00214https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXhtlaqtLjI&md5=35aa6da53feb11c3cc2be230c537701cDistribution of perfluorinated compounds in surface seawaters between Asia and AntarcticaWei, S.; Chen, L. Q.; Taniyasu, S.; So, M. K.; Murphy, M. B.; Yamashita, N.; Yeung, L. W. Y.; Lam, P. K. S.Marine Pollution Bulletin (2007), 54 (11), 1813-1818CODEN: MPNBAZ; ISSN:0025-326X. (Elsevier B.V.)There is no expanded citation for this reference.
- 15Yamashita, N.; Taniyasu, S.; Petrick, G.; Wei, S.; Gamo, T.; Lam, P. K. S.; Kannan, K. Perfluorinated Acids as Novel Chemical Tracers of Global Circulation of Ocean Waters. Chemosphere 2008, 70 (7), 1247– 1255, DOI: 10.1016/j.chemosphere.2007.07.07915https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXivVyjsw%253D%253D&md5=276d7ee4ebdaef9d76ac1a3cc879991fPerfluorinated acids as novel chemical tracers of global circulation of ocean watersYamashita, Nobuyoshi; Taniyasu, Sachi; Petrick, Gert; Wei, Si; Gamo, Toshitaka; Lam, Paul K. S.; Kannan, KurunthachalamChemosphere (2008), 70 (7), 1247-1255CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Perfluorinated acids (PFAs) such as perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) are global environmental contaminants. The physicochem. properties of PFAs are unique in that they have high water solubilities despite the low reactivity of C-F bond, which also imparts high stability in the environment. Because of the high water solubilities, the open-ocean water column is suggested to be the final sink for PFOS and PFOA. However, little is known on the distribution of PFAs in the oceans around the world. We describe the horizontal (spatial) and vertical distribution of PFAs in ocean waters worldwide. PFOS and PFOA concns. in the North Atlantic Ocean ranged from 8.6 to 36 pg/L and from 52 to 338 pg/L, resp., whereas the corresponding concns. in the Mid Atlantic Ocean were 13-73 and 67-439 pg/L. These were completely different from the surface waters of the South Pacific Ocean and the Indian Ocean (overall range of <5-11 pg/L for PFOS and PFOA). Vertical profiles of PFAs in the marine water column were assocd. with the global ocean circulation theory. Vertical profiles of PFAs in water columns from the Labrador Sea reflected the influx of the North Atlantic Current in surface waters, the Labrador Current in subsurface waters, and the Denmark Strait Overflow Water in deep layers below 2000 m. Striking differences in the vertical and spatial distribution of PFAs, depending on the oceans, suggest that these persistent acids can serve as useful chem. tracers to allow us to study oceanic transport by major water currents. The results provide evidence that PFA concns. and profiles in the oceans adhere to a pattern consistent with the global Broecker's Conveyor Belt theory of open ocean water circulation.
- 16Ahrens, L.; Barber, J. L.; Xie, Z.; Ebinghaus, R. Longitudinal and Latitudinal Distribution of Perfluoroalkyl Compounds in the Surface Water of the Atlantic Ocean. Environ. Sci. Technol. 2009, 43 (9), 3122– 3127, DOI: 10.1021/es803507p16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXjvFalsb0%253D&md5=bdee241499275203506b1132065db770Longitudinal and Latitudinal Distribution of Perfluoroalkyl Compounds in the Surface Water of the Atlantic OceanAhrens, Lutz; Barber, Jonathan L.; Xie, Zhiyong; Ebinghaus, RalfEnvironmental Science & Technology (2009), 43 (9), 3122-3127CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Perfluoroalkyl compds. (PFCs) were detd. in 2 L surface water samples collected in the Atlantic Ocean onboard the research vessels Maria S. Merian along the longitudinal gradient from Las Palmas (Spain) to St. Johns (Canada) (15° W to 52° W) and Polarstern along the latitudinal gradient from the Bay of Biscay to the South Atlantic Ocean (46° N to 26° S) in spring and fall 2007, resp. After filtration the dissolved and particulate phases were extd. sep., and PFC concns. were detd. using HPLC interfaced to tandem mass spectrometry. No PFCs were detected in the particulate phase. This study provides the 1st concn. data of perfluorooctanesulfonamide (FOSA), perfluorohexanoic acid, and perfluoroheptanoic acid from the Atlantic Ocean. Results indicate that trans-Atlantic Ocean currents caused the decreasing concn. gradient from the Bay of Biscay to the South Atlantic Ocean and the concn. drop-off close to the Labrador Sea. Maximum concns. were found for FOSA, perfluorooctanesulfonate, and perfluorooctanoic acid at 302, 291, and 229 pg/L, resp. However, the concn. of each single compd. was usually in the tens of pg/L range. South of the equator only FOSA and below 4° S no PFCs could be detected.
- 17Ahrens, L.; Xie, Z.; Ebinghaus, R. Distribution of Perfluoroalkyl Compounds in Seawater from Northern Europe, Atlantic Ocean, and Southern Ocean. Chemosphere 2010, 78 (8), 1011– 1016, DOI: 10.1016/j.chemosphere.2009.11.03817https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXhtlWkurw%253D&md5=f76cffde333395dabc06cebddc6a9e72Distribution of perfluoroalkyl compounds in seawater from Northern Europe, Atlantic Ocean, and Southern OceanAhrens, Lutz; Xie, Zhiyong; Ebinghaus, RalfChemosphere (2010), 78 (8), 1011-1016CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)The global distribution of perfluoroalkyl compds. (PFCs) were investigated in surface water samples collected onboard the Polarstern in Northern Europe, Atlantic and Southern Ocean (52°N-69°S) in 2008. The water samples were solid-phase extd. with Oasis WAX cartridges and analyzed using the high-performance liq. chromatog. interfaced to tandem mass spectrometry. Concns. of various PFCs, including C4, C6, C8 perfluoroalkyl sulfonates (PFSAs), perfluorooctane sulfinate (PFOSi), C5-C12 perfluoroalkyl carboxylic acids (PFCA) and perfluorooctane sulfonamide (FOSA) were quantified. Perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) were the predominant compds. with a max. concn. of 232 and 223 pg L-1, resp. Results indicate that industrial areas like the European Continent act as source of PFCs, while ocean water is an important as a sink as well as the transport medium of these compds. Interestingly, in the equator area the .sum.PFC concn. increased, which indicates that there exists an atm. or other unknown input source of PFCs. In the Southern Ocean only PFOS was detected which could be caused by atm. transport of its precursors.
- 18Zhao, Z.; Xie, Z.; Möller, A.; Sturm, R.; Tang, J.; Zhang, G.; Ebinghaus, R. Distribution and Long-Range Transport of Polyfluoroalkyl Substances in the Arctic, Atlantic Ocean and Antarctic Coast. Environ. Pollut. 2012, 170, 71– 77, DOI: 10.1016/j.envpol.2012.06.00418https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC38XhtF2rsr%252FN&md5=a783ed6e2adc4a4b7b1a3c973107d3d1Distribution and long-range transport of polyfluoroalkyl substances in the Arctic, Atlantic Ocean and Antarctic coastZhao, Zhen; Xie, Zhiyong; Moeller, Axel; Sturm, Renate; Tang, Jianhui; Zhang, Gan; Ebinghaus, RalfEnvironmental Pollution (Oxford, United Kingdom) (2012), 170 (), 71-77CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)The global distribution and long-range transport of polyfluoroalkyl substances (PFASs) were investigated using seawater samples collected from the Greenland Sea, East Atlantic Ocean, and the Southern Ocean in 2009-2010. Elevated levels of ΣPFASs were detected in the North Atlantic Ocean with the concns. ranging from 130-650 pg/L. In the Greenland Sea, the ΣPFASs concns. ranged from 45-280 pg/L, and 5 most frequently detected compds. were perfluorooctanoic acid (PFOA), perfluorohexanesulfonate (PFHxS), perfluorohexanoic acid (PFHxA), perfluorooctane sulfonate (PFOS), and perfluorobutane sulfonate (PFBS). PFOA (15 pg/L) and PFOS (25-45 pg/L) were occasionally found in the Southern Ocean. In the Atlantic Ocean, the ΣPFASs concn. decreased from 2007-2010. The elevated PFOA level that resulted from melting snow and ice in Greenland Sea implies that the Arctic may were driven by climate change and turned to be a source of PFASs for the marine ecosystem. Polyfluoroalkyl substances (PFASs) were reported for the Arctic, Atlantic, and the Southern Ocean, which improves understanding the fate of PFASs in the global oceans.
