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Mark C. Marvin-DiPasquale

Publications and source records attributed to Mark C. Marvin-DiPasquale.

At least 19 recordsLinked to original sources

Select elements of concern in surface water of three hydrologic basins (Delaware River, Illinois River, and Upper Colorado River)—Data screening for the development of spatial and temporal models

The report focuses on the screening of previously published concentration data associated with 12 elements of concern (aluminum, arsenic, cadmium, chromium, copper, iron, mercury, manganese, lead, selenium, uranium, and zinc) measured in stream surface waters of three hydrologic basins (Delaware River Basin, Illinois River Basin, and the Upper Colorado River Basin). The purpose of this analysis is to determine what subsets of the original dataset (containing more than 1,500,000 observations) may be most suitable for each of two types of modeling efforts. The first type of modeling envisions a machine learning approach to determine which geospatial attributes are most significant in describing the spatial distribution of elemental concentrations within a basin. The second type of modeling envisions a stepwise regression approach to develop multivariable models that can be used to determine high resolution time-series estimates of elemental concentrations or loads at discrete U.S. Geological Survey real-time stream surface water sites. These site-specific temporal models are based on continuous measurements of available discharge and (or) in situ sensor data (temperature, pH, turbidity, dissolved oxygen, specific conductance, and (or) fluorescent dissolved organic matter) as the explanatory variables. The data screening for both model types considered historical trends in analytical methods and detection quantitation limits, the extent of censored data, data density, and environmental relevance with respect to three U.S. Environmental Protection Agency water quality thresholds (drinking water guidelines, human health criteria, and aquatic life criteria). The result of this analysis was the production of a final list of potential models deemed suitable for further development based upon the data exclusion (or inclusion) scheme developed herein for each model type. In both cases, the final models included mostly the three crustal elements (iron, manganese, and aluminum) that are found at comparatively high concentrations in surface water, whereas most of the more pernicious elements were excluded from the final model lists owing to various data limitations. The one exception to this was arsenic, for which the existing data were sufficient at three U.S. Geological Survey real-time sites for potential further development of time-series models.

Colorado, Delaware, Illinois, Indiana, Maryland, N

Longitudinal and seasonal changes of organic matter sources through a semi-arid river-reservoir system

The quality and quantity of organic matter (OM) in a river system directly affects ecosystem health; thus, managers benefit from an in-depth understanding of the drivers and sources of OM. In the Snake River, a highly altered river-reservoir system in the semi-arid western United States, OM production and loading are key drivers of reservoir anoxia, which leads to several deleterious processes such as mercury methylation. However, sources and quantities of OM to the Snake River, and the effects of impoundment on OM moving through the river-reservoir system, are not well understood. Particulate organic carbon (POC), dissolved organic carbon (DOC), particulate nitrogen (PN), chlorophyll a (chl- a ), and δ 15 N–PN and δ 13 C–POC isotopic ratios were measured bi-weekly for over 2 years at four locations through the Snake River Hells Canyon Reservoir Complex to determine spatial and temporal patterns of OM quantities and sources. POC concentrations increased through the riverine zone upstream of the reservoirs, likely due to in situ primary production and/or inputs from tributaries and agricultural drains; then decreased through the most upstream reservoir likely due to particle settling. Isotopic ratios and other OM source indicators (δ 15 N–PN, δ 13 C–POC, POC:PN, chl- a :POC) show that the dominant source of particulate OM was phytoplankton with seasonal terrestrial/macrophytic inputs. Results highlight the effects of major tributary and agricultural drain inputs, primary production, and impoundment on OM composition and concentration through a large river-reservoir system and may inform water quality management efforts in this and similar systems.

