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1.
J Environ Qual ; 53(3): 327-339, 2024.
Article in English | MEDLINE | ID: mdl-38468600

ABSTRACT

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


Subject(s)
Agricultural Irrigation , Environmental Monitoring , Mercury , Oryza , Soil Pollutants , Soil , Water Pollutants, Chemical , Mercury/analysis , Soil/chemistry , Soil Pollutants/analysis , Water Pollutants, Chemical/analysis , California , Methylmercury Compounds/analysis
2.
Environ Sci Technol ; 57(48): 19263-19273, 2023 Dec 05.
Article in English | MEDLINE | ID: mdl-37956992

ABSTRACT

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


Subject(s)
Mercury , Methylmercury Compounds , Water Pollutants, Chemical , Animals , Mercury/analysis , Food Chain , Wetlands , Bioaccumulation , Water Pollutants, Chemical/analysis , Water , Environmental Monitoring/methods , Geologic Sediments/chemistry
3.
Ecotoxicology ; 29(8): 1207-1220, 2020 Oct.
Article in English | MEDLINE | ID: mdl-31643013

ABSTRACT

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


Subject(s)
Environmental Monitoring , Environmental Pollutants/analysis , Mercury/analysis , Puerto Rico
4.
Environ Pollut ; 256: 113280, 2020 Jan.
Article in English | MEDLINE | ID: mdl-31718826

ABSTRACT

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


Subject(s)
Birds/metabolism , Environmental Monitoring/methods , Geologic Sediments/chemistry , Methylmercury Compounds/metabolism , Water Pollutants, Chemical/metabolism , Wetlands , Animals , Bioaccumulation , Diet , Ferrous Compounds/analysis , Food Chain , Humans , Methylmercury Compounds/analysis , Rivers/chemistry , San Francisco , Water Pollutants, Chemical/analysis
5.
Environ Toxicol Chem ; 38(10): 2178-2196, 2019 10.
Article in English | MEDLINE | ID: mdl-31343757

ABSTRACT

Wetland environments provide numerous ecosystem services but also facilitate methylmercury (MeHg) production and bioaccumulation. We developed a wetland-management technique to reduce MeHg concentrations in wetland fish and water. We physically modified seasonal wetlands by constructing open- and deep-water treatment cells at the downstream end of seasonal wetlands to promote naturally occurring MeHg-removal processes. We assessed the effectiveness of reducing mercury (Hg) concentrations in surface water and western mosquitofish that were caged at specific locations within 4 control and 4 treatment wetlands. Methylmercury concentrations in wetland water were successfully decreased within treatment cells during only the third year of study; however, treatment cells were not effective for reducing total Hg concentrations. Furthermore, treatment cells were not effective for reducing total Hg concentrations in wetland fish. Mercury concentrations in fish were not correlated with total Hg concentrations in filtered, particulate, or whole water; and the slope of the correlation with water MeHg concentrations differed between months. Fish total Hg concentrations were weakly correlated with water MeHg concentrations in April when fish were introduced into cages but were not correlated in May when fish were retrieved from cages. Fish total Hg concentrations were greater in treatment wetlands than in control wetlands the year after the treatment wetlands' construction but declined by the second year. During the third year, fish total Hg concentrations increased in both control and treatment wetlands after an unexpected regional flooding event. Overall, we found limited support for the use of open- and deep-water treatment cells at the downstream end of wetlands to reduce MeHg concentrations in water but not fish. We suggest that additional evaluation over a longer period of time is necessary. Environ Toxicol Chem 2019;38:2178-2196. Published 2019 Wiley Periodicals, Inc. on behalf of SETAC. This article is a US government work, and as such, is in the public domain in the United States of America..