- 19Benskin, J. P.; Muir, D. C. G.; Scott, B. F.; Spencer, C.; De Silva, A. O.; Kylin, H.; Martin, J. W.; Morris, A.; Lohmann, R.; Tomy, G.; Rosenberg, B.; Taniyasu, S.; Yamashita, N. Perfluoroalkyl Acids in the Atlantic and Canadian Arctic Oceans. Environ. Sci. Technol. 2012, 46 (11), 5815– 5823, DOI: 10.1021/es300578x19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC38XmtlOlt7Y%253D&md5=7921afb5ff8600731268538bb0fc969fPerfluoroalkyl Acids in the Atlantic and Canadian Arctic OceansBenskin, Jonathan P.; Muir, Derek C. G.; Scott, Brian F.; Spencer, Christine; De Silva, Amila O.; Kylin, Henrik; Martin, Jonathan W.; Morris, Adam; Lohmann, Rainer; Tomy, Gregg; Rosenberg, Bruno; Taniyasu, Sachi; Yamashita, NobuyoshiEnvironmental Science & Technology (2012), 46 (11), 5815-5823CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The spatial distribution of C4, C6, and C8 perfluoroalkyl sulfonates; C6-C14 perfluoroalkyl carboxylates; and perfluorooctanesulfonamide in Atlantic and Arctic oceans, including previously unstudied coastal water of North and South America,and the Canadian Arctic Archipelago, is reported. Perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) were typically the dominant perfluoroalkyl acids (PFAA) in Atlantic water. In the mid-northwest Atlantic/Gulf Stream, sum PFAA concns. (.sum.PFAA) were low (77-190 pg/L) but increased rapidly upon crossing into US coastal water (≤5800 pg/L near Rhode Island). .sum.PFAA in the northeast Atlantic were highest north of the Canary Islands (280-980 pg/L) and decreased with latitude. In the South Atlantic, concns. increased near Rio de la Plata (Argentina/Uruguay; 350-540 pg/L .sum.PFAA), possibly due to insecticides contg. N-Et perfluorooctanesulfonamide or proximity to Montevideo and Buenos Aires. In all other southern hemisphere locations, .sum.PFAA were <210 pg/L. PFOA:PFOS ratios were typically ≥1 in the northern hemisphere, ∼1 near the equator, and ≤1 in the southern hemisphere. In the Canadian Arctic, .sum.PFAA occurred at 40-250 pg/; perfluoroheptanoate, PFOA, and PFOS were among PFAA detected in highest concns. PFOA:PFOS ratios (typically »1) decreased from Baffin Bay to Amundsen Gulf, possibly due to increased atm. inputs. These data help validate global emission models and contribute to understanding PFAA long-range transport pathways and sources in remote regions.
- 20González-Gaya, B.; Dachs, J.; Roscales, J. L.; Caballero, G.; Jiménez, B. Perfluoroalkylated Substances in the Global Tropical and Subtropical Surface Oceans. Environ. Sci. Technol. 2014, 48 (22), 13076– 13084, DOI: 10.1021/es503490z20https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhslKgtLzL&md5=b41a06cc3867126d167223c52368810dPerfluoroalkylated Substances in the Global Tropical and Subtropical Surface OceansGonzalez-Gaya, Belen; Dachs, Jordi; Roscales, Jose L.; Caballero, Gemma; Jimenez, BegonaEnvironmental Science & Technology (2014), 48 (22), 13076-13084CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Perfluoroalkylated substances (PFASs) were analyzed in 92 surface seawater samples taken during the Malaspina 2010 expedition which covered all the tropical and subtropical Atlantic, Pacific and Indian oceans. Nine ionic PFASs including C6-C10 perfluoroalkyl carboxylic acids (PFCAs), C4 and C6-C8 perfluoroalkyl sulfonic acids (PFSAs) and 2 neutral precursors perfluoroalkyl sulfonamides (PFASAs), were identified and quantified. The Atlantic Ocean presented the broader range in concns. of total PFASs (131-10900 pg/L, median 645 pg/L, n =45) compared to the other oceanic basins, probably due to a better spatial coverage. Total concns. in the Pacific were 344-2500 pg/L (median =527 pg/L, n =27) and in the Indian Ocean 176-1976 pg/L (median =329, n =18). Perfluorooctanesulfonic acid (PFOS) was the most abundant compd., accounting for 33% of the total PFASs globally, followed by perfluorodecanoic acid (PFDA, 22%) and perfluorohexanoic acid (PFHxA, 12%), being the rest of the individual congeners under 10% of total PFASs, even for perfluorooctane carboxylic acid (PFOA, 6%). PFASAs accounted for <1% of the total PFASs concn. This study reports the ubiquitous occurrence of PFCAs, PFSAs, and PFASAs in the global ocean, being the first attempt, to our knowledge, to show a comprehensive assessment in surface water samples collected in a single oceanic expedition covering tropical and subtropical oceans. The potential factors affecting their distribution patterns were assessed including the distance to coastal regions, oceanic subtropical gyres, currents and biogeochem. processes. Field evidence of biogeochem. controls on the occurrence of PFASs was tentatively assessed considering environmental variables (solar radiation, temp., chlorophyll a concns. among others), and these showed significant correlations with some PFASs, but explaining small to moderate percentages of variability. This suggests that a no. of phys. and biogeochem. processes collectively drive the oceanic occurrence and fate of PFASs in a complex manner.
- 21Yeung, L. W. Y.; Dassuncao, C.; Mabury, S.; Sunderland, E. M.; Zhang, X.; Lohmann, R. Vertical Profiles, Sources, and Transport of PFASs in the Arctic Ocean. Environ. Sci. Technol. 2017, 51 (12), 6735– 6744, DOI: 10.1021/acs.est.7b0078821https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXnvVyjsb0%253D&md5=22400217c247069fd43980eb8a1a5953Vertical Profiles, Sources, and Transport of PFASs in the Arctic OceanYeung, Leo W. Y.; Dassuncao, Clifton; Mabury, Scott; Sunderland, Elsie M.; Zhang, Xianming; Lohmann, RainerEnvironmental Science & Technology (2017), 51 (12), 6735-6744CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The relative importance of atm. vs. oceanic transport for poly- and perfluorinated alkyl substances (PFASs) reaching the Arctic Ocean is not well understood. Vertical profiles from the Central Arctic Ocean and shelf water, snow and meltwater samples were collected in 2012; 13 PFASs (C6-C12 PFCAs; C6, 8, 10 PFSAs; MeFOSAA and EtFOSAA; and FOSA) were routinely detected (range: <5-343 pg/L). PFASs were only detectable above 150 m depth in the polar mixed layer (PML) and halocline. Enhanced concns. were obsd. in snow and melt pond samples, implying atm. deposition as an important source of PFASs. Model results suggested atm. inputs to account for 34-59% (∼11-19 pg/L) of measured PFOA concns. in the PML (mean 32 ± 15 pg/L). Modeled surface and halocline measurements for PFOS based on North Atlantic inflow (11-36 pg/L) agreed with measurements (mean, 17, range <5-41 pg/L). Modeled deep water concns. below 200 m (5-15 pg/L) were slightly higher than measurements (<5 pg/L), suggesting the lower bound of PFAS emissions ests. from wastewater and rivers may provide the best est. of inputs to the Arctic. Despite low concns. in deep water, this reservoir is expected to contain most of the PFOS mass in the Arctic (63-180 Mg) and is projected to continue increasing to 2038.
