Geology Reports⌕ Search

Geology topics

Mark Marvin-DiPasquale

Publications and source records attributed to Mark Marvin-DiPasquale.

15 recordsLinked to original sources

Mercury cycling in agricultural and managed wetlands of California: experimental evidence of vegetation-driven changes in sediment biogeochemistry and methylmercury production

The role of live vegetation in sediment methylmercury (MeHg) production and associated biogeochemistry was examined in three types of agricultural wetlands (domesticated or white rice, wild rice, and fallow fields) and adjacent managed natural wetlands (cattail- and bulrush or tule-dominated) in the Yolo Bypass region of California's Central Valley, USA. During the active growing season for each wetland, a vegetated:de-vegetated paired plot experiment demonstrated that the presence of live plants enhanced microbial rates of mercury methylation by 20 to 669% (median = 280%) compared to de-vegetated plots. Labile carbon exudation by roots appeared to be the primary mechanism by which microbial methylation was enhanced in the presence of vegetation. Pore-water acetate (pw[Ac]) decreased significantly with de-vegetation (63 to 99%) among all wetland types, and within cropped fields, pw[Ac] was correlated with both root density (r = 0.92) and microbial Hg(II) methylation (k meth . r = 0.65). Sediment biogeochemical responses to de-vegetation were inconsistent between treatments for “reactive Hg” (Hg(II)R), as were reduced sulfur and sulfate reduction rates. Sediment MeHg concentrations in vegetated plots were double those of de-vegetated plots (median = 205%), due in part to enhanced microbial MeHg production in the rhizosphere, and in part to rhizoconcentration via transpiration-driven pore-water transport. Pore-water concentrations of chloride, a conservative tracer, were elevated (median = 22%) in vegetated plots, suggesting that the higher concentrations of other constituents around roots may also be a function of rhizoconcentration rather than microbial activity alone. Elevated pools of amorphous iron (Fe) in vegetated plots indicate that downward redistribution of oxic surface waters through transpiration acts as a stimulant to Fe(III)-reduction through oxidation of Fe(II)pools. These data suggest that vegetation significantly affected rhizosphere biogeochemistry through organic exudation and transpiration-driven concentration of pore-water constituents and oxidation of reduced compounds. While the relative role of vegetation varied among wetland types, macrophyte activity enhanced MeHg production.

California↗

Methylmercury production in sediment from agricultural and non-agricultural wetlands in the Yolo Bypass, California, USA

As part of a larger study of mercury (Hg) biogeochemistry and bioaccumulation in agricultural (rice growing) and non-agricultural wetlands in California's Central Valley, USA, seasonal and spatial controls on methylmercury (MeHg) production were examined in surface sediment. Three types of shallowly-flooded agricultural wetlands (white rice, wild rice, and fallow fields) and two types of managed (non-agricultural) wetlands (permanently and seasonally flooded) were sampled monthly-to-seasonally. Dynamic seasonal changes in readily reducible ‘reactive’ mercury (Hg(II) R ), Hg(II)-methylation rate constants (k meth ), and concentrations of electron acceptors (sulfate and ferric iron) and donors (acetate), were all observed in response to field management hydrology, whereas seasonal changes in these parameters were more muted in non-agricultural managed wetlands. Agricultural wetlands exhibited higher sediment MeHg concentrations than did non-agricultural wetlands, particularly during the fall through late-winter (post-harvest) period. Both sulfate- and iron-reducing bacteria have been implicated in MeHg production, and both were demonstrably active in all wetlands studied. Stoichiometric calculations suggest that iron-reducing bacteria dominated carbon flow in agricultural wetlands during the growing season. Sulfate-reducing bacteria were not stimulated by the addition of sulfate-based fertilizer to agricultural wetlands during the growing season, suggesting that labile organic matter, rather than sulfate, limited their activity in these wetlands. Along the continuum of sediment geochemical conditions observed, values of k meth increased approximately 10,000-fold, whereas Hg(II) R decreased 100-fold. This suggests that, with respect to the often opposing trends of Hg(II)-methylating microbial activity and Hg(II) availability for methylation, microbial activity dominated the Hg(II)-methylation process, and that along this biogeochemical continuum, conditions that favored microbial sulfate reduction resulted in the highest calculated MeHg production potential rates. Rice straw management options aimed at limiting labile carbon supplies to surface sediment during the post-harvest fall–winter period may be effective in limiting MeHg production within agricultural wetlands.