Subject(s)
Bioaccumulation , Fishes/physiology , Methylmercury Compounds/analysis , Wetlands , Animals , Body Weight/drug effects , Environmental Monitoring , Floods , Methylmercury Compounds/toxicity , Seasons , Water Pollutants, Chemical/analysis
6.
Sci Total Environ ; 651(Pt 1): 851-858, 2019 Feb 15.
Article in English | MEDLINE | ID: mdl-30253367

ABSTRACT

Active floodplains can putatively store large amounts of organic carbon (SOC) in subsoils originating from catchment erosion processes with subsequent floodplain deposition. Our study focussed on the assessment of SOC pools associated with alluvial floodplain soils that are affected by human-induced changes in floodplain deposition and in situ SOC mineralisation due to land use change and drainage. We evaluated depth-dependent SOC contents based on 23 soil cores down to 3 m and 10 drillings down to 7 m in a floodplain area of the lower Cosumnes River. An estimate of 266 Mg C ha-1 or about 59% of the entire SOC stored within the 7 m profiles was found in the upper 2 m. Most profiles (n = 25) contained discrete buried A horizons at depths of approximately 0.8 m. These profiles had up to 130% higher SOC stocks. The mean δ13C of all deep soil profiles clearly indicated that arable land use has already altered the stable isotopic signature in the first meter of the profile. Radiocarbon dating showed that the 14C age in the buried horizon was younger than in overlaying soils indicating a substantial sedimentation phase for the overlaying soils. An additional analysis of total mercury contents in the soil profiles indicated that this sedimentation was associated with upstream hydraulic gold mining after the 1850s. In summary, deep alluvial soils in floodplains store large amounts of SOC not yet accounted for in global carbon models. Historic data give evidence that large amounts of sediment were transported into the floodplains of most rivers of the Central Valley and deposited over organically rich topsoil, which promoted the stabilization of SOC, and needs to be considered to improve our understanding of the human-induced interference with C cycling.


Subject(s)
Carbon Sequestration , Carbon/analysis , California , Ecology , Environmental Monitoring , Humans
7.
J Environ Qual ; 47(4): 830-838, 2018 Jul.
Article in English | MEDLINE | ID: mdl-30025065

ABSTRACT

Few studies have considered how methylmercury (MeHg, a toxic form of Hg produced in anaerobic soils) production in rice ( L.) fields can affect water quality, and little is known about MeHg dynamics in rice fields. Surface water MeHg and total Hg (THg) imports, exports, and storage were studied in two commercial rice fields in the Sacramento Valley, California, where soil THg was low (25 and 57 ng g). The median concentration of MeHg in drainage water exiting the fields was 0.17 ng g (range: <0.007-2.1 ng g). Compared with irrigation water, drainage water had similar MeHg concentrations, and lower THg concentrations during the growing season. Significantly elevated drainage water MeHg and THg concentrations were observed in the fallow season compared with the growing season. An analysis of surface water loads indicates that fields were net importers of both MeHg (76-110 ng m) and THg (1947-7224 ng m) during the growing season, and net exporters of MeHg (35-200 ng m) and THg (248-6496 ng m) during the fallow season. At harvest, 190 to 700 ng MeHg m and 1400 to 1700 ng THg m were removed from fields in rice grain. Rice straw, which contained 120 to 180 ng MeHg m and 7000-10,500 ng m THg was incorporated into the soil. These results indicate that efforts to reduce MeHg and THg exports in rice drainage water should focus on the fallow season. Substantial amounts of MeHg and THg were stored in plants, and these pools should be considered in future studies.


Subject(s)
Methylmercury Compounds/analysis , Oryza , Water Pollutants, Chemical/analysis , California , Environmental Monitoring , Mercury , Methylmercury Compounds/chemistry , Soil , Water Pollutants, Chemical/chemistry
8.
Environ Pollut ; 229: 1006-1018, 2017 Oct.
Article in English | MEDLINE | ID: mdl-28781180

ABSTRACT

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


Subject(s)
Environmental Monitoring , Mercury/analysis , Methylmercury Compounds/analysis , Water Pollutants, Chemical/analysis , Animals , Birds , Cities , Fresh Water , Mining , Nevada , Rivers , Water/analysis , Water Movements
9.
Sci Total Environ ; 581-582: 495-506, 2017 Mar 01.
Article in English | MEDLINE | ID: mdl-28057343

ABSTRACT

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.