Idaho, Oregon

Influence of irrigation water and soil on annual mercury dynamics in Sacramento Valley rice fields

Methylmercury (MeHg) is a human and environmental toxin produced in flooded soils. Little is known about MeHg in rice ( Oryza Sativa L.) fields in Sacramento Valley, California. The objectives of this study were to quantify mercury fractions in irrigation water and within rice fields and to determine their mercury pools in surface water, soil, and grain. Soil, grain, and surface water (dissolved and particulate) MeHg and total mercury (THg) were monitored in six commercial rice fields throughout a winter fallow season and subsequent growing season. Both dissolved and particulate mercury fractions were higher in fallow season rice field water. Total suspended solids and particulate mercury concentrations were positively correlated ( r = 0.99 and 0.98 for THg and MeHg, respectively), suggesting that soil MeHg was suspended in the water column and potentially exported. Dissolved THg and MeHg concentrations were positively correlated with absorbance at 254 nm ( r = 0.47 and 0.58, respectively) in fallow season field water. In the growing season, fields with higher irrigation water MeHg concentrations (due to recycled water use) had elevated field-water MeHg ( r = 0.86) and grain MeHg concentrations ( r = 0.96). Based on a mass balance analysis, soil mercury pools were orders of magnitude larger than surface water or grain mercury pools; however, fallow season drainage and grain harvest were the primary pathways for MeHg export. Based on these findings, reducing (1) discharge when water is turbid, (2) straw inputs, and (3) use of recycled irrigation water could help reduce mercury exports in rice field drainage water.

California

Linking meso-scale spatial variation in methylmercury production to bioaccumulation in tidal marsh food webs

Differences in sediment biogeochemistry among tidal marsh features with different hydrological and geomorphological characteristics, including marsh interiors, marsh edges, first-order channels, and third-order channels, can result in spatial variation in MeHg production and availability. To better understand the link between MeHg production in sediments and bioaccumulation in primary and secondary consumer invertebrates and fish, we characterized mesoscale spatial variation in sediment biogeochemistry and MeHg concentrations of sediments, water, and consumer tissues among marsh features. Our results indicated that marsh interiors had biogeochemical conditions, including greater concentrations of organic matter and sulfate reduction rates, that resulted in greater MeHg concentrations in sediments and surface water particulates from marsh interiors compared to other features. Tissue MeHg concentrations of consumers also differed among features, with greater concentrations from marsh edges and interiors compared to channels. This spatial mismatch of MeHg concentrations in sediments and water compared to those in consumers may have resulted from differences in behavior and physiology among consumers that influenced the spatial scale over which MeHg was integrated into tissues. Our results highlight the importance of sampling across a suite of marsh features and considering the behavioral and physiological traits of sentinel taxa for contaminant monitoring studies.

Environmental Science and Technology

Successful hindcast of 7 years of mud morphodynamics influenced by salt pond restoration in south San Francisco Bay

Alviso Slough in South San Francisco Bay has been experiencing restoration of adjacent former salt-production ponds into muted tidal ponds, tidal ponds, and salt marsh. As a result, tidal prism through Alviso Slough has increased and mercury-contaminated sediment has been remobilized. We developed a 2D, high-resolution, process-based model (Delft3D FM-wave) to hindcast observed morpho-dynamic developments and to investigate associated sediment flux in the slough and pond system. Our results contrastingly demonstrate that a successful hindcast of the observed morphodynamic trend is made while reproducing observed intratidal suspended sediment concentrations in Alviso Slough remains a challenge. Our explanation is that the model is able to capture spatial gradients in the tide-residual sediment transports as the result of the large-scale management actions in the system, i.e., the opening of the salt ponds. These tide-residual processes are generally difficult to measure over an entire domain, but are very relevant to model the morphodynamic development. Our model provides a promising tool to trace eroding contaminated sediments to the benefit of restoration project managers and to support planning and design phases of adaptive management measures.

California

Long-term mercury loading and trapping dynamics in a Western North America reservoir