California↗

Incorporation of inorganic mercury (Hg2+) in pelagic food webs of ultraoligotrophic and oligotrophic lakes: the role of different plankton size fractions and species assemblages

In lake food webs, pelagic basal organisms such as bacteria and phytoplankton incorporate mercury (Hg 2+ ) from the dissolved phase and pass the adsorbed and internalized Hg to higher trophic levels. This experimental investigation addresses the incorporation of dissolved Hg 2+ by four plankton fractions (picoplankton: 0.2–2.7 μm; pico + nanoplankton: 0.2–20 μm; microplankton: 20–50 μm; and mesoplankton: 50–200 μm) obtained from four Andean Patagonian lakes, using the radioisotope 197 Hg 2+ . Species composition and abundance were determined in each plankton fraction. In addition, morphometric parameters such as surface and biovolume were calculated using standard geometric models. The incorporation of Hg 2+ in each plankton fraction was analyzed through three concentration factors: BCF (bioconcentration factor) as a function of cell or individual abundance, SCF (surface concentration factor) and VCF (volume concentration factor) as functions of individual exposed surface and biovolume, respectively. Overall, this investigation showed that through adsorption and internalization, pico + nanoplankton play a central role leading the incorporation of Hg 2+ in pelagic food webs of Andean lakes. Larger planktonic organisms included in the micro- and mesoplankton fractions incorporate Hg 2+ by surface adsorption, although at a lesser extent. Mixotrophic bacterivorous organisms dominate the different plankton fractions of the lakes connecting trophic levels through microbial loops (e.g., bacteria–nanoflagellates–crustaceans; bacteria–ciliates–crustaceans; endosymbiotic algae–ciliates). These bacterivorous organisms, which incorporate Hg from the dissolved phase and through their prey, appear to explain the high incorporation of Hg 2+ observed in all the plankton fractions.

Patagonia↗

Differential mercury transfer in the aquatic food web of a double basined lake associated with selenium and habitat

Food web trophodynamics of total mercury (THg) and selenium (Se) were assessed for the double-basined ultraoligotrophic system of Lake Moreno, Patagonia. Each basin has differing proportions of littoral and pelagic habitats, thereby providing an opportunity to assess the importance of habitat (e.g. food web structure or benthic MeHg production) in the transfer of Hg and Se to top trophic fish species. Pelagic plankton, analyzed in three size classes (10–53, 53–200, and > 200 μm), had very high [THg], exceeding 200 μg g − 1 dry weight (DW) in the smallest, and a low ratio of MeHg to THg (0.1 to 3%). In contrast, [THg] in littoral macroinvertebrates showed lower values (0.3 to 1.8 μg g − 1 DW). Juvenile and small fish species feeding upon plankton had higher [THg] (0.2 to 8 μg g − 1 muscle DW) compared to large piscivore fish species (0.1 to 1.6 μg g − 1 muscle DW). Selenium concentrations exhibited a much narrower variation range than THg in the food web, varying from 0.5 to 2.7 μg g − 1 DW. Molar Se:Hg ratios exceeded 1 for the majority of organisms in both basins, with most ratios exceeding 10. Using stable nitrogen isotopes as indicator of trophic level, no significant correlations were found with [THg], [Se] or Se:Hg. The apparent lack of biomagnification trends was attributed to elevated [THg] in plankton in the inorganic form mostly, as well as the possibility of consistent Se supply reducing the biomagnification in the food web of the organic portion of THg.

Patagonia;Lake Moreno↗

How to overcome inter-electrode variability and instability to quantify dissolved oxygen, Fe(II), mn(II), and S(−II) in undisturbed soils and sediments using voltammetry

Background - Although uniquely capable of measuring multiple redox constituents nearly simultaneously with no or minimal sample pretreatment, voltammetry is currently underutilized in characterizing redox conditions in aquatic and terrestrial systems. Investigation of undisturbed media such as pore water requires a solid-state electrode, and such electrodes can be difficult to fabricate reproducibly. An approach to determine the concentrations of electroactive constituents using indirectly calibrated electrodes has been developed, but the protocol for and accuracy of this approach—the pilot ion method—has not been documented in detail. Results - A detailed procedure for testing electrode quality is provided, and the application and limitations of the pilot ion method have been documented. To quantify Fe(II) and Mn(II), subtraction of non-linear baseline functions from voltammetric signals produced better calibration curves than did linear baselines, enabled lower detection limits and reliable deconvolution of overlapping signals, and was successfully applied to sediment pore water signals. We observed that electrode sensitivities often vary by tens of percent, and that the sensitivity declines over time. The ratio of calibration slopes of Mn(II) to Fe(II) varied by no more than 11% from one Hg/Au electrode to another and Fe(II) concentrations predicted by the Mn(II) pilot ion were, on average, 13% different from their actual values. However, concentration predictions by the pilot ion method were worse for less than 15 μM Fe(II) (46% different on average). The ratio of calibration slopes of Mn(II) to S(−II) varied by almost 20% from one Hg/Au electrode to another, and S(−II) predicted concentrations were as much as 58% different from their actual values. These predictions of Fe(II) and S(−II) concentrations indicate that the accuracy of the pilot ion method depends on how independent calibration slope ratios are from the electrode used. At medium-to-high concentration for the ocean, naturally derived dissolved organic carbon did not significantly affect the baseline-corrected electrode response of Mn(II) and Fe(II), but did significantly affect the response of S(−II). Conclusions - Despite their intrinsic variability, Hg/Au electrodes fabricated by hand can be used to quantify O2, S(−II), Fe(II), and Mn(II) without calibrating every electrode for every constituent of interest. The pilot ion method can achieve accuracies to within 20% or less, provided that the underlying principle—the independence of slope ratios—is demonstrated for all voltammetric techniques used, and effects of the physicochemical properties of the system on voltammetric signals are addressed through baseline subtraction.