Subject(s)
Mercury/analysis , Methylmercury Compounds/analysis , Salinity , Water Microbiology , Water Pollutants, Chemical/analysis , Archaea , Bacteria , Environmental Monitoring , Geologic Sediments , Lakes , Methylation , RNA, Ribosomal, 16S/analysis , Utah
10.
Sci Total Environ ; 571: 364-79, 2016 Nov 15.
Article in English | MEDLINE | ID: mdl-27378154

ABSTRACT

Widespread mercury (Hg) contamination of aquatic systems in the Sierra Nevada of California, U.S., is associated with historical use to enhance gold (Au) recovery by amalgamation. In areas affected by historical Au mining operations, including the western slope of the Sierra Nevada and downstream areas in northern California, such as San Francisco Bay and the Sacramento River-San Joaquin River Delta, microbial conversion of Hg to methylmercury (MeHg) leads to bioaccumulation of MeHg in food webs, and increased risks to humans and wildlife. This study focused on developing a predictive model for THg in stream fish tissue based on geospatial data, including land use/land cover data, and the distribution of legacy Au mines. Data on total mercury (THg) and MeHg concentrations in fish tissue and streambed sediment collected during 1980-2012 from stream sites in the Sierra Nevada, California were combined with geospatial data to estimate fish THg concentrations across the landscape. THg concentrations of five fish species (Brown Trout, Rainbow Trout, Sacramento Pikeminnow, Sacramento Sucker, and Smallmouth Bass) within stream sections were predicted using multi-model inference based on Akaike Information Criteria, using geospatial data for mining history and landscape characteristics as well as fish species and length (r(2)=0.61, p<0.001). Including THg concentrations in streambed sediment did not improve the model's fit, however including MeHg concentrations in streambed sediment, organic content (loss on ignition), and sediment grain size resulted in an improved fit (r(2)=0.63, p<0.001). These models can be used to estimate THg concentrations in stream fish based on landscape variables in the Sierra Nevada in areas where direct measurements of THg concentration in fish are unavailable.


Subject(s)
Fishes/metabolism , Geologic Sediments/analysis , Mercury/metabolism , Methylmercury Compounds/metabolism , Water Pollutants, Chemical/metabolism , Animals , California , Ecosystem , Environmental Monitoring , Mercury/analysis , Methylmercury Compounds/analysis , Mining , Rivers/chemistry , Water Pollutants, Chemical/analysis
11.
Sci Total Environ ; 568: 1213-1226, 2016 Oct 15.
Article in English | MEDLINE | ID: mdl-27320732

ABSTRACT

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


Subject(s)
Environmental Pollutants/metabolism , Mercury/metabolism , Methylmercury Compounds/metabolism , Vertebrates/metabolism , Animals , Canada , Environmental Monitoring , Environmental Pollutants/analysis , Fishes/metabolism , Mercury/analysis , Methylmercury Compounds/analysis , Mexico , United States
12.
Sci Total Environ ; 568: 1192-1203, 2016 Oct 15.
Article in English | MEDLINE | ID: mdl-27234290