Study Region The Carson River including Lahontan Reservoir in Northwestern Nevada, USA Study Focus The discovery, mining, and processing of silver and gold from the Comstock Lode in northwestern Nevada heavily contaminated the Carson River system with mercury (Hg). The river now contains some of the highest recorded water column and bed sediment Hg concentrations reported in peer-reviewed literature. Acute Hg contamination in river and reservoir bed sediment has led to elevated methylmercury (MeHg) concentrations across all trophic levels of Lahontan Reservoir, culminating in significant health risks to humans. Lahontan Reservoir, located downstream from the mills that processed Comstock ore, has served as a Hg trap since the completion of the dam in 1915. Starting in 1997 and extending through 2021, the U.S. Geological Survey has collected and analyzed hundreds of discrete water samples entering and exiting Lahontan Reservoir for unfiltered total Hg (uf.THg), thereby providing a first-of-its-kind opportunity for studying long-term Hg trapping efficiencies within a western North American reservoir. Continuous time series of uf.THg concentration and flux above and below the reservoir were estimated using the weighted regressions on time, discharge, and season with the Kalman filtering (WRTDS-K) method employed with newly developed methods to account for non-natural (i.e., managed) hydrographs below a reservoir. New hydrological insights for the region An estimated 31,650 kg (34.89 US tons) of uf.THg entered Lahontan Reservoir during the 25 year period of analysis, accounting for approximately 0.5% of the total uf.THg estimated to have been released to the Carson River system [6.8 million kg (7500 US tons)] over a multi-decade mining boom. Moreover, approximately 92% of the estimated uf.THg entering Lahontan Reservoir was trapped. On an annual basis, however, trapping efficiencies range between 34% and 98%, and are closely related to the total annual discharge. Results also indicate that flow-normalized uf.THg concentrations and loads above and below the reservoir are trending down.

Nevada

The relative importance of mercury methylation and demethylation in rice paddy soil varies depending on the presence of rice plants

Neurotoxic methylmercury (MeHg) accumulates in rice grain from paddy soil, where its concentration is controlled by microbial mercury methylation and demethylation. Both up- and down-regulation of methylation is known to occur in the presence of rice plants in comparison to non-vegetated paddy soils; the influence of rice plant presence/absence on demethylation is unknown. To assess the concurrent influence of rice plant presence/absence on methylation and demethylation, and to determine which process was more dominant in controlling soil MeHg concentrations, we maintained six rhizoboxes of paddy soil with and without rice plants. At the peak of plant growth, we simultaneously measured ambient MeHg, ambient inorganic mercury (IHg), and potential rate constants of methylation and demethylation (K meth and K demeth ) in soil using stable isotope tracers and ID-GC-ICPMS. We also measured organic matter content, elemental S, and water-extractable sulfate. We found MeHg concentrations were differentially controlled by MeHg production and degradation processes, depending on whether plants were present. In non-vegetated boxes, MeHg concentration was controlled by K meth , as evidenced by a strong and positive correlation, while K demeth had no relation to MeHg concentration. These results indicate methylation was the dominant driver of MeHg concentration in non-vegetated soil. In vegetated boxes, K demeth strongly and negatively predicted MeHg concentration, indicating that demethylation was the dominant control in soil with plants. MeHg concentration, K meth , and % MeHg all had significantly less variance in vegetated than in non-vegetated soils due to a consistent elimination of greater values. This pattern suggests that reduced MeHg production capacity was a secondary control on MeHg concentrations in vegetated soils. We observed no difference in the magnitude or variance of K demeth between treatments, suggesting that demethylation was robust to soil chemical conditions influenced by the plant, perhaps because of a wider taxonomic diversity of demethylators. Our results suggest that methylation and demethylation processes could both be leveraged to alter MeHg concentrations in rice paddy soil.

Ecotoxicology and Environmental Safety

Disentangling the effects of habitat biogeochemistry, food web structure, and diet composition on mercury bioaccumulation in a wetland bird

Methylmercury (MeHg) is a globally pervasive contaminant with known toxicity to humans and wildlife. Several sources of variation can lead to spatial differences in MeHg bioaccumulation within a species including: biogeochemical processes that influence MeHg production and availability within an organism’s home range; trophic positions of consumers and MeHg biomagnification efficiency in food webs; and individual prey preferences that influence diet composition. To better understand spatial variation in MeHg bioaccumulation within a species, we evaluated the effects of habitat biogeochemistry, food web structure, and diet composition in the wetland-obligate California black rail ( Laterallus jamaicensis coturniculus ) at three wetlands along the Petaluma River in northern San Francisco Bay, California, USA. The concentration of MeHg in sediments differed significantly among wetlands. We identified three sediment and porewater measurements that contributed significantly to a discriminant function explaining differences in habitat biogeochemistry among wetlands: the porewater concentration of ferrous iron, the percent organic matter, and the sediment MeHg concentration. Food web structure and biomagnification efficiency were similar among wetlands, with trophic magnification factors for MeHg ranging from 1.84 to 2.59. In addition, regurgitation samples indicated that black rails were dietary generalists with similar diets among wetlands (percent similarity indices > 70%). Given the similarities in diet composition, food web structure, and MeHg biomagnification efficiency among wetlands, we concluded that variation in habitat biogeochemistry and associated sediment MeHg production was the primary driver of differences in MeHg concentrations among black rails from different wetlands.