Geochemical Transactions↗

Spatial and seasonal variability of dissolved methylmercury in two stream basins in the Eastern United States

We assessed methylmercury (MeHg) concentrations across multiple ecological scales in the Edisto (South Carolina) and Upper Hudson (New York) River basins. Out-of-channel wetland/floodplain environments were primary sources of filtered MeHg (F-MeHg) to the stream habitat in both systems. Shallow, open-water areas in both basins exhibited low F-MeHg concentrations and decreasing F-MeHg mass flux. Downstream increases in out-of-channel wetlands/floodplains and the absence of impoundments result in high MeHg throughout the Edisto. Despite substantial wetlands coverage and elevated F-MeHg concentrations at the headwater margins, numerous impoundments on primary stream channels favor spatial variability and lower F-MeHg concentrations in the Upper Hudson. The results indicated that, even in geographically, climatically, and ecologically diverse streams, production in wetland/floodplain areas, hydrologic transport to the stream aquatic environment, and conservative/nonconservative attenuation processes in open water areas are fundamental controls on dissolved MeHg concentrations and, by extension, MeHg availability for potential biotic uptake.

New York, South Carolina↗

The effects of sediment and mercury mobilization in the South Yuba River and Humbug Creek confluence area, Nevada County, California: Concentrations, speciation, and environmental fate – Part 1: Field characterization

Millions of pounds of mercury (Hg) were deposited in the river and stream channels of the Sierra Nevada from placer and hard-rock mining operations in the late 1800s and early 1900s. The resulting contaminated sediments are relatively harmless when buried and isolated from the overlying aquatic environment. The entrained Hg in the sediment constitutes a potential risk to human and ecosystem health should it be reintroduced to the actively cycling portion of the aquatic system, where it can become methylated and subsequently bioaccumulated in the food web. Each year, sediment is mobilized within these fluvial systems during high stormflows, transporting hundreds of tons of Hg-laden sediment downstream. The State of California and resource-management agencies, including the Bureau of Land Management (BLM) and the U.S. Forest Service, are concerned about additional disturbances, such as from suction gold dredging activities, which have the potential to mobilize Hg associated with buried sediment layers elevated in Hg that are otherwise likely to remain buried under normal storm conditions. The BLM initiated a study looking at the feasibility of removing Hg-contaminated sediment at the confluence of the South Yuba River and Humbug Creek in the northern Sierra Nevada of California by using standard suction-dredge technology. Additionally, the California State Water Resources Control Board (SWRCB) supported a comprehensive characterization of the intended dredge site. Together, the BLM and SWRCB supported a comprehensive characterization of Hg contamination at the site and the potential effects of sediment disturbance at locations with historical hydraulic mining debris on downstream environments. The comprehensive study consisted of two primary components: field studies and laboratory experiments. The field component, described in this report, had several study elements: 1) a preliminary, smallscale, in-stream dredge test; 2) comprehensive characterization of grain size distribution, Hg speciation, and mineralogy of bed and suspended sediment; 3) a determination of the past and current sources of sediment in the study area; 4) an assessment of Hg bioaccumulation in the local invertebrate population; and 5) a comparison of potential Hg transport caused by natural storm disturbances with potential Hg mobilization caused by suction dredging as a method of Hg removal at the study site. The laboratory component of the study assessed the potential influence of the disturbance of Hg-contaminated sediment through experiments designed to simulate in-stream transport, deposition, and potential methylation of Hg, described in a companion report (see Marvin-DiPasquale and others, 2011). Results of the field studies indicate that the fine-grained fraction (silt-clay, less than 0.063 millimeters) contains the greatest concentration of Hg in contaminated sediment. Because the fine-grained fraction is the most susceptible to longrange fluvial transport, disturbance of Hg-contaminated sediment is likely to increase the concentration and load of Hg in downstream waters. The preliminary, small-scale dredge test showed an increase in the concentration of fine particles and Hg in the water column caused by the dredge activity, despite relatively low concentrations of fine particles and Hg (about 300 nanograms per gram) at the dredge site. Characterization of sediment from two test pits and other sites in the vicinity of the confluence of the South Yuba River and Humbug Creek revealed a highly variable distribution of fine- and coarse-grained sediment. The highest levels of Hg contamination (up to 11,100 ng/g) were associated with the fine-grained fraction of sediment from the bedrock contact zone of Pit 2, a horizon which also yielded grains of gold and gold-Hg amalgam. A closed-circuit tank experiment with a venturi dredge at the base of Pit 1, in a gravel bar within the South Yuba River, resulted in fine-grained suspended sediment remaining in suspension more than 40 hours following the disturbance simulation. Although the volumetric concentration of Hg declined over time as particles settled out, the concentration of Hg on the suspended particles increased over time as the suspended material became finer grained, because Hg is preferentially adsorbed on to clay-sized particles. Mineralogical and chemical analyses indicated that the buried fine-grained material with the greatest Hg contamination was derived from hydraulic mining debris, which consist primarily of Eocene gravels mined in the Malakoff Diggins, North Bloomfield, and Lake City areas within the South Yuba River watershed. Coarse material and more recently deposited sediment were derived primarily from upstream sources on the South Yuba River. The biota assessment indicated that invertebrate taxa collected from all sites on the South Yuba River in 2007, including lower Humbug Creek, had elevated concentrations of total mercury (THg) and methylmercury (MeHg) compared to a reference site on the Bear River, upstream of mining effects. Differences with the reference site were less pronounced in 2008 when a significant reduction in MeHg concentrations was observed in biota across all taxa from concentrations in 2007. It is possible that the inter-annual variation was related to the fact that suction dredging was active in the South Yuba River in 2007 but not in 2008 when a local moratorium was imposed by the BLM. There were significant variations among taxa for both THg and MeHg concentrations, with the water striders (Gerridae) having the highest concentrations of both THg and MeHg; variation among sites was not as strong as between years or among taxa. These results suggest that additional monitoring would be helpful to investigate the possible linkage between variations in MeHg bioaccumulation and levels of suction dredge activity in areas of historical gold mining. Results from the field studies indicate that disturbance of the finegrained Hg-contaminated sediment would likely lead to enhanced mobilization of Hg to downstream environments; therefore, the use of suction dredging to remove Hg at the South Yuba River and Humbug Creek confluence area would likely result in enhanced Hg transport downstream relative to natural conditions.

