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Spatial, Phase, And Temporal Distributions of Perfluorooctane Sulfonate (PFOS) and Perfluorooctanoate (PFOA) in Tokyo Bay, Japan
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National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
* Corresponding author fax: +81 298 50 2920; e-mail: [email protected]
†Current address: Center for Marine Environmental Studies (CMES), Ehime University, Matsuyama, Japan.
‡Current address: Faculty of Fisheries, Nagasaki University, Nagasaki, Japan.
§Current address: Faculty of Agriculture, Ehime University, Matsuyama, Japan.
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Environmental Science & Technology

Cite this: Environ. Sci. Technol. 2010, 44, 11, 4110–4115
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https://doi.org/10.1021/es1007609
Published April 29, 2010

Copyright © 2010 American Chemical Society. This publication is licensed under these Terms of Use.

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Abstract

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The spatial distribution, partitioning, and time trends of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) were investigated in the water column and bottom sediment of Tokyo Bay, Japan, during 2004−2006. A total of 480 water and 60 sediment samples obtained by regular 20-station samplings ascertained the three-dimensional distributions of these compounds and changes in the seawater structure in the whole bay. The median of volume-based average water-borne concentrations of PFOS and PFOA was 3.7 and 12 ng/L, respectively. The median concentrations in sediment were 0.61 (PFOS) and 0.20 (PFOA) ng/g-dry. Vertical mixing of the water column probably affected the vertical distribution of these compounds. The negative correlations between PFOS and PFOA concentrations and water salinity and the horizontal distributions of their concentrations suggested that freshwater inputs into the bay were the source of these compounds. A mixing model estimated the average PFOS concentration in the freshwater inputs to be 29 ng/L. The common logarithm of the partition coefficients between the dissolved and suspended-particle-sorbed phases varied among samples, with the average of 4.2 (PFOS) and 3.5 (PFOA). Our analyses indicated no apparent time trends in the concentrations of these compounds during 2004−2006 in either the freshwater input or the bay.

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Synopsis

Seawater structure and freshwater inputs control PFOS and PFOA concentrations in Tokyo Bay. No time trends were observed in the concentrations during 2004−2006.

Introduction

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Perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) have been detected worldwide in humans (1, 2), wildlife (2, 3), ambient water (4-10), and aquatic sediment (11). These compounds have been a focus of concern because of their persistence in the environment (12), retention in human body (13), and toxicities (12, 14, 15). PFOS was recently added to the Stockholm Convention on Persistent Organic Pollutants list (16). These compounds are members of perfluorinated alkylated substances which have been produced for more than 50 years (12). Product applications developed using perfluorooctanesulfonyl fluoride (POSF) through formation of N-alkyl perfluorooctane sulfonamides have been used in surfactants and surface coatings and protections. These POSF-based products may have ultimately degraded or metabolized to PFOS (13). Salts of PFOA, particularly ammonium perfluorooctanoate, have been used as surfactants and processing aids in the production of fluoropolymers and fluoroelastomers (13).
The purpose of our study was to comprehensively elucidate the spatial distribution, partitioning, and time trends of PFOS and PFOA in the water column and bottom sediment of Tokyo Bay, Japan, during 2004−2006, based on quarterly samplings at 20 stations. Ambient water and bottom sediment may be appropriate media for monitoring levels of these compounds in the environment because of their relatively low vapor pressures and high water solubilities (12, 17). The Tokyo Bay area is one of the world’s most populous areas with many kinds of human activities (18). Elevated PFOS and PFOA concentrations have been reported in the bay and its inflowing rivers (4-9), but their detailed spatial distribution and partitioning in the bay have not been elucidated. Seasonal samplings are necessary to fully understand their three-dimensional distributions because the seawater structure of the bay changes seasonally (19, 20). The extent of mixing of bay water with freshwater inputs may affect the concentrations of these compounds in the bay. Spatial distributions and partitioning of these compounds are an essential basis for predicting their transfer to and potential effects on aquatic organisms, whose habitats are generally localized both horizontally and vertically in the bay (21). Their spatial distributions can also provide information on their probable sources. Time trends in the concentrations of these persistent compounds in the environment are of particular interest, but reports of their time trends in ambient water are scarce.

Materials and Methods

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Sampling

Twenty sampling stations were established that covered Tokyo Bay horizontally and vertically (Figure 1, Table 1). Tokyo Bay and its catchment area are described in the Supporting Information (SI). One-day sampling campaigns were conducted quarterly during 2004−2006, using two or three boats, on 19 February, 26 May, 22 August, and 28 October 2004; 24 February, 12 May, 17 August, and 26 October 2005; and 22 February, 17 May, 16 August, and 16 November 2006. Water samples were collected with GO-FLO Water Samplers (model 1080, General Oceanics, Inc., Miami, FL) at 10% and 90% of water depths, representing the upper and lower water layers at each sampling station, immediately transferred to a solvent-rinsed glass bottle, cooled during transport, and stored in a cool and dark place. They were normally extracted within four days. Surface sediment samples (about 5 cm depth) were collected by using Smith-MacIntyre grab samplers once each year (August) at the same stations, transferred to a stainless-steel container, cooled during transport, and stored at −20 °C. The sediment samples can be viewed as representing sedimentation of roughly 10 years before sampling, considering the sedimentation rates (22) and surface mixing in the bay. To demonstrate water sample variability, triplicate samples were obtained by repeated deployment of a sampler at each depth at st. 8 on 17 May 2006 and analyzed separately. Salinity and water temperature, which are important measures of water-column structure and freshwater mixing, were recorded at the sampling depths at each station with a conductivity, temperature and depth profiler (XR 420-CTD, RBR Ltd., ON, Canada; or Sonde 4a, HYDROLAB, Loveland, CO). Additionally, during the May, August, and November 2006 samplings, continuous vertical profiles of salinity and water temperature were recorded at st. 1−10. Suspicious salinity measurements were removed before data analysis. Seawater density was calculated (23) from the measured temperature and salinity.

Figure 1

Figure 1. Tokyo Bay and the sampling stations.

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Table 1. Sampling Stations, Water Depth, Suspended Solid (SS) Concentration in Water, Total Organic Carbon (TOC) Content in Sediment, and PFOS and PFOA Concentrations in the Upper (10% depth) and Lower (90% Depth) Water Layers and in Sedimenta
sampling stationlongitude (°N)latitude (°E)depth (m)SS upper (mg/L)SS lower (mg/L)TOC (mg/g-dry)PFOS upper (ng/L)PFOS lower (ng/L)PFOS sediment (ng/g-dry)PFOA upper (ng/L)PFOA lower (ng/L)PFOA sediment (ng/g-dry)
135.6172139.966711157.4226.33.50.7422150.35
235.5975140.0344128.38.2125.53.30.6325110.31
335.5900139.846712118.2239.03.90.4616110.22
435.5794139.8897148.57.4316.53.11.4149.20.29
535.5644139.9431166.66.5336.42.91.1169.10.27
635.5481139.9931177.28.0345.73.20.71169.70.26
735.5478139.826419118.6228.52.90.35167.70.17
835.5358139.858121107.8316.42.60.77157.90.23
935.5250139.8953229.17.3314.92.50.60173.50.21
1035.5033139.9531208.19.1335.22.60.66177.70.27
1135.4658139.7775328.07.5296.02.00.65164.80.11
12b35.4639139.8367318.18.4295.11.80.57174.30.16
1335.4500139.8725238.47.9274.42.00.55175.30.20
1435.4158139.7183378.210176.11.40.21162.90.11
1535.4083139.7614198.16.99.64.52.60.43175.00.39
1635.3856139.8150146.97.03.54.03.20.25138.60.11
1735.3528139.6881446.811185.21.00.31132.10.15
1835.3486139.7253267.16.53.33.32.20.13116.30.19
1935.3433c139.7753147.68.62.73.12.40.20126.60.19
2035.3103139.7167d528.06.27.34.70.880.13141.70.16
a

Medians of measured values among samplings during 2004−2006 are shown for depth, SS, TOC, PFOS, and PFOA.

b

35.4603°N, 139.8267°E in 2004 and February 2005.

c

35.3389°N in 2004 and February 2005.

d

139.7081°E in 2004 and February 2005.

