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Continental-Scale Increase in Lake and Stream Phosphorus: Are Oligotrophic Systems Disappearing in the United States?

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† United States Environmental Protection Agency, 200 Southwest 35th Street, Corvallis, Oregon 97333, United States
§ Department of Fish and Wildlife, Oregon State University, Corvallis, Oregon 97331, United States
∥ Department of Earth and Environmental Science, University of British Columbia, Kelowna, British Columbia V1V 1V7, Canada
⊥ Office of Water, United States Environmental Protection Agency, Washington, D.C. 20460, United States
*Telephone: 541-754-4441. Fax: 541-754-4716. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2016, 50, 7, 3409–3415
Publication Date (Web):February 25, 2016
https://doi.org/10.1021/acs.est.5b05950
Copyright © 2016 American Chemical Society
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Abstract

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We describe continental-scale increases in lake and stream total phosphorus (TP) concentrations, identified through periodic probability surveys of thousands of water bodies in the conterminous U.S. The increases, observed over the period 2000–2014 were most notable in sites in relatively undisturbed catchments and where TP was initially low (e.g., less than 10 μg L–1). Nationally, the percentage of stream length in the U.S. with TP ≤ 10 μg L–1 decreased from 24.5 to 10.4 to 1.6% from 2004 to 2009 to 2014; the percentage of lakes with TP ≤ 10 μg L–1 decreased from 24.9 to 6.7% between 2007 and 2012. Increasing TP concentrations appear to be ubiquitous, but their presence in undeveloped catchments suggests that they cannot be entirely attributed to either point or common non-point sources of TP.

1 Introduction

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Phosphorus (P) is a critical nutrient that limits the productivity of many temperate freshwater ecosystems.(1, 2) Extensive research in the late 1950s to the 1970s revealed how anthropogenic sources of P, especially from industrial and municipal wastewater, facilitated the eutrophication of lakes and streams. Measures have since been implemented to control the supply of P from these point sources, but eutrophication attributable to non-point sources of P (e.g., agricultural, stormwater, and wastewater runoff) continues to be widespread.(3) Recent sizable and economically critical blooms of harmful algae(4) have been attributed to these non-point sources.
Because of its critical role in aquatic ecosystems, total phosphorus (TP) has been one of the key variables included in the United States Environmental Protection Agency (U.S. EPA)’s national program of aquatic resources surveys. In this paper, we present stream and lake data collected in periodic national surveys conducted cooperatively by the U.S. EPA and the States/Tribes and initiated in 2000. Results from these randomized, unequal probability surveys provide unbiased estimates of a range of biological, chemical, and physical variables at a continental scale and allow the users to determine the percentage of all lakes and streams that exceeds specific levels of these variables. The data provide a powerful source of information for examining the conditions of water resources and their stressors, across geopolitical, ecological, and hydrologic boundaries.

2 Materials and Methods

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2.1 Survey Design

All of the national surveys described in this paper are randomized, unequally weighted probability surveys(5) overseen by the U.S. EPA’s Office of Water (http://www.epa.gov/nheerl/arm/designpages/monitdesign/survey_overview.htm) with the goal of creating unbiased assessments of aquatic resources across the 48 conterminous states. Details of the stream(6) and lake(7) survey designs have been published elsewhere.
The first of these surveys sampled wadeable (first through fourth Strahler order) streams in the conterminous U.S. between 2000 and 2004.(8, 9) Additional stream and river surveys have been repeated on a 5 year schedule, with results from the 2008–2009 and 2013–2014 efforts available for the current investigation. A national lake survey was conducted in 2007 and repeated in 2012.(10) Each site in each survey was sampled once during a summer index period. In the second and third stream surveys and the second lake survey, approximately half of the sampled sites were a random subsample of sites also sampled in the previous survey. Details on sample sizes in each survey and the numbers of resurveyed sites are shown in Table S1 of the Supporting Information.
The surveys use standardized sampling methods that did not change over our the reported time period. At each stream site, a 4 L grab sample was collected from an area of flowing water at or near the designated geographic coordinates assigned to the site as part of the survey design.(11) At each lake site, a 4 L integrated water sample was collected from a point on the lake that represented the deepest point of natural lakes or from the midpoint area of reservoirs.(12) All samples were shipped on ice as soon as possible after collection to an analytical laboratory (overnight courier service was used when necessary and available). Samples typically arrived at a laboratory within 24–48 h of collection.

2.2 Creation of Minimally Disturbed Data Set

To quantify changes in TP in relatively undisturbed catchments and to examine potential mechanisms operating in the absence of significant anthropogenic development, we created a minimally disturbed subset of the resurveyed samples collected as part of each pair of surveys. The contributing watershed area was delineated for each sample site (lake or stream), and percentages of various land use categories were calculated for each, using the 2006 National Land Cover Data set (http://www.mrlc.gov/nlcd2006.php). In addition, the density of roads (km of roads/km2 of catchment) was calculated for the catchment of each site based on the 2006 TIGER database (https://www.census.gov/geo/maps-data/data/tiger.html). Finally, we calculated riparian disturbance at each stream and lake site based on data collected at the time of each survey. In brief, riparian disturbance was estimated from direct observations of 12 specific forms of human riparian disturbance, tallied in either 22 (streams) or 10 (lakes) riparian plots along the stream or lakeshore.(13, 14) We defined minimally disturbed(15) sites as those with catchments exhibiting <5% agricultural land use, <1.5% urban land use, <2 km km–2 road density, and <1.25 riparian disturbance index value.

2.3 Laboratory Analyses

All of the concentrations that we report are estimated from water samples analyzed by a single laboratory, using analytical methods that have not changed over the course of the surveys.
An unfiltered aliquot was prepared from each bulk stream and lake sample for analysis of TP and total nitrogen (TN). TP was determined by a manual alkaline persulfate digestion, followed by automated colorimetric analysis (ammonium molybdate and antimony potassium tartrate under acidic conditions, with absorbance at 880 nm) using a flow injection analyzer. TN was determined by a manual alkaline persulfate digestion, followed by automated colorimetric analysis (cadmium reduction, followed by treatment with sulfanilamide and ethylenediamine dihydrochloride, with absorbance at 520 nm) using a flow injection analyzer.
Specific conductance (μS/cm at 25 °C) was determined on an unfiltered aliquot using a conductivity meter. Dissolved silica (as mg of SiO2 L–1) was determined from a filtered (0.4 μm) unpreserved aliquot from each lake and stream sample by automated colorimetric analysis (ammonium molybdate under acidic conditions, followed by reduction with stannous chloride, with absorbance at 820 nm). Dissolved magnesium was determined on a filtered, acid-preserved aliquot from each stream and lake sample by inductively coupled plasma–atomic emission spectroscopy.
The estimated method detection limits (MDLs) for the laboratory analyzing survey TP samples ranged from less than 3 to 5.5 μg L–1 (Table S2 of the Supporting Information). The proportion of the population with values below the corresponding MDL decreased over time, from 10.8% (2000–2004) to 0.3% (2013–2014) in streams and from 7.1% (2007) to 0% (2012) in lakes. Similarly, the proportion of minimally disturbed sites with TP values below detection decreased from a high of 26% (24/91) in streams in 2000–2004 to 0% in both the latest streams and latest lake surveys (Table S2 of the Supporting Information).
In subsequent analyses, all TP values lower than the MDL for the given survey (Table S2 of the Supporting Information) were set to 1/2 of the corresponding MDL for that survey.
Analytical precision was estimated from duplicate samples prepared from approximately 5% of the unfiltered aliquots. For duplicate pairs with TP concentration of ≤20 μg L–1 (n = 169), the mean difference was 1 ± 0.2 μg L–1 (95% confidence interval). For duplicate pairs with the first replicate TP concentration of >20 μg L–1 (n = 256), the mean relative percent difference was 3 ± 0.6%.
We tested the consistency and accuracy of laboratory TP estimates by compiling the results of blind audit analyses conducted by the U.S. EPA laboratory responsible for analyzing lake/stream survey water samples during 2000–2014. The U.S. EPA laboratory participated in multi-laboratory performance studies coordinated by the National Water Research Institute of Environment Canada (http://www.ec.gc.ca/inre-nwri/default.asp?lang=En&n=7A20877C-1, accessed April 27, 2015). There were two studies per year, with each study consisting of 10 acid-preserved aliquots for analysis of TP. Aliquots were prepared from natural samples and fortified so that each set of samples represented a broad range of TP concentrations. The “true” audit value of each sample was assigned to be the median of concentrations reported by all participating laboratories.
Figure S1 of the Supporting Information plots the measured TP concentration reported by the U.S. EPA lab against the corresponding estimate assigned by the audit process, for 243 samples analyzed by the laboratory from 2000 to 2014. Differences between measured and assigned (audit) concentrations were small, with a mean difference (measured – audit) over the 14 year period of −4.6 μg L–1 (95% confidence interval from −2.9 to −6.2 μg L–1), with no visual evidence that the differences were related to the concentrations. There was no significant linear trend in the (measured – audit) differences over time (slope = 0.255 μg L–1 year–1; p = 0.19).