California

Resolving a paradox—high mercury deposition, but low bioaccumulation in northeastern Puerto Rico

At a “clean air” trade winds site in northeastern Puerto Rico, we found an apparent paradox: atmospheric total mercury (THg) deposition was highest of any site in the USA Mercury Deposition Network, but assimilation into the local food web was quite low. Avian blood THg concentrations (n = 31, from eight species in five foraging guilds) ranged widely from 0.2 to 32 ng g −1 (median of 4.3 ng g −1 ). Within this population, THg was significantly greater at a low-elevation site near a wetland compared to an upland montane site, even when the comparison was limited to a single species. Overall, however, THg concentrations were approximately an order of magnitude lower than comparable populations in the continental U.S. In surface soil and sediment, potential rates of demethylation were 3 to 9-fold greater than those for Hg(II)-methylation (based on six radiotracer amendment incubations), but rates of change of ambient MeHg pools showed a slight net positive Hg(II)-methylation. Thus, the resolution of the paradox is that MeHg degradation approximately keeps pace with MeHg production in this landscape. Further, any net production of MeHg is subject to frequent flushing by high rainfall on chronically wet soils. The interplay of these microbial processes and hydrology appears to shield the local food web from adverse effects of high atmospheric mercury loading. This scenario may play out in other humid tropical ecosystems as well, but it is difficult to evaluate because coordinated studies of Hg deposition, methylation, and trophic uptake have not been conducted at other tropical sites.

Puerto Rico

Wetland management strategy to reduce mercury export in water and bioaccumulation in fish

Wetland environments provide numerous ecosystem services but also facilitate methylmercury (MeHg) production and bioaccumulation. We developed a wetland‐management technique to reduce MeHg concentrations in wetland fish and water. We physically modified seasonal wetlands by constructing open‐ and deep‐water treatment cells at the downstream end of seasonal wetlands to promote naturally occurring MeHg‐removal processes. We assessed the effectiveness of reducing mercury (Hg) concentrations in surface water and western mosquitofish that were caged at specific locations within 4 control and 4 treatment wetlands. Methylmercury concentrations in wetland water were successfully decreased within treatment cells during only the third year of study; however, treatment cells were not effective for reducing total Hg concentrations. Furthermore, treatment cells were not effective for reducing total Hg concentrations in wetland fish. Mercury concentrations in fish were not correlated with total Hg concentrations in filtered, particulate, or whole water; and the slope of the correlation with water MeHg concentrations differed between months. Fish total Hg concentrations were weakly correlated with water MeHg concentrations in April when fish were introduced into cages but were not correlated in May when fish were retrieved from cages. Fish total Hg concentrations were greater in treatment wetlands than in control wetlands the year after the treatment wetlands’ construction but declined by the second year. During the third year, fish total Hg concentrations increased in both control and treatment wetlands after an unexpected regional flooding event. Overall, we found limited support for the use of open‐ and deep‐water treatment cells at the downstream end of wetlands to reduce MeHg concentrations in water but not fish. We suggest that additional evaluation over a longer period of time is necessary.

Environmental Toxicology and Chemistry

Slough evolution and legacy mercury remobilization induced by wetland restoration in South San Francisco Bay

Coastal wetlands have a long history of degradation and destruction due to human development. Now recognized as one of the most productive ecosystems in the world, substantial efforts are being made to restore this critical habitat. While wetland restoration efforts are generally viewed as beneficial in terms of providing wildlife habitat and flood control, they are often accompanied by dramatic physical and chemical changes that may result in unintended consequences, which are rarely studied. Alviso Slough, a tidal slough in South San Francisco Bay, California, is the site of an ongoing effort to restore former salt-production ponds to intertidal marsh habitat. Restoration is complicated by the fact that (1) the ponds undergoing restoration are severely subsided and (2) subsurface sediments within the slough and surrounding ponds are contaminated with legacy mercury deposits. Due to concerns regarding mercury remobilization, restoration has proceeded in a cautious, methodical manner. To assess the amount of legacy mercury remobilized since restoration began, we developed a technique of combining high-resolution, biannual measurements of bathymetric scour with mercury concentration measurements from sediment cores. We estimate that 52 kg (±3) of mercury was remobilized in the 6 years since restoration began. Net bathymetric change analyses revealed seasonal trends of peak erosion during the winter months and little to no net change during summer months. Our analyses provide crucial insight on the spatial and temporal scales of geomorphic evolution within a tidal slough resulting from both natural (seasonal) variability and restoration actions. The technique presented here could be applied to other study sites and various sediment-associated contaminants of concern to aid in the design and management of restoration projects aiming to minimize negative impacts from legacy contaminants.