Chemical Analysis

See SI for details (4, 5, 24). For determination of total (dissolved + particulate) concentrations of PFOS and PFOA in water, about 100 mL aliquots of the samples were filtered through a precombusted glass-fiber filter. The methanol extract of the freeze-dried filter was obtained by sonication and centrifuged, and the supernatant was concentrated. The filtrate and the concentrated supernatant were combined, spiked with labeled surrogate compound(s) in methanol (depending on the sampling date; 5 ng of sodium dodecyl-d25 sulfate, 1 ng of 13C2-labeled PFOA, or 1 ng each of13C4-labeled PFOS and 13C2-labeled PFOA), and then purified by using a C18 solid-phase extraction (SPE). The SPE eluate was concentrated and finally dissolved in 500 μL of 1:1 (v/v) methanol in Milli-Q water. For the separate determination of dissolved and particulate concentrations, about 500 mL aliquots of the water samples were filtered through a precombusted glass-fiber filter. The filtrate and filter were spiked with the surrogate compound(s), and then separately purified similarly as described above. Freeze-dried sediment samples of about 1.0 g-dry were extracted and purified by the same procedure used for the filter samples. All samples were acidified just prior to SPE. Identification and quantification were conducted by injecting an aliquot of the final concentrated extract into a liquid chromatograph (LC) connected to a triple-quadrupole-type tandem mass spectrometer equipped with a C18 LC column. Quantification was based on the internal standard method. Concentrations were reported when the signal-to-noise ratio (S/N) of the peak was >8. Phase-separated concentrations were measured in 62 samples (31 upper layer samples) collected at the May (n = 2), August (40), and November (20) 2006 samplings. Total concentrations are reported unless otherwise specified. Suspended solids (SS) were determined by passing the water sample through a precombusted glass-fiber filter and weighing the dried residue on the filter. The particulate organic carbon (POC) content in water and the organic carbon (OC) content in the sediment were measured with an elemental analyzer after removing inorganic carbonate with hydrochloric acid.

Data Quality Assurance and Quality Control

See SI for details. Analytical reproducibility and method recovery of PFOS and PFOA in the water and sediment samples were confirmed to be satisfactory. Method and sampling blanks were confirmed to be negligible. The agreement between the total concentration and the sum of the separately determined dissolved and particulate concentrations was good.

Data Analysis

Median values are adopted as representative of the central tendency of the observed concentrations, considering the data distribution (see Results). The difference in concentrations between the two layers was examined by the Wilcoxon signed rank test (i.e., sampling stations matched) against the null hypothesis that the central tendencies of the distributions were equal, and the associated Hodges−Lehmann estimator (25). To focus on relative horizontal spatial trends in each layer at each sampling, the 20 sampling stations were ranked in descending order according to the observed concentrations of each compound, and the ranks of each sampling station were averaged over the 12 water or three sediment samplings. These average ranks were used to assess the spatial distributions, in addition to the median concentrations at each sampling station. To assess the central tendency of ratios, the geometric mean and the 95% confidence interval (95% CI) based on the t-statistic of the log-transformed ratios were used. The 95% CI of population correlation coefficients was estimated by Fisher’s z transformation. These 95% CIs are indicated in square brackets. Statistical analyses were carried out with Microsoft Excel (ver. 2003, Microsoft, Redmond, WA), SPSS for Windows (ver. 15.0J, SPSS Inc., Chicago, IL), Statistica (ver. 7.1, StatSoft, Inc., Tulsa, OK), and StatXact (ver. 8, Cytel Inc., Cambridge, MA).
Linear regression analysis was conducted to assess the possible dependence of PFOS and PFOA concentrations on salinity: (1) where C, Cfresh, and Cocean are the concentration of PFOS or PFOA in each sample, in the freshwater inputs to the bay, and in Pacific Ocean water, respectively. αfresh and αocean are the respective ratios of freshwater and ocean water in the water samples (αfresh + αocean = 1). Equation 1 transforms to eq 2 by assuming that αocean equals salinity of each sample (S) divided by salinity of Pacific Ocean seawater (Socean). The parameters a0 and a1 in eq 2 were estimated by weighted least-squares (WLS) regression by using C−2 as the weight. (2) Equation 2 was then used to estimate Cfresh by setting S = 0 and Cocean by setting S = Socean. In this study, Socean was set to 35.5 because the maximum observed salinity in the bay was 35.4. Another least-squares regression without weighting (OLS) of log(PFOS concentration) was conducted against log(freshwater ratio (1 − S/Socean)) to confirm the WLS regression results.
To evaluate partitioning between the suspended-particle-sorbed (or OC-sorbed) and apparently dissolved phases, observed partition coefficients were calculated for particle−water (KPlinear, eq 3) and OC-water (KOClinear, eq 4), assuming linear relationships. (3) where Cparticulate (/kg dry matter) is the concentration in the particulate phase and Cdis (/L water) is the concentration in the apparently dissolved phase. Similarly, (4) where [OC] (−) is the OC content (dry mass basis) of the suspended particles.
Volume-based average concentrations of PFOS and PFOA in Tokyo Bay water were calculated by taking into account their three-dimensional distributions and the seawater structure of the bay. The total mass of each compound in the bay water was first estimated, and then divided by the volume of water in the bay. The mass of each compound in the bay water was estimated by dividing the bay horizontally into 500 × 500 m grid squares and coastal subareas, and vertically into two layers corresponding to the upper and lower layer samples, and by summing the masses present in each grid square or subarea. The water column was divided into two layers when stratification was present, by using observed and reported vertical density profiles (19, 26-28). PFOS and PFOA concentrations and pycnocline depth at the closest sampling station were assigned to each grid square or subarea. See SI for details. The total mass of each compound in the water column was divided by the estimated water residence-time in the bay (1.0−1.6 months ( (19, 29))) to estimate their fluxes through the water column. Their sedimentation fluxes were calculated by multiplying the concentrations in the sediment by the reported sedimentation rates in the bay (22).

Results

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Concentration

Table 1 shows the median values at each sampling station of the SS concentration in water, the total organic carbon (TOC) content in sediment, and the PFOS and PFOA concentrations in the upper and lower water layers and sediment. SI Figure S1 shows the data distributions of the PFOS and PFOA concentrations in the upper and lower layers of the water column and in the sediment. The data distributions in normal scale have a long tail to higher values but are roughly symmetrical in log scale. As the median concentrations of both compounds were clearly higher in the upper water layer than in the lower layer (SI Figure S1), data from the two layers were analyzed separately. The median concentrations (range) were PFOS, upper layer, 5.5 ng/L (0.78−17), and lower layer, 2.5 ng/L (not detected [ND]-14); PFOA, upper layer, 16 ng/L (2.7−63), and lower layer, 6.2 ng/L (0.29−35); PFOS, sediment, 0.61 ng/g-dry (0.062−3.6); and PFOA, sediment, 0.20 ng/g-dry (ND-1.4). In the lower layer, log(PFOS concentration) and log(PFOA concentration) were relatively highly correlated (r = 0.83 [0.79−0.87], n = 240) compared with the other correlations between the log concentrations of each compound in each layer (0.22−0.55).
The variability, including both sampling and analytical variability, was demonstrated to be roughly 10% in the water data, as the three consecutive deployment of the water sampler yielded coefficient of variation (CV) in concentration of 2.1% (average = 7.5 ng/L), 6.2% (3.1 ng/L), 3.2% (36 ng/L), and 12% (17 ng/L) for PFOS in the upper and lower layers and PFOA in the upper and lower layers, respectively. In the case of one PFOS ND value in water and four PFOA ND values in sediment, the detection limits (S/N = 8) were estimated to be about 0.4 ng/L and 0.05−0.08 ng/g-dry, respectively. Half the detection limit was assigned to these ND values when necessary in the data analysis.