- 22Zhang, X.; Lohmann, R.; Sunderland, E. M. Poly- and Perfluoroalkyl Substances in Seawater and Plankton from the Northwestern Atlantic Margin. Environ. Sci. Technol. 2019, 53 (21), 12348– 12356, DOI: 10.1021/acs.est.9b0323022https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhvVOisbnL&md5=b35412e79f05eba5e1dc04de532c1d4bPoly- and Perfluoroalkyl Substances in Seawater and Plankton from the Northwestern Atlantic MarginZhang, Xianming; Lohmann, Rainer; Sunderland, Elsie M.Environmental Science & Technology (2019), 53 (21), 12348-12356CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The ocean probably is the terminal sink for poly- and perfluoroalkyl substances (PFAS) that have been produced and released in large quantities for >60 years. Regulatory actions have curbed prodn. of legacy compds. such as perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) but impacts on releases to the marine environment are poorly understood. Here we report new data for 21 targeted PFASs in marine seawater and plankton from the coast, shelf and slope of the Northwestern Atlantic Ocean. We find strong inverse correlations between salinity and concns. of most PFASs, indicating ongoing continental discharges are the major source to the marine environment. For legacy PFASs such as PFOS and PFOA, a comparison of inland and offshore measurements from the same year suggests there are ongoing releases to the marine environment from sources such as submarine groundwater discharges. Vertical transport of most PFASs assocd. with settling particles from the surface 10 m to deeper waters is small compared to advective transport except for perfluorodecanoic acid: PFDA (35% of vertical flux) and precursor compds. to PFOS (up to 86%). We find higher than expected bioaccumulation factors (BAFs = Cplankton/Cwater) for perfluorinated carboxylic acids (PFCAs) with 5 and 6 carbons (log BAFs = 2.9-3.4) and linear PFOS (log BAF = 2.6-4.3) in marine plankton compared to PFCAs with 7-11 carbons. We postulate that this reflects addnl. contributions from precursor compds. Known precursor compds. detected in this study have among the highest BAFs (log BAFs > 3.0) for all PFASs suggesting addnl. research on the bioaccumulation potential of unknown organoflourine compds. is urgently needed.
- 23Miranda, D. de A.; Leonel, J.; Benskin, J. P.; Johansson, J.; Hatje, V. Perfluoroalkyl Substances in the Western Tropical Atlantic Ocean. Environ. Sci. Technol. 2021, 55 (20), 13749– 13758, DOI: 10.1021/acs.est.1c0179423https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXitFymsbnP&md5=9f6acc5b10a719a49972daa723e811b2Perfluoroalkyl Substances in the Western Tropical Atlantic OceanMiranda, Daniele de A.; Leonel, Juliana; Benskin, Jonathan P.; Johansson, Jana; Hatje, VanessaEnvironmental Science & Technology (2021), 55 (20), 13749-13758CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)The dispersion of perfluoroalkyl substances (PFAS) in surface and deep-water profiles (down to 5845 m deep) was evaluated through the Western Tropical Atlantic Ocean (TAO) between 15°N and 23°S. The sum concns. for eight quantifiable PFAS (.sum.8PFAS) in surface waters ranged from 11 to 69 pg/L, which is lower than previously reported in the same area as well as in higher latitudes. Perfluoroalkyl carboxylic acids (PFCAs) were the predominant PFASs present in the Western TAO. The 16 surface samples showed variable PFAS distributions, with the predominance of perfluorooctanoic acid (PFOA) along the transect (67%; 11 ± 8 pg/L) and detection of perfluoroalkyl sulfonic acids (PFSAs) only in the Southern TAO. Perfluoroheptanoic acid (PFHpA) was often detected in the vertical profiles. PFAS distribution patterns (i.e., profiles and concns.) varied with depth throughout the TAO latitudinal sectors (North, Equator, South Atlantic, and in the Brazilian coastal zone). Vertical profiles in coastal samples displayed decreasing PFAS concns. with increasing depth, whereas offshore samples displayed higher PFAS detection frequencies in the intermediate water masses. Together with the surface currents and coastal upwelling, the origin of the water masses was an important factor in explaining PFAS concns. and profiles in the TAO.
- 24Yamazaki, E.; Taniyasu, S.; Wang, X.; Yamashita, N. Per- and Polyfluoroalkyl Substances in Surface Water, Gas and Particle in Open Ocean and Coastal Environment. Chemosphere 2021, 272, 129869, DOI: 10.1016/j.chemosphere.2021.12986924https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXks1Krs7g%253D&md5=63c6f8515ff39275df6c045eb5f8797ePer- and polyfluoroalkyl substances in surface water, gas and particle in open ocean and coastal environmentYamazaki, Eriko; Taniyasu, Sachi; Wang, Xinhong; Yamashita, NobuyoshiChemosphere (2021), 272 (), 129869CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)A simultaneous sampling of atm. and seawater samples was performed in the Taiwan Western Strait, western Arctic Ocean, and the Antarctic Ocean. Anal. of both particle and gas phase PFAS in oceanic air was conducted using cascade impactor particle fractionator, cryogenic air sampler and activated charcoal fiber sorbent for the first time with application in the Taiwan Western Strait. Mean concn. of Σ12PFAS in surface seawater and atm. samples were 1178 pg/L and 24 pg/m3 in the Taiwan Western Strait, 430 pg/L and 6 pg/m3 in the western Arctic Ocean, and 456 pg/L and 3 pg/m3 in the Antarctic Ocean. In oceanic air from the Taiwan Western Strait, fluorotelomer alc. (FTOH) and the ionic PFAS [perfluoroalkyl sulfonic acid (PFSA) and perfluoroalkyl carboxylic acid (PFCA)] were found in 76% and 7% resp. Regional comparison of air/water exchange (KAW) and gas-particle (Kp) partition coeffs. of PFAS in the oceanic environment indicated potential partitioning of ionic PFAS between surface seawater and oceanic air. These findings highlight the advancement in atm. PFAS measurements through combined novel technologies, namely size-fractionated particle sampling with cryogenic air trapping and/or activated charcoal sorption. Correlation between Kp and carbon chain length of PFAS was obsd. using both hyphenated techniques.
- 25Han, T.; Chen, J.; Lin, K.; He, X.; Li, S.; Xu, T.; Xin, M.; Wang, B.; Liu, C.; Wang, J. Spatial Distribution, Vertical Profiles and Transport of Legacy and Emerging per- and Polyfluoroalkyl Substances in the Indian Ocean. Journal of Hazardous Materials 2022, 437, 129264, DOI: 10.1016/j.jhazmat.2022.12926425https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XhsFertL%252FP&md5=d0502df999a50c61e63dd9a25cb156aaSpatial distribution, vertical profiles and transport of legacy and emerging per- and polyfluoroalkyl substances in the Indian OceanHan, Tongzhu; Chen, Junhui; Lin, Kun; He, Xiuping; Li, Shujiang; Xu, Tengfei; Xin, Ming; Wang, Baodong; Liu, Chenguang; Wang, JiangtaoJournal of Hazardous Materials (2022), 437 (), 129264CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)The contamination status and transport of per- and polyfluoroalkyl substances (PFASs) in the seawater of the Indian Ocean (IO) and an adjacent subregion of the Northwest Pacific Ocean (NWPO) were investigated. Eight legacy PFASs were widely distributed in the surface seawater, and perfluoroheptanoic acid (PFHpA) and perfluorooctanoic acid (PFOA) were the two predominant PFASs. ΣPFAS concn. decreased in the following order: NWPO>Joining area of Asia and Indian-Pacific Oceans (JAIPO)>Northeast Indian Ocean>Southwest Indian Ocean. Hexafluoropropylene oxide-dimer acid, a replacement surfactant for PFOA was extensively detected in the IO (∼34.8 pg/L) for the first time, showing an early sign of emerging PFAS spread in global open oceans. Eight depth profiles across the JAIPO (down to 5433 m depth) revealed a 'surface-enrichment' and 'depth-depletion' pattern for PFASs in the water column, and two noticeable fluctuations were mainly located at depths of 150-200 and 200-500 m. Phys. processes, including eddy diffusion, and the origin and trajectory of water mass were crucial factors for structuring PFAS vertical profiles. Mass transport ests. revealed a remarkable PFOA contribution through the JAIPO to IO carried by the Indonesian Throughflow, and a nonnegligible PFHpA contribution from Antarctic Immediate Water to deep water of the JAIPO driven by thermohaline circulation.