ABSTRACT

Monomethyl mercury (MMHg) and total mercury (THg) concentrations and Hg stable isotope ratios (δ(202)Hg and Δ(199)Hg) were measured in sediment and aquatic organisms from Cache Creek (California Coast Range) and Yolo Bypass (Sacramento Valley). Cache Creek sediment had a large range in THg (87 to 3870ng/g) and δ(202)Hg (-1.69 to -0.20‰) reflecting the heterogeneity of Hg mining sources in sediment. The δ(202)Hg of Yolo Bypass wetland sediment suggests a mixture of high and low THg sediment sources. Relationships between %MMHg (the percent ratio of MMHg to THg) and Hg isotope values (δ(202)Hg and Δ(199)Hg) in fish and macroinvertebrates were used to identify and estimate the isotopic composition of MMHg. Deviation from linear relationships was found between %MMHg and Hg isotope values, which is indicative of the bioaccumulation of isotopically distinct pools of MMHg. The isotopic composition of pre-photodegraded MMHg (i.e., subtracting fractionation from photochemical reactions) was estimated and contrasting relationships were observed between the estimated δ(202)Hg of pre-photodegraded MMHg and sediment IHg. Cache Creek had mass dependent fractionation (MDF; δ(202)Hg) of at least -0.4‰ whereas Yolo Bypass had MDF of +0.2 to +0.5‰. This result supports the hypothesis that Hg isotope fractionation between IHg and MMHg observed in rivers (-MDF) is unique compared to +MDF observed in non-flowing water environments such as wetlands, lakes, and the coastal ocean.


Subject(s)
Environmental Exposure , Fishes/metabolism , Geologic Sediments/analysis , Invertebrates/metabolism , Mercury/metabolism , Methylmercury Compounds/metabolism , Animals , California , Environmental Monitoring , Geologic Sediments/chemistry , Mercury/analysis , Methylmercury Compounds/analysis , Mining , Rivers , Water Pollutants, Chemical/analysis , Wetlands
13.
Sci Total Environ ; 568: 727-738, 2016 Oct 15.
Article in English | MEDLINE | ID: mdl-27130329

ABSTRACT

Large-scale assessments are valuable in identifying primary factors controlling total mercury (THg) and monomethyl mercury (MeHg) concentrations, and distribution in aquatic ecosystems. Bed sediment THg and MeHg concentrations were compiled for >16,000 samples collected from aquatic habitats throughout the West between 1965 and 2013. The influence of aquatic feature type (canals, estuaries, lakes, and streams), and environmental setting (agriculture, forest, open-water, range, wetland, and urban) on THg and MeHg concentrations was examined. THg concentrations were highest in lake (29.3±6.5µgkg(-1)) and canal (28.6±6.9µgkg(-1)) sites, and lowest in stream (20.7±4.6µgkg(-1)) and estuarine (23.6±5.6µgkg(-1)) sites, which was partially a result of differences in grain size related to hydrologic gradients. By environmental setting, open-water (36.8±2.2µgkg(-1)) and forested (32.0±2.7µgkg(-1)) sites generally had the highest THg concentrations, followed by wetland sites (28.9±1.7µgkg(-1)), rangeland (25.5±1.5µgkg(-1)), agriculture (23.4±2.0µgkg(-1)), and urban (22.7±2.1µgkg(-1)) sites. MeHg concentrations also were highest in lakes (0.55±0.05µgkg(-1)) and canals (0.54±0.11µgkg(-1)), but, in contrast to THg, MeHg concentrations were lowest in open-water sites (0.22±0.03µgkg(-1)). The median percent MeHg (relative to THg) for the western region was 0.7%, indicating an overall low methylation efficiency; however, a significant subset of data (n>100) had percentages that represent elevated methylation efficiency (>6%). MeHg concentrations were weakly correlated with THg (r(2)=0.25) across western North America. Overall, these results highlight the large spatial variability in sediment THg and MeHg concentrations throughout western North America and underscore the important roles that landscape and land-use characteristics have on the MeHg cycle.


Subject(s)
Environmental Monitoring/methods , Geologic Sediments/analysis , Mercury/analysis , Methylmercury Compounds/analysis , Water Pollutants, Chemical/analysis , Northwest Territories , Northwestern United States
14.
Sci Total Environ ; 568: 697-711, 2016 Oct 15.
Article in English | MEDLINE | ID: mdl-26994752