Spatial Distributions

Observed differences in the density of seawater between the upper and the lower layers indicate the extent of stratification of the water column (SI Figure S2). The lower density of the upper layer was most pronounced in August, followed May, consistent with previous reports of seasonal changes in the seawater structure in the bay, and reflecting greater dilution of the salinity by freshwater from inflowing rivers and heating of the water’s surface in warmer seasons (19, 20).
The ranges of PFOS and PFOA concentrations in each layer as well as differences in the concentrations between the two layers were shown in Figure 2. Their concentrations in the upper layer were statistically significantly higher (p < 0.05, n = 20) than those in the lower layer at each of the 12 samplings, except for PFOS in November 2006 and PFOA in February 2005 at which the concentrations in the two layers were comparable. In addition, larger differences in PFOS and PFOA concentrations were observed between the two layers along with larger differences in seawater densities between the layers, particularly in August and May (Figure 2 and SI Figure S2), consistent with the greater stratification of the water column in August and May. The range of concentrations in the water column was 3.9, 6.4, 4.8, and 12 for PFOS in the upper layer, PFOS in the lower layer, PFOA in the upper layer, and PFOA in the lower layer, respectively, as represented by the median among the 12 samplings of the maximum-to-minimum concentration ratio at the 20 stations.

Figure 2

Figure 2. Seasonal distributions of PFOS (a) and PFOA (b) concentrations in the upper and lower layers of the water column of Tokyo Bay. Each point represents one sample. Horizontal offsets were chosen arbitrarily to minimize overlap of the points. For each sampling, the upper layer data (open symbols) are plotted on the left and the lower layer data (closed symbols) on the right. ND (⊕) is plotted as the detection limit of the sample.

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The concentrations of PFOS and PFOA were generally higher at northern sampling stations (st. 1−10) (SI Figure S3). For both compounds in both layers, the three highest-ranking stations were among st. 1−11, and the three lowest-ranking stations were among st. 14−20. For both compound in the lower layer, the three highest-ranking stations were st. 4 or more northern stations, whereas in the upper layer, they were st. 11 or more northern stations. In the upper layer, PFOS concentrations during each sampling were higher at the northwestern stations (3, 7, and 11, in descending order of concentration), whereas PFOA concentrations were higher at the northeastern stations (2, 1, and 10). PFOS and PFOA concentrations in sediment were also generally higher at the northern sampling stations. However, correlations of the log concentrations of the two compounds between the sediment and the lower water layer were weak (PFOS, r = 0.39 [0.15−0.59], n = 60; PFOA, r = 0.42 [0.18−0.62], n = 56). The highest-ranking stations for PFOS concentrations in sediment were st. 4 and 5, which were different from those for PFOS concentrations in the lower layer water (st. 3 and 1). These relative horizontal trends based on the average ranks generally accord with the horizontal trends based on median concentrations (Table 1).
PFOS concentrations in both layers of the water column showed a clear increasing trend (r = 0.78 [0.73−0.81], log−log scale, n = 405) in relation to the freshwater ratio (1 − S/Socean) (Figure 3). The WLS regression of PFOS concentration against salinity (n = 405) yielded [PFOS concentration/(ng L−1)] = (29.2 ± 2.6) − (0.823 ± 0.077) × salinity (parameters: point estimates ± half of 95% CI). PFOS Cfresh was determined to be 29 ng/L [27−32], and Cocean to be close to zero (−0.011 ng/L [−0.14 to 0.12]), by extrapolation. Similar regressions for the seasonal data suggested that PFOS Cfresh was higher in winter (February) (48 ng/L versus about 29−32 ng/L in other seasons). The regression result for log(PFOS concentration) against log(freshwater ratio) supported these results by yielding an extrapolated PFOS Cfresh of 23 ng/L [20−27] (Figure 3), with similar differences among seasons. Yearly regression estimates of Cfresh were inconsistent between the two regression methods (WLS and OLS of log concentrations); the former suggested slightly higher Cfresh in 2006, whereas the latter suggested that Cfresh was highest in 2005. Although PFOA concentrations also tended to increase as the freshwater ratio increased, the correlation was lower (r = 0.57 [0.50−0.63], log−log scale) and the data were more scattered.

Figure 3

Figure 3. Relationship between the PFOS concentration and the freshwater ratio (FWR = 1 − ((sample salinity)/(Pacific Ocean seawater salinity))) in the water column. Open and closed symbols indicate upper and lower water layer samples, respectively. Circles, triangles, and squares indicate samples collected in 2004, 2005, and 2006, respectively. Blue, green, pink, and brown indicate samples collected in winter (February), spring (May), summer (August), and autumn (October or November), respectively. The equation of the regression line is log[PFOS concentration/(ng L−1)] = (1.36 ± 0.07) − (0.738 ± 0.059) × log FWR (parameters: point estimates ± half of 95% CI).

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Partitioning

Partition coefficients were calculated for the 58 and 49 samples with detected concentrations in both phases, for PFOS and PFOA, respectively. These partition coefficients varied by more than 1 order of magnitude among samples. For PFOS and PFOA, logKPlinear ranged 3.4−5.0 (log of the geometric mean, 4.2) and 2.7−4.2 (3.5), respectively, and logKOClinear from 4.5−5.9 (5.2) and from 3.4−5.5 (4.5), respectively (SI Figure S4). KOC values were calculated under the assumption that these compounds were predominantly sorbed to the OC fraction of the particles. In November 2006, the water column was more vertically mixed, compared with the more stratified water column in May and August 2006. Therefore, the partition coefficients of samples from November 2006 may reflect more homogeneous conditions. The partition coefficients for this data subset (PFOS, n = 16; PFOA, n = 8; water temperature, 17.2−18.9 °C) did fall within a narrower range, but the median values were similar to those of the whole data set (see SI Figure S4).

Volume-Based Average Concentrations in the Water Column, And Fluxes through the Bay

The volume-based average concentrations of PFOS ranged 1.9−5.9 (median of 12 samplings, 3.7) ng/L and that of PFOA ranged 2.7−22 (median, 12) ng/L, whereas the mass of PFOS in the bay ranged 29−87 (median, 54) kg and that of PFOA 40−320 (median, 170) kg (Figure 4). The volume-based average concentrations of the two compounds changed similarly over time (r = 0.71 [0.23−0.91], n = 12), but neither showed any apparent or statistically significant linear trend in relation to time (n = 12; PFOS, r = −0.14 [−0.66 to 0.47]; PFOA, r = −0.24 [−0.71 to 0.39]). The estimated fluxes of PFOS and PFOA through the water column of Tokyo Bay were 210−1000 and 300−3900 kg/y, respectively, which were about 2−3 orders of magnitude higher than the sedimentation fluxes in the bay (0.84−4.2 and 0.23−0.83 kg/y, respectively).

Figure 4

Figure 4. Time series of masses and volume-based average concentrations of PFOS (a) and PFOA (b) in the water column of Tokyo Bay. Error bars indicate uncertainty due to assignment of pycnocline depth as well as that due to sampling and analytical variability.