California

Human-induced and natural carbon storage in floodplains of the Central Valley of California

Active floodplains can putatively store large amounts of organic carbon (SOC) in subsoils originating from catchment erosion processes with subsequent floodplain deposition. Our study focussed on the assessment of SOC pools associated with alluvial floodplain soils that are affected by human-induced changes in floodplain deposition and in situ SOC mineralisation due to land use change and drainage. We evaluated depth-dependent SOC contents based on 23 soil cores down to 3 m and 10 drillings down to 7 m in a floodplain area of the lower Cosumnes River. An estimate of 266 Mg C ha −1 or about 59% of the entire SOC stored within the 7 m profiles was found in the upper 2 m. Most profiles (n = 25) contained discrete buried A horizons at depths of approximately 0.8 m. These profiles had up to 130% higher SOC stocks. The mean δ 13 C of all deep soil profiles clearly indicated that arable land use has already altered the stable isotopic signature in the first meter of the profile. Radiocarbon dating showed that the 14 C age in the buried horizon was younger than in overlaying soils indicating a substantial sedimentation phase for the overlaying soils. An additional analysis of total mercury contents in the soil profiles indicated that this sedimentation was associated with upstream hydraulic gold mining after the 1850s. In summary, deep alluvial soils in floodplains store large amounts of SOC not yet accounted for in global carbon models. Historic data give evidence that large amounts of sediment were transported into the floodplains of most rivers of the Central Valley and deposited over organically rich topsoil, which promoted the stabilization of SOC, and needs to be considered to improve our understanding of the human-induced interference with C cycling.

California

Geochemical data for water, streambed sediment, and fish tissue from the Sierra Nevada Mercury Impairment Project, 2011–12

This report presents geochemical data for surface water, streambed sediment, and fish tissue samples collected during low-flow conditions in 20 to 24 Sierra Nevada streams during 2011 and 2012. The dataset is part of a larger study designed to assess the factors that control mercury concentrations in fish tissue and to develop a model that predicts mercury concentration in the tissue of selected fish species in Sierra Nevada streams. The ranges of total mercury concentration observed in different matrices of water and sediment from 24 locations were as follows: below detection to 0.86 nanograms per liter in filtered water, below detection to 4.06 nanograms per liter in suspended particulates (greater than 0.3 micrometer in diameter), 1.1 to 381 nanograms per gram in bed sediment less than 2 millimeters, and 28.1 to 1,410 nanograms per gram in bed sediment less than 0.063 millimeters. The ratio of monomethyl mercury to total mercury ranged as follows: below detection to 19.2 percent in filtered water, below detection to 51.7 percent in suspended particles (greater than 0.3 micrometer), and below detection to 7.6 percent in streambed sediment less than 2 millimeters. Fish from 3 species collected at 20 locations had the following range in total mercury concentration (all concentrations wet weight): 10 to 292 nanograms per gram in rainbow trout (293 fish, 19 locations), 13 to 386 nanograms per gram in brown trout (33 fish, 10 locations), and 159 nanograms per gram in hardhead (1 fish). Concentrations of selenium in fish (wet weight) ranged from 60 to 420 nanograms per gram in rainbow trout (66 fish, 19 locations) and from 180 to 240 nanograms per gram in brown trout (6 fish, 2 locations).