California↗

Methylmercury cycling, bioaccumulation, and export from agricultural and non-agricultural wetlands in the Yolo Bypass

This 18-month field study addresses the seasonal and spatial patterns and processes controlling methylmercury (MeHg) production, bioaccumulation, and export from natural and agricultural wetlands of the Yolo Bypass Wildlife Area (YBWA). The data were collected in conjuntion with a Proposition 40 grant from the State Water Resources Control Board in support of the development of Best Management Practices (BMP's) for reducing MeHg loading from agricultural lands in the wetland-dominated Yolo Bypass to the Sacramento-San Joaquin River Delta. The four managemenr-based questions addressed in this study were: 1. Is there a different among agricultural and managfed wetland types in terms of Me Hg dynamic (production, degradation, bioaccumulation, or export)? 2. Does water residence time influence MeHg dynamics? 3. Does the application of sulfate-based fertilizer impact MeHg production rates? 4. Does the presence (or absence) of vegetation influence MeHg production rates? Measurements of MeHg concentrations in sediment, water, and biota (plants, invertebrates, and fish) were made to assess management-level patterns in five wetland types, which included three type of shallowly-flooded agricultural wetlands (white rice, wild rice, and fallow) and two types of managed wetlands (permanently and seasonally flooded). To strengthen our understanding of the processes underlying the seasonal and spatial patterns of MeHg cycling, additional exploratory factors were measured including ancillary sediment and water quality parameters, stable isotope fractionation (oxygen, sulfur, carbon, and nitrogen), photodemethylation rates, and daily-integrated hydrologic budgets. Samples and field data were collected from May 2007 to July 2008, and nearly all sample analyses were completed by September 2008 as per the Quality Assurance Program Plan (QAPP) requirements. Although wetland type was a major factor that drove the study design, within-field hydrology also proved to be an important factor controlling aqueous MeHg and total mercury (THg) concentrations and export. Overall, agricultural wetlands exhibited higher MeHg concentrations in overlying water, sediment, and biota than did managed seasonal and permanent wetlands. This appears to be partly due to higher rates of sediment in microbial production of MeHg on agricultural wetlands during the fall through spring period. Both sulfate- and iron-reducing bacteria have been implicated in the MeHg production process, and both were demonstrably active in all wetlands studied; however, sulfate-reducing bacteria were not stimulated by the addition of sulfate-based fertilizer to agricultural wetlands, suggesting that easily-degraded (labile) organic matter, rather than sulfate, was limiting their activity in these field types. The data suggest that agriculturally-managed soils promoted MeHg production through 1) enhanced microbial activity via higher temperatures and larger pools of labile carbon, and 2) enhanced pools of microbially available inorganic divalent mercury (Hg(II)) resulting from a decrease in reduced-sulfur, solid-phase minerals under oxic or only mildly reducing conditions. MeHg mass balances were assessed by comparing filed-specific MeHg loads for inlets vs. outlet flows. The overall mass balance for MeHg in surface water during the summer irrigation period (June - September 2007) indicated little to no net MeHg export from the six agricultural wetlands taken as a whole. Of the six agricultural wetlands, there was net overall MeHg export from two fields (one fallow and one white rice) during August, and from four of the six fields (one fallow, one white rice, and two wild rice) during September) Over the entire summer irrigation period, two of the fields (one fallow and one wild rive) showed net MeHg export, and the other four fields showed wither net import or no significant change. Rates of measured photomethylation and exchange between sediment and water pools suggest that both processes may be responsible for the lack of MeHg export. Despite significant differences during winter months between fields in surface water concentrations of MeHg, MeHg loads were not calculated in mid-winter because flood waters had overtopped field boundaries and field fidelity could not be established. During the summer 2007 irrigation season, surface water out-flows from agricultural wetlands were 9%-36% of inlet flows, and evaporation rates explained most of this water loss, with infiltration likely accounting for the remainder. Unfiltered aqueous MeHg concentrations increased from <1 ng L -1 in source waters to up to 10 ng L -1 in agricultural wetland drains during the summer irrigation period. Increases in solute concentration caused by evapoconcentration were estimated by determining concentration factors (outflow/inflow) for chloride (a conservative dissolved constituent) and by measuring oxygen isotope ratios ( 18 O/ 16 O, expressed as δ 18 O) in water. Increases in MeHg concentration from inflows-to-outflows exceeded those caused by evapoconcentration on several fields during the summer irrigation season. This was especially true when initial surface water MeHg concentrations were low, as