- 26Muir, D.; Miaz, L. T. Spatial and Temporal Trends of Perfluoroalkyl Substances in Global Ocean and Coastal Waters. Environ. Sci. Technol. 2021, 55 (14), 9527– 9537, DOI: 10.1021/acs.est.0c0803526https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXlt1Kks7k%253D&md5=7688dc2dc3986cf4a03b1632185fca7eSpatial and temporal trends of perfluoroalkyl substances in global ocean and coastal watersMuir, Derek; Miaz, Luc T.Environmental Science & Technology (2021), 55 (14), 9527-9537CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Per- and polyfluoroalkyl substances (PFAS) have been widely detected in global surface waters since the early 2000s. Here, we have compiled and analyzed the published data for perfluorocarboxylates (PFCAs) and perfluorosulfonates (PFSAs) in surface waters of coastal seas, the Great Lakes, and open oceans to examine temporal and geospatial trends. Mass discharges from major rivers were also estd. A large no. of measurements of individual PFAS have been made in these surface waters (29 500 values), with seven C4-C10 PFSAs and nine C4-C12 PFCAs accounting for 83% of all data. However, most results (85% for PFSAs; 80% for PFCAs) were for the coastal seas of Western Europe, China, Korea, and Japan, while results were limited for coastal North America and lacking for South America and Africa. Highest median concns. of PFCAs and PFSAs were reported in the Bohai and Yellow Seas region of China as well as in the North and Baltic seas in Europe. Significant declines in median PFSAs and C7-C12 PFCAs were also obsd. for the period 2012-2018 in these same regions, and for 2004-2017 in the Great Lakes. Mass discharge ests. indicated continued substantial riverine emissions of long chain (C7-C12) PFCAs in the period 2015-2019 for the coastal seas of China and redns. in emissions for Western European rivers compared to earlier time periods.
- 27Al Amin, Md.; Sobhani, Z.; Liu, Y.; Dharmaraja, R.; Chadalavada, S.; Naidu, R.; Chalker, J. M.; Fang, C. Recent Advances in the Analysis of Per- and Polyfluoroalkyl Substances (PFAS)─A Review. Environmental Technology & Innovation 2020, 19, 100879, DOI: 10.1016/j.eti.2020.100879There is no corresponding record for this reference.
- 28Yamazaki, E.; Taniyasu, S.; Ruan, Y.; Wang, Q.; Petrick, G.; Tanhua, T.; Gamo, T.; Wang, X.; Lam, P. K. S.; Yamashita, N. Vertical Distribution of Perfluoroalkyl Substances in Water Columns around the Japan Sea and the Mediterranean Sea. Chemosphere 2019, 231, 487– 494, DOI: 10.1016/j.chemosphere.2019.05.13228https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhtVGgsLvM&md5=c34f6b4539684fd7460f8a08c3228ed1Vertical distribution of perfluoroalkyl substances in water columns around the Japan sea and the Mediterranean SeaYamazaki, Eriko; Taniyasu, Sachi; Ruan, Yuefei; Wang, Qi; Petrick, Gert; Tanhua, Toste; Gamo, Toshitaka; Wang, Xinhong; Lam, Paul K. S.; Yamashita, NobuyoshiChemosphere (2019), 231 (), 487-494CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Perfluoroalkyl substances (PFASs) have become an important class of global environmental contaminants, yet their vertical profile in the marine water column is still less understood, esp. for the semi-closed seas. In this study, the contamination level and spatial distribution of 8 PFASs were investigated in both surface and vertical water samples from two semi-closed seas, the Japan Sea and the Mediterranean Sea. Similar levels and compns. of PFASs were found between these two seas. The vertical profile of PFASs in the Mediterranean Sea was variable while that was relatively steady in the Japan Sea, probably due to their different pollution sources. The accumulation rate of PFASs from the East China Sea to the Japan Sea was calcd., for which perfluorooctanesulfonic acid and perfluorooctanoic acid were found to have high accumulation potency in both surface and deep water; most of the investigated PFASs were accumulated in the deep water due to the long residence time while they were more likely to escape to the Pacific Ocean in the surface water. This work aimed (i) to study the distribution of PFASs in both surface and vertical water samples in two semi-closed seas, namely the Japan Sea and for the first time the Mediterranean Sea, (ii) to assess the temporal trend in the Japan Sea, and (iii) to firstly investigate the potential transport of PFASs from the East China Sea and Taiwan Strait in order to est. the inventory of PFASs in whole water mass in the Japan Sea.
- 29Joerss, H.; Xie, Z.; Wagner, C. C.; von Appen, W.-J.; Sunderland, E. M.; Ebinghaus, R. Transport of Legacy Perfluoroalkyl Substances and the Replacement Compound HFPO-DA through the Atlantic Gateway to the Arctic Ocean─Is the Arctic a Sink or a Source?. Environ. Sci. Technol. 2020, 54 (16), 9958– 9967, DOI: 10.1021/acs.est.0c0022829https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXhsVGrtrfI&md5=89a245af5de56bd32490b61b466c6418Transport of legacy perfluoroalkyl substances and the replacement compound HFPO-DA through the Atlantic gateway to the Arctic Ocean: Is the Arctic a sink or a source?Joerss, Hanna; Xie, Zhiyong; Wagner, Charlotte C.; von Appen, Wilken-Jon; Sunderland, Elsie M.; Ebinghaus, RalfEnvironmental Science & Technology (2020), 54 (16), 9958-9967CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The spatial distribution of 29 per- and polyfluoroalkyl substances (PFASs) in seawater was investigated along a sampling transect from Europe to the Arctic and two transects within Fram Strait, located between Greenland and Svalbard, in the summer of 2018. Hexafluoropropylene oxide-dimer acid (HFPO-DA), a replacement compd. for perfluorooctanoic acid (PFOA), was detected in Arctic seawater for the first time. This provides evidence for its long-range transport to remote areas. The total PFAS concn. was significantly enriched in the cold, low-salinity surface water exiting the Arctic compared to warmer, higher-salinity water from the North Atlantic entering the Arctic (260 ± 20 pg/L vs. 190 ± 10 pg/L). The higher ratio of perfluoroheptanoic acid (PFHpA) to perfluorononanoic acid (PFNA) in outflowing water from the Arctic suggests a higher contribution of atm. sources compared to ocean circulation. An east-west cross section of the Fram Strait, which included seven depth profiles, revealed higher PFAS concns. in the surface water layer than in intermediate waters and a negligible intrusion into deep waters (>1000 m). Mass transport ests. indicated a net inflow of PFASs with ≥8 perfluorinated carbons via the boundary currents and a net outflow of shorter-chain homologues. We hypothesize that this reflects higher contributions from atm. sources to the Arctic outflow and a higher retention of the long-chain compds. in melting snow and ice.
- 30Sanchez-Vidal, A.; Llorca, M.; Farré, M.; Canals, M.; Barceló, D.; Puig, P.; Calafat, A. Delivery of Unprecedented Amounts of Perfluoroalkyl Substances towards the Deep-Sea. Science of The Total Environment 2015, 526, 41– 48, DOI: 10.1016/j.scitotenv.2015.04.08030https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXnt1entbY%253D&md5=c6a75618587f5274fae092a0580ac47aDelivery of unprecedented amounts of perfluoroalkyl substances towards the deep-seaSanchez-Vidal, Anna; Llorca, Marta; Farre, Marinella; Canals, Miquel; Barcelo, Damia; Puig, Pere; Calafat, AntoniScience of the Total Environment (2015), 526 (), 41-48CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)The finding of perfluoroalkyl substances (PFASs) in particles sinking to the deep northwestern Mediterranean Sea confirms the role of the latter as ballast for the transfer of pollutants to the deep sea. The transfer of particulate matter down to the deep is enhanced during atm.-driven, high-energy phys. oceanog. processes like dense shelf water cascading (DSWC), which is caused by winter surface heat losses and evapn. We present data from samples collected during winter 2012, when dense shelf water formation and subsequent cascading triggered the flushing of large amts. of PFASs through a submarine canyon to depths in excess of 1000 m. The finding of quantifiable concns. of long-chain PFOA, PFOS and PFNA substances and significantly high concns. of the short-chain substances PFHxA and PFBA indicates that these compds., sorbed onto particulate matter, are quickly and directly transferred to the ocean's interior, thus highlighting the role of DSWC in removing those pollutants from the coastal ocean. Eventually, uncertainties about our results arising from the limited no. of samples available are counterbalanced by their intrinsic value as intense DSWC events, like the one in 2012, occur only every 5-7 yr in the study area, which seriously restricts sampling opportunities. Our results add PFASs to the list of persistent org. pollutants like polychlorinated biphenyls, chlorobenzenes or polycyclic arom. hydrocarbons known to be conveyed to the deep marine environment.