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Discussion

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This study elucidated the three-dimensional distributions of PFOS and PFOA in the whole bay taking into account the seasonal change in the seawater structure. 480 measurements were obtained from the water column and 60 from the sediment of Tokyo Bay for each of these compounds, among which only five were ND values. This comprehensive data set thus provides a basis for evaluating potential risks associated with these compounds in the aquatic environment of the bay. Previously reported concentrations of these compounds in Tokyo Bay (4-7) are within or close to the ranges observed in our study. All data analyses in this study assumed no degradation of the two compounds in the bay.
The correlations between [PFOS or PFOA concentration difference between the upper and lower layers] and [the density difference between the two layers] suggest that water column stratification or vertical mixing affects the vertical distributions of these compounds. The concentrations in the upper layer, however, were generally higher than those in the lower layer (although the difference was smaller), even when no vertical density gradient was present (e.g., at most stations at the February samplings), probably reflecting fresh water input into the upper layer and still incomplete vertical mixing.
The higher concentrations in the upper layer and at more northern stations suggest that these compounds enter the bay at its northern part and are input mainly into the upper layer. This inference is supported by the reported considerable input of these compounds via inflowing rivers and effluent of sewage treatment plants (STPs) (7, 8) mainly into the northern part of the bay. The higher PFOA concentrations in the northeastern part of the bay suggest that the geographical source distribution of PFOA or its behavior may be different from those of PFOS. North to south concentration gradients in the water column and sediment of Tokyo Bay have also been reported for other persistent organic chemicals of anthropogenic origin (dioxins (18), fluorescent whitening agents (20), and polychlorinated biphenyls (30)), so this horizontal distribution may be characteristic for such compounds in Tokyo Bay.
Our simple mixing model (eq 1) provided valuable information regarding the average concentration of PFOS and its seasonal change in the freshwater inputs to Tokyo Bay. The model assumes that the concentrations of PFOS or PFOA in each sample (C) result from mixing of freshwater and ocean water inputs in the bay. The conservative behavior of salinity and the persistence of PFOS and PFOA support the use of this model. The concentration of a compound in freshwater (Cfresh) represents the average of its concentration in the various freshwater inputs. Salinity, or the freshwater ratio, represents the extent of mixing of seawater with freshwater. Thus, the negative correlation between the PFOS concentration and salinity indicates that freshwater inputs were the predominant source of PFOS to the bay. The estimated PFOS Cfresh falls within its reported concentration ranges in rivers flowing into Tokyo Bay (2.1−140 ng/L) (5, 7-10), and within its concentration range in effluent from the STPs on the shore of the bay (17−1100 ng/L; Serizawa et al., National Institute for Environmental Studies, unpublished data). No data on seasonal differences in the PFOS concentrations of waters flowing into Tokyo Bay are available, however, if the PFOS load from the catchment is relatively constant, the lower water flow in winter due to lower precipitation would account for the higher estimated concentration in the freshwater input in winter. Our regression result for PFOS Cocean is consistent with the reported low concentrations in ocean water not affected by Tokyo Bay (40−75 pg/L in the offshore of Japan (6)). The similar trend of PFOA against salinity to that of PFOS and the similar trend between PFOS and PFOA over time suggest that these compounds in Tokyo Bay share a common major source. The greater variability of the PFOA concentration against the freshwater ratio may reflect a wider spatial distribution of emission sources or a higher variability in the emission rate.
Variability in particulate matter composition and the extent to which equilibrium had been obtained in the sampled waters may account for the variation in partition coefficients between dissolved and suspended-particle-sorbed phases. The partition coefficients of PFOS and PFOA in ambient seawater obtained in this study were several orders of magnitude higher than previously reported limited number of values measured using environmental samples. Odaka and Masunaga (7) reported a field-observed PFOS log Kd of 2.8 (Kd = 600 L/kg) in Tokyo Bay (we compared reported Kd values with our KPlinear values). The difference from our results is primarily due to the lower particulate-phase concentrations in their study (dissolved concentrations and SS levels were comparable). Since their samples used for Kd calculations were collected near the mouths of major inflowing rivers, their lower Kd values may reflect particular conditions in these rivers on the sampling day. Even lower partition coefficients (PFOS log Kd, 0.88 (31); PFOS log KOC, 2.4−2.7 (31, 32) PFOA log KOC, 2.11 (32)) have been obtained in experiments using freshwater sediments. However, these experimental values may not be directly comparable to ours because of the much higher ranges of concentrations used in these laboratory experiments (about 103−106 higher dissolved concentrations than those observed in this study), and the difference in cation concentrations (e.g., [Ca2+]) (32) between freshwater and seawater. It is interesting to note that PFOS and PFOA concentrations at the August 2006 sampling in the lower layer per particulate mass were respectively roughly 68 (geometric mean) (range, 9.5−780) and 82 (12−340) times those in the bottom sediment collected at the same station at the same time, and respectively 16 (4.4−59) and 20 (4.2−180) times on an OC basis, possibly reflecting differences in source or composition between sediment particles and suspended particulate matter.
Our results showed no apparent trend in the concentration of either compound in the freshwater input or the bay with time. This lack of a linear trend in PFOS during the 12 seasons is consistent with the PFOS Cfresh regression results showing no consistent yearly trend. No governmental regulations have been implemented on these compounds in Japan until 2009. Few domestic records of their industrial production, import, or emission are available. Since the fluxes of PFOS and PFOA through the water column were much higher than their sedimentation fluxes, the water column may be the more appropriate medium in which to monitor the levels of these compounds in Tokyo Bay. The potential relationships of the concentrations of these compounds with the stratification of the water column in Tokyo Bay and with the freshwater inputs as indicated by the salinity should be taken into account in the interpretation of such monitoring results. Investigation of degradation rates in the aquatic environment of precursor compounds of PFOS and PFOA may be necessary for a more precise evaluation of their fluxes and partitioning therein.

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Author Information

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  • Corresponding Author
    • Takeo Sakurai - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan;  Email: [email protected]
  • Authors
    • Shigeko Serizawa - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Tomohiko Isobe - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Jun Kobayashi - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Keita Kodama - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Gen Kume - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Jeong-Hoon Lee - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Hideaki Maki - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Yoshitaka Imaizumi - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Noriyuki Suzuki - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Toshihiro Horiguchi - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Masatoshi Morita - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan
    • Hiroaki Shiraishi - National Institute for Environmental Studies, Onogawa 16-2, Tsukuba, Ibaraki 305-8506, Japan

Acknowledgment

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Dr. Tomohiro Nishikawa, Mr. Masashi Hirota, and Mr. Masaaki Oyama helped in the sampling. Ms Izumi Hirai helped in the chemical analysis.

References

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This article references 32 other publications.

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    Since the early 1980s, there has been a steady increase in the use of nonvolatile fluorinated org. compds. for a variety of industrial and com. applications. The industrial use of these relatively stable compds. has initiated debate over the fate of fluorochems. in the environment and, ultimately, the bioavailability of these compds. In this manuscript, we present quant. results from a study of 65 human sera samples purchased from biol. supply companies that provide characterization of specific org. fluorochems. present in the sera of nonindustrially exposed humans. Summed together, the compd.-specific characterization data reported here agree closely with levels of nonspeciated org. fluorine that were originally reported to be present in sera in 1970. The compd.-specific method for the extn. of extremely low levels of several com. org. fluorochems. from sera and liver with quant. detection by neg. ion electrospray tandem mass spectrometry described represents a robust, previously undescribed approach to quantifying specific org. fluorochems. in biol. matrixes.
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    The global distribution of perfluorooctanesulfonate (PFOS), a fluorinated org. contaminant. PFOS measured in the tissues of wildlife, including, fish, birds, and marine mammals is reported. Some of the species studied include bald eagles, polar bears, albatrosses, and various species of seals. Samples were collected from urbanized areas in North America, esp. the Great Lakes region and coastal marine areas and rivers, and Europe. Samples were also collected from a no. of more remote, less urbanized locations such as the Arctic and the North Pacific Oceans. The results demonstrated that PFOS is widespread in the environment. Concns. of PFOS in animals from relatively more populated and industrialized regions, such as the North American Great Lakes, Baltic Sea, and Mediterranean Sea, were greater than those in animals from remote marine locations. Fish-eating, predatory animals such as mink and bald eagles contained concns. of PFOS that were greater than the concns. in their diets. This suggests that PFOS can bioaccumulate to higher trophic levels of the food chain. Currently available data indicate that the concns. of PFOS in wildlife are less than those required to cause adverse effects in lab. animals.
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    Journal of Occupational Health (2004), 46 (1), 49-59CODEN: JOCHFV; ISSN:1341-9145. (Japan Society for Occupational Health)
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    Perfluorochems. (PFCs) are the subject of increasingly intense environmental research. Despite their detection both in biota and in aq. systems, little attention was paid to the possible presence of this class of compds. in solid environmental matrixes. The limited available data indicate that some PFCs such as perfluorooctane sulfonate (PFOS) may strongly sorb to solids, and sewage sludge is widely suspected as a major sink of PFCs entering municipal waste streams. A quant. anal. method was developed that consists of liq. solvent extn. of the analytes from sediments and sludge, cleanup via solid-phase extn., and injection of the exts. with internal stds. into a HPLC system coupled to a tandem mass spectrometer (LC/MS/MS). The limits of detections of the method were analyte and matrix dependent, but ranged from 0.7 to 2.2 ng/g and 0.041 to 0.246 ng/g (dry wt.) for sludge and sediment, resp. A demonstration of the method was performed by conducting a limited survey of domestic sludge and sediments. The concn. of PFCs in domestic sludge ranged from 5 to 152 ng/g for total perfluorocarboxylates and 55 to 3370 ng/g for total perfluoroalkyl sulfonyl-based chems. Data from a survey of San Francisco Bay Area sediments suggest widespread occurrence of PFCs in sediments at the low ng/g to sub-ng/g level. Also, substances that may be transformed to PFOS, such as 2-(N-ethylperfluorooctanesulfonamido) acetic acid (N-EtFOSAA) and 2-(N-methylperfluorooctanesulfonamido) acetic acid (N-MeFOSAA), are present in both sediments and sludge at levels often exceeding PFOS.
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  • Figure 1

