Spatiotemporal patterns of mercury accumulation in lake sediments of western North America.

For the Western North America Mercury Synthesis, we compiled mercury records from 165 dated sediment cores from 138 natural lakes across western North America. Lake sediments are accepted as faithful recorders of historical mercury accumulation rates, and regional and sub-regional temporal and spatial trends were analyzed with descriptive and inferential statistics. Mercury accumulation rates in sediments have increased, on average, four times (4×) from 1850 to 2000 and continue to increase by approximately 0.2µg/m(2) per year. Lakes with the greatest increases were influenced by the Flin Flon smelter, followed by lakes directly affected by mining and wastewater discharges. Of lakes not directly affected by point sources, there is a clear separation in mercury accumulation rates between lakes with no/little watershed development and lakes with extensive watershed development for agricultural and/or residential purposes. Lakes in the latter group exhibited a sharp increase in mercury accumulation rates with human settlement, stabilizing after 1950 at five times (5×) 1850 rates. Mercury accumulation rates in lakes with no/little watershed development were controlled primarily by relative watershed size prior to 1850, and since have exhibited modest increases (in absolute terms and compared to that described above) associated with (regional and global) industrialization. A sub-regional analysis highlighted that in the ecoregion Northwestern Forest Mountains, <1% of mercury deposited to watersheds is delivered to lakes. Research is warranted to understand whether mountainous watersheds act as permanent sinks for mercury or if export of "legacy" mercury (deposited in years past) will delay recovery when/if emissions reductions are achieved.

Spatial trends and factors affecting mercury bioaccumulation in freshwater fishes of Washington State, USA.

Twenty-four lakes in Washington State, United States, were sampled for largemouth and smallmouth bass as well as water chemistry parameters during 2005 to 2009 to evaluate trends in mercury (Hg) concentrations. We analyzed spatial patterns in bass Hg levels across a gradient of land and climate types, lake chemistry parameters, and physical watershed characteristics to identify factors influencing Hg bioaccumulation. Across the state, bass Hg levels followed rainfall patterns and were statistically greater on the coastal west side of the state and lowest in the drier eastern region. Lake and watershed variables with the strongest correlations to Hg bioaccumulation in bass were annual watershed precipitation (+) and lake alkalinity (-). Principal component analysis (PCA) explaining 50.3 % of the variance in the dataset indicated that wet, forested landscapes were more likely to contain lakes with greater fish Hg levels than alkaline lakes in drier agriculture-dominated or open space areas. The PCA did not show wetland abundance and lake DOC levels as variables influencing bass Hg levels, but these were generally associated with small, shallow lakes containing greater chlorophyll levels. The effect of in-lake productivity may have counteracted the role of wetlands in Hg bioaccumulation among this study's lakes.

Relative importance of wastewater treatment plants and non-point sources of perfluorinated compounds to Washington State rivers.

Perfluorinated compounds (PFCs) were measured in 10 Washington State rivers and 4 wastewater treatment plants (WWTPs) under periods of low and high flows to investigate the relative importance of point and non-point sources to rivers. PFCs were detected in all samples with summed values ranging from 1.11 to 74.9 ng/L in surface waters and 62.3-418 ng/L in WWTP effluent. Concentrations in 6 of the 10 rivers exhibited a positive relationship with flow, indicating runoff as a contributing source, with PFC loads greatest at all 10 waterbodies during high flows. Perfluoroheptanoic acid:perfluorooctanoic acid homologue ratios suggest atmospheric contributions to the waterbodies are important throughout the year. Principal component analysis (PCA) indicated distinct homologue profiles for high flow, low flow, and effluent samples. The PCA demonstrates that during the spring when flows and loads are at their greatest; WWTP discharges are not the primary sources of PFCs to the river systems. Taken together, the evidence provided signifies non-point inputs are a major pathway for PFCs to surface waters in Washington State.

Wastewater dilution index partially explains observed polybrominated diphenyl ether flame retardant concentrations in osprey eggs from Columbia River Basin, 2008-2009.

Several polybrominated biphenyl ether (PBDE) congeners were found in all 175 osprey (Pandion haliaetus) eggs collected from the Columbia River Basin between 2002 and 2009. ΣPBDE concentrations in 2008-2009 were highest in osprey eggs from the two lowest flow rivers studied; however, each river flowed through relatively large and populous metropolitan areas (Boise, Idaho and Spokane, Washington). We used the volume of Wastewater Treatment Plant (WWTP) discharge, a known source of PBDEs, as a measure of human activity at a location, and combined with river flow (both converted to millions of gallons/day) created a novel approach (an approximate Dilution Index) to relate waterborne contaminants to levels of these contaminants that reach avian eggs. This approach provided a useful understanding of the spatial osprey egg concentration patterns observed. Individual osprey egg concentrations along the Upper Willamette River co-varied with the Dilution Index, while combined egg data (geometric means) from rivers or segments of rivers showed a strong, significant relationship to the Dilution Index with one exception, the Boise River. There, we believe osprey egg concentrations were lower than expected because Boise River ospreys foraged perhaps 50-75% of the time off the river at ponds and lakes stocked with fish that contained relatively low ΣPBDE concentrations. Our limited temporal data at specific localities (2004-2009) suggests that ΣPBDE concentrations in osprey eggs peaked between 2005 and 2007, and then decreased, perhaps in response to penta- and octa-PBDE technical mixtures no longer being used in the USA after 2004. Empirical estimates of biomagnification factors (BMFs) from fish to osprey eggs were 3.76-7.52 on a wet weight (ww) basis or 4.37-11.0 lipid weight. Our earlier osprey study suggested that ΣPBDE egg concentrations >1,000 ng/g ww may reduce osprey reproductive success. Only two of the study areas sampled in 2008-2009 contained individual eggs with ΣPBDE concentrations >1,000 ng/g, and non-significant (P > 0.30) negative relationships were found between ΣPBDEs and reproductive success. Additional monitoring is required to confirm not only the apparent decline in PBDE concentrations in osprey eggs that occurred during this study, but also to better understand the relationship between PBDEs in eggs and reproductive success.

Mercury accumulation in sediment cores from three Washington state lakes: evidence for local deposition from a coal-fired power plant.

Mercury accumulation rates measured in age-dated sediment cores were compared at three Washington state lakes. Offutt Lake and Lake St. Clair are located immediately downwind (18 and 28 km, respectively) of a coal-fired power plant and Lake Sammamish is located outside of the immediate area of the plant (110 km). The sites immediately downwind of the power plant were expected to receive increased mercury deposition from particulate and reactive mercury not deposited at Lake Sammamish. Mercury accumulation in cores was corrected for variable sedimentation, background, and sediment focusing to estimate the anthropogenic contribution (Hg(A,F)). Results indicated lakes immediately downwind of the power plant contained elevated Hg(A,F) levels with respect to the reference lake. Estimated fluxes to Lake Sammamish were compared to measured values from a nearby mercury wet deposition collector to gauge the efficacy of the core deconstruction techniques. Total deposition calculated through the sediment core (20.7 µg/m²/year) fell just outside of the upper estimate (18.9 µg/m²/year) of total deposition approximated from the wet deposition collector.