- 31Casal, P.; González-Gaya, B.; Zhang, Y.; Reardon, A. J. F.; Martin, J. W.; Jiménez, B.; Dachs, J. Accumulation of Perfluoroalkylated Substances in Oceanic Plankton. Environ. Sci. Technol. 2017, 51 (5), 2766– 2775, DOI: 10.1021/acs.est.6b0582131https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXis1Sqs7s%253D&md5=76d98670f30edc056c5155f5e73bd905Accumulation of Perfluoroalkylated Substances in Oceanic PlanktonCasal, Paulo; Gonzalez-Gaya, Belen; Zhang, Yifeng; Reardon, Anthony J. F.; Martin, Jonathan W.; Jimenez, Begona; Dachs, JordiEnvironmental Science & Technology (2017), 51 (5), 2766-2775CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The bioaccumulation of perfluoroalkylated substances (PFASs) in plankton has previously been evaluated only in freshwater and regional seas, but not for the large oligotrophic global oceans. Plankton samples from the tropical and subtropical Pacific, Atlantic and Indian Oceans were collected during the Malaspina 2010 circumnavigation expedition, and analyzed for 14 ionizable PFASs, including perfluorooctanoate (PFOA), perfluorooctanesulfonate (PFOS) and their resp. linear and branched isomers. PFOA and PFOS concns. in plankton ranged from 0.1 to 43 ng gdw-1 and from 0.5 to 6.7 ng gdw-1, resp. The relative abundance of branched PFOA in the northern hemisphere was correlated with distance to North America, consistent with the historical prodn. and coherent with previously reported patterns in seawater. The plankton samples showing the highest PFOS concns. also presented the largest relative abundances of branched PFOS, suggesting a selective cycling/fractionation of branched PFOS in the surface ocean mediated by plankton. Bioaccumulation factors (BAFs) for plankton were calcd. for six PFASs, including short chain PFASs. PFASs Log BAFs (wet wt.) ranged from 2.6±0.8 for perfluorohexanesulfonic acid (PFHxS), to 4.4±0.6 for perfluoroheptanoic acid (PFHpA). The vertical transport of PFASs due to the settling of org. matter bound PFAS (biol. pump) was estd. from an org. matter settling fluxes climatol. and the PFAS concns. in plankton. The global av. sinking fluxes were 0.8±1.3 ng m-2d-1 for PFOA, and 1.1±2.1 ng m-2d-1 for PFOS. The residence times of PFAS in the surface ocean, assuming the biol. pump as the unique sink, showed a wide range of variability, from few years to millennia, depending on the sampling site and individual compd. Further process-based studies are needed to constrain the oceanic sink of PFAS.
- 32González-Gaya, B.; Casal, P.; Jurado, E.; Dachs, J.; Jiménez, B. Vertical Transport and Sinks of Perfluoroalkyl Substances in the Global Open Ocean. Environmental Science: Processes & Impacts 2019, 21 (11), 1957– 1969, DOI: 10.1039/C9EM00266A32https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXhsV2is7bN&md5=a45cbb2a3e67600204da56a10311a1d1Vertical transport and sinks of perfluoroalkyl substances in the global open oceanGonzalez-Gaya, Belen; Casal, Paulo; Jurado, Elena; Dachs, Jordi; Jimenez, BegonaEnvironmental Science: Processes & Impacts (2019), 21 (11), 1957-1969CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)The ubiquitous occurrence of perfluoroalkyl substances (PFAS) in the open ocean has been previously documented, but their vertical transport and oceanic sinks have not been comprehensively characterized and quantified at the oceanic scale. During the Malaspina 2010 circumnavigation expedition, 21 PFAS were measured at the surface and at the deep chlorophyll max. (DCM) in the Atlantic, Indian and Pacific oceans. In this work, we report an extended data set of PFAS dissolved phase concns. at the DCM. .sum.PFAS at the DCM varied from 130 to 11 000 pg L-1, with a global av. value of 500 pg L-1. Perfluorooctanesulfonate (PFOS) abundance contributed 39% of .sum.PFAS, followed by perfluorodecanoate (PFDA, 17%), and perfluorohexanoate (PFHxA, 12%). The relative contribution of the remaining compds. was below 10%, with perfluorooctanoate (PFOA) contributing only 5% to PFAS measured at the DCM. Ests. of vertical diffusivity, derived from microstructure turbulence observations in the upper (<300 m) water column, allowed the derivation of PFAS eddy diffusive fluxes from concurrent field measurements of eddy diffusivity and PFAS concns. The PFAS concns. at the DCM predicted from an eddy diffusivity model were lower than field-measured concns., suggesting a relevant role of other vertical transport mechanisms. Settling fluxes of org. matter bound PFAS (biol. pump), oceanic circulation and potential, yet un-reported, biol. transformations are discussed.
- 33Löfstedt Gilljam, J.; Leonel, J.; Cousins, I. T.; Benskin, J. P. Is Ongoing Sulfluramid Use in South America a Significant Source of Perfluorooctanesulfonate (PFOS)? Production Inventories, Environmental Fate, and Local Occurrence. Environ. Sci. Technol. 2016, 50 (2), 653– 659, DOI: 10.1021/acs.est.5b0454433https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC28vptFGksg%253D%253D&md5=830a5494e7b8cf5b3ef92ffa46b9fad1Is Ongoing Sulfluramid Use in South America a Significant Source of Perfluorooctanesulfonate (PFOS)? Production Inventories, Environmental Fate, and Local OccurrenceLofstedt Gilljam John; Cousins Ian T; Benskin Jonathan P; Leonel JulianaEnvironmental science & technology (2016), 50 (2), 653-9 ISSN:.Despite international phase-out initiatives, production and use of perfluorooctanesulfonate (PFOS) and related substances continues in some countries. In Brazil, the PFOS-precursor N-ethyl perfluorooctane sulfonamide (EtFOSA) is used in Sulfluramid, a pesticide for controlling leaf-cutting ants. New data on production, environmental fate, and occurrence of Brazilian Sulfluramid are reported herein. From 2003 to 2013, Brazilian Sulfluramid manufacturing increased from 30 to 60 tonnes yr(-1) EtFOSA. During this time <1.3 tonnes yr(-1) were imported, while exports increased from ∼0.3 to 2 tonnes yr(-1). From 2004 to 2015, most EtFOSA was exported to Argentina (7.2 tonnes), Colombia (2.07 tonnes), Costa Rica (1.13 tonnes), Equador (2.16 tonnes), and Venezuela (2.4 tonnes). Within Brazil, sales occurred primarily in the states of Minas Gerais, Sao Paulo, Mato Grosso do Sul, Espirito Santo, and Bahia. Model simulations predict EtFOSA will partition to soils, while transformation products perfluorooctane sulfonamide (FOSA) and PFOS are sufficiently mobile to leach into surface waters. In support of these predictions, up to 3400 pg L(-1) of FOSA and up to 1100 pg L(-1) of PFOS were measured in Brazilian surface water, while EtFOSA was not detected. The high FOSA/PFOS ratio observed here (up to 14:1) is unprecedented in the scientific literature to our knowledge. Depending on the extent of conversion of EtFOSA, cumulative Brazilian Sulfluramid production and import from 2004 to 2015 may contribute between 167 and 487 tonnes of PFOS/FOSA to the environment. These levels are clearly nontrivial and of concern since production is continuing unabated.
- 34Catherine, M.; Nadège, B.; Charles, P.; Yann, A. Perfluoroalkyl Substances (PFASs) in the Marine Environment: Spatial Distribution and Temporal Profile Shifts in Shellfish from French Coasts. Chemosphere 2019, 228, 640– 648, DOI: 10.1016/j.chemosphere.2019.04.20534https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXovFentLY%253D&md5=b83d174035f7bdbc7fe5d83d9f435e1bPerfluoroalkyl substances (PFASs) in the marine environment: Spatial distribution and temporal profile shifts in shellfish from French coastsCatherine, Munschy; Nadege, Bely; Charles, Pollono; Yann, AminotChemosphere (2019), 228 (), 640-648CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Perfluoroalkyl substances (PFASs) were investigated in filter-feeding shellfish collected from 2013-2017 along the English Channel, Atlantic and Mediterranean coasts of France. PFOS (perfluorooctane sulfonate), PFTrDA (perfluorotridecanoic acid), PFTeDA (perfluorotetradecanoic acid), PFDoDA (perfluorododecanoic acid) and PFUnDA (perfluoroundecanoic acid) were detected in more than 80% of samples, thus indicating widespread contamination of the French coastal environment by these chems. The distribution of PFAS concns. showed differences according to sampling locations and years. PFOS was the predominant PFAS in most samples collected from English Channel and Atlantic coasts until 2014, but the opposite was obsd. in 2015, 2016 and 2017, while perfluoroalkyl carboxylic acids (PFCAs) prevailed in Mediterranean samples in all study years. Among PFCAs, PFTrDA showed the highest max. (1.36 ng g-1 ww) and median (0.077 ng g-1 ww) concns. in 2016-2017. Other PFAS median concns. were within the 0.014 (PFNA) - 0.055 (PFTeDA) ng g-1 ww range. The profiles detd. each year in most Mediterranean samples suggest distinctive sources. PFOS median concns. showed a significant decrease over the study years, from 0.118 to 0.126 ng g-1 ww in 2013-2015 to 0.066 ng g-1 ww in 2016 and 2017. .sum.PFCAs showed no trends in concn. ranges over the same years. The shift in PFAS profiles from PFOS to long-chain PFCAs over the study period reflects PFOS prodn. phase-out, combined with continuous inputs of PFCAs into the marine environment. These results provide ref. data for future studies of the occurrence of contaminants of emerging concern on European coasts.