ABSTRACT

The biogeochemical cycling of metals and other contaminants in river-floodplain corridors is controlled by microbial activity responding to dynamic redox conditions. Riverine flooding thus has the potential to affect speciation of redox-sensitive metals such as mercury (Hg). Therefore, inundation history over a period of decades potentially holds information on past production of bioavailable Hg. We investigate this within a Northern California river system with a legacy of landscape-scale 19th century hydraulic gold mining. We combine hydraulic modeling, Hg measurements in sediment and biota, and first-order calculations of mercury transformation to assess the potential role of river floodplains in producing monomethylmercury (MMHg), a neurotoxin which accumulates in local and migratory food webs. We identify frequently inundated floodplain areas, as well as floodplain areas inundated for long periods. We quantify the probability of MMHg production potential (MPP) associated with hydrology in each sector of the river system as a function of the spatial patterns of overbank inundation and drainage, which affect long-term redox history of contaminated sediments. Our findings identify river floodplains as periodic, temporary, yet potentially important, loci of biogeochemical transformation in which contaminants may undergo change during limited periods of the hydrologic record. We suggest that inundation is an important driver of MPP in river corridors and that the entire flow history must be analyzed retrospectively in terms of inundation magnitude and frequency in order to accurately assess biogeochemical risks, rather than merely highlighting the largest floods or low-flow periods. MMHg bioaccumulation within the aquatic food web in this system may pose a major risk to humans and waterfowl that eat migratory salmonids, which are being encouraged to come up these rivers to spawn. There is a long-term pattern of MPP under the current flow regime that is likely to be accentuated by increasingly common large floods with extended duration.


Subject(s)
Environmental Monitoring/methods , Mercury/analysis , Methylmercury Compounds/analysis , Rivers/chemistry , Water Pollutants, Chemical/analysis , California , Environmental Monitoring/history , Floods , Gold , History, 20th Century , History, 21st Century , Hydrology , Mercury/chemistry , Methylation , Methylmercury Compounds/chemistry , Mining , Models, Chemical , Rivers/microbiology , Water Pollutants, Chemical/chemistry
15.
Environ Pollut ; 212: 366-373, 2016 May.
Article in English | MEDLINE | ID: mdl-26874318

ABSTRACT

Wetlands are hotspots for production of toxic methylmercury (MeHg) that can bioaccumulate in the food web. The objective of this study was to determine whether the application of zero-valent iron (ZVI) or granular activated carbon (GAC) to wetland sediment could reduce MeHg production and bioavailability to benthic organisms. Field mesocosms were installed in a wetland fringing Hodgdon Pond (Maine, USA), and ZVI and GAC were applied. Pore-water MeHg concentrations were lower in treated compared with untreated mesocosms; however, sediment MeHg, as well as total Hg (THg), concentrations were not significantly different between treated and untreated mesocosms, suggesting that smaller pore-water MeHg concentrations in treated sediment were likely due to adsorption to ZVI and GAC, rather than inhibition of MeHg production. In laboratory experiments with intact vegetated sediment clumps, amendments did not significantly change sediment THg and MeHg concentrations; however, the mean pore-water MeHg and MeHg:THg ratios were lower in the amended sediment than the control. In the laboratory microcosms, snails (Lymnaea stagnalis) accumulated less MeHg in sediment treated with ZVI or GAC. The study results suggest that both GAC and ZVI have potential for reducing MeHg bioaccumulation in wetland sediment.


Subject(s)
Charcoal/chemistry , Environmental Monitoring , Environmental Restoration and Remediation , Geologic Sediments/chemistry , Iron/chemistry , Mercury/chemistry , Soil Pollutants/chemistry , Wetlands , Biological Availability , Charcoal/analysis , Environmental Restoration and Remediation/methods , Geologic Sediments/analysis , Humans , Iron/analysis , Mercury/analysis , Methylmercury Compounds , Soil Pollutants/analysis , United States , Water Pollutants, Chemical/analysis
16.
Environ Sci Technol ; 50(4): 1691-702, 2016 Feb 16.
Article in English | MEDLINE | ID: mdl-26789018