    Figure 1. Tokyo Bay and the sampling stations.

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    Figure 2

    Figure 2. Seasonal distributions of PFOS (a) and PFOA (b) concentrations in the upper and lower layers of the water column of Tokyo Bay. Each point represents one sample. Horizontal offsets were chosen arbitrarily to minimize overlap of the points. For each sampling, the upper layer data (open symbols) are plotted on the left and the lower layer data (closed symbols) on the right. ND (⊕) is plotted as the detection limit of the sample.

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    Figure 3

    Figure 3. Relationship between the PFOS concentration and the freshwater ratio (FWR = 1 − ((sample salinity)/(Pacific Ocean seawater salinity))) in the water column. Open and closed symbols indicate upper and lower water layer samples, respectively. Circles, triangles, and squares indicate samples collected in 2004, 2005, and 2006, respectively. Blue, green, pink, and brown indicate samples collected in winter (February), spring (May), summer (August), and autumn (October or November), respectively. The equation of the regression line is log[PFOS concentration/(ng L−1)] = (1.36 ± 0.07) − (0.738 ± 0.059) × log FWR (parameters: point estimates ± half of 95% CI).

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    Figure 4

    Figure 4. Time series of masses and volume-based average concentrations of PFOS (a) and PFOA (b) in the water column of Tokyo Bay. Error bars indicate uncertainty due to assignment of pycnocline depth as well as that due to sampling and analytical variability.

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  • References

    This article references 32 other publications.