2.4 Hydrologic Analysis

We compiled estimated quarterly runoff values for the eight digit hydrologic units in which each minimally disturbed site is located (http://waterwatch.usgs.gov), matched by quarter and year with the dates of each survey sample. Differences in quarterly runoff between surveys at each site were analyzed using unweighted paired t tests.

2.5 Data Analyses

Population estimates (Figure 1 and Table S1 of the Supporting Information) are based on a single sample from each lake/stream and use weighted Horvitz–Thompson estimation.(16) We used the local mean variance estimator to develop confidence intervals around population estimates.(17) Computations were conducted using the spsurvey package in R.

Figure 1

Figure 1. Cumulative frequency distributions of TP concentrations in the population of (a) streams and (b) lakes in the conterminous U.S. Vertical axes are the cumulative proportion of stream length or lake count with concentrations less than or equal to the corresponding horizontal axis value. Lines are weighted population estimates and 95% confidence intervals for (a) total stream length in 2000–2004, 2008–2009, and 2013–2014 (2008–2009 and 2013–2014 data exclude rivers, which were not included in the 2000–2004 survey) and (b) total numbers of lakes in 2007 versus 2012 (excludes lakes with surface area of <4 ha, which were not included in the 2007 survey).

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3 Results

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Population estimates for TP concentrations in streams and lakes are shown in Figure 1. In all cases, TP concentrations increased over the 5 year periods between surveys. Median TP in streams increased from 26 μg L–1 (2000–2004) to 48 μg L–1 (2008–2009) to 56 μg L–1 (2013–2014); median TP in lakes increased from 20 μg L–1 (2007) to 37 μg L–1 (2012). The most disturbing increases have occurred at the lower end of the TP concentration gradient. During the study, the percentage of stream length in the U.S. with TP of ≤10 μg L–1 decreased from 24.5 to 10.4 to 1.6 from 2004 to 2009 to 2014; the percentage of lakes with TP of ≤10 μg L–1 decreased from 24.9 to 6.7 between 2007 and 2012. These estimates indicate that there has been a dramatic decline in the number of naturally oligotrophic water bodies (<10 μg of TP L–1) over this time period.
To explore the magnitude of TP changes at the lower end of the TP concentration gradient and the possible mechanisms responsible for them, we created a subset of resurveyed sites from each pair of surveys that occupy relatively undisturbed catchments (see the Materials and Methods). Comparisons of TP values between surveys for this minimally disturbed set of sites are shown in Figure 2. Unweighted median annual TP increases at resurveyed sites occupying relatively undeveloped catchments were +2.5 μg L–1 year–1 for streams from 2000 to 2014 (+2.2 μg L–1 year–1 from 2000/2004 to 2008/2009; +2.9 μg L–1 year–1 from 2008/2009 to 2013/2014) and +1.6 μg L–1 year–1 for lakes from 2007 to 2012. Increasing TP in minimally disturbed sites has occurred throughout the U.S. (Figure 3).

Figure 2

Figure 2. Comparison of (a–c) TP concentrations and (d–f) TN concentrations at sites in minimally disturbed catchments for (a and d) 91 streams included in both the 2000–2004 and 2008–2009 surveys, (b and e) 47 resurveyed sites from the 2007 and 2012 lake surveys, and (c and f) 52 resurveyed sites from the 2008–2009 and 2013–2014 stream surveys. Lines are 1:1 lines. In each case, points above the 1:1 line indicate increased concentrations in the later survey. The p values are from weighted, paired-sample t tests. Values below analytical detection limits (MDLs) have been set to 1/2 of the MDL for that time period (observable, for example, at the far left of panel a).

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Figure 3

Figure 3. Locations of resurveyed sites in minimally disturbed watersheds and annual rate of TP change measured between paired surveys. Rates of change are μg L–1 year–1.

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We also note that virtually every minimally disturbed resurveyed site that began with TP below ca. 10 μg L–1 exhibited an increase in TP between surveys. The unweighted percentage of resurveyed streams with TP concentrations of <10 μg L–1 decreased from 46 in the 2000–2004 survey to 23 in the 2008–2009 survey to 4 in the 2013–2014 survey. The percentage of resurveyed lakes with TP of <10 μg L–1 in these undisturbed catchments decreased from 51 in 2007 to 20 in 2012.
Nationally, TN is strongly correlated with TP in both lakes and streams,(9, 10) probably reflecting common sources (e.g., agricultural and urban runoff). Unlike TP, however, TN does not appear to be increasing at minimally disturbed sites (Figure 2). Importantly, all other major constituents follow the pattern of TN in Figure 2 rather than that of TP. We illustrate the contrast between the behavior of TP and selected examples of other constituents in Figure S2 of the Supporting Information.

4 Discussion

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The results of repeated national surveys demonstrate that increases in TP are dramatic and widespread but provide limited direct information about potential causes. Several observations help constrain the possible sources of additional TP to streams and lakes: (1) The increases are continental in scale, with higher concentrations occurring throughout the conterminous U.S.; therefore, potential causes are also likely to be large scale. (2) TP is increasing at sites covering a wide range of human land use, but the increases are especially notable at minimally disturbed sites. Plausible sources for added TP are likely to result from processes that operate at both disturbed and relatively undisturbed sites. (3) TP appears to be the only major ion showing directional change. TN has not increased (Figure 2) nor have any other major constituents (selected examples in Figure S2 of the Supporting Information). Likely causative mechanisms are therefore limited to those that might affect TP disproportionally and that operate in undeveloped areas.
One might expect that a change in the dominant sources of TP to lakes and streams (runoff from agriculture, wastewater, or stormwater) is responsible for the observed TP increases. The notable increases observed in lakes and streams occupying minimally disturbed catchments, however, make these sources very unlikely sole causes. Changes in these sources might also be expected to drive an increase in TN, which we have not observed (Figure 2 and Figure S2 of the Supporting Information).
Other processes that might be important in undeveloped areas are also improbable because changes in them are unlikely to be found at continental scales. Increasing inputs from migratory birds, for example, might produce increases in some local areas but not at the spatial scale of the TP increases that we report. Forest dieback is known to produce increased rates of nutrient flux from forested catchments(18, 19) but is heterogeneous spatially and could not by itself produce the large-scale patterns that we observe. Increasing TP has recently been linked to recovery from atmospheric acidification,(20) driven by a decrease in acidity and an increase in leaching of dissolved organic carbon (DOC) from catchment soils. This mechanism would be limited to a small proportion of our minimally disturbed sites that occupy acid-sensitive terrain.(9, 10) For the nation as a whole, there are no systematic changes in DOC observable in the data (Figure S2 of the Supporting Information).
Much of the natural movement of phosphorus from the land to receiving waters is in the form of particulate P associated with soil particles and is mediated by high-runoff hydrologic events and erosion. Because increased hydrologic runoff from catchments has the potential to influence TP concentrations in lakes and streams over time, we examined whether runoff has changed during the 2000–2014 period covered by this study. We found no systematic increase in quarterly runoff between surveys for streams in minimally disturbed catchments (Figure S3 of the Supporting Information) but a small increase in the 2012 lake survey relative to the 2007 survey (mean increase of 12.5 mm year–1; p = 0.001). This coarse analysis of runoff data suggests that large-scale increases in runoff have not occurred but the quarterly data may not capture any potential increase in episodic high-runoff events, of the type more likely to precipitate TP movement from catchments to receiving waters.
One remaining potential explanation for rising TP concentrations is an increase in the atmospheric contribution of P to lakes and streams; such increases might be most evident in undeveloped catchments, where other P sources do not cloud the signal. Although historically atmospheric deposition has been considered a negligible source relative to watershed sources(21) and TP is not a published component of the National Atmospheric Deposition Program, deposition has recently been identified as a potentially important source of TP to alpine lakes and streams in Europe and North America.(22-25)
The contribution of atmospheric P loads to freshwaters varies globally. Local- to regional-scale sources of atmospheric P are often derived from primary biogenic particles,(21) while regional- to long-range transported P is typically derived from the wind erosion of soils, biomass burning (e.g., forest fires), and combustion of fossil fuels.(26, 27) All of these sources are more likely to produce a TP signal in the dry component of deposition rather than in rain or snow. Dry particulate deposition (dust) has the potential to enrich naturally oligotrophic lake ecosystems primarily through the association with organic compounds, which may be up to 40% of the dust material,(28, 29) and potentially through phosphorus-rich minerals.(30) Recent studies have documented increases in lake TP as a result of dust deposition in the western U.S.(22, 23) and Europe.(25) While direct deposition of TP to lake surfaces is a plausible mechanism for increasing TP concentrations, our observation of increased TP in streams is more problematic. It is not clear that increased dry deposition of TP to a catchment would necessarily increase the TP concentrations of the streams that drain them.
Dramatic reductions in the number of naturally oligotrophic streams and lakes (<10 μg of TP L–1) create a potential for extensive ecosystem consequences, including increased incidence of algal blooms and altered habitat for a variety of aquatic organisms, birds, and amphibians. Additional research on the cause(s) of these trends is certainly warranted. In particular, two of the most plausible mechanisms may be influenced by the changing climate. Recent studies have demonstrated increases in the frequency of extreme precipitation events in the U.S.(31) and in extreme hydrologic events in some regions of the U.S.(32) Because TP is often mobilized during such extreme events, we recommend further investigation on the potential association of increasing TP and more frequent extreme hydrologic events. Recent simulations have also suggested a global increase in atmospheric deposition of TP, by 1.4 times the pre-industrial rate, largely as a result of increased dust and biomass-burning emissions.(33) Additional work on the potential role of atmospheric deposition, particularly dust, in driving TP trends in lakes and streams is also warranted.