seen in the southern block of fields receiving irrigation water directly from the Toe Drain. The northern block of fields received irrigation water from Greens Lake, which included Toe Drain water plus recirculated drain water from other agricultural fields within the Yolo Bypass and west of the Yolo Bypass; as such, the northern fields showed a smaller percentage increase in MeHg concentration because initial MeHg concentrations in surface water inflows were greater than in inputs to the southern fields. Mercury concentrations in fish were greater in agricultural wetlands white rice and wild rice) than in the two permanently flooded wetlands. Additionally, Hg concentrations in biota showed a general increase from inlets to outlets withing agricultural wetlands, but not within permanent wetlands. This was particular evident in white rice fields where caged western mosquitofish at the outlets had Hg concentrations that were more than 4 times higher than in caged fish held at the inlets. Similar spatial patterns in Hg bioaccumulation in agricultural and permanent wetlands were seen for wild populations of western mosquitofish and Mississippi silversides. In contrast to fish, invertebrates, such as water-boatman (Corixidae) and back swimmers (Notonectidae), had greater Hg concentrations in permanent wetlands than in tempoarirly flooded agricultural wetlands, Fish THg concentrations were weakly correlated with water MeHg,a and not correlated with sediment MeHg. In contrast, invertebrate MeHg concentrations were more strongly correlated with sediment MeHg than with water MeHg concentrations. These results illustrate the complexity of MeHg bioaccumulation through food webs and indicate the importance of simultaneously using multiple biosentinels when monitoring MeHg production and bioaccumulation. Despite high sediment production rates and water concentrations in agricultural wetlands, MeHg export was physically limited by hydrologic export for all wetlands studied. We suggest that load reduction is maximized by limiting water throughout, but that on-site biota exposure is maximized by this loner water residence time. While field-specific hydrologic loads could not be fully quantified during flood conditions in February 2008, we suggest that the primary period of MeHg export from Yolo Bypass Wildlife Area is during those winter flooding periods when overall microbial activity and MeHg production in agricultural soils is fueled by the decomposition of rice straw, and when hydrologic flowthrough is maximal. Local stakeholders participated in two workshops related to this study, demonstrating an interest in understanding factors controlling MeHg production, export, and bioaccumulation. The results of this field study show that permanently flooded, naturally vegetated wetlands are unlikely to a large source of MeHg production within the YBWA, in contrast with agriculturally-managed wetlands. MeHg loading to Toe Drain waters of the Yolo Bypass may be reduced by lowering rated of hydrologic export from agricultural wetlands during the growing season and especially during rice harvest, However, under these water-holding conditions, biota living within agricultural wetlands may thus be exposed to higher MeHg concentrations in surface water, As observed in this study, rapid bioacculumaltion over a 2-month period led to MeHg concentrations in invertebrates and fish more than 6 and 11 times higher, respectively, than proposed TMDL target values to protect wildlife (0.03 ppm ww). The results of this field study, together with the information from YBWA stakeholders, provide a more definitive understanding of how MeHg cycling and bioaccumulation respond to habitat differences and specific management practices. These results directly address 4 core components of CBDA's Mercury Strategy for the Bay-Delta Ecosystem (Wiener et al., 2003a): a) Quantification and evaluation of THg and MeHg sources, b) Quantification of effects of ecosystem restoration on MeHg exposure, c) Assessment of ecological risk, and d) Identification and testing of potential management approaches for reducing MeHg contamination. In addition, the quantitative results reported here assess the effect of current land use practices in the Yolo Bypass MeHg production, bioaccumulation and export, and provide process-based advice towards achieving current goals of the RWQCB-CVR's Sacramento -- San Joaquin Delta Estuary TMDL for Methyl & Total Mercury (Wood et al., 2010b). Further work is necessary to evaluate biotic exposure in the Yolo Bypass Wildlife Area at higher trophic levels (e.g. birds), to quantify winter hydrologic flux of MeHg to the larger Delta ecosystem, and to evaluate rice straw management options to limit labile carbon supplies to surface sediment during winter months. In summary, agricultural management of rice fields -- specifically the periodic flooding and production of easily degraded organic matter -- promotes the production of MeHg beyond rates seen in naturally vegetated wetlands, whether seasonally or permanently flooded., The exported load from MeHg from these agricultural wetlands may be controlled by limiting hydrologic export from fields to enhance on-site MeHg removal processes, but the tradeoff is that this impoundement increases Me Hg exposure to resident organisms.