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      Compound-Specific, Quantitative Characterization of Organic Fluorochemicals in Biological Matrices
      Hansen, Kristen J.; Clemen, Lisa A.; Ellefson, Mark E.; Johnson, Harold O.
      Environmental Science and Technology (2001), 35 (4), 766-770CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Since the early 1980s, there has been a steady increase in the use of nonvolatile fluorinated org. compds. for a variety of industrial and com. applications. The industrial use of these relatively stable compds. has initiated debate over the fate of fluorochems. in the environment and, ultimately, the bioavailability of these compds. In this manuscript, we present quant. results from a study of 65 human sera samples purchased from biol. supply companies that provide characterization of specific org. fluorochems. present in the sera of nonindustrially exposed humans. Summed together, the compd.-specific characterization data reported here agree closely with levels of nonspeciated org. fluorine that were originally reported to be present in sera in 1970. The compd.-specific method for the extn. of extremely low levels of several com. org. fluorochems. from sera and liver with quant. detection by neg. ion electrospray tandem mass spectrometry described represents a robust, previously undescribed approach to quantifying specific org. fluorochems. in biol. matrixes.
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      Houde, M.; Martin, J. W.; Letcher, R. J.; Solomon, K. R.; Muir, D. C. G. Biological monitoring of polyfluoroalkyl substances: A review Environ. Sci. Technol. 2006, 40, 3463– 3473
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      Biological Monitoring of Polyfluoroalkyl Substances: A Review
      Houde, Magali; Martin, Jonathan W.; Letcher, Robert J.; Solomon, Keith R.; Muir, Derek C. G.
      Environmental Science & Technology (2006), 40 (11), 3463-3473CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      A review. Polyfluoroalkyl substances (PFSs) are used in industrial and com. products and can degrade to persistent perfluorocarboxylates (PFCAs) and perfluoroalkyl sulfonates (PFSAs). Temporal trend studies using human, fish, bird, and marine mammal samples indicate that exposure to PFSs has increased significantly over the past 15-25 years. This review summarizes the biol. monitoring of PFCAs, PFSAs, and related PFSs in wildlife and humans, compares concns. and contamination profiles among species and locations, evaluates the bioaccumulation/biomagnification in the environment, discusses possible sources, and identifies knowledge gaps. PFSs can reach elevated concns. in humans and wildlife inhabiting industrialized areas of North America, Europe, and Asia (2-30 000 ng/mL or ng/g of wet wt. (ww)). PFSs have also been detected in organisms from the Arctic and mid-ocean islands (≤3000 ng/g ww). In humans, PFSAs and PFCAs have been shown to vary among ethnic groups and PFCA/PFSA profiles differ from those in wildlife with high proportions of perfluorooctanoic acid and perfluorooctane sulfonate. The pattern of contamination in wildlife varied among species and locations suggesting multiple emission sources. Food web analyses have shown that PFCAs and PFSAs can bioaccumulate and biomagnify in marine and freshwater ecosystems. Knowledge gaps with respect to the transport, accumulation, biodegrdn., temporal/spatial trends and PFS precursors have been identified. Continuous monitoring with key sentinel species and standardization of anal. methods are recommended.
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      Giesy, J. P.; Kannan, K. Global distribution of perfluorooctane sulfonate in wildlife Environ. Sci. Technol. 2001, 35, 1339– 1342
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      Global distribution of perfluorooctane sulfonate in wildlife
      Giesy, John P.; Kannan, Kurunthachalam
      Environmental Science and Technology (2001), 35 (7), 1339-1342CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The global distribution of perfluorooctanesulfonate (PFOS), a fluorinated org. contaminant. PFOS measured in the tissues of wildlife, including, fish, birds, and marine mammals is reported. Some of the species studied include bald eagles, polar bears, albatrosses, and various species of seals. Samples were collected from urbanized areas in North America, esp. the Great Lakes region and coastal marine areas and rivers, and Europe. Samples were also collected from a no. of more remote, less urbanized locations such as the Arctic and the North Pacific Oceans. The results demonstrated that PFOS is widespread in the environment. Concns. of PFOS in animals from relatively more populated and industrialized regions, such as the North American Great Lakes, Baltic Sea, and Mediterranean Sea, were greater than those in animals from remote marine locations. Fish-eating, predatory animals such as mink and bald eagles contained concns. of PFOS that were greater than the concns. in their diets. This suggests that PFOS can bioaccumulate to higher trophic levels of the food chain. Currently available data indicate that the concns. of PFOS in wildlife are less than those required to cause adverse effects in lab. animals.
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    4. 4
      Taniyasu, S.; Kannan, K.; Horii, Y.; Hanari, N.; Yamashita, N. A survey of perfluorooctane sulfonate and related perfluorinated organic compounds in water, fish, birds, and humans from Japan Environ. Sci. Technol. 2003, 37, 2634– 2639
      4
      A Survey of Perfluorooctane Sulfonate and Related Perfluorinated Organic Compounds in Water, Fish, Birds, and Humans from Japan
      Taniyasu, Sachi; Kannan, Kurunthachalam; Horii, Yuichi; Hanari, Nobuyasu; Yamashita, Nobuyoshi
      Environmental Science and Technology (2003), 37 (12), 2634-2639CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Occurrence of perfluorooctanesulfonate (PFOS) in the tissues of humans and wildlife is well documented. In this study, concns. and distribution of PFOS, perfluorohexanesulfonate (PFHS), and perfluorobutanesulfonate (PFBS) were detd. in samples of surface water, fish and bird blood and livers, and human blood collected in Japan. Notable concns. of PFOS were found in surface water and fish from Tokyo Bay, Japan. PFOS was found in all of the 78 samples of fish blood and liver analyzed. Based on the concns. of PFOS in water and in fish livers, bioconcn. factors were calcd. to range from 274 to 41,600. The concns. of PFOS in the blood of Japanese human volunteers ranged from 2.4 to 14 ng/mL. PFHS was detected in 33% of the fishes analyzed, at concns. severalfold less than those of PFOS.
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    5. 5
      Saito, N.; Harada, K.; Inoue, K.; Sasaki, K.; Yoshinaga, T.; Koizumi, A. Perfluorooctanoate and perfluorooctane sulfonate concentrations in surface water in Japan J. Occup. Health 2004, 46, 49– 59
      5
      Perfluorooctanoate and perfluorooctane sulfonate concentrations in surface water in Japan
      Saito, Norimitsu; Harada, Kouji; Inoue, Kayoko; Sasaki, Kazuaki; Yoshinaga, Takeo; Koizumi, Akio
      Journal of Occupational Health (2004), 46 (1), 49-59CODEN: JOCHFV; ISSN:1341-9145. (Japan Society for Occupational Health)
      Perfluorooctanoate (PFOA) and perfluorooctane sulfonate (PFOS) are synthetic surfactants used in Japan. An epidemiol. study of workers exposed to PFOA showed a significant increase in prostate cancer mortality. A cross-sectional study of PFOA-exposed workers showed PFOA perturbed sex hormone homeostasis. Concns. of these pollutants in surface water collected throughout Japan were detd. by LC/mass spectrometry following solid phase extn. Lowest limits of detection (LOD, ng/L) were 0.06 for PFOA and 0.04 for PFOS. Lowest limits of quantification (LOQ, ng/L) were 0.1 for both analytes. Levels (geometric mean [GM]; geometric std. deviation [GS], ng/L) of PFOA and PFOS in surface water were GM (GS): 0.97 (3.06) and 1.19 (2.44) for Hokkaido-Tohoku (n = 16); 2.84 (3.56) and 3.69 (3.93) for Kanto (n = 14); 2.50 (2.23) and 1.07 (2.36) for Chubu (n = 17); 21.5 (2.28) and 5.73 (3.61) for Kinki (n = 8); 1.51 (2.28) and 1.00 (3.42) for Chugoku (n = 9); and 1.93 (2.40) and 0.89 (3.09) for Kyushu-Shikoku (n = 15). PFOA GM in Kinki was significantly higher than in other areas (ANOVA, p <0.01). Systematic searches of Yodo and Kanzaki rivers showed 2 highly polluted sites, a public water disposal site for PFOA, and an airport for PFOS. The former was estd. to release 18 kg PFOA/day. PFOA in drinking water in Osaka [40 (1.07) ng/L] was significantly higher than in other areas. Results confirmed that recognizable concns. of PFOA are released in the Osaka area and that people are exposed to PFOA via drinking water ingestion.
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    6. 6
      Yamashita, N.; Kannan, K.; Taniyasu, S.; Horii, Y.; Petrick, G.; Gamo, T. A global survey of perfluorinated acids in oceans Mar. Pollut. Bull. 2005, 51, 658– 668
      6
      A global survey of perfluorinated acids in oceans
      Yamashita, Nobuyoshi; Kannan, Kurunthachalam; Taniyasu, Sachi; Horii, Yuichi; Petrick, Gert; Gamo, Toshitaka
      Marine Pollution Bulletin (2005), 51 (8-12), 658-668CODEN: MPNBAZ; ISSN:0025-326X. (Elsevier B.V.)
      Perfluorinated acids and their salts have emerged as an important class of global environmental contaminants. Biol. monitoring surveys conducted using tissues of marine organisms reported the occurrence of perfluorooctanesulfonate (PFOS) and related perfluorinated compds. in biota from various seas and oceans, including the Arctic and the Antarctic Oceans. Occurrence of perfluorinated compds. in remote marine locations is of concern and indicates the need for studies to trace sources and pathways of these compds. to the oceans. Detn. of sub-parts-per-trillion (ng/L) or parts-per-quadrillion (pg/L) concns. of aq. media was impeded by relatively high background levels arising from procedural or instrumental blanks. The research group has developed a reliable and highly sensitive anal. method by which to monitor perfluorinated compds. in oceanic waters. The method developed is capable of detecting PFOS, perfluorohexanesulfonate (PFHS), perfluorobutanesulfonate (PFBS), perfluorooctanoate (PFOA), perfluorononanoate (PFNA), and perfluorooctanesulfonamide (PFOSA) at a few pg/L in oceanic waters. The method was applied to seawater samples collected during several international research cruises undertaken during 2002-2004 in the central to eastern Pacific Ocean (19 locations), South China Sea and Sulu Seas (5), north and mid Atlantic Ocean (12), and the Labrador Sea (20). An addnl. 50 samples of coastal seawater from several Asian countries (Japan, China, Korea) were analyzed. PFOA was found at levels ranging from several thousands of pg/L in water samples collected from coastal areas in Japan to a few tens of pg/L in the central Pacific Ocean. PFOA was the major contaminant detected in oceanic waters, followed by PFOS. Further studies are being conducted to elucidate the distribution and fate of perfluorinated acids in oceans.
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    7. 7
      Odaka, R.; Masunaga, S. Environmental behavior of perfluorinated surfactants in Tokyo Bay J. Jpn. Soc. Water Environ. 2006, 29, 221– 228

      (in Japanese)