Supporting Information

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.5b05950.

  • Years of data collection and details of sample sizes for lake and stream surveys used in this analysis (Table S1), MDLs for TP analyses for years representing each survey analyzed in this paper, the proportion of the population (percent stream length or percentage of lake number) with values below the MDL, and the number of resurveyed sites in the minimally disturbed data set (total number in parentheses) with TP less than the corresponding MDL (Table S2), results of blind audit sample analysis for the U.S. EPA laboratory responsible for analyzing survey samples for 2000–2014, corresponding to the time span of statistical surveys reported in this paper (Figure S1), box and whisker plots of unweighted, normalized differences between surveys at minimally disturbed resurveyed sites for TP and selected other chemical variables (TN, conductivity, silica, magnesium, DOC, calcium, and total suspended solids) for (a) stream surveys in 2000–2004 versus 2008–2009, (b) lake surveys in 2007 versus 2012, and (c) stream surveys in 2008–2009 versus 2013–2014, with normalized differences calculated as (survey 2 – survey 1)/mean (survey 1 and survey 2) (Figure S2), and comparison of quarterly runoff (matched to date of each survey sample) in eight digit hydrologic units for each least disturbed catchment from (a) stream surveys in 2000–2004 versus 2008–2009, (b) lake surveys in 2007 versus 2012, and (c) stream surveys in 2008–2009 versus 2013–2014 (lines being 1:1 lines), with only the lake data showing a significant change in runoff between surveys (Figure S3) (PDF)

The authors declare no competing financial interest.

‡Author Status

John Van Sickle: Retired.

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Acknowledgment

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This manuscript has been subjected to U.S. EPA review and has been approved for publication. The views expressed in this paper are those of the authors and do not necessarily reflect the views or policies of the U.S. EPA. Mention of trade names or commercial products does not constitute endorsement or recommendation for use. This work has benefited from constructive review comments from Charles T. Driscoll, Donald T. Monteith, Jana E. Compton, Brian H. Hill, Dana Thomas, Jim Markwiese, and two anonymous reviewers. The data reported in this paper are available publically through the U.S. EPA at http://water.epa.gov/type/watersheds/monitoring/aquaticsurvey_index.cfm.

