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Mark Marvin-DiPasquale

Publications and source records attributed to Mark Marvin-DiPasquale.

At least 19 recordsLinked to original sources

South San Francisco Bay Salt Pond Restoration Project—A synthesis of Phase-1 mercury studies

The South Bay Salt Pond Restoration Project (SBSPRP) encompasses over 6,000 hectares of former salt production ponds along the south edge of the San Francisco Bay and represents the largest wetland restoration effort on the west coast of North America. A series of studies associated with Phase 1 (2010–2018) restoration activities that are focused on a historically mercury contaminated slough and series of ponds within the restoration area have recently been completed. This report brings together the key findings of these loosely coordinated studies and integrates the results into a more comprehensive and holistic product that informs future restoration activities associated with the SBSPRP and elsewhere. This report documents key findings associated with the breach of pond A6: (1) a short-term spike in slough fish (Mississippi silverside) total mercury concentration in lower Alviso Slough; (2) a short-term spike in surface-water particulate total mercury in lower Alviso Slough; (3) significant sediment scour in Alviso Slough adjacent to and downstream of the breach points; (4) a decrease in surface-sediment methylmercury (as a percentage of total mercury) in lower Alviso Slough; (5) the transport of 70 kilograms per year of sediment-associated total mercury into pond A6 during the first 2 years following the breach but with much of this coming from outside of Alviso Slough, presumably from the nearby shallows, Guadalupe Slough, and the larger southern San Francisco Bay area; and (6) a slowing of bed sediment erosion in lower Alviso Slough 3–5 years after the breaching of pond A6. Although this report is not intended to be prescriptive in terms of the next steps the SBSPRP should or should not take, the totality of the findings presented provide critical process-level information regarding the extent and the duration of spikes in mercury levels in water, sediment, fish, and birds, which appeared to result from the two management actions under study. Thus, these results can be used to anticipate similar ecosystem responses associated with similar management actions that may be considered in the future. We also conclude this report by highlighting unanswered questions associated with mercury dynamics as it relates to the restoration project, and possible future directions for research.

California

Biogeochemical and physical processes controlling mercury methylation and bioaccumulation in Lake Powell, Glen Canyon National Recreation Area, Utah and Arizona, 2014 and 2015