      7
      Environmental behavior of perfluorinated surfactants in Tokyo Bay
      Odaka, Ryosuke; Masunaga, Shigeki
      Mizu Kankyo Gakkaishi (2006), 29 (4), 221-228CODEN: MKGAEY; ISSN:0916-8958. (Nippon Mizu Kankyo Gakkai)
      The perfluorinated surfactants, perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) have been reported to be present in the environment. Their behavior in the environmental, however, is still unknown. We measured their concns. in seawater and sediment from Tokyo Bay and in the waters of 6 major rivers that run into the bay. Then, their mass balances and behavior in the bay were estd. PFOS and PFOA existed mainly in the dissolved phase in water. The estd. annual input of PFOS from the rivers was 74-346 Kg/yr, which was similar to the total amt. of PFOS outflow to the ocean (20-350 Kg/yr) and the amt. of PFOS sedimentation to the bottom of the bay (1.3 Kg/yr). On the other hand, the estd. annual input of PFOA from the rivers was 29-148 Kg/yr, which was much smaller than the total amt. of PFOA outflow to the ocean (140-1900 Kg/yr). The amt. of PFOA sedimentation was estd. to be negligible. These results suggest that the major source of PFOS in the bay is riverine transport. The results also indicate the existence of unknown PFOA sources around the coast of the bay and/or the possibility of a significant PFOA atm. deposition to the bay. The sediment was not a significant sink for the 2 compds. Their environmental behavior, therefore, is quite different from that of persistent organochlorine compds.
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    8. 8
      Murakami, M.; Imamura, E.; Shinohara, H.; Kiri, K.; Muramatsu, Y.; Harada, A.; Takada, H. Occurrence and sources of perfluorinated surfactants in rivers in Japan Environ. Sci. Technol. 2008, 42, 6566– 6572
      There is no corresponding record for this reference.
    9. 9
      Zushi, Y.; Takeda, T.; Masunaga, S. Existence of nonpoint source of perfluorinated compounds and their loads in the Tsurumi River basin, Japan Chemosphere 2008, 71, 1566– 1573
      There is no corresponding record for this reference.
    10. 10
      Takazawa, Y.; Nishino, T.; Sasaki, Y.; Yamashita, H.; Suzuki, N.; Tanabe, K.; Shibata, Y. Occurrence and distribution of perfluorooctane sulfonate and perfluorooctanoic acid in the rivers of Tokyo Water, Air, Soil Pollut. 2009, 202, 57– 67
      10
      Occurrence and distribution of perfluorooctane sulfonate and perfluorooctanoic acid in the rivers of Tokyo
      Takazawa, Y.; Nishino, T.; Sasaki, Y.; Yamashita, H.; Suzuki, N.; Tanabe, K.; Shibata, Y.
      Water, Air, & Soil Pollution (2009), 202 (1-4), 57-67CODEN: WAPLAC; ISSN:0049-6979. (Springer)
      Comprehensive survey of major rivers in the Tokyo metropolitan area was conducted for clarifying the emission sources of perfluorooctane sulfonate (PFOS) in Tokyo. PFOS was found at all sampling sites at concns. ranging from 0.5 to 58 ng L-1; in addn. to this, it was also indicated that unknown PFOS emission sources are present in the midstream of the Tama River basin. The relationship between PFOS and perfluorooctanoic acid (PFOA) was const. at a ratio of 10:3 (PFOS/PFOA) throughout the Tama River basin. The sum of daily load amts. of PFOS from Tokyo's major rivers to Tokyo Bay reached 215 g day-1. This value corresponds to 12.8 μg day-1 per person using the sum of wastewater treatment district populations. In contrast, an estn. of PFOS contribution of domestic wastewater was also attempted, and the contribution was 1.6 μg day-1 per person. Samples were taken up trunk sewers in the Tama River and finally the highest PFOS concn. (58,000 ng L-1) were found at one of the wastewater of the electronic parts manufg. facilities.
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    11. 11
      Higgins, C. P.; Field, J. A.; Criddle, C. S.; Luthy, R. G. Quantitative determination of perfluorochemicals in sediments and domestic sludge Environ. Sci. Technol. 2005, 39, 3946– 3956
      11
      Quantitative Determination of Perfluorochemicals in Sediments and Domestic Sludge
      Higgins, Christopher P.; Field, Jennifer A.; Criddle, Craig S.; Luthy, Richard G.
      Environmental Science and Technology (2005), 39 (11), 3946-3956CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Perfluorochems. (PFCs) are the subject of increasingly intense environmental research. Despite their detection both in biota and in aq. systems, little attention was paid to the possible presence of this class of compds. in solid environmental matrixes. The limited available data indicate that some PFCs such as perfluorooctane sulfonate (PFOS) may strongly sorb to solids, and sewage sludge is widely suspected as a major sink of PFCs entering municipal waste streams. A quant. anal. method was developed that consists of liq. solvent extn. of the analytes from sediments and sludge, cleanup via solid-phase extn., and injection of the exts. with internal stds. into a HPLC system coupled to a tandem mass spectrometer (LC/MS/MS). The limits of detections of the method were analyte and matrix dependent, but ranged from 0.7 to 2.2 ng/g and 0.041 to 0.246 ng/g (dry wt.) for sludge and sediment, resp. A demonstration of the method was performed by conducting a limited survey of domestic sludge and sediments. The concn. of PFCs in domestic sludge ranged from 5 to 152 ng/g for total perfluorocarboxylates and 55 to 3370 ng/g for total perfluoroalkyl sulfonyl-based chems. Data from a survey of San Francisco Bay Area sediments suggest widespread occurrence of PFCs in sediments at the low ng/g to sub-ng/g level. Also, substances that may be transformed to PFOS, such as 2-(N-ethylperfluorooctanesulfonamido) acetic acid (N-EtFOSAA) and 2-(N-methylperfluorooctanesulfonamido) acetic acid (N-MeFOSAA), are present in both sediments and sludge at levels often exceeding PFOS.
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    12. 12
      Giesy, J. P.; Kannan, K. Perfluorochemical surfactants in the environment Environ. Sci. Technol. 2002, 36, 146A– 152A
      12
      Perfluorochemical surfactants in the environment
      Giesy, John P.; Kannan, Kurunthachalam
      Environmental Science and Technology (2002), 36 (7), 146A-152ACODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      A review. Topics discussed include properties of fluorinated org. compds. (FOCs), prodn. and use, anal. issues, transport uncertainties, perfluorooctane sulfonate in animals, bioconcn. factors and Henry's law consts., occurrence in humans, and toxicity issues and concerns.
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    13. 13
      Olsen, G. W.; Burris, J. M.; Ehresman, D. J.; Froehlich, J. W.; Seacat, A. M.; Butenhoff, J. L.; Zobel, L. R. Half-life of serum elimination of perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorooctanoate in retired fluorochemical production workers Environ Health Perspect. 2007, 115, 1298– 1305
      13
      Half-life of serum elimination of perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorooctanoate in retired fluorochemical production workers
      Olsen, Geary W.; Burris, Jean M.; Ehresman, David J.; Froehlich, John W.; Seacat, Andrew M.; Butenhoff, John L.; Zobel, Larry R.
      Environmental Health Perspectives (2007), 115 (9), 1298-1305CODEN: EVHPAZ; ISSN:0091-6765. (U. S. Department of Health and Human Services, Public Health Services)
      Background: The presence of perfluorooctanesulfonate (PFOS), perfluorohexanesulfonate (PFHS), and perfluorooctanoate (PFOA) has been reported in humans and wildlife. Pharmacokinetic differences have been obsd. in lab. animals. Objective: The purpose of this observational study was to est. the elimination half-life of PFOS, PFHS, and PFOA from human serum. Methods: Twenty-six (24 male, 2 female) retired fluorochem. prodn. workers, with no addnl. occupational exposure, had periodic blood samples collected over 5 years, with serum stored in plastic vials at -80°C. At the end of the study, we used HPLC-mass spectrometry to analyze the samples, with quantification based on the ion ratios for PFOS and PFHS and the internal std. 18O2-PFOS. For PFOA, quantitation was based on the internal std. 13C2-PFOA. Results: The arithmetic mean initial serum concns. were as follows: PFOS, 799 ng/mL (range, 145-3,490); PFHS, 290 ng/mL (range, 16-1,295); and PFOA, 691 ng/mL (range, 72-5,100). For each of the 26 subjects, the elimination appeared linear on a semi-log plot of concn. vs. time; therefore, we used a first-order model for estn. The arithmetic and geometric mean half-lives of serum elimination, resp., were 5.4 years [95% confidence interval (CI), 3.9-6.9] and 4.8 years (95% CI, 4.0-5.8) for PFOS; 8.5 years (95% CI, 6.4-10.6) and 7.3 years (95% CI, 5.8-9.2) for PFHS; and 3.8 years (95% CI, 3.1-4.4) and 3.5 years (95% CI, 3.0-4.1) for PFOA. Conclusions: Based on these data, humans appear to have a long half-life of serum elimination of PFOS, PFHS, and PFOA. Differences in species-specific pharmacokinetics may be due, in part, to a saturable renal resorption process.
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      Ankley, G. T.; Kuehl, D. W.; Kahl, M. D.; Jensen, K. M.; Butterworth, B. C.; Nichols, J. W. Partial life-cycle toxicity and bioconcentration modeling of perfluorooctanesulfonate in the northern leopard frog (Rana pipiens) Environ. Toxicol. Chem. 2004, 23, 2745– 2755
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      Sakurai, T.; Kim, J. G.; Suzuki, N.; Matsuo, T.; Li, D. Q.; Yao, Y. A.; Masunaga, S.; Nakanishi, J. Polychlorinated dibenzo-p-dioxins and dibenzofurans in sediment, soil, fish, shellfish and crab samples from Tokyo Bay area, Japan Chemosphere 2000, 40, 627– 640
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      Managaki, S.; Takada, H.; Kim, D.-M.; Horiguchi, T.; Shiraishi, H. Three-dimensional distributions of sewage markers in Tokyo Bay water—fluorescent whitening agents (FWAs) Mar. Pollut. Bull. 2006, 52, 281– 292
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      Kume, G.; Horiguchi, T.; Goto, A.; Shiraishi, H.; Shibata, Y.; Morita, M.; Shimizu, M. Seasonal distribution, age, growth, and reproductive biology of marbled sole Pleuronectes yokohamae in Tokyo Bay, Japan Fisheries Science 2006, 72, 289– 298
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      The sedimentary environment in the Tokyo Bay
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      Chikyu Kagaku (Nippon Chikyu Kagakkai) (1983), 17 (1), 27-32CODEN: CKNKDM; ISSN:0386-4073.
      A review with 10 refs.
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      Hansen, K. J.; Johnson, H. O.; Eldridge, J. S.; Butenhoff, J. L.; Dick, L. A. Quantitative characterization of trace levels of PFOS and PFOA in the Tennessee River Environ. Sci. Technol. 2002, 36, 1681– 1685
      24
      Quantitative Characterization of Trace Levels of PFOS and PFOA in the Tennessee River
      Hansen, K. J.; Johnson, H. O.; Eldridge, J. S.; Butenhoff, J. L.; Dick, L. A.
      Environmental Science and Technology (2002), 36 (8), 1681-1685CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Although there is evidence of widespread distribution of org. fluorochems., e.g., perfluorooctane sulfonate and perfluorooctanoate, in the environment, the versatility of these compds. in industrial and com. applications complicates characterization of pathways into the environment. A solid-phase extn. method coupled with HPLC-neg. ion electrospray tandem mass spectrometry was developed to quant. measure trace concns. of org. fluorochems. in drinking and surface water. With this method, certain fluorochems. can be quant. measured in water samples down to 25 ppt, a level well below calcd. drinking water advisory levels. To assess fluorochem. distribution in a localized geog. and to ascertain whether fluorochem. manufg. facilities contribute to environmental fluorochem. levels, 40 water samples were collected on an 80-mi stretch of the Tennessee River near a fluorochem. manufg. site in Decatur, Alabama. Low perfluorooctane sulfonate concns. (ppt) were detd. throughout the stretch of river sampled. Concns. of measured fluorochems. increased downstream from the fluorochem. manufg. facility, indicating that manufg. effluent is one likely source of org. fluorochems. in the river.
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    25. 25
      Hollander, M.; Wolfe, D. A., Nonparametric Statistical Methods., 2nd ed.; John Wiley & Sons, Inc: New York, 1999; p 816.
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      Yazawa, K.;; Ikeda, F. Distribution of the anoxic water mass in Tokyo Bay and effect of dissolved oxygen on mantis shrimp (Oratosquilla oratoria De Haan). In Research Report of the Kanagawa Prefectural Fisheries Experimental Station, 1988; pp 95− 100 (