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    United States Environmental Protection Agency (U.S. EPA). Wadeable Streams Assessment. A Collaborative Survey of the Nation’s Streams; Office of Research and Development/Office of Water, U.S. EPA: Washington, D.C., 2006; EPA 841-B-06-002.
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    United States Environmental Protection Agency (U.S. EPA). National Lakes Assessment: A Collaborative Survey of the Nation’s Lakes; Office of Water and Office of Research and Development, U.S. EPA: Washington, D.C., 2009; p 118.
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    United States Environmental Protection Agency (U.S. EPA). National Rivers and Streams Assessment Field Operations Manual; U.S. EPA: Washington, D.C., 2009.
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    United States Environmental Protection Agency (U.S. EPA). 2012 National Lakes Assessment Field Operations Manual; U.S. EPA: Washington, D.C., 2012.
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    Kaufmann, P. R.; Hughes, R. M.; Van Sickle, J.; Whittier, T. R.; Seeliger, C. W.; Paulsen, S. G. Lakeshore and littoral physical habitat structure: A field survey method and its precision Lake Reservoir Manage. 2014, 30 (2) 157– 176 DOI: 10.1080/10402381.2013.877543
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    13
    Lakeshore and littoral physical habitat structure: A field survey method and its precision
    Kaufmann, Philip R.; Hughes, Robert M.; Van Sickle, John; Whittier, Thomas R.; Seeliger, Curt W.; Paulsen, Steven G.
    Lake and Reservoir Management (2014), 30 (2), 157-176CODEN: LRMAEY; ISSN:1040-2381. (Taylor & Francis Ltd.)
    Measures of near-shore phys. habitat structure have only recently been employed in large-scale assessments of lake ecol. condition. We outline and evaluate a rapid approach for quantifying lake phys. habitat structure and disturbance that was piloted in the Northeast United States by the US Environmental Protection Agency in its Environmental Monitoring and Assessment Program (EMAP-NE), then improved and applied in the 2007 National Lakes Assessment (NLA). This approach measures littoral habitat complexity, fish cover, substrate, aquatic macrophytes, riparian vegetation, and human disturbances. Of 46 NLA phys. habitat metrics, 34 had repeat-visit std. deviations <10% of their potential ranges, indicating repeatability sufficient to distinguish 4 to 5 levels of habitat condition within that range. For 23 metrics, the signal to noise ratio (S/N) of among-lake to same-year repeat-visit variance was moderate to high (3-10), indicating that noise variance was a relatively small confounding factor in their interpretation. Most NLA metrics were 30-40% more precise than those of EMAP-NE, largely because NLA used a greater no. of habitat percent cover classes. We conclude that the metrics and indexes derived from the NLA phys. habitat field approach are precise enough to quantify near-shore habitat structure for contributing to national, state, and ecoregional assessments of lake condition.
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  14. 14
    Kaufmann, P. R.; Levine, P.; Robison, E. G.; Seeliger, C.; Peck, D.Quantifying Physical Habitat in Wadeable Streams; United States Environmental Protection Agency (U.S. EPA): Washington, D.C., 1999; EPA/620/R-99/003.
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    Stoddard, J. L.; Larsen, D. P.; Hawkins, C. P.; Johnson, R. K.; Norris, R. H. Setting expectations for the ecological condition of running waters: the concept of reference condition Ecological Applications 2006, 16, 1267– 1276 DOI: 10.1890/1051-0761(2006)016[1267:SEFTEC]2.0.CO;2
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    15
    Setting expectations for the ecological condition of streams: the concept of reference condition
    Stoddard John L; Larsen David P; Hawkins Charles P; Johnson Richard K; Norris Richard H
    Ecological applications : a publication of the Ecological Society of America (2006), 16 (4), 1267-76 ISSN:1051-0761.
    An important component of the biological assessment of stream condition is an evaluation of the direct or indirect effects of human activities or disturbances. The concept of a "reference condition" is increasingly used to describe the standard or benchmark against which current condition is compared. Many individual nations, and the European Union as a whole, have codified the concept of reference condition in legislation aimed at protecting and improving the ecological condition of streams. However, the phrase "reference condition" has many meanings in a variety of contexts. One of the primary purposes of this paper is to bring some consistency to the use of the term. We argue the need for a "reference condition" term that is reserved for referring to the "naturalness" of the biota (structure and function) and that naturalness implies the absence of significant human disturbance or alteration. To avoid the confusion that arises when alternative definitions of reference condition are used, we propose that the original concept of reference condition be preserved in this modified form of the term: "reference condition for biological integrity," or RC(BI). We further urge that these specific terms be used to refer to the concepts and methods used in individual bioassessments to characterize the expected condition to which current conditions are compared: "minimally disturbed condition" (MDC); "historical condition" (HC); "least disturbed condition" (LDC); and "best attainable condition" (BAC). We argue that each of these concepts can be narrowly defined, and each implies specific methods for estimating expectations. We also describe current methods by which these expectations are estimated including: the reference-site approach (condition at minimally or least-disturbed sites); best professional judgment; interpretation of historical condition; extrapolation of empirical models; and evaluation of ambient distributions. Because different assumptions about what constitutes reference condition will have important effects on the final classification of streams into condition classes, we urge that bioassessments be consistent in describing the definitions and methods used to set expectations.
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    Lohr, S. L. Sampling: Design and Analysis; Brooks/Cole Publishing: Pacific Grove, CA, 1999.
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    Stevens, D. L.; Olsen, A. R. Variance estimation for spatially balanced samples of environmental resources Environmetrics 2003, 14 (6) 593– 610 DOI: 10.1002/env.606
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    Kana, J.; Tahovska, K.; Kopacek, J. Response of soil chemistry to forest dieback after bark beetle infestation Biogeochemistry 2013, 113 (1–3) 369– 383 DOI: 10.1007/s10533-012-9765-5
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    Response of soil chemistry to forest dieback after bark beetle infestation
    Kana, Jiri; Tahovska, Karolina; Kopacek, Jiri
    Biogeochemistry (2013), 113 (1-3), 369-383CODEN: BIOGEP; ISSN:0168-2563. (Springer)
    We evaluated changes in the chem. of the uppermost soil horizons in an unmanaged spruce forest (National Park Bohemian Forest, Czech Republic) for 3 years after dieback caused by a bark beetle infestation, and compared these changes with a similar undisturbed forest area. The soils below the disturbed forest received 2-6 times more elements via litter fall compared to the unaffected plot. The subsequent decompn. of litter and reduced nutrient uptake by trees resulted in a steep increase in soil concns. of sol. N (NH4-N, org.-bound N) and P forms in the disturbed plot. The av. concns. of NH4-N and sol. reactive P increased from 0.8 to 4.4 mmol kg-1 and from 0.04 to 0.9 mmol kg-1, resp., in the uppermost soil horizon. Decompn. of litter at the disturbed plot elevated soil concns. of Ca2+, Mg2+ and K+, which replaced Al3+ and H+ ions from the soil sorption complex. Consequently, soil concns. of exchangeable base cations increased from 120 to 200 meq kg-1, while exchangeable Al3+ and H+ decreased 66 and 50 %, resp., and soil base satn. increased from 40 to 70 %. The Al3+ liberation did not elevate concns. of ionic Al in the soil soln., because most of the liberated Al3+ was rapidly complexed by dissolved org. carbon (DOC) and transformed to DOC-Al complexes. The chem. parameters investigated at the unaffected plot remained stable during the study.
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    Mikkelson, K. M.; Bearup, L. A.; Maxwell, R. M.; Stednick, J. D.; McCray, J. E.; Sharp, J. O. Bark beetle infestation impacts on nutrient cycling, water quality and interdependent hydrological effects Biogeochemistry 2013, 115 (1–3) 1– 21 DOI: 10.1007/s10533-013-9875-8
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    19
    Bark beetle infestation impacts on nutrient cycling, water quality and interdependent hydrological effects
    Mikkelson, Kristin M.; Bearup, Lindsay A.; Maxwell, Reed M.; Stednick, John D.; McCray, John E.; Sharp, Jonathan O.
    Biogeochemistry (2013), 115 (1-3), 1-21CODEN: BIOGEP; ISSN:0168-2563. (Springer)
    Bark beetle populations have drastically increased in magnitude over the last several decades leading to the largest-scale tree mortality ever recorded from an insect infestation on multiple wooded continents. When the trees die, the loss of canopy and changes in water and nutrient uptake lead to observable changes in hydrol. and biogeochem. cycling. This review aims to synthesize the current research on the effects of the bark beetle epidemic on nutrient cycling and water quality while integrating recent and relevant hydrol. findings, along with suggesting necessary future research avenues. Studies generally agree that snow depth will increase in infested forests, though the magnitude is uncertain. Changes in evapotranspiration are more variable as decreased transpiration from tree death may be offset by increased understory evapotranspiration and ground evapn. As a result of such competing hydrol. processes that can affect watershed biogeochem. along with the inherent variability of natural watershed characteristics, water quality changes related to beetle infestation are difficult to predict and may be regionally distinct. However, tree-scale changes to soil-water chem. (N, P, DOC and base cation concns. and compn.) are being obsd. in assocn. with beetle outbreaks which ultimately could lead to larger-scale responses. The different temporal and spatial patterns of bark beetle infestations due to different beetle and tree species lead to inconsistent infestation impacts. Climatic variations and large-scale watershed responses provide a further challenge for predictions due to spatial heterogeneities within a single watershed; conflicting reports from different regions suggest that hydrol. and water quality impacts of the beetle on watersheds cannot be generalized. Research regarding the subsurface water and chem. flow-paths and residence times after a bark beetle epidemic is lacking and needs to be rigorously addressed to best predict watershed or regional-scale changes to soil-water, groundwater, and stream water chem.
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  20. 20
    Kopacek, J.; Hejzlar, J.; Kana, J.; Norton, S. A.; Stuchlik, E. Effects of Acidic Deposition on in-Lake Phosphorus Availability: A Lesson from Lakes Recovering from Acidification Environ. Sci. Technol. 2015, 49 (5) 2895– 2903 DOI: 10.1021/es5058743
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    20
    Effects of Acidic Deposition on in-Lake Phosphorus Availability: A Lesson from Lakes Recovering from Acidification
    Kopacek, Jiri; Hejzlar, Josef; Kana, Jiri; Norton, Stephen A.; Stuchlik, Evzen
    Environmental Science & Technology (2015), 49 (5), 2895-2903CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Lake water concns. of P recently increased in some mountain areas due to elevated atm. input of P-rich dust. We show that increasing P concns. also occur during stable atm. P inputs in central European alpine lakes recovering from atm. acidification. The elevated P availability in the lakes results from (1) increasing terrestrial export of P accompanying elevated leaching of dissolved org. C and decreasing phosphate-adsorption ability of soils due to their increasing pH, and (2) decreasing in-lake P immobilization by Al hydroxide due to decreasing leaching of ionic Al from the recovering soils. The P availability in the recovering lakes is modified by the extent of soil acidification, soil compn., and proportion of till and meadow soils in the catchment. These mechanisms explain several conflicting observations of the acid rain effects on surface water P concns.
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  21. 21
    Tipping, E.; Benham, S.; Boyle, J. F.; Crow, P.; Davies, J.; Fischer, U.; Guyatt, H.; Helliwell, R.; Jackson-Blake, L.; Lawlor, A. J.; Monteith, D. T.; Rowe, E. C.; Toberman, H. Atmospheric deposition of phosphorus to land and freshwater Environ. Sci.-Process Impacts 2014, 16 (7) 1608– 1617 DOI: 10.1039/C3EM00641G
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    21
    Atmospheric deposition of phosphorus to land and freshwater
    Tipping, E.; Benham, S.; Boyle, J. F.; Crow, P.; Davies, J.; Fischer, U.; Guyatt, H.; Helliwell, R.; Jackson-Blake, L.; Lawlor, A. J.; Monteith, D. T.; Rowe, E. C.; Toberman, H.
    Environmental Science: Processes & Impacts (2014), 16 (7), 1608-1617CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)
    We compiled published and newly-obtained data on the directly-measured atm. deposition of total phosphorus (TP), filtered total phosphorus (FTP), and inorg. phosphorus (PO4-P) to open land, lakes, and marine coasts. The resulting global data base includes data for c. 250 sites, covering the period 1954 to 2012. Most (82%) of the measurement locations are in Europe and North America, with 44 in Africa, Asia, Oceania, and South-Central America. The deposition rates are log-normally distributed, and for the whole data set the geometric mean deposition rates are 0.027, 0.019 and 0.14 g m-2 a-1 for TP, FTP and PO4-P resp. At smaller scales there is little systematic spatial variation, except for high deposition rates at some sites in Germany, likely due to local agricultural sources. In cases for which PO4-P was detd. as well as one of the other forms of P, strong parallels between logarithmic values were found. Based on the directly-measured deposition rates to land, and published ests. of P deposition to the oceans, we est. a total annual transfer of P to and from the atm. of 3.7 Tg. However, much of the phosphorus in larger particles (principally primary biol. aerosol particles) is probably redeposited near to its origin, so that long-range transport, important for tropical forests, large areas of peatland and the oceans, mainly involves fine dust from deserts and soils, as described by the simulations of Mahowald et al. (Global Biogeochem. Cycles 22, GB4026, 2008). We suggest that local release to the atm. and subsequent deposition bring about a pseudo-diffusive redistribution of P in the landscape, with P-poor ecosystems, for example ombrotrophic peatlands and oligotrophic lakes, gaining at the expense of P-rich ones. Simple calcns. suggest that atm. transport could bring about significant local redistribution of P among terrestrial ecosystems. Although most atmospherically transported P is natural in origin, local transfers from fertilised farmland to P-poor ecosystems may be significant, and this requires further research.