- 35Santucci, L.; Carol, E.; Tanjal, C. Industrial Waste as a Source of Surface and Groundwater Pollution for More than Half a Century in a Sector of the Río de La Plata Coastal Plain (Argentina). Chemosphere 2018, 206, 727– 735, DOI: 10.1016/j.chemosphere.2018.05.08435https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXpvVOjsr0%253D&md5=01ff6e05a13954ac1c91198ff8fedcf7Industrial waste as a source of surface and groundwater pollution for more than half a century in a sector of the Rio de la Plata coastal plain (Argentina)Santucci, Lucia; Carol, Eleonora; Tanjal, CarolinaChemosphere (2018), 206 (), 727-735CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Environmental liabilities have become one of the most important problems of the last years, esp. those of contaminated sites located in urban areas which have been abandoned by pollution intensive industries. Such sites may contain hazardous materials that pose risks to human health and the environment. Industrial waste from the ancient sulfuric acid industry is scattered in a local area at the petrochem. pole in a sector of the Rio de la Plata coastal plain. A survey of soil and waste deposit was carried out and samples were examd. by X-ray diffraction, under a scanning electron microscope and a polarizing microscope. Surface water and groundwater samples, both to the unconfined and semi-confined aquifers, were collected to det. elec. cond., pH and major elements. The results show the presence of minerals composed of sulfur assocd. with jarosite and iron oxides on superficial sediments. The detailed study of soil sediments together with that of the water physicochem. characteristics make it possible to understand the geochem. processes developed in soil that cause the high concns. of sulfates in groundwater. Furthermore, high SO-24 concn. registered in the semi-confined aquifer due to its infiltration from the unconfined aquifer shows that the industrial pollution has an important impact at local level. These results may contribute to the understanding of chem. processes and pollutants distribution in highly industrialized coastal plain areas.
- 36Bentancur, S.; López-Vázquez, C. M.; García, H. A.; Duarte, M.; Travers, D.; Brdjanovic, D. Resource Recovery Assessment at a Pulp Mill Wastewater Treatment Plant in Uruguay. Journal of Environmental Management 2020, 255, 109718, DOI: 10.1016/j.jenvman.2019.10971836https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXit12ksbvJ&md5=8870c6739def37c59cd8e21a66878664Resource recovery assessment at a pulp mill wastewater treatment plant in UruguayBentancur, S.; Lopez-Vazquez, C. M.; Garcia, H. A.; Duarte, M.; Travers, D.; Brdjanovic, D.Journal of Environmental Management (2020), 255 (), 109718CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)Using a math. model, a resource recovery assessment was carried out at a pulp mill activated sludge wastewater treatment plant (WWTP) located in Uruguay. Through the evaluation of different scenarios, the potential prodn. of methane from secondary sludge, with its inherent energy savings, and the recovery of phosphorus (P) as struvite were estd. Considering the current WWTP configuration with a sludge retention time (SRT) of 32 days, and according to the model, which is a simplification of reality, the assessment indicates that the implementation of an anaerobic digester (AD) to treat the excess sludge can lead to a methane prodn. of approx. 1736 m3 CH4 d-1, being a promising alternative to increase the WWTP treatment performance. Furthermore, the model predictions suggest that by shortening the SRT from 32 to 5 days, the methane prodn. could increase by up to 5568 m3 CH4 d-1. If the methane produced is used to generate elec. energy to operate the WWTP, energy savings of about 88% can be achieved. Regarding the potential recovery of P as struvite, the addn. of a struvite reactor could be an efficient option to recover approx. 1611 mg L-1 of struvite (corresponding to a load of about 433 kg d-1). By optimizing the process performance, these findings highlight the potential recovery of resources in pulp mill WWTP, while complying with stringent effluent discharge stds. In addn., further research activities such as pilot-test or detailed lab. studies may be needed to validate the previous recommendations for industrial scale application.
- 37Langberg, H. A.; Arp, H. P. H.; Breedveld, G. D.; Slinde, G. A.; Høiseter, Å.; Grønning, H. M.; Jartun, M.; Rundberget, T.; Jenssen, B. M.; Hale, S. E. Paper Product Production Identified as the Main Source of Per- and Polyfluoroalkyl Substances (PFAS) in a Norwegian Lake: Source and Historic Emission Tracking. Environ. Pollut. 2021, 273, 116259, DOI: 10.1016/j.envpol.2020.11625937https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhsVersL8%253D&md5=b0d9b392894c9a2b7663141b945556eaPaper product production identified as the main source of per- and polyfluoroalkyl substances (PFAS) in a Norwegian lake: Source and historic emission trackingLangberg, Haakon A.; Arp, Hans Peter H.; Breedveld, Gijs D.; Slinde, Goeril A.; Hoeiseter, Aase; Groenning, Hege M.; Jartun, Morten; Rundberget, Thomas; Jenssen, Bjoern M.; Hale, Sarah E.Environmental Pollution (Oxford, United Kingdom) (2021), 273 (), 116259CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)The entirety of the sediment bed in lake Tyrifjorden, Norway, is contaminated by per- and polyfluoroalkyl substances (PFAS). A factory producing paper products and a fire station were investigated as possible sources. Fire station emissions were dominated by the eight carbon perfluoroalkyl sulfonic acid (PFSA), perfluorooctanesulfonic acid (PFOS), from aq. film forming foams. Factory emissions contained PFOS, PFOS precursors (preFOS and SAmPAP), long chained fluorotelomer sulfonates (FTS), and perfluoroalkyl carboxylic acids (PFCA). Concns. and profiles in sediments and biota indicated that emissions originating from the factory were the main source of pollution in the lake, while no clear indication of fire station emissions was found. Ratios of linear-to branched-PFOS increased with distance from the factory, indicating that isomer profiles can be used to trace a point source. A dated sediment core contained higher concns. in older sediments and indicated that two different PFAS products have been used at the factory, referred to here as Scotchban and FTS mixt. Modeling, based on the sediment concns., indicated that 42-189 tons Scotchban, and 2.4-15.6 tons FTS mixt., were emitted. Prodn. of paper products may be a major PFAS point source, that has generally been overlooked. It is hypothesized that paper fibers released from such facilities are important vectors for PFAS transport in the aquatic environment.
- 38No a La Sulfluramida: Razones para la Prohibición Mundial de este Agrótoxico. IPEN. https://ipen.org/documents/no-la-sulfluramida (accessed 2022–11–28).There is no corresponding record for this reference.
- 39Rogerson, M.; Rohling, E. J.; Weaver, P. P. E.; Murray, J. W. The Azores Front since the Last Glacial Maximum. Earth and Planetary Science Letters 2004, 222 (3), 779– 789, DOI: 10.1016/j.epsl.2004.03.03939https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2cXkvVSnsL8%253D&md5=5b1235dfc274873e0f1a9247b6c4b19dThe Azores Front since the Last Glacial MaximumRogerson, M.; Rohling, E. J.; Weaver, P. P. E.; Murray, J. W.Earth and Planetary Science Letters (2004), 222 (3-4), 779-789CODEN: EPSLA2; ISSN:0012-821X. (Elsevier Science B.V.)The spatial distribution of warm surface water in the Atlantic Ocean reflects the state of the thermohaline circulation. The Azores Current/Front, which is a recirculation of the Gulf Stream, marks the northeastern boundary of the North Atlantic subtropical gyre. Its position is therefore diagnostic of the width of the Atlantic warm water sphere. Here we report high resoln. stable isotope and faunal abundance records of planktonic foraminifera in a sediment core from the Gulf of Cadiz (southwest Spain) which reflects shifting of the Azores Front since the Last Glacial Maximum (LGM). Today, the Azores Front does not penetrate into the Gulf of Cadiz, even though the front resides at the same latitude as the Gulf of Cadiz in the Atlantic. Our results indicate that the Azores Front is a robust feature of the Atlantic surface circulation, and that is present both in interglacial times and during the LGM at roughly the same latitude. However, during the LGM prior to 16 ka BP and during the Younger Dryas, the Azores Front did penetrate eastward into the Gulf of Cadiz.