California↗

Experimental removal of wetland emergent vegetation leads to decreased methylmercury production in surface sediment

We performed plant removal (devegetation) experiments across a suite of ecologically diverse wetland settings (tidal salt marshes, river floodplain, rotational rice fields, and freshwater wetlands with permanent or seasonal flooding) to determine the extent to which the presence (or absence) of actively growing plants influences the activity of the Hg(II)-methylating microbial community and the availability of Hg(II) to those microbes. Vegetated control plots were paired with neighboring devegetated plots in which photosynthetic input was terminated 4–8 months prior to measurements, through clipping aboveground biomass, severing belowground connections, and shading the sediment surface to prevent regrowth. Across all wetlands, devegetation decreased the activity of the Hg(II)-methylating microbial community (k meth ) by 38%, calculated MeHg production potential (MP) rates by 36%, and pore water acetate concentration by 78%. Decreases in MP were associated with decreases in microbial sulfate reduction in salt marsh settings. In freshwater agricultural wetlands, decreases in MP were related to indices of microbial iron reduction. Sediment MeHg concentrations were also significantly lower in devegetated than in vegetated plots in most wetland settings studied. Devegetation effects were correlated with live root density (percent volume) and were most profound in vegetated sites with higher initial pore water acetate concentrations. Densely rooted wetlands had the highest rates of microbial Hg(II)-methylation activity but often the lowest concentrations of bioavailable reactive Hg(II). We conclude that the exudation of labile organic carbon (e.g., acetate) by plants leads to enhanced microbial sulfate and iron reduction activity in the rhizosphere, which results in high rates of microbial Hg(II)-methyation and high MeHg concentrations in wetland sediment.

Journal of Geophysical Research: Biogeosciences↗

Procedures for collecting and processing streambed sediment and pore water for analysis of mercury as part of the National Water-Quality Assessment Program

Mercury (Hg) contamination is an issue of national concern, affecting both wildlife and human health. The U.S. Geological Survey (USGS) National Water-Quality Assessment (NAWQA) Program, in association with the USGS Toxic Substances Hydrology Program and the USGS National Research Program, has initiated two levels of studies to investigate Hg contamination of the Nation's streams: reconnaissance and detailed studies. Reconnaissance studies entailed one-time sampling events at 266 stream sites across the Nation. Detailed studies entailed intensive spatial and temporal sampling of a small number of streams across the Nation in an effort to develop a more complete, process-level understanding of benthic Hg geochemistry and the underlying factors controlling it. This report summarizes the sampling methods used for the collection and processing of streambed sediment and pore water in association with both of these study levels. Bed-sediment characteristics, such as organic content and grain size, strongly influence Hg geochemistry; detailed characterization of these constituents within a stream reach will allow for the extrapolation of related Hg biogeochemical constituents to the reach scale.

Open-File Report↗

Legacy mercury in Alviso Slough, south San Francisco Bay, California: Concentration, speciation and mobility

Mercury (Hg) is a significant contaminant in the waters, sediment and biota of San Francisco Bay, largely resulting from extensive historic regional mining activities. Alviso Slough represents one of the most mercury contaminated waterways entering south San Francisco Bay, as it is associated with the drainage of the New Almaden mercury mining district. Wetland habitat restoration of former salt manufacturing ponds adjacent to Alviso Slough is currently being planned. One management scenario being considered is a levee breach between Alviso Slough and Pond A8, which will allow reconnection of the salt pond with the tidal slough. This action is projected to increase the tidal prism within Alviso Slough and result in some degree of sediment remobilization as the main channel deepens and widens. The focus of the current study is to assess: a) the current mercury species composition and concentration in sediments within the Alviso Slough main channel and its associated fringing marsh plain, b) how much of each mercury species will be mobilized as a result of projected channel deepening and widening, and c) potential changes in inorganic reactive mercury bioavailability (for conversion to toxic methylmercury) associated with the mobilized sediment fraction. The current report details the field sampling approach and all laboratory analyses conducted, as well as provides the complete dataset associated with this project including a) a quantitative assessment of mercury speciation (total mercury, reactive mercury and methylmercury), b) estimates of the quantity of sediment and mercury mobilized based on 20-foot and 40-foot levee wall notch scenarios, and c) results from a sediment scour experiment examining the changes in the reactive mercury pool under four treatment conditions (high / low salinity and oxic / anoxic water). Ancillary sediment data also collected and reported herein include bulk density, organic content, magnetic susceptibility, percent dry weight, grain size, pH, oxidation-reduction potential, core photography, and detailed lithographic descriptions.