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  22. 22
    Brahney, J.; Ballantyne, A.; Kociolek, P.; Spaulding, S. A.; Otu, M.; Porwoll, T.; Neff, J. C. Dust mediated transfer of phosphorus to alpine lake ecosystems of the Wind River Range, Wyoming Biogeochemistry 2014, 120 (1–3) 259– 278 DOI: 10.1007/s10533-014-9994-x
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    22
    Dust mediated transfer of phosphorus to alpine lake ecosystems of the Wind River Range, Wyoming, USA
    Brahney, J.; Ballantyne, A. P.; Kociolek, P.; Spaulding, S.; Otu, M.; Porwoll, T.; Neff, J. C.
    Biogeochemistry (2014), 120 (1-3), 259-278CODEN: BIOGEP; ISSN:0168-2563. (Springer)
    Alpine lakes receive a large fraction of their nutrients from atm. sources and are consequently sensitive to variations in both the amt. and chem. of atm. deposition. In this study we explored the spatial changes in lake water chem. and biol. along a gradient of dust deposition in the Wind River Range, Wyoming. Regional differences were explored using the variation in bulk deposition, lake water, sediment, and bedrock geochem. and catchment characteristics. Dust deposition rates in the Southwestern region averaged 3.34 g m-2 year-1, approx. three times higher than deposition rates in the Northwestern region (av. 1.06 g m-2 year-1). Dust-P deposition rates ranged from 87 μg P m2 day-1 in the Northwestern region to 276 μg P m2 day-1 in the Southwestern region. Subalpine and alpine lakes in the Southwestern region had greater total phosphorus (TP) concns. (5-13 μg L-1) and greater sediment phosphorus (SP) concns. (2-5 mg g-1) than similar lakes elsewhere in the region (1-8 μg L-1 TP, 0.5-2 mg g-1 SP). Lake phosphorus concns. were related to dissolved org. carbon (DOC) across vegetation gradients, but related to the percent of bare rock, catchment area to lake area, and catchment steepness across dust deposition gradients. Modern phytoplankton and zooplankton biomasses were two orders of magnitude greater in the Southwest than in the Northwest, and alpine lakes in the Southwest had a unique diatom species assemblage with relatively higher concns. of Asterionella formosa, Pseudostaurosirapseudoconstruens, and Pseudostaurosira brevistriata. These results suggests that catchment controls on P export to lakes (i.e. DOC) are overridden in dominantly bare rock basins where poor soils cannot effectively retain dust deposited P.
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  23. 23
    Brahney, J.; Ballantyne, A. P.; Kociolek, P.; Leavitt, P. R.; Farmer, G. L.; Neff, J. C. Ecological changes in two contrasting lakes associated with human activity and dust transport in western Wyoming Limnol. Oceanogr. 2015, 60, 678– 695 DOI: 10.1002/lno.10050
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    23
    Ecological changes in two contrasting lakes associated with human activity and dust transport in western Wyoming
    Brahney, J.; Ballantyne, A. P.; Kociolek, P.; Leavitt, P. R.; Farmer, G. L.; Neff, J. C.
    Limnology and Oceanography (2015), 60 (2), 678-695CODEN: LIOCAH; ISSN:0024-3590. (John Wiley & Sons, Inc.)
    The atm. transport and deposition of aerosols has the potential to influence the chem. and biol. of oligotrophic alpine lakes. In recent decades, dust and nitrogen emissions to alpine ecosystems have increased across large areas of the western U.S., including Wyoming. Here, we use sediment geochem. and 87Sr/86Sr and 143Nd/144Nd isotopes to examine historical dust deposition rates to alpine lakes in the southwestern region of the Wind River Range, Wyoming. We evaluate the biol. response using diatom fossil assemblages and sediment pigment concns. Sediment core analyses indicated that prior to a recent rise in dust flux, phosphorus concns. and species compn. were similar to those found in other alpine lakes in the region. Concomitant with a ∼50 fold increase in dust flux to the sediments circa 1940, sediment proxies revealed a two- to threefold increase in normalized sediment phosphorus content, an increase in the diatom-inferred total dissolved phosphorus concn. from ∼ 4 to 9-12 μg L-1, a tenfold increase in diatom prodn., and a relative increase in cyanobacteria abundance. The increase in dust influx during the 20th century appears to be due in part to human factors and demonstrates the potential for dust and other atm. pollutants to significantly alter remote aquatic ecosystems.
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    Homyak, P. M.; Sickman, J. O.; Melack, J. M. Pools, transformations, and sources of P in high-elevation soils: Implications for nutrient transfer to Sierra Nevada lakes Geoderma 2014, 217–218, 65– 73 DOI: 10.1016/j.geoderma.2013.11.003
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    Pools, transformations, and sources of P in high-elevation soils: Implications for nutrient transfer to Sierra Nevada lakes
    Homyak, Peter M.; Sickman, James O.; Melack, John M.
    Geoderma (2014), 217-218 (), 65-73CODEN: GEDMAB; ISSN:0016-7061. (Elsevier B.V.)
    In high-elevation lakes of the Sierra Nevada (California), increases in P supply have been inferred from shifts in P to N limitation. To examine factors possibly leading to changes in P supply, we measured pools and transformations in soil P, and developed a long-term mass balance to est. the contribution of parent material weathering to soil P stocks. Common Sierra Nevada soils were found to not be P-deficient and to be retentive of P due to the influence of Fe- and Al-oxides. Total P averaged 867 μg P g- 1 in the top 10 cm of soil (O and A horizons) and 597 μg P g- 1 in the 10-60 cm depth (B horizons), of which 70% in A horizons and 60% in B horizons was freely exchangeable or assocd. with Fe and Al. Weathering of parent material explained 69% of the P found in soils and lost from the catchment since deglaciation, implying that long-term atm. P deposition (0.02 kg ha- 1 yr- 1) represented the balance of P inputs (31%) during the past 10,000 years of soil development. During spring snowmelt ∼ 27% of the total soil P was transferred between org. and inorg. pools; av. inorg. P pools decreased by 232 μg P g- 1, while org. P pools increased by 242 μg P g- 1. Microbial biomass P was highest during winter and decreased six-fold to a min. in the fall. Interactions between hydrol. and biol. processes strongly influence the rate of P transfer from catchment soils to lakes.
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    Morales-Baquero, R.; Pulido-Villena, E.; Reche, I. Atmospheric inputs of phosphorus and nitrogen to the southwest Mediterranean region: Biogeochemical responses of high mountain lakes Limnol. Oceanogr. 2006, 51 (2) 830– 837 DOI: 10.4319/lo.2006.51.2.0830
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    25
    Atmospheric inputs of phosphorus and nitrogen to the southwest mediterranean region: biogeochemical responses of high mountain lakes
    Morales-Baquero, Rafael; Pulido-Villena, Elvira; Reche, Isabel
    Limnology and Oceanography (2006), 51 (2), 830-837CODEN: LIOCAH; ISSN:0024-3590. (American Society of Limnology and Oceanography)
    We quantified dry and wet deposition of dust, nitrogen, and phosphorus over the southwest Mediterranean region (Sierra Nevada, Spain) and assessed its effects on the nutrient status and the chlorophyll a (Chl a) concn. in two high mountain lakes. Atm. deposition of particulate matter (PM) and total phosphorus (TP) were mainly assocd. with dryfall and showed a seasonal pattern similar to that reported for Saharan dust export toward the Mediterranean region, with maxima during spring and summer. In contrast, total nitrogen (TN) deposition was related to rainfall and did not follow the pattern obsd. for PM and TP. The molar TN:TP ratio was significantly lower (i.e., phosphorus-enriched) in dry deposition (TN vs. TP slope = 11.2) than in wet deposition (TN vs. TP slope = 95.5). In the study lakes, the molar TN:TP ratios and the Chl a concns. were significantly influenced by the molar TN:TP ratio and the TP content of atm. deposition, resp. Lake responses were more pronounced in the more phosphorous-limited system. These results establish a direct connection between atm. deposition and lake nutrient status and Chl a, making evident that in the Mediterranean region these inputs are an important source of phosphorous affecting biogeochem. of oligotrophic systems.
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  26. 26
    Mahowald, N.; Jickells, T. D.; Baker, A. R.; Artaxo, P.; Benitez-Nelson, C. R.; Bergametti, G.; Bond, T. C.; Chen, Y.; Cohen, D. D.; Herut, B.; Kubilay, N.; Losno, R.; Luo, C.; Maenhaut, W.; McGee, K. A.; Okin, G. S.; Siefert, R. L.; Tsukuda, S. Global distribution of atmospheric phosphorus sources, concentrations and deposition rates, and anthropogenic impacts Global Biogeochemical Cycles 2008, 22, GB4026 DOI: 10.1029/2008GB003240
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    Global distribution of atmospheric phosphorus sources, concentrations and deposition rates, and anthropogenic impacts
    Mahowald, Natalie; Jickells, Timothy D.; Baker, Alex R.; Artaxo, Paulo; Benitez-Nelson, Claudia R.; Bergametti, Gilles; Bond, Tami C.; Chen, Ying; Cohen, David D.; Herut, Barak; Kubilay, Nilgun; Losno, Remi; Luo, Chao; Maenhaut, Willy; McGee, Kenneth A.; Okin, Gregory S.; Siefert, Ronald L.; Tsukuda, Seigen
    Global Biogeochemical Cycles (2008), 22 (4), GB4026/1-GB4026/19, 6 platesCODEN: GBCYEP; ISSN:0886-6236. (American Geophysical Union)
    A worldwide compilation of atm. total phosphorus (TP) and phosphate (PO4) concn. and deposition flux observations are combined with transport model simulations to derive the global distribution of concns. and deposition fluxes of TP and PO4. Our results suggest that mineral aerosols are the dominant source of TP on a global scale (82%), with primary biogenic particles (12%) and combustion sources (5%) important in nondusty regions. Globally averaged anthropogenic inputs are estd. to be ∼5 and 15% for TP and PO4, resp., and may contribute as much as 50% to the deposition over the oligotrophic ocean where productivity may be phosphorus-limited. There is a net loss of TP from many (but not all) land ecosystems and a net gain of TP by the oceans (560 Gg P a-1). More measurements of atm. TP and PO4 will assist in reducing uncertainties in our understanding of the role that atm. phosphorus may play in global biogeochem.
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    Wang, R.; Balkanski, Y.; Boucher, O.; Ciais, P.; Penuelas, J.; Tao, S. Significant contribution of combustion-related emissions to the atmospheric phosphorus budget Nat. Geosci. 2014, 8 (1) 48– 54 DOI: 10.1038/ngeo2324
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    Dahms, D. E.; Rawlins, C. L. A two-year record of eolian sedimentation in the Wind River Range, Wyoming, USA Arct. Alp. Res. 1996, 28 (2) 210– 216 DOI: 10.2307/1551762
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    Lawrence, C. R.; Neff, J. The contemporary physical and chemical flux of Aeolian dust: a synthesis of direct measurements of dust deposition Chem. Geol. 2009, 267 (1–2) 46– 63 DOI: 10.1016/j.chemgeo.2009.02.005
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    The contemporary physical and chemical flux of aeolian dust: A synthesis of direct measurements of dust deposition
    Lawrence, Corey R.; Neff, Jason C.
    Chemical Geology (2009), 267 (1-2), 46-63CODEN: CHGEAD; ISSN:0009-2541. (Elsevier B.V.)
    The deposition of aeolian, or windblown, dust is widely recognized as an important phys. and chem. flux to ecosystems. Dust deposition adds exogenous mineral and org. material to terrestrial surfaces and can be important for the biogeochem. cycling of nutrients. There have been many studies that characterize the phys. and chem. compn. of dust. However, few studies have synthesized these observations in order to examine patterns geochem. fluxes. We have compiled observations of dust deposition rates, particle size distributions (PSD), mineralogy and bulk elemental and org. chem. The rates of dust deposition obsd. across the globe vary from almost 0 to ≥ 450 g/m2.yr. Sites receiving dust deposition can be partitioned into broad categories based on there distance from dust source regions. When compared to global dust models our results suggest some models may underestimate dust deposition rates at the regional and local scales. The distance from the source region that dust is deposited also influences the particle size distributions, mineralogy, and chem. compn. of dust; however, more consistent dust sampling and geochem. analyses are needed to better constrain these spatial patterns. On av., the concns. of most major elements (Si, Al, Fe, Mg, Ca, K) in aeolian dust tend to be similar (± 20%) to the compn. of the upper continental crust (UCC), but there is substantial variability from sample to sample. In contrast, some elements tend to be depleted (Na) or enriched (Ti) in dust, likely as a result of soil weathering processes prior to dust emissions. Trace elements, esp. heavy metals, are consistently enriched in dust relative to the UCC. Ecol. important nutrients, such as N and P, are also present in dust deposition. The geochem. flux attributable to dust deposition can be substantial in ecosystems located proximal to dust source regions. We calc. ests. of elemental flux rates based on the av. chem. compn. of aeolian dust and varying rates of deposition. These estd. flux rates are useful as a rough gauge of the degree to which dust deposition may influence biogeochem. cycling in terrestrial ecosystems and should be utilized to better constrain deposition ests. of global dust models.
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  • Abstract