Sierra Nevada

Mercury on a landscape scale—Balancing regional export with wildlife health

The Cosumnes River watershed requires a 57–64 percent reduction in loads to meet the new Delta methylmercury (MeHg) total maximum daily load allocation, established by the Central Valley Regional Water Quality Control Board. Because there are no large point sources of MeHg in the watershed, the focus of MeHg load reductions will fall upon non-point sources, particularly the expansive wetlands considered to be a primary source of MeHg in the region. Few management practices have been implemented and tested in order to meet load reductions in managed wetlands, but recent efforts have shown promise. This project examines a treatment approach to reduce MeHg loads to the Sacramento-San Joaquin River Delta by creating open-water deep cells with a small footprint at the downstream end of wetlands to promote net demethylation of MeHg and to minimize MeHg and Hg loads exiting wetlands at the Cosumnes River Preserve. Specifically, the deep cells were were located immediately up gradient of the wetland’s outflow weir and were deep enough (75–91 centimeter depth) to be vegetation-free. The topographic and hydrologic structure of each treatment wetland was modified to include open-water deep cells so that the removal of aqueous MeHg might be enhanced through (1) particle settling, (2) photo-degradation, and (3) benthic microbial demethylation. These deep cells were, therefore, expected to clean MeHg from surface water prior to its discharge to the Cosumnes River and the downstream Delta. Our goal was to test whether the implementation of the deep cells within wetlands would minimize MeHg and total Hg export. Further, we sought to test whether continuous flow-through hydrology, would lower MeHg concentrations in resident biota, compared to traditional wetland management operations. The dominant practice in seasonal wetlands management is the “fill-and-maintain” approach, in which wetlands are filled with water and the water levels maintained without substantial draining until drawdown. Our approach was to create and characterize replicate treatment wetland complexes, in conjunction with monitoring of hydrologic, biologic, and chemical indicators of MeHg exposure for two full annual cycles within winter-spring flooded seasonal wetlands. In addition to the creation of deep cells within treatment wetlands, hydrology was manipulated so that there was a constant flow-through of water, while the control wetlands utilized the fill-and-maintain approach. Specifically, the treatment wetlands were maintained in a flow-through manner, while the control wetlands were maintained in a fill-and-maintain manner from September through May, to test the hypothesis that the flow of water through the seasonal wetland can lower fish bioaccumulation through dilution of MeHg-concentrated water within the wetland by constant inflows of water into the wetland. The major tasks of this study included: (1) field design and implementation, (2) water and wetland management, (3) hydrologic monitoring and water quality sampling, (4) MeHg export and load estimates, (5) caged fish experiments for examining MeHg bioaccumulation, (6) site and process characterization to improve understanding and transferability of results, (7) adaptive management, transferability, and outreach, and (8) reporting of results and conclusions. This report summarizes the key findings of this study, which focuses on MeHg load estimates from control and treatment wetlands, quantification of three MeHg removal mechanisms (particulate settling, benthic demethylation, and photo-demethylation) in the deep cells within the treatment wetlands, and MeHg bioaccumulation in wetland fishes. Key findings include: Over two years of study, mean whole-water MeHg load decreased 37 percent in deep cells, when comparing inlet of check weir flows to outlet. Of the 37 percent MeHg load removed within the deep cell, photodegradation accounted for 7 percent and particle flux to the benthos accounted for 24 percent of the mass removed, with the remaining 6 percent apparent MeHg loss unexplained. Benthic MeHg degradation did not appear to be a major MeHg removal process in the deep cells, as changes in the ambient MeHg pool over 7-day bottle incubations showed that the surface sediment exhibited net MeHg production in the majority (87 percent) of incubation experiments. In only 13 percent of the incubations (3 out of 24) was net MeHg degradation observed. Estimates of benthic diffusive flux of MeHg across the sediment/water interface were small relative to particulate flux and variable (positive or negative), suggesting this is likely a minor term in the overall MeHg budget within the deep cells. Although the deep cells served as net MeHg sink overall, MeHg export from the flow-through treatment wetlands (shallow and deep combined) exceeded export from the fill-and-maintain managed control wetlands, because of the differences in hydrologic management between the two wetland types. Shallow wetlands under flow-through conditions generated a net export of MeHg. Most of the annual MeHg export from the treatment wetlands occurred within the first 3 months of flood up (September to November), shortly after hydrologic management began. Despite the effectiveness of the deep cell in lowering MeHg export concentrations, total mercury (THg) concentration did not decrease in biosentinel fish ( Gambusia affinis , Mosquitofish) between the deep cell inlet and outlet. Mosquitofish THg concentrations were higher in treatment wetlands than in control wetlands during the first year of study, likely because of an associated increase in MeHg availability immediately following wetland construction activities. Mosquitofish THg concentrations declined in the treatment wetlands during the second year of study, and fish THg concentrations in treatment wetlands were no different from those in the control. Similarly, the increased hydrologic flow rates in the treatment wetlands did not lower fish THg concentrations nor aqueous MeHg concentrations in the shallow cells, suggesting that MeHg flux from the sediment to water column exceeded the flow-through flushing rate in the shallow portion of the treatment wetlands. Reductions in MeHg concentrations of surface water and fish may require higher flow rates than used in the study to achieve the region’s regulatory goals. However, the flow rates necessary may not be feasible for these managed wetlands because of limited water supply and the associated costs for water and pumping. The use of deep cells in seasonal wetlands were effective in lowering MeHg exports under continuous water flow-through hydrology. However, fill-and-maintain hydrology had lower exports overall, because of a single major drainage event at the end of the flood season. Future studies focused on limiting MeHg export should consider combining deep cells with the fill-and-maintain or fill-and-trickle hydrologic management approach.