ABSTRACT

We measured total mercury (THg) and monomethyl mercury (MMHg) concentrations and mercury (Hg) isotopic compositions in sediment and aquatic organisms from the Yuba River (California, USA) to identify Hg sources and biogeochemical transformations downstream of a historical gold mining region. Sediment THg concentrations and δ(202)Hg decreased from the upper Yuba Fan to the lower Yuba Fan and the Feather River. These results are consistent with the release of Hg during gold mining followed by downstream mixing and dilution. The Hg isotopic composition of Yuba Fan sediment (δ(202)Hg = -0.38 ± 0.17‰ and Δ(199)Hg = 0.04 ± 0.03‰; mean ± 1 SD, n = 7) provides a fingerprint of inorganic Hg (IHg) that could be methylated locally or after transport downstream. The isotopic composition of MMHg in the Yuba River food web was estimated using biota with a range of %MMHg (the percent of THg present as MMHg) and compared to IHg in sediment, algae, and the food web. The estimated δ(202)Hg of MMHg prior to photodegradation (-1.29 to -1.07‰) was lower than that of IHg and we suggest this is due to mass-dependent fractionation (MDF) of up to -0.9‰ between IHg and MMHg. This result is in contrast to net positive MDF (+0.4 to +0.8‰) previously observed in lakes, estuaries, coastal oceans, and forests. We hypothesize that this unique relationship could be due to differences in the extent or pathway of biotic MMHg degradation in stream environments.


Subject(s)
Environmental Pollutants/chemistry , Gold , Mercury/chemistry , Methylmercury Compounds/chemistry , Mining/methods , Animals , California , Chemical Fractionation , Estuaries , Food Chain , Lakes/chemistry , Rivers/chemistry , Water Pollutants, Chemical/analysis
17.
Environ Sci Technol ; 50(2): 573-83, 2016 Jan 19.
Article in English | MEDLINE | ID: mdl-26651265

ABSTRACT

The San Francisco Bay-Delta Estuary watershed is a major source of freshwater for California and a profoundly human-impacted environment. The water quality monitoring that is critical to the management of this important water resource and ecosystem relies primarily on a system of fixed water-quality monitoring stations, but the limited spatial coverage often hinders understanding. Here, we show how the latest technology in visible/near-infrared imaging spectroscopy can facilitate water quality monitoring in this highly dynamic and heterogeneous system by enabling simultaneous depictions of several water quality indicators at very high spatial resolution. The airborne portable remote imaging spectrometer (PRISM) was used to derive high-spatial-resolution (2.6 × 2.6 m) distributions of turbidity, and dissolved organic carbon (DOC) and chlorophyll-a concentrations in a wetland-influenced region of this estuary. A filter-passing methylmercury vs DOC relationship was also developed using in situ samples and enabled the high-spatial-resolution depiction of surface methylmercury concentrations in this area. The results illustrate how high-resolution imaging spectroscopy can inform management and policy development in important inland and estuarine water bodies by facilitating the detection of point- and nonpoint-source pollution, and by providing data to help assess the complex impacts of wetland restoration and climate change on water quality and ecosystem productivity.


Subject(s)
Bays/analysis , Environmental Monitoring/methods , Estuaries , Remote Sensing Technology , Water Quality , California , Spectrophotometry, Ultraviolet
18.
Environ Toxicol Chem ; 34(7): 1649-58, 2015 Jul.
Article in English | MEDLINE | ID: mdl-25732794