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    Figure 1

    Figure 1. Cumulative frequency distributions of TP concentrations in the population of (a) streams and (b) lakes in the conterminous U.S. Vertical axes are the cumulative proportion of stream length or lake count with concentrations less than or equal to the corresponding horizontal axis value. Lines are weighted population estimates and 95% confidence intervals for (a) total stream length in 2000–2004, 2008–2009, and 2013–2014 (2008–2009 and 2013–2014 data exclude rivers, which were not included in the 2000–2004 survey) and (b) total numbers of lakes in 2007 versus 2012 (excludes lakes with surface area of <4 ha, which were not included in the 2007 survey).

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    Figure 2

    Figure 2. Comparison of (a–c) TP concentrations and (d–f) TN concentrations at sites in minimally disturbed catchments for (a and d) 91 streams included in both the 2000–2004 and 2008–2009 surveys, (b and e) 47 resurveyed sites from the 2007 and 2012 lake surveys, and (c and f) 52 resurveyed sites from the 2008–2009 and 2013–2014 stream surveys. Lines are 1:1 lines. In each case, points above the 1:1 line indicate increased concentrations in the later survey. The p values are from weighted, paired-sample t tests. Values below analytical detection limits (MDLs) have been set to 1/2 of the MDL for that time period (observable, for example, at the far left of panel a).

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    Figure 3

    Figure 3. Locations of resurveyed sites in minimally disturbed watersheds and annual rate of TP change measured between paired surveys. Rates of change are μg L–1 year–1.

