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Title: Mercury speciation, bioavailability, and biomagnification in contaminated streams on the Savannah River Site (SC, USA)

Abstract

Water, sediment, and biota from two streams on the Savannah River Site were sampled to study mercury (Hg) biogeochemistry. Total and methyl-Hg (MHg) concentrations were measured for all samples, speciation models were used to explore Hg speciation in the water, and Diffusive Gradients in Thin Films (DGT) were applied to indicate the vertical profiles of labile Hg (DGT-Hg). Trophic position (δ15N) was estimated for biota and used to establish MHg biomagnification model. Furthermore, the speciation model indicated Hg methylation in the water occurred on settling particles and the most bioavailable Hg species to bacteria were complexes of inorganic Hg and labile organic ligands. Correspondingly, dissolved organic carbon concentrations were positively related to MHg concentrations in the water. In the sediment, the sharp increase of DGT-Hg around the sediment water interface underscores the importance of this interface, which determines the differences in the accumulation and generation of labile Hg among different waterbodies. The positive correlation between sediment MHg and sulfate concentrations suggested possible methylation reaction by dissimilatory sulfate reducing bacteria in the sediment. The food web magnification factors of MHg were 9.6 (95% CI: 4.0 - 23.4) and 4.4 (95% 31 CI: 2.5 - 7.7) for the two streams established withmore » trophic data of biofilm, invertebrates, and fish. Meanwhile, DGT-Hg concentrations in the water were positively correlated to biofilm Hg concentrations, which can be combined with the MHg biomagnification model to generate a modified biomagnification model that estimate MHg bioaccumulation with only labile Hg concentrations in the water. With this approach, Hg accumulation in abiotic and biotic environmental compartments were connected and the different bioaccumulation patterns of Hg in different waterbodies were explained with both geochemical and biological factors.« less

Authors:
ORCiD logo [1];  [1];  [1];  [2]
  1. Univ. of Georgia, Aiken, SC (United States)
  2. Univ. of Georgia, Aiken, SC (United States); Univ. of South Florida, Tampa, FL (United States)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States). Savannah River Ecology Lab. (SREL)
Sponsoring Org.:
USDOE
Contributing Org.:
Univ. of South Florida
OSTI Identifier:
1819450
Alternate Identifier(s):
OSTI ID: 1528639
Grant/Contract Number:  
FC09-07SR22506; EM0004391
Resource Type:
Accepted Manuscript
Journal Name:
Science of the Total Environment
Additional Journal Information:
Journal Volume: 668; Journal ID: ISSN 0048-9697
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Mercury; Speciation; Methylation; Bioavailability; Biomagnification; Diffusive gradients in thin films

Citation Formats

Xu, Xiaoyu, Bryan, Albert L., Mills, Gary L., and Korotasz, Alexis M. Mercury speciation, bioavailability, and biomagnification in contaminated streams on the Savannah River Site (SC, USA). United States: N. p., 2019. Web. doi:10.1016/j.scitotenv.2019.02.301.
Xu, Xiaoyu, Bryan, Albert L., Mills, Gary L., & Korotasz, Alexis M. Mercury speciation, bioavailability, and biomagnification in contaminated streams on the Savannah River Site (SC, USA). United States. https://