Mercury monitoring results from about 300 Morone saxatilis (striped bass) muscle tissue samples collected by the State of Utah from Lake Powell resulted in a Utah/Arizona fish consumption advisory issued in 2012 for approximately the lower 100 kilometers of the reservoir. Chemical, physical, and biological data were collected during two synoptic sampling cruises on Lake Powell during May/June 2014 and August 2015 to test three hypotheses associated with a conceptual model developed to explain the observed geographic concentration gradient of Hg in fish tissue samples. This model proposes that in the transition from a primarily riverine system to a reservoir, there is a change in the concentration and composition of water-column particulate material, increasing in the proportion of organic content moving downstream, as the larger size fractions of the inorganic particulate load are deposited in the upper reservoir. This change alleviates light limitation of phytoplankton production and leads to a higher proportion of autochthonous primary production in the downstream direction. This, in turn, drives increased microbial methylmercury (MeHg) production in the benthos and potentially the water column, in the downstream direction, and results in the observed elevated fish Hg levels in the lower part of the reservoir. The model also proposes that there are differences between the main stem of Lake Powell and side canyons, embayments, or secondary rivers entering the reservoir, in terms of Hg cycling dynamics and bioaccumulations, driven mainly by differences in hydrology. Finally, seasonal differences in Hg dynamics within the reservoir are proposed, based on seasonal dynamics associated with primary production and the physical process of seasonal stratification. A total of three statistically testable hypotheses were proposed and postulated that measurable differences in key Hg and non-Hg metrics exist between: (1) the upper and lower reservoir; (2) main stem and river arm/side canyon/embayment sites; and (3) early-season (May/June 2014, less stratified) and late-season (August 2015, stratified) conditions. Statistically modeled least square means in combination with the graphical analysis of Hg and non-Hg parameters were used to examine the data collected during the study and test these hypotheses. Data collected during the study are included in a U.S. Geological Survey data release and are available online at https://doi.org/10.5066/F74X560J . In general, water-column, plankton, and surface sediment samples collected during the synoptic sampling cruises are supportive of the three hypotheses associated with the conceptual model. In support of hypothesis 1 (comparing upper and lower reservoir sites), the least square mean for turbidity was higher in the upper reservoir. In contrast, surface water particulate organic carbon (as a percentage of total particulate mass), particulate MeHg (by mass [in nanograms per gram] and as a percentage of total mercury [THg]), and particulate-dissolved partitioning coefficients for THg and MeHg were higher in the lower reservoir. Plankton THg concentrations also were significantly (probability [ p ] less than (<) 0.05) higher in the lower reservoir. Surface sediment metrics in support of hypothesis 1 include higher MeHg production potential rates in the lower reservoir. In contrast, there were no statistically significant differences between the upper and lower reservoir for surface sediment percent of MeHg and MeHg concentration, percent MeHg, or methylation rate constants. These spatial trends associated with hypothesis 1 indicate a pathway for enhanced Hg bioavailability in the lower reservoir. Hypothesis 2, which tested for differences between main stem and river arm/side canyon/embayment sites, was supported by a number of water-column parameters, including particulate THg and MeHg concentrations by mass (in nanograms per gram) and percent particulate MeHg being significantly ( p <0.05) higher in the river arms, side canyons, and embayments relative to the main stem channel. Plankton MeHg concentrations (by mass [in nanograms per gram] and volume [in nanograms per liter] and as a percentage of THg) were elevated in river arm/side canyon/embayment sites compared to main stem sites, indicating an enhanced potential for MeHg bioaccumulation at the base of the pelagic food web in river arms, side canyons, and embayments. In contrast, few of the sediment metrics differed between main stem and river arm/side canyon/embayment sampling sites; however, the potential for MeHg degradation in surface sediment was significantly higher in the main stem. The data indicate that river arm/side canyon/embayment sites may experience enhanced Hg bioaccumulation, compared to the main stem, because of higher MeHg levels at the base of the pelagic food web. This conclusion is supported by the elevated Hg detected in striped bass muscle tissue samples collected in the San Juan Arm during this study (2014). Fish collected from the lower reservoir exhibited a distinct Hg isotopic signature that was enriched in delta (δ) 202 Hg and capital delta (Δ) 199 Hg relative to fish samples collected from either Good Hope Bay or the San Juan Arm. Hypothesis 3 tested for differences between early (May/June) high-flow and late (August) low-flow seasons. This test was supported by a range of non-Hg metrics (nitrate, phosphate, chlorophyll a , dissolved oxygen, fluorescent dissolved organic matter, temperature, and pH) that reflect the increase in chlorophyll a , decrease in nutrients, and buildup of stratified conditions in the transition from early- to late-season sampling periods. Significant seasonal differences also were noted for multiple Hg metrics, including (a) water-column filtered and particulate (by mass) MeHg and THg concentrations; (b) plankton MeHg and THg concentration (by mass); and (c) sediment percent MeHg, Hg(II)-methylation rate constant, and microbial ribosomal ribonucleic acid, small subunit 16 (16S rRNA) abundance, all of which were higher during the late-season synoptic sampling. Overall, the surface sediment metrics are consistent with a seasonal shift from the early-season synoptic results, when the availability of Hg(II) exerts a primary control on MeHg production, to the late-season synoptic sampling, when microbial activity is a dominant driver of MeHg production.

Arizona, Utah

Effect of salinity on mercury methylating benthic microbes and their activities in Great Salt Lake, Utah

Surface water and biota from Great Salt Lake (GSL) contain some of the highest documented concentrations of total mercury (THg) and methylmercury (MeHg) in the United States. In order to identify potential biological sources of MeHg and controls on its production in this ecosystem, THg and MeHg concentrations, rates of Hg(II)-methylation and MeHg degradation, and abundances and compositions of archaeal and bacterial 16 rRNA gene transcripts were determined in sediment along a salinity gradient in GSL. Rates of Hg(II)-methylation were inversely correlated with salinity and were at or below the limits of detection in sediment sampled from areas with hypersaline surface water. The highest rates of Hg(II)-methylation were measured in sediment with low porewater salinity, suggesting that benthic microbial communities inhabiting less saline environments are supplying the majority of MeHg in the GSL ecosystem. The abundance of 16S rRNA gene transcripts affiliated with the sulfate reducer Desulfobacterium sp. was positively correlated with MeHg concentrations and Hg(II)-methylation rates in sediment, indicating a potential role for this taxon in Hg(II)-methylation in low salinity areas of GSL. Reactive inorganic Hg(II) (a proxy used for Hg(II) available for methylation) and MeHg concentrations were inversely correlated with salinity. Thus, constraints imposed by salinity on Hg(II)-methylating populations and the availability of Hg(II) for methylation are inferred to result in higher MeHg production potentials in lower salinity environments. Benthic microbial MeHg degradation was also most active in lower salinity environments. Collectively, these results suggest an important role for sediment anoxia and microbial sulfate reducers in the production of MeHg in low salinity GSL sub-habitats and may indicate a role for salinity in constraining Hg(II)-methylation and MeHg degradation activities by influencing the availability of Hg(II) for methylation.