- 40Neuer, S.; Cianca, A.; Helmke, P.; Freudenthal, T.; Davenport, R.; Meggers, H.; Knoll, M.; Santana-Casiano, J. M.; González-Davila, M.; Rueda, M.-J.; Llinás, O. Biogeochemistry and Hydrography in the Eastern Subtropical North Atlantic Gyre. Results from the European Time-Series Station ESTOC. Progress in Oceanography 2007, 72 (1), 1– 29, DOI: 10.1016/j.pocean.2006.08.001There is no corresponding record for this reference.
- 41Law, K. L.; Morét-Ferguson, S.; Maximenko, N. A.; Proskurowski, G.; Peacock, E. E.; Hafner, J.; Reddy, C. M. Plastic Accumulation in the North Atlantic Subtropical Gyre. Science 2010, 329 (5996), 1185– 1188, DOI: 10.1126/science.119232141https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXhtV2hsr7J&md5=13b19b8068ceb9d2217fcac9e833a4d7Plastic Accumulation in the North Atlantic Subtropical GyreLaw, Kara Lavender; Moret-Ferguson, Skye; Maximenko, Nikolai A.; Proskurowski, Giora; Peacock, Emily E.; Hafner, Jan; Reddy, Christopher M.Science (Washington, DC, United States) (2010), 329 (5996), 1185-1188CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Plastic marine pollution is a major environmental concern, yet a quant. description of the scope of this problem in the open ocean is lacking. Here, we present a time series of plastic content at the surface of the western North Atlantic Ocean and Caribbean Sea from 1986 to 2008. More than 60% of 6136 surface plankton net tows collected buoyant plastic pieces, typically millimeters in size. The highest concn. of plastic debris was obsd. in subtropical latitudes and assocd. with the obsd. large-scale convergence in surface currents predicted by Ekman dynamics. Despite a rapid increase in plastic prodn. and disposal during this time period, no trend in plastic concn. was obsd. in the region of highest accumulation.
- 42Reißig, S.; Nürnberg, D.; Bahr, A.; Poggemann, D.-W.; Hoffmann, J. Southward Displacement of the North Atlantic Subtropical Gyre Circulation System During North Atlantic Cold Spells. Paleoceanography and Paleoclimatology 2019, 34 (5), 866– 885, DOI: 10.1029/2018PA003376There is no corresponding record for this reference.
- 43Ter Halle, A.; Jeanneau, L.; Martignac, M.; Jardé, E.; Pedrono, B.; Brach, L.; Gigault, J. Nanoplastic in the North Atlantic Subtropical Gyre. Environ. Sci. Technol. 2017, 51 (23), 13689– 13697, DOI: 10.1021/acs.est.7b0366743https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2sXhvVaqtrfK&md5=7480dbf6584ac7d3d0ed2ecda43d3499Nanoplastic in the North Atlantic Subtropical GyreTer Halle, Alexandra; Jeanneau, Laurent; Martignac, Marion; Jarde, Emilie; Pedrono, Boris; Brach, Laurent; Gigault, JulienEnvironmental Science & Technology (2017), 51 (23), 13689-13697CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Plastics can be found in all ecosystems across the globe. This type of environmental pollution is important, even if its impact is not fully understood. The presence of small plastic particles at the micro- and nanoscales is of growing concern, but nanoplastic has not yet been obsd. in natural samples. We examd. 4 size fractions (meso-, large micro-, small micro-, and nanoplastics) of debris collected in the North Atlantic subtropical gyre. To obtain the nanoplastic portion, we isolated the colloidal fraction of seawater. After ultrafiltration, the occurrence of nanoscale particles was demonstrated using dynamic light scattering expts. The chem. fingerprint of the colloids was obtained by pyrolysis coupled with gas chromatog.-mass spectrometry. We demonstrated that the signal was anthropogenic and attributed to a combination of plastics. The polymer compn. varied among the size classes. At the micro- and nanoscales, polyvinyl chloride, polyethylene terephthalate, polystyrene and polyethylene were obsd. We also obsd. changes in the pyrolytic signals of polyethylene with decreasing debris size, which could be related to the structural modification of this plastic as a consequence of weathering.
- 44Egger, M.; Sulu-Gambari, F.; Lebreton, L. First Evidence of Plastic Fallout from the North Pacific Garbage Patch. Sci. Rep 2020, 10 (1), 7495, DOI: 10.1038/s41598-020-64465-844https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXptVeiu7Y%253D&md5=88ca6178113431518b16e98b9a20e5ccFirst evidence of plastic fallout from the North Pacific Garbage PatchEgger, Matthias; Sulu-Gambari, Fatimah; Lebreton, LaurentScientific Reports (2020), 10 (1), 7495CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)He infamous garbage patches on the surface of subtropical oceanic gyres are proof that plastic is polluting the ocean on an unprecedented scale. The fate of floating plastic debris 'trapped' in these gyres, however, remains largely unknown. Here, we provide the first evidence for the vertical transfer of plastic debris from the North Pacific Garbage Patch (NPGP) into the underlying deep sea. The numerical and mass concns. of plastic fragments (500μm to 5 cm in size) suspended in the water column below the NPGP follow a power law decline with water depth, reaching values <0.001 pieces/m3 and <0.1μg/m3 in the deep sea. The plastic particles in the NPGP water column are mostly in the size range of particles that are apparently missing from the ocean surface and the polymer compn. of plastic in the NPGP water column is similar to that of floating debris circulating in its surface waters (i.e. dominated by polyethylene and polypropylene). Our results further reveal a pos. correlation between the amt. of plastic debris at the sea surface and the depth-integrated concns. of plastic fragments in the water column. We therefore conclude that the presence of plastics in the water column below the NPGP is the result of 'fallout' of small plastic fragments from its surface waters.
- 45Mato, Y.; Isobe, T.; Takada, H.; Kanehiro, H.; Ohtake, C.; Kaminuma, T. Plastic Resin Pellets as a Transport Medium for Toxic Chemicals in the Marine Environment. Environ. Sci. Technol. 2001, 35 (2), 318– 324, DOI: 10.1021/es001049845https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXosFyqt70%253D&md5=751d40a75427a1cea06bd8555aca2d0aPlastic Resin Pellets as a Transport Medium for Toxic Chemicals in the Marine EnvironmentMato, Yukie; Isobe, Tomohiko; Takada, Hideshige; Kanehiro, Haruyuki; Ohtake, Chiyoko; Kaminuma, TsuguchikaEnvironmental Science and Technology (2001), 35 (2), 318-324CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Plastic resin pellets (small granules 0.1-0.5 cm diam.) are widely distributed in the ocean worldwide. They are an industrial raw material for the plastic industry and are unintentionally released to the environment during manufg. and transport. They are sometimes ingested by seabirds and other marine organisms; their adverse effects on organisms are a concern. In this, polychlorinated biphenyls (PCB), DDE, and nonylphenols (NP) were detected in polypropylene (PP) resin pellets collected from 4 Japanese coasts. Concns. of PCB (4-117 ng/g), DDE (0.16-3.1 ng/g), and NP (0.13-16 μg/g) varied among sample site. Concns. were comparable to those for suspended particles and bottom sediment collected from the same area as the pellets. Field adsorption expts. using PP virgin pellets demonstrated a significant, steady increase in PCB and DDE concns. throughout a 6-day expt., indicating the source of PCB and DDE is ambient seawater and that adsorption to pellet surfaces is the mechanism of enrichment. The major source of NP in the marine PP resin pellets was thought to be plastic additives and/or their degrdn. products. Comparison of PCB and DDE concns. in marine PP resin pellets with those in seawater suggested their high degree of accumulation (apparent adsorption coeff.: 105-106). The high accumulation potential suggested that plastic resin pellets serve as a transport medium and a potential source of toxic chems. in the marine environment.