California↗

Geochemistry of Mercury and other trace elements in fluvial tailings upstream of Daguerre Point Dam, Yuba River, California, August 2001

This study was designed to characterize the particle-size distribution and the concentrations of total mercury (HgT), methylmercury (MeHg), and other constituents in sediments trapped behind Daguerre Point Dam, a 28-foot-high structure on the lower Yuba River in California. The results of the study will assist other agencies in evaluating potential environmental impacts from mobilization of sediments if Daguerre Point Dam is modified or removed to improve the passage of anadromous fish. Methylmercury is of particular concern owing to its toxicity and propensity to bioaccumulate. A limited amount of recent work on hydraulic and dredge tailings in other watersheds has indicated that mercury and MeHg concentrations may be elevated in the fine-grained fractions of placer mining debris, particularly clay and silt. Mercury associated with tailings from placer gold mines is a source of continued contamination in Sierra Nevada watersheds and downstream water bodies, including the Sacramento?San Joaquin Delta and the San Francisco Bay of northern California. Churn drilling was used to recover sediments and heavy minerals at 5-foot intervals from six locations upstream of Daguerre Point Dam. Maximum depth of penetration ranged from 17.5 to 35 feet below land surface, resulting in 31 discreet drilled intervals. Drilling in permeable, unconsolidated sediments below the streambed of the Yuba River released a significant volume of water along with the sediment, which complicated the sampling and characterization effort. Overflow of a silty fraction sampled at the drill site contained suspended sediment consisting predominantly of silt and clay, with HgT concentration ranging from 33 to 1,100 ng/g (nanogram per gram) dry weight. A sandy fraction, collected after sieving sediment through a 2-millimeter vibratory screen, contained from 14 to 82 percent sand and 1 to 29 percent silt plus clay, and had HgT concentrations ranging from 6.8 to 81 ng/g dry weight. A clay-silt fraction, sampled from material remaining in suspension after the sandy fraction settled for 15-20 minutes, contained mercury concentrations from 23 to 370 ng/g dry weight. Concentrations of MeHg were less than the detection limit (<0.001 ng/g dry weight) in 30 of 31 samples of the sandy fraction. In the suspended clay-silt fraction, MeHg was detected in 16 of 31 samples, in which it ranged in concentration from 0.04 (estimated) to 0.61 ng/g wet weight. Potential rates of mercury methylation and demethylation were evaluated in seven samples using radiotracer methods. Mercury methylation (MeHg production) potentials were generally low, ranging from less than 0.15 to about 1.6 ng/g/d (nanogram per gram of dry sediment per day). Mercury demethylation (MeHg degradation) potentials were moderately high, ranging from 1.0 to 2.2 ng/g/d. The ratio of methylation potential (MP) to demethylation potential (DP) ranged from less than 0.14 to about 1.4 (median = 0.24, mean = 0.44, number of samples = 7), suggesting that the potential for net production of MeHg in deep sediments is generally low. The MeHg production rates and MP/DP ratios were higher in the shallower interval in two of the three holes where two depth intervals were assessed, whereas the MeHg concentrations were higher in the shallower interval for all three holes. A similar spatial distribution was found for concentrations of solid-phase sulfide (measured as total reduced sulfur and likely representing iron-sulfide and iron-disulfide compounds), which were much higher in shallower samples (about 700 to about 2,100 nanomoles per gram, dry sediment) than in deeper samples (32 to 55 nanomoles per gram, dry sediment) in these three holes. If reduced sulfur compounds are oxidized to sulfate as a consequence of sediment disturbance, the activity of sulfate-reducing bacteria might be stimulated, causing a short-term increase in methylation of inorganic Hg(II) (divalent mercury).

California↗

Sediment-water interactions affecting dissolved-mercury distributions in Camp Far West Reservoir, California

Field and laboratory studies were conducted in April and November 2002 to provide the first direct measurements of the benthic flux of dissolved (0.2-micrometer filtered) mercury species (total and methylated forms) between the bottom sediment and water column at three sampling locations within Camp Far West Reservoir, California: one near the Bear River inlet to the reservoir, a second at a mid-reservoir site of comparable depth to the inlet site, and the third at the deepest position in the reservoir near the dam (herein referred to as the inlet, midreservoir and near-dam sites, respectively; Background, Fig. 1). Because of interest in the effects of historic hydraulic mining and ore processing in the Sierra Nevada foothills just upstream of the reservoir, dissolved-mercury species and predominant ligands that often control the mercury speciation (represented by dissolved organic carbon, and sulfides) were the solutes of primary interest. Benthic flux, sometimes referred to as internal recycling, represents the transport of dissolved chemical species between the water column and the underlying sediment. Because of the affinity of mercury to adsorb onto particle surfaces and to form insoluble precipitates (particularly with sulfides), the mass transport of mercury in mining-affected watersheds is typically particle dominated. As these enriched particles accumulate at depositional sites such as reservoirs, benthic processes facilitate the repartitioning, transformation, and transport of mercury in dissolved, biologically reactive forms (dissolved methylmercury being the most bioavailable for trophic transfer). These are the forms of mercury examined in this study.