Utah

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

The effects of wetland restoration on mercury bioaccumulation in the South Bay Salt Pond Restoration Project: Using the biosentinel toolbox to monitor changes across multiple habitats and spatial scales

The project was initiated in April 2010, and to date has included four sampling events of surface water (April, May, June/July, and August 2010) and five sampling events of biota (April, May, June/July, August, and September 2010) and three sampling events for surface sediment (May, June/July, and August 2010). This annual report briefly summarizes our progress to date.

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

Mercury, methylmercury, and other constituents in sediment and water from seasonal and permanent wetlands in the Cache Creek settling basin and Yolo Bypass, Yolo County, California, 2005-06

This report presents surface water and surface (top 0-2 cm) sediment geochemical data collected during 2005-2006, as part of a larger study of mercury (Hg) dynamics in seasonal and permanently flooded wetland habitats within the lower Sacramento River basin, Yolo County, California. The study was conducted in two phases. Phase I represented reconnaissance sampling and included three locations within the Cache Creek drainage basin; two within the Cache Creek Nature Preserve (CCNP) and one in the Cache Creek Settling Basin (CCSB) within the creek's main channel near the southeast outlet to the Yolo Bypass. Two additional downstream sites within the Yolo Bypass Wildlife Area (YBWA) were also sampled during Phase I, including one permanently flooded wetland and one seasonally flooded wetland, which had began being flooded only 1–2 days before Phase I sampling. Results from Phase I include: (a) a negative correlation between total mercury (THg) and the percentage of methylmercury (MeHg) in unfiltered surface water; (b) a positive correlation between sediment THg concentration and sediment organic content; (c) surface water and sediment THg concentrations were highest at the CCSB site; (d) sediment inorganic reactive mercury (Hg(II) R ) concentration was positively related to sediment oxidation-reduction potential and negatively related to sediment acid volatile sulfur (AVS) concentration; (e) sediment Hg(II) R concentrations were highest at the two YBWA sites; (f) unfiltered surface water MeHg concentration was highest at the seasonal wetland YBWA site, and sediment MeHg was highest at the permanently flooded YBWA site; (g) a 1,000-fold increase in sediment pore water sulfate concentration was observed in the downstream transect from the CCNP to the YBWA; (h) low sediment pore water sulfide concentrations (<1 µmol/L) across all sites; and (i) iron (Fe) speciation data suggest a higher potential for microbial Fe(III)-reduction in the YBWA compared to the CCSB. Phase II sampling did not include the original three Cache Creek sites, but instead focused on the original two sites within the YBWA and a similarly paired set of seasonally and permanently flooded wetland sites within the CCSB. Sediment sampling at the YBWA and CCSB occurred approximately 28 days and 52 days, respectively, after the initial flooding of the respective seasonal wetlands, and again towards the end of the seasonal flooding period (end of May 2006). Results from Phase II sampling include: (a) sediment MeHg concentration and the percentage of THg as MeHg (%MeHg) in unfiltered surface waters were generally higher in the YBWA compared to the CCSB; (b) suspended sediment concentration (SCC) in surface water was positively correlated with both THg and MeHg in unfiltered water across all sites, although the relationship between SCC and MeHg differed for the two regions, suggesting local MeHg sources; (c) MeHg concentration in unfiltered surface water was positively correlated to sediment MeHg concentrations across all sites, supporting the suggestion of unique local (sediment) sources of MeHg to the water column; (d) THg concentration in filtered water was positively correlated with both total Fe and dissolved organic carbon (DOC), offering additional support for the role of these constituents in the partitioning of THg between particulate and dissolved phases; (e) flooding of the YBWA seasonal wetland resulted in a rapid and significant (5-fold) rise in sediment MeHg concentration within 3–4 weeks following inundation; and (f) temporal changes in sediment S and Fe speciation suggest that rates of both microbial sulfate reduction and Fe(III)-reduction were significantly higher at YBWA, compared to CCSB, during the period between flooding and drying. The geochemical data presented in this report indicate that (a) strong spatial and temporal differences in Hg speciation and transformations can occur within the range of wetland habitats found in the lower Sacramento River basin; (b) flooding of seasonal wetlands can be accompanied by a rapid increase in benthic MeHg production and the release of previously formed MeHg (generated during or since the previous flooding season) to the overlying water column; (c) S and Fe chemistry, and associated microbial reduction pathways, play an important role in mediating the speciation and transformation of Hg in these wetland habitats; (d) hydroperiod is a primary forcing function in mediating MeHg production among various wetland types; and (e) MeHg production appears to be more active in the YBWA compared to the CCSB.

California

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