      in Japanese

      ).
      There is no corresponding record for this reference.
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      Koike, Y.; Matsuyama, M.; Hayashi, T.; Kitade, Y.; Kitazawa, A.; Yoshida, J. Distribution and behavior of bottom water in Tokyo Bay in summer J. Tokyo Univ. Fish. 1997, 84, 43– 51

      (in Japanese)

      There is no corresponding record for this reference.
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      Hibino, T.; Nakayama, K.; Okada, T. Current field in Tokyo Bay during stratification period Proc. Coast. Eng., JSCE 2000, 47, 1056– 1060

      (in Japanese)

      There is no corresponding record for this reference.
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      Okada, T.; Takao, T.; Nakayama, K.; Furukawa, K. Change in freshwater discharge and residence time of seawater in Tokyo Bay J. Hydraul., Coastal Environ. Eng. 2007, 63, 67– 72

      (in Japanese)

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    30. 30
      Kobayashi, J.; Serizawa, S.; Sakurai, T.; Imaizumi, Y.; Suzuki, N.; Horiguchi, T. Spatial distribution and partitioning of polychlorinated biphenyls in Tokyo Bay, Japan J. Environ. Monit. 2010, 12, 838– 845
      There is no corresponding record for this reference.
    31. 31
      Johnson, R. L.; Anschutz, A. J.; Smolen, J. M.; Simcik, M. F.; Penn, R. L. The adsorption of perfluorooctane sulfonate onto sand, clay, and iron oxide surfaces J. Chem. Eng. Data 2007, 52, 1165– 1170
      31
      The Adsorption of Perfluorooctane Sulfonate onto Sand, Clay, and Iron Oxide Surfaces
      Johnson, Ramona L.; Anschutz, Amy J.; Smolen, Jean M.; Simcik, Matt F.; Penn, R. Lee
      Journal of Chemical & Engineering Data (2007), 52 (4), 1165-1170CODEN: JCEAAX; ISSN:0021-9568. (American Chemical Society)
      Fluorinated anionic surfactants have drawn considerable attention due to recent work showing significant concns. in surface waters and biota from around the globe. A detailed understanding of the transport and fate of fluorinated surfactants through soil and like media must include an elucidation of mineral surface chem. Five materials were equilibrated with solns. of perfluorooctane sulfonate (PFOS) to characterize adsorption: kaolinite, Ottawa sand std., synthetic goethite, Lake Michigan sediment, and iron-coated sand from Mappsville, VA. Aq. and adsorbed PFOS was quantified with LC/MS (mass balance av.: 101 ± 12 %, n = 37). The materials showed a near linear increase in adsorption as the equil. concns. increased. Isotherms and calcd. solid/soln. distribution ratio expts. indicated that PFOS adsorption is significant but smaller than hydrocarbon analogs or org. compds. of similar mol. wt. Surface area normalized adsorption increased for the materials in the following order: goethite < kaolinite < high iron sand < Ottawa sand std. Exptl. results and comparisons to published data suggest that org. carbon may play an important role in sorption whereas electrostatic attraction may play a role when org. carbon is not present.
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    32. 32
      Higgins, C. P.; Luthy, R. G. Sorption of perfluorinated surfactants on sediments Environ. Sci. Technol. 2006, 40, 7251– 7256
      32
      Sorption of Perfluorinated Surfactants on Sediments
      Higgins, Christopher P.; Luthy, Richard G.
      Environmental Science & Technology (2006), 40 (23), 7251-7256CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The sorption of anionic perfluorochem. (PFC) surfactants of varying chain lengths to sediments was investigated using natural sediments of varying iron oxide and org. carbon content. Three classes of PFC surfactants were evaluated for sorptive potential: perfluorocarboxylates, perfluorosulfonates, and perfluorooctyl sulfonamide acetic acids. PFC surfactant sorption was influenced by both sediment-specific and soln.-specific parameters. Sediment org. carbon, rather than sediment iron oxide content, was the dominant sediment-parameter affecting sorption, indicating the importance of hydrophobic interactions. However, sorption also increased with increasing soln. [Ca2+] and decreasing pH, suggesting that electrostatic interactions play a role. Perfluorocarbon chain length was the dominant structural feature influencing sorption, with each CF2 moiety contributing 0.50-0.60 log units to the measured distribution coeffs. The sulfonate moiety contributed an addnl. 0.23 log units to the measured distribution coeff., when compared to carboxylate analogs. In addn., the perfluorooctyl sulfonamide acetic acids demonstrated substantially stronger sorption than perfluorooctane sulfonate (PFOS). These data should prove useful for modeling the environmental fate of this class of contaminants.
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