California↗

Flux of dissolved forms of mercury across the sediment-water interface in Lahontan Reservoir, Nevada

Field and laboratory studies were conducted between April 30, 2001 and July 19, 2001 to provide the first direct measurements of the benthic flux of dissolved (0.2-micrometer filtered) mercury species (total and methylated forms) between the bottom sediment and water column at three sites: two in the southern lobe and one in the northern lobe of Lahontan Reservoir, Nevada (Background, Fig. 1). Dissolved-mercury species and predominant ligands (represented by dissolved organic carbon, and sulfides) were the solutes of primary interest. Benthic flux, sometimes referred to as internal recycling, represents the transport of dissolved chemical species between the water column and the underlying sediment. Water-quality managers often assess and prioritize remediation strategies for aquatic systems, in particular Super Fund sites that have been adversely affected by anthropogenic activities. In the case of the Lahontan Reservoir along the Carson River, mercury associated with historic gold and silver extraction has been fluvially transported and accumulated in the bottom sediments. Frequent demands have been made by Super Fund site managers and the general public to quantify the connections between fluxes of contaminants and the health, abundance, and distribution of biological resources (Kuwabara and others, 1999). As part of a comprehensive examination of transport processes affecting mercury dynamics in Lahontan Reservoir, this study focuses on a poorly understood, yet potentially predominant, source of mercury to the reservoir water column, which is internal recycling, or benthic flux of mercury species and associated ligands. Mobilization, flux, and biological availability of mercury into the water column of the reservoir are affected by physical (e.g., advection and diffusion), chemical (i.e., oxidationreduction reactions, complexation and repartitioning) and biological processes (Flegal and others, 1991; Kuwabara and others, 1996; Grenz and others, 2000, Topping and others, 2001). The results described herein followed from the integration of current project studies with information needs identified by the U.S. Environmental Protection Agency, Region 9 (USEPA) to provide initial determinations of dissolved total and methyl-mercury fluxes from the sediments into the water column of Lahontan Reservoir. Recent mercury distribution and transformation studies in the Carson River system by Marvin-Dipasquale and others (2001) indicated the potential importance of sediment-water interactions in describing mercury speciation, its sources and sinks. Quantifying and understanding the magnitude and variability of these interactions are critical to the accurate assessment of contaminant sources and loads as well as to the development of process-integrated water-quality models for this mining-affected system. With a variety of strategies under consideration to determine how to most efficiently improve the water quality in the Carson River system, the primary question posed in this study was, “What processes regulate the fate and transport of mercury species in Lahontan Reservoir? In particular, are sources and sinks of dissolved total and methyl mercury associated with the bottom sediment within Lahontan Reservoir significant relative to major surface-water inputs from the Carson River?” The question was motivated by a number of factors. First, extraction of precious metals up gradient of the reservoir provide a historic source of elemental mercury that continues to be fluvially transported in dissolved and particulate phases (Hoffman and Taylor, 1998; Carroll and others, 2000; Carroll and Warwick, 2001). Elevated total and methyl mercury concentrations into the reservoir have been well documented (Priessler and others, 1999; Jones and others, 1999; Allander and others, 2001, Marvin-Dipasquale and others, 2001). Therefore, determining whether some fraction of this sediment-associated mercury can remobilize for transport to the overlying water and subsequently to down-stream portions of the Carson River is necessary. Second, elevated concentrations of mercury species in reservoir water, sediment, and fish have prompted a compilation, and comparison of dominant contaminant sources so that appropriate remedial strategies can be designed and implemented. Third, changes in oxidizing or reducing (redox) conditions and nutrient availability near the sediment-water interface (e.g., during phytoplankton blooms) can dramatically alter the mobility of metals and ligands associated with the bottom sediment as episodic sources of carbon settle out and accumulate (Thompson and others, 1981). Finally, there is a growing body of evidence from other aquatic systems that benthic flux or internal recycling of contaminants and nutrients is an important process to consider in developing appropriate ecosystem water-quality models (Wood and others, 1995; Kuwabara and others, 2000). The need for more refined numerical and conceptual models for mercury dynamics within the Carson River system thus clearly exists. This report is formatted unconventionally in a pyramid-like structure to effectively serve the needs of diverse parties interested in reviewing or acquiring information at various levels of detail (Appendix 1). The report enables quick transitions between the initial summary information (figuratively at the top of the pyramid) and later details of methods or results (that is, figuratively towards the base) using hyperlinks to supporting figures and tables, and an electronically linked Table of Contents.

Nebraska↗