California

Alternate wetting and drying decreases methylmercury in flooded rice (Oryza sativa) systems

In flooded soils, including those found in rice ( Oryza sativa L.) fields, microbes convert inorganic Hg to more toxic methylmercury (MeHg). Methylmercury is accumulated in rice grain, potentially affecting health. Methylmercury in rice field surface water can bioaccumulate in wildlife. We evaluated how introducing aerobic periods into an otherwise continuously flooded rice growing season affects MeHg dynamics. Conventional continuously flooded (CF) rice field water management was compared with alternate wetting and drying, where irrigation was stopped twice during the growing season, allowing soil to dry to 35% volumetric moisture content, at which point plots were reflooded (AWD-35). Methylmercury studies began at harvest in Year 3 and throughout Year 4 of a 4-yr replicated field experiment. Bulk soil, water, and plant samples were analyzed for MeHg and total Hg (THg), and iron (Fe) speciation was measured in soil samples. Rice grain yield over 4 yr did not differ between treatments. Soil chemistry responded quickly to AWD-35 dry-downs, showing significant oxidation of Fe(II) accompanied by a significant reduction of MeHg concentration (76% reduction at harvest) compared with CF. Surface water MeHg decreased by 68 and 39% in the growing and fallow seasons, respectively, suggesting that the effects of AWD-35 management can last through to the fallow season. The AWD-35 treatment reduced rice grain MeHg and THg by 60 and 32%, respectively. These results suggest that the more aerobic conditions caused by AWD-35 limited the activity of Hg(II)-methylating microbes and may be an effective way to reduce MeHg concentrations in rice ecosystems.

Soil Science Society of America Journal

Geochemistry of mercury and other constituents in subsurface sediment—Analyses from 2011 and 2012 coring campaigns, Cache Creek Settling Basin, Yolo County, California

Cache Creek Settling Basin was constructed in 1937 to trap sediment from Cache Creek before delivery to the Yolo Bypass, a flood conveyance for the Sacramento River system that is tributary to the Sacramento–San Joaquin Delta. Sediment management options being considered by stakeholders in the Cache Creek Settling Basin include sediment excavation; however, that could expose sediments containing elevated mercury concentrations from historical mercury mining in the watershed. In cooperation with the California Department of Water Resources, the U.S. Geological Survey undertook sediment coring campaigns in 2011–12 (1) to describe lateral and vertical distributions of mercury concentrations in deposits of sediment in the Cache Creek Settling Basin and (2) to improve constraint of estimates of the rate of sediment deposition in the basin. Sediment cores were collected in the Cache Creek Settling Basin, Yolo County, California, during October 2011 at 10 locations and during August 2012 at 5 other locations. Total core depths ranged from approximately 4.6 to 13.7 meters (15 to 45 feet), with penetration to about 9.1 meters (30 feet) at most locations. Unsplit cores were logged for two geophysical parameters (gamma bulk density and magnetic susceptibility); then, selected cores were split lengthwise. One half of each core was then photographed and archived, and the other half was subsampled. Initial subsamples from the cores (20-centimeter composite samples from five predetermined depths in each profile) were analyzed for total mercury, methylmercury, total reduced sulfur, iron speciation, organic content (as the percentage of weight loss on ignition), and grain-size distribution. Detailed follow-up subsampling (3-centimeter intervals) was done at six locations along an east-west transect in the southern part of the Cache Creek Settling Basin and at one location in the northern part of the basin for analyses of total mercury; organic content; and cesium-137, which was used for dating. This report documents site characteristics; field and laboratory methods; and results of the analyses of each core section and subsample of these sediment cores, including associated quality-assurance and quality-control data.