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  • References

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      Environmental Science & Technology (2015), 49 (5), 2895-2903CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Lake water concns. of P recently increased in some mountain areas due to elevated atm. input of P-rich dust. We show that increasing P concns. also occur during stable atm. P inputs in central European alpine lakes recovering from atm. acidification. The elevated P availability in the lakes results from (1) increasing terrestrial export of P accompanying elevated leaching of dissolved org. C and decreasing phosphate-adsorption ability of soils due to their increasing pH, and (2) decreasing in-lake P immobilization by Al hydroxide due to decreasing leaching of ionic Al from the recovering soils. The P availability in the recovering lakes is modified by the extent of soil acidification, soil compn., and proportion of till and meadow soils in the catchment. These mechanisms explain several conflicting observations of the acid rain effects on surface water P concns.
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    21. 21
      Tipping, E.; Benham, S.; Boyle, J. F.; Crow, P.; Davies, J.; Fischer, U.; Guyatt, H.; Helliwell, R.; Jackson-Blake, L.; Lawlor, A. J.; Monteith, D. T.; Rowe, E. C.; Toberman, H. Atmospheric deposition of phosphorus to land and freshwater Environ. Sci.-Process Impacts 2014, 16 (7) 1608– 1617 DOI: 10.1039/C3EM00641G
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      21
      Atmospheric deposition of phosphorus to land and freshwater
      Tipping, E.; Benham, S.; Boyle, J. F.; Crow, P.; Davies, J.; Fischer, U.; Guyatt, H.; Helliwell, R.; Jackson-Blake, L.; Lawlor, A. J.; Monteith, D. T.; Rowe, E. C.; Toberman, H.
      Environmental Science: Processes & Impacts (2014), 16 (7), 1608-1617CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)
      We compiled published and newly-obtained data on the directly-measured atm. deposition of total phosphorus (TP), filtered total phosphorus (FTP), and inorg. phosphorus (PO4-P) to open land, lakes, and marine coasts. The resulting global data base includes data for c. 250 sites, covering the period 1954 to 2012. Most (82%) of the measurement locations are in Europe and North America, with 44 in Africa, Asia, Oceania, and South-Central America. The deposition rates are log-normally distributed, and for the whole data set the geometric mean deposition rates are 0.027, 0.019 and 0.14 g m-2 a-1 for TP, FTP and PO4-P resp. At smaller scales there is little systematic spatial variation, except for high deposition rates at some sites in Germany, likely due to local agricultural sources. In cases for which PO4-P was detd. as well as one of the other forms of P, strong parallels between logarithmic values were found. Based on the directly-measured deposition rates to land, and published ests. of P deposition to the oceans, we est. a total annual transfer of P to and from the atm. of 3.7 Tg. However, much of the phosphorus in larger particles (principally primary biol. aerosol particles) is probably redeposited near to its origin, so that long-range transport, important for tropical forests, large areas of peatland and the oceans, mainly involves fine dust from deserts and soils, as described by the simulations of Mahowald et al. (Global Biogeochem. Cycles 22, GB4026, 2008). We suggest that local release to the atm. and subsequent deposition bring about a pseudo-diffusive redistribution of P in the landscape, with P-poor ecosystems, for example ombrotrophic peatlands and oligotrophic lakes, gaining at the expense of P-rich ones. Simple calcns. suggest that atm. transport could bring about significant local redistribution of P among terrestrial ecosystems. Although most atmospherically transported P is natural in origin, local transfers from fertilised farmland to P-poor ecosystems may be significant, and this requires further research.
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    22. 22
      Brahney, J.; Ballantyne, A.; Kociolek, P.; Spaulding, S. A.; Otu, M.; Porwoll, T.; Neff, J. C. Dust mediated transfer of phosphorus to alpine lake ecosystems of the Wind River Range, Wyoming Biogeochemistry 2014, 120 (1–3) 259– 278 DOI: 10.1007/s10533-014-9994-x
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      22
      Dust mediated transfer of phosphorus to alpine lake ecosystems of the Wind River Range, Wyoming, USA
      Brahney, J.; Ballantyne, A. P.; Kociolek, P.; Spaulding, S.; Otu, M.; Porwoll, T.; Neff, J. C.
      Biogeochemistry (2014), 120 (1-3), 259-278CODEN: BIOGEP; ISSN:0168-2563. (Springer)
      Alpine lakes receive a large fraction of their nutrients from atm. sources and are consequently sensitive to variations in both the amt. and chem. of atm. deposition. In this study we explored the spatial changes in lake water chem. and biol. along a gradient of dust deposition in the Wind River Range, Wyoming. Regional differences were explored using the variation in bulk deposition, lake water, sediment, and bedrock geochem. and catchment characteristics. Dust deposition rates in the Southwestern region averaged 3.34 g m-2 year-1, approx. three times higher than deposition rates in the Northwestern region (av. 1.06 g m-2 year-1). Dust-P deposition rates ranged from 87 μg P m2 day-1 in the Northwestern region to 276 μg P m2 day-1 in the Southwestern region. Subalpine and alpine lakes in the Southwestern region had greater total phosphorus (TP) concns. (5-13 μg L-1) and greater sediment phosphorus (SP) concns. (2-5 mg g-1) than similar lakes elsewhere in the region (1-8 μg L-1 TP, 0.5-2 mg g-1 SP). Lake phosphorus concns. were related to dissolved org. carbon (DOC) across vegetation gradients, but related to the percent of bare rock, catchment area to lake area, and catchment steepness across dust deposition gradients. Modern phytoplankton and zooplankton biomasses were two orders of magnitude greater in the Southwest than in the Northwest, and alpine lakes in the Southwest had a unique diatom species assemblage with relatively higher concns. of Asterionella formosa, Pseudostaurosirapseudoconstruens, and Pseudostaurosira brevistriata. These results suggests that catchment controls on P export to lakes (i.e. DOC) are overridden in dominantly bare rock basins where poor soils cannot effectively retain dust deposited P.
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    23. 23
      Brahney, J.; Ballantyne, A. P.; Kociolek, P.; Leavitt, P. R.; Farmer, G. L.; Neff, J. C. Ecological changes in two contrasting lakes associated with human activity and dust transport in western Wyoming Limnol. Oceanogr. 2015, 60, 678– 695 DOI: 10.1002/lno.10050
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      23
      Ecological changes in two contrasting lakes associated with human activity and dust transport in western Wyoming
      Brahney, J.; Ballantyne, A. P.; Kociolek, P.; Leavitt, P. R.; Farmer, G. L.; Neff, J. C.
      Limnology and Oceanography (2015), 60 (2), 678-695CODEN: LIOCAH; ISSN:0024-3590. (John Wiley & Sons, Inc.)
      The atm. transport and deposition of aerosols has the potential to influence the chem. and biol. of oligotrophic alpine lakes. In recent decades, dust and nitrogen emissions to alpine ecosystems have increased across large areas of the western U.S., including Wyoming. Here, we use sediment geochem. and 87Sr/86Sr and 143Nd/144Nd isotopes to examine historical dust deposition rates to alpine lakes in the southwestern region of the Wind River Range, Wyoming. We evaluate the biol. response using diatom fossil assemblages and sediment pigment concns. Sediment core analyses indicated that prior to a recent rise in dust flux, phosphorus concns. and species compn. were similar to those found in other alpine lakes in the region. Concomitant with a ∼50 fold increase in dust flux to the sediments circa 1940, sediment proxies revealed a two- to threefold increase in normalized sediment phosphorus content, an increase in the diatom-inferred total dissolved phosphorus concn. from ∼ 4 to 9-12 μg L-1, a tenfold increase in diatom prodn., and a relative increase in cyanobacteria abundance. The increase in dust influx during the 20th century appears to be due in part to human factors and demonstrates the potential for dust and other atm. pollutants to significantly alter remote aquatic ecosystems.
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      Homyak, P. M.; Sickman, J. O.; Melack, J. M. Pools, transformations, and sources of P in high-elevation soils: Implications for nutrient transfer to Sierra Nevada lakes Geoderma 2014, 217–218, 65– 73 DOI: 10.1016/j.geoderma.2013.11.003
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      Pools, transformations, and sources of P in high-elevation soils: Implications for nutrient transfer to Sierra Nevada lakes
      Homyak, Peter M.; Sickman, James O.; Melack, John M.
      Geoderma (2014), 217-218 (), 65-73CODEN: GEDMAB; ISSN:0016-7061. (Elsevier B.V.)
      In high-elevation lakes of the Sierra Nevada (California), increases in P supply have been inferred from shifts in P to N limitation. To examine factors possibly leading to changes in P supply, we measured pools and transformations in soil P, and developed a long-term mass balance to est. the contribution of parent material weathering to soil P stocks. Common Sierra Nevada soils were found to not be P-deficient and to be retentive of P due to the influence of Fe- and Al-oxides. Total P averaged 867 μg P g- 1 in the top 10 cm of soil (O and A horizons) and 597 μg P g- 1 in the 10-60 cm depth (B horizons), of which 70% in A horizons and 60% in B horizons was freely exchangeable or assocd. with Fe and Al. Weathering of parent material explained 69% of the P found in soils and lost from the catchment since deglaciation, implying that long-term atm. P deposition (0.02 kg ha- 1 yr- 1) represented the balance of P inputs (31%) during the past 10,000 years of soil development. During spring snowmelt ∼ 27% of the total soil P was transferred between org. and inorg. pools; av. inorg. P pools decreased by 232 μg P g- 1, while org. P pools increased by 242 μg P g- 1. Microbial biomass P was highest during winter and decreased six-fold to a min. in the fall. Interactions between hydrol. and biol. processes strongly influence the rate of P transfer from catchment soils to lakes.
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      Morales-Baquero, R.; Pulido-Villena, E.; Reche, I. Atmospheric inputs of phosphorus and nitrogen to the southwest Mediterranean region: Biogeochemical responses of high mountain lakes Limnol. Oceanogr. 2006, 51 (2) 830– 837 DOI: 10.4319/lo.2006.51.2.0830
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      Atmospheric inputs of phosphorus and nitrogen to the southwest mediterranean region: biogeochemical responses of high mountain lakes
      Morales-Baquero, Rafael; Pulido-Villena, Elvira; Reche, Isabel
      Limnology and Oceanography (2006), 51 (2), 830-837CODEN: LIOCAH; ISSN:0024-3590. (American Society of Limnology and Oceanography)