- 46Rios, L. M.; Moore, C.; Jones, P. R. Persistent Organic Pollutants Carried by Synthetic Polymers in the Ocean Environment. Mar. Pollut. Bull. 2007, 54 (8), 1230– 1237, DOI: 10.1016/j.marpolbul.2007.03.02246https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXotlKju7w%253D&md5=5d8f8b494e8d2390bc96fb0b9a0da4e3Persistent organic pollutants carried by synthetic polymers in the ocean environmentRios, Lorena M.; Moore, Charles; Jones, Patrick R.Marine Pollution Bulletin (2007), 54 (8), 1230-1237CODEN: MPNBAZ; ISSN:0025-326X. (Elsevier B.V.)Thermoplastic resin pellets are melted and formed into an enormous no. of inexpensive consumer goods, many of which are discarded after a relatively short period of use, dropped haphazardly onto watersheds and then make their way to the ocean where some get ingested by marine life. In 2003 and 2004 pre-prodn. thermoplastic resin pellets and post-consumer plastic fragments were collected and analyzed for contamination for persistent org. pollutants (POPs). Samples were taken from the North Pacific Gyre, and selected sites in California, Hawaii, and from Guadalupe Island, Mexico. The total concn. of PCBs was 27-980 ng/g, DDTs 22-7100 ng/g and PAHs 39-1200 ng/g, and aliph. hydrocarbons 1.1-8600 μg/g. Anal. methods were developed to ext., conc. and identify POPs that may have accumulated on plastic fragments and plastic pellets. The results confirm that plastic debris is a trap for POPs.
- 47Wang, F.; Shih, K. M.; Li, X. Y. The Partition Behavior of Perfluorooctanesulfonate (PFOS) and Perfluorooctanesulfonamide (FOSA) on Microplastics. Chemosphere 2015, 119, 841– 847, DOI: 10.1016/j.chemosphere.2014.08.04747https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhsVOmsb%252FM&md5=597ed4f5bad0f7c51ce06918be93b60fThe partition behavior of perfluorooctanesulfonate (PFOS) and perfluorooctanesulfonamide (FOSA) on microplasticsWang, Fei; Shih, Kai Min; Li, Xiao YanChemosphere (2015), 119 (), 841-847CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Microplastics have been recognized as transport vectors for heavy metals and org. pollutants to marine animals. Thus, the sorption behavior of contaminant on microplastic is crucial to their transport in marine system. In this study, the sorption behavior of PFOS and FOSA (two perfluorochems.) on three kinds of microplastics (PE, PS, and PVC) are reported. The isotherm study showed that the sorption of PFOS and FOSA on microplastics is highly linear, and it indicated that partition by hydrophobic interaction is the predominant sorption mechanism. The Kd values of FOSA on three kinds of microplastics are all higher than those of PFOS, and the reason is attributed to their different functional groups. The Kd value of FOSA on three types of microplastics followed the order as: PE > PVC > PS. Such finding may indicate that the mol. compn. and structure of microplastics play important roles in their sorption processes of org. pollutants. The PFOS sorption levels on PE and PS particles were increased with the increase of NaCl and CaCl2 concns., while the ion concns. have no effect on FOSA sorption. The study on the pH effects on PFOS and FOSA sorption indicated FOSA could partition under various pH conditions on three types of microplastics while PFOS sorption on PE and PS were favored with lower pH.
- 48Islam, N.; Garcia da Fonseca, T.; Vilke, J.; Gonçalves, J. M.; Pedro, P.; Keiter, S.; Cunha, S. C.; Fernandes, J. O.; Bebianno, M. J. Perfluorooctane Sulfonic Acid (PFOS) Adsorbed to Polyethylene Microplastics: Accumulation and Ecotoxicological Effects in the Clam Scrobicularia Plana. Marine Environmental Research 2021, 164, 105249, DOI: 10.1016/j.marenvres.2020.10524948https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhs1yhs74%253D&md5=64ca3fd9a72e84d1dd0e6bc3dd8476b1Perfluorooctane sulfonic acid (PFOS) adsorbed to polyethylene microplastics: Accumulation and ecotoxicological effects in the clam Scrobicularia planaIslam, Naimul; Garcia da Fonseca, Taina; Vilke, Juliano; Goncalves, Joanna M.; Pedro, Paulo; Keiter, Steffen; Cunha, Sara C.; Fernandes, Jose O.; Bebianno, M. J.Marine Environmental Research (2021), 164 (), 105249CODEN: MERSDW; ISSN:0141-1136. (Elsevier Ltd.)Microplastics are widespread in the marine environment, whereby the uptake of these tiny particles by organisms, can cause adverse biol. responses. Plastic debris also act as a vector of many contaminants, herein depending on type, size, shape and chem. properties, possibly intensifying their effects on marine organisms. This study aimed to assess the accumulation and potential toxicity of different sizes of microplastics with and without adsorbed perfluorooctane sulfonic acid (PFOS) in the clam Scrobicularia plana. Clams were exposed to low-d. polyethylene microplastics (1 mg L-1) of two different sizes (4-6 and 20-25μm) virgin and contaminated with PFOS (55.7 ± 5.3 and 46.1 ± 2.9μg g-1 resp.) over 14 days. Microplastic ingestion, PFOS accumulation and filtration rate were detd. along with a multi biomarker approach to assess the biol. effects of microplastics ingestion. Biomarkers include oxidative stress (superoxide dismutase, catalase, glutathione peroxidases), biotransformation enzymes (glutathione-S-transferases activity), neurotoxicity (acetylcholinesterase activity), oxidative damage and apoptosis. Microplastics ingestion and PFOS accumulation was microplastic size dependent but not PFOS dependent and filtration rate was reduced at the end of the exposure. Reactive oxygen species in gills and digestive gland were generated as a result of exposure to both types of microplastics, confirming the disturbance of the antioxidant system. Larger virgin microparticles lead to stronger impacts, when compared to smaller ones which was also supported by the Integrated Biomarker Responses index calcd. for both tissues. An anti-apoptotic response was detected in digestive glands under exposure to any of the MPs treatments.
- 49Brumovský, M.; Karásková, P.; Borghini, M.; Nizzetto, L. Per- and Polyfluoroalkyl Substances in the Western Mediterranean Sea Waters. Chemosphere 2016, 159, 308– 316, DOI: 10.1016/j.chemosphere.2016.06.01549https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XpvFaktbk%253D&md5=5b326d75056b5680640376ac78643802Per- and polyfluoroalkyl substances in the Western Mediterranean Sea watersBrumovsky, Miroslav; Karaskova, Pavlina; Borghini, Mireno; Nizzetto, LucaChemosphere (2016), 159 (), 308-316CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)The spatial and temporal distribution of per- and polyfluoroalkyl substances (PFASs) in the open Western Mediterranean Sea waters was investigated in this study for the first time. In addn. to surface water samples, a deep water sample (1390 m depth) collected in the center of the western basin was analyzed. Perfluorohexanoic acid (PFHxA), perfluoroheptanoic acid (PFHpA), perfluorooctanoic acid (PFOA), perfluorohexanesulfonate (PFHxS) and perfluorooctanesulfonate (PFOS) were detected in all samples and were the dominant PFASs found. The sum of PFAS concns. (ΣPFASs) ranged 246-515 pg/L for surface water samples. PFASs in surface water had a relatively homogeneous distribution with levels similar to those previously measured in the Atlantic near the Strait of Gibraltar, in water masses feeding the inflow to the Mediterranean Sea. Higher concns. of PFHxA, PFHpA and PFHxS were, however, found in the present study. Inflowing Atlantic water and river/coastal discharges are likely the major sources of PFASs to the Western Mediterranean basin. Slightly lower (factor of 2) ΣPFASs was found in the deep water sample (141 pg/L). Such a relatively high contamination of deep water is likely to be linked to recurring deep water renewal fed by downwelling events in the Gulf of Lion and/or Ligurian Sea.
- 50García-Gallardo, Á.; Grunert, P.; Piller, W. E. Variations in Mediterranean–Atlantic Exchange across the Late Pliocene Climate Transition. Climate of the Past 2018, 14 (3), 339– 350, DOI: 10.5194/cp-14-339-2018There is no corresponding record for this reference.
- 51Lyu, X.; Xiao, F.; Shen, C.; Chen, J.; Park, C. M.; Sun, Y.; Flury, M.; Wang, D. Per- and Polyfluoroalkyl Substances (PFAS) in Subsurface Environments: Occurrence, Fate, Transport, and Research Prospect. Reviews of Geophysics 2022, 60 (3), e2021RG000765 DOI: 10.1029/2021RG000765There is no corresponding record for this reference.
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