ABSTRACT

In Berlin, New Hampshire, USA, the Androscoggin River flows adjacent to a former chlor-alkali facility that is a US Environmental Protection Agency Superfund site and source of mercury (Hg) to the river. The present study was conducted to determine the fate and bioaccumulation of methylmercury (MeHg) to lower trophic-level taxa in the river. Surface sediment directly adjacent to the source showed significantly elevated MeHg (10-40× increase, mean ± standard deviation [SD]: 20.1 ± 24.8 ng g(-1) dry wt) and total mercury (THg; 10-30× increase, mean ± SD: 2045 ± 2669 ng g(-1) dry wt) compared with all other reaches, with sediment THg and MeHg from downstream reaches elevated (3-7× on average) relative to the reference (THg mean ± SD: 33.5 ± 9.33 ng g(-1) dry wt; MeHg mean ± SD: 0.52 ± 0.21 ng g(-1) dry wt). Water column THg concentrations adjacent to the point source for both particulate (0.23 ng L(-1)) and dissolved (0.76 ng L(-1)) fractions were 5-fold higher than at the reference sites, and 2-fold to 5-fold higher than downstream. Methylmercury production potential of periphyton material was highest (2-9 ng g(-1) d(-1) dry wt) adjacent to the Superfund site; other reaches were close to or below reporting limits (0. 1 ng g(-1) d(-1) dry wt). Total Hg and MeHg bioaccumulation in fauna was variable across sites and taxa, with no clear spatial patterns downstream of the contamination source. Crayfish, mayflies, and shiners showed a weak positive relationship with porewater MeHg concentration.


Subject(s)
Astacoidea/metabolism , Environmental Monitoring , Fishes/metabolism , Insecta/metabolism , Mercury/analysis , Mercury/metabolism , Water Pollutants, Chemical/analysis , Animals , Astacoidea/chemistry , Geologic Sediments/chemistry , Industry , Insecta/chemistry , Methylmercury Compounds/analysis , Methylmercury Compounds/metabolism , Rivers/chemistry
19.
Sci Total Environ ; 511: 489-500, 2015 Apr 01.
Article in English | MEDLINE | ID: mdl-25576792

ABSTRACT

We examined mercury (Hg) speciation in water and sediment of the Great Salt Lake and surrounding wetlands, a locale spanning fresh to hypersaline and oxic to anoxic conditions, in order to test the hypothesis that spatial and temporal variations in Hg concentration and methylation rates correspond to observed spatial and temporal trends in Hg burdens previously reported in biota. Water column, sediment, and pore water concentrations of methylmercury (MeHg) and total mercury (THg), as well as related aquatic chemical parameters were examined. Inorganic Hg(II)-methylation rates were determined in selected water column and sediment subsamples spiked with inorganic divalent mercury (204Hg(II)). Net production of Me204Hg was expressed as apparent first-order rate constants for methylation (kmeth), which were also expanded to MeHg production potential (MPP) rates via combination with tin reducible 'reactive' Hg(II) (Hg(II)R) as a proxy for bioavailable Hg(II). Notable findings include: 1) elevated Hg concentrations previously reported in birds and brine flies were spatially proximal to the measured highest MeHg concentrations, the latter occurring in the anoxic deep brine layer (DBL) of the Great Salt Lake; 2) timing of reduced Hg(II)-methylation rates in the DBL (according to both kmeth and MPP) coincides with reduced Hg burdens among aquatic invertebrates (brine shrimp and brine flies) that act as potential vectors of Hg propagation to the terrestrial ecosystem; 3) values of kmeth were found to fall within the range reported by other studies; and 4) MPP rates were on the lower end of the range reported in methodologically comparable studies, suggesting the possibility that elevated MeHg in the anoxic deep brine layer results from its accumulation and persistence in this quasi-isolated environment, due to the absence of light (restricting abiotic photo demethylation) and/or minimal microbiological demethylation.


Subject(s)
Environmental Monitoring , Lakes/chemistry , Methylmercury Compounds/analysis , Water Pollutants, Chemical/analysis , Methylation , Salinity , Utah
20.
Sci Total Environ ; 494-495: 65-73, 2014 Oct 01.
Article in English | MEDLINE | ID: mdl-25033466

ABSTRACT

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.


Subject(s)
Food Chain , Lakes/chemistry , Mercury/metabolism , Plankton/metabolism , Water Pollutants, Chemical/metabolism , Environmental Monitoring , Mercury/analysis , Plankton/classification , Water Pollutants, Chemical/analysis
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