California

Long-term trends of surface-water mercury and methylmercury concentrations downstream of historic mining within the Carson River watershed

The Carson River is a vital water resource for local municipalities and migratory birds travelling the Pacific Flyway. Historic mining practices that used mercury (Hg) to extract gold from Comstock Lode ore has left much of the river system heavily contaminated with Hg, a practice that continues in many parts of the world today. Between 1998 and 2013, the United States Geological Survey (USGS) collected and analyzed Carson River water for Hg and methylmercury (MeHg) concentrations resulting in a sixteen year record of unfiltered total mercury (uf.THg), filtered (dissolved) Hg (f.THg), total methylmercury (uf.MeHg), filtered MeHg (f.MeHg), and particulate-bound THg (p.THg) and MeHg (p.MeHg) concentrations. This represents one of the longest continuous records of Hg speciation data for any riverine system, thereby providing a unique opportunity to evaluate long-term trends in concentrations and annual loads. During the period of analysis, uf.THg concentration and load trended downward at rates of −0.85% and −1.8% per year, respectively. Conversely, the f.THg concentration increased at a rate of 1.7% per year between 1998 and 2005, and 4.9% per year between 2005 and 2013. Trends in flow-normalized partition coefficients for both Hg and MeHg suggest a statistically significant shift from the particulate to the filtered phase. The upwardly accelerating f.THg concentration and observed shift from the solid phase to the aqueous phase among the pools of Hg and MeHg within the river water column signals an increased risk of deteriorating ecological conditions in the lower basin with respect to Hg contamination. More broadly, the 16-year trend analysis, completed 140 years after the commencement of major Hg releases to the Carson River, provides a poignant example of the ongoing legacy left behind by gold and silver mining techniques that relied on Hg amalgamation, and a cautionary tale for regions still pursuing the practice in other countries.

Nevada

Mercury in western North America: A synthesis of environmental contamination, fluxes, bioaccumulation, and risk to fish and wildlife

Western North America is a region defined by extreme gradients in geomorphology and climate, which support a diverse array of ecological communities and natural resources. The region also has extreme gradients in mercury (Hg) contamination due to a broad distribution of inorganic Hg sources. These diverse Hg sources and a varied landscape create a unique and complex mosaic of ecological risk from Hg impairment associated with differential methylmercury (MeHg) production and bioaccumulation. Understanding the landscape-scale variation in the magnitude and relative importance of processes associated with Hg transport, methylation, and MeHg bioaccumulation requires a multidisciplinary synthesis that transcends small-scale variability. The Western North America Mercury Synthesis compiled, analyzed, and interpreted spatial and temporal patterns and drivers of Hg and MeHg in air, soil, vegetation, sediments, fish, and wildlife across western North America. This collaboration evaluated the potential risk from Hg to fish, and wildlife health, human exposure, and examined resource management activities that influenced the risk of Hg contamination. This paper integrates the key information presented across the individual papers that comprise the synthesis. The compiled information indicates that Hg contamination is widespread, but heterogeneous, across western North America. The storage and transport of inorganic Hg across landscape gradients are largely regulated by climate and land-cover factors such as plant productivity and precipitation. Importantly, there was a striking lack of concordance between pools and sources of inorganic Hg, and MeHg in aquatic food webs. Additionally, water management had a widespread influence on MeHg bioaccumulation in aquatic ecosystems, whereas mining impacts where relatively localized. These results highlight the decoupling of inorganic Hg sources with MeHg production and bioaccumulation. Together the findings indicate that developing efforts to control MeHg production in the West may be particularly beneficial for reducing food web exposure instead of efforts to simply control inorganic Hg sources.

Science of the Total Environment