      We quantified dry and wet deposition of dust, nitrogen, and phosphorus over the southwest Mediterranean region (Sierra Nevada, Spain) and assessed its effects on the nutrient status and the chlorophyll a (Chl a) concn. in two high mountain lakes. Atm. deposition of particulate matter (PM) and total phosphorus (TP) were mainly assocd. with dryfall and showed a seasonal pattern similar to that reported for Saharan dust export toward the Mediterranean region, with maxima during spring and summer. In contrast, total nitrogen (TN) deposition was related to rainfall and did not follow the pattern obsd. for PM and TP. The molar TN:TP ratio was significantly lower (i.e., phosphorus-enriched) in dry deposition (TN vs. TP slope = 11.2) than in wet deposition (TN vs. TP slope = 95.5). In the study lakes, the molar TN:TP ratios and the Chl a concns. were significantly influenced by the molar TN:TP ratio and the TP content of atm. deposition, resp. Lake responses were more pronounced in the more phosphorous-limited system. These results establish a direct connection between atm. deposition and lake nutrient status and Chl a, making evident that in the Mediterranean region these inputs are an important source of phosphorous affecting biogeochem. of oligotrophic systems.
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      Mahowald, N.; Jickells, T. D.; Baker, A. R.; Artaxo, P.; Benitez-Nelson, C. R.; Bergametti, G.; Bond, T. C.; Chen, Y.; Cohen, D. D.; Herut, B.; Kubilay, N.; Losno, R.; Luo, C.; Maenhaut, W.; McGee, K. A.; Okin, G. S.; Siefert, R. L.; Tsukuda, S. Global distribution of atmospheric phosphorus sources, concentrations and deposition rates, and anthropogenic impacts Global Biogeochemical Cycles 2008, 22, GB4026 DOI: 10.1029/2008GB003240
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      Global distribution of atmospheric phosphorus sources, concentrations and deposition rates, and anthropogenic impacts
      Mahowald, Natalie; Jickells, Timothy D.; Baker, Alex R.; Artaxo, Paulo; Benitez-Nelson, Claudia R.; Bergametti, Gilles; Bond, Tami C.; Chen, Ying; Cohen, David D.; Herut, Barak; Kubilay, Nilgun; Losno, Remi; Luo, Chao; Maenhaut, Willy; McGee, Kenneth A.; Okin, Gregory S.; Siefert, Ronald L.; Tsukuda, Seigen
      Global Biogeochemical Cycles (2008), 22 (4), GB4026/1-GB4026/19, 6 platesCODEN: GBCYEP; ISSN:0886-6236. (American Geophysical Union)
      A worldwide compilation of atm. total phosphorus (TP) and phosphate (PO4) concn. and deposition flux observations are combined with transport model simulations to derive the global distribution of concns. and deposition fluxes of TP and PO4. Our results suggest that mineral aerosols are the dominant source of TP on a global scale (82%), with primary biogenic particles (12%) and combustion sources (5%) important in nondusty regions. Globally averaged anthropogenic inputs are estd. to be ∼5 and 15% for TP and PO4, resp., and may contribute as much as 50% to the deposition over the oligotrophic ocean where productivity may be phosphorus-limited. There is a net loss of TP from many (but not all) land ecosystems and a net gain of TP by the oceans (560 Gg P a-1). More measurements of atm. TP and PO4 will assist in reducing uncertainties in our understanding of the role that atm. phosphorus may play in global biogeochem.
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      Wang, R.; Balkanski, Y.; Boucher, O.; Ciais, P.; Penuelas, J.; Tao, S. Significant contribution of combustion-related emissions to the atmospheric phosphorus budget Nat. Geosci. 2014, 8 (1) 48– 54 DOI: 10.1038/ngeo2324
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      Lawrence, C. R.; Neff, J. The contemporary physical and chemical flux of Aeolian dust: a synthesis of direct measurements of dust deposition Chem. Geol. 2009, 267 (1–2) 46– 63 DOI: 10.1016/j.chemgeo.2009.02.005
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      The contemporary physical and chemical flux of aeolian dust: A synthesis of direct measurements of dust deposition
      Lawrence, Corey R.; Neff, Jason C.
      Chemical Geology (2009), 267 (1-2), 46-63CODEN: CHGEAD; ISSN:0009-2541. (Elsevier B.V.)
      The deposition of aeolian, or windblown, dust is widely recognized as an important phys. and chem. flux to ecosystems. Dust deposition adds exogenous mineral and org. material to terrestrial surfaces and can be important for the biogeochem. cycling of nutrients. There have been many studies that characterize the phys. and chem. compn. of dust. However, few studies have synthesized these observations in order to examine patterns geochem. fluxes. We have compiled observations of dust deposition rates, particle size distributions (PSD), mineralogy and bulk elemental and org. chem. The rates of dust deposition obsd. across the globe vary from almost 0 to ≥ 450 g/m2.yr. Sites receiving dust deposition can be partitioned into broad categories based on there distance from dust source regions. When compared to global dust models our results suggest some models may underestimate dust deposition rates at the regional and local scales. The distance from the source region that dust is deposited also influences the particle size distributions, mineralogy, and chem. compn. of dust; however, more consistent dust sampling and geochem. analyses are needed to better constrain these spatial patterns. On av., the concns. of most major elements (Si, Al, Fe, Mg, Ca, K) in aeolian dust tend to be similar (± 20%) to the compn. of the upper continental crust (UCC), but there is substantial variability from sample to sample. In contrast, some elements tend to be depleted (Na) or enriched (Ti) in dust, likely as a result of soil weathering processes prior to dust emissions. Trace elements, esp. heavy metals, are consistently enriched in dust relative to the UCC. Ecol. important nutrients, such as N and P, are also present in dust deposition. The geochem. flux attributable to dust deposition can be substantial in ecosystems located proximal to dust source regions. We calc. ests. of elemental flux rates based on the av. chem. compn. of aeolian dust and varying rates of deposition. These estd. flux rates are useful as a rough gauge of the degree to which dust deposition may influence biogeochem. cycling in terrestrial ecosystems and should be utilized to better constrain deposition ests. of global dust models.
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      Smith, E. A.; Mayfield, C. I.; Wong, P. T. S. Naturally Occurring Apatite as a Source of Ortho-Phosphate for Growth of Bacteria and Algae Microb. Ecol. 1977, 4 (2) 105– 117 DOI: 10.1007/BF02014281
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      Naturally occurring apatite as a source of orthophosphate for growth of bacteria and algae
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      Several naturally occurring calcium-phosphate apatites which varied in crystalline structure and ionic composition were added as crystals of different particle size to P-free (<1μg/liter total P) nutrient media. Sufficient ortho-PO 4 (3-) was released by the partial dissolution of apatite crystals at limnetic pH levels (pH 7.8) to support growth of several unialgal-mixed bacterial cultures. The biomass produced by mixed populations increased as the amount of available apatite was increased and as the pH of the media and the particle size of the apatite crystals were decreased. These findings suggest that although apatite characteristically displays reduced solubility under alkaline conditions, the tons of apatite which are continuously entering aquatic environments as erosion material may be contributing to the P loading of those ecosystems.
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      Brahney, J.; Mahowald, N.; Ward, D. S.; Ballantyne, A. P.; Neff, J. C. Is atmospheric phosphorus pollution altering global alpine Lake stoichiometry? Global Biogeochemical Cycles 2015, 29 (9) 1369– 1383 DOI: 10.1002/2015GB005137
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      Is atmospheric phosphorus pollution altering global alpine Lake stoichiometry?
      Brahney, Janice; Mahowald, Natalie; Ward, Daniel S.; Ballantyne, Ashley P.; Neff, Jason C.
      Global Biogeochemical Cycles (2015), 29 (9), 1369-1383CODEN: GBCYEP; ISSN:1944-9224. (Wiley-Blackwell)
      Anthropogenic activities have significantly altered atm. chem. and changed the global mobility of key macronutrients. Here we show that contemporary global patterns in nitrogen (N) and phosphorus (P) emissions drive large hemispheric variation in pptn. chem. These global patterns of nutrient emission and deposition (N:P) are in turn closely reflected in the water chem. of naturally oligotrophic lakes (r2 = 0.81, p < 0.0001). Obsd. increases in anthropogenic N deposition play a role in nutrient concns. (r2 = 0.20, p < 0.05); however, atm. deposition of P appears to be major contributor to this pattern (r2 = 0.65, p < 0.0001). Atm. simulations indicate a global increase in P deposition by 1.4 times the preindustrial rate largely due to increased dust and biomass burning emissions. Although changes in the mass flux of global P deposition are smaller than for N, the impacts on primary productivity may be greater because, on av., one unit of increased P deposition has 16 times the influence of one unit of N deposition. These stoichiometric considerations, combined with the evidence presented here, suggest that increases in P deposition may be a major driver of alpine Lake trophic status, particularly in the Southern Hemisphere. These results underscore the need for the broader scientific community to consider the impact of atm. phosphorus deposition on the water quality of naturally oligotrophic lakes.
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    • Years of data collection and details of sample sizes for lake and stream surveys used in this analysis (Table S1), MDLs for TP analyses for years representing each survey analyzed in this paper, the proportion of the population (percent stream length or percentage of lake number) with values below the MDL, and the number of resurveyed sites in the minimally disturbed data set (total number in parentheses) with TP less than the corresponding MDL (Table S2), results of blind audit sample analysis for the U.S. EPA laboratory responsible for analyzing survey samples for 2000–2014, corresponding to the time span of statistical surveys reported in this paper (Figure S1), box and whisker plots of unweighted, normalized differences between surveys at minimally disturbed resurveyed sites for TP and selected other chemical variables (TN, conductivity, silica, magnesium, DOC, calcium, and total suspended solids) for (a) stream surveys in 2000–2004 versus 2008–2009, (b) lake surveys in 2007 versus 2012, and (c) stream surveys in 2008–2009 versus 2013–2014, with normalized differences calculated as (survey 2 – survey 1)/mean (survey 1 and survey 2) (Figure S2), and comparison of quarterly runoff (matched to date of each survey sample) in eight digit hydrologic units for each least disturbed catchment from (a) stream surveys in 2000–2004 versus 2008–2009, (b) lake surveys in 2007 versus 2012, and (c) stream surveys in 2008–2009 versus 2013–2014 (lines being 1:1 lines), with only the lake data showing a significant change in runoff between surveys (Figure S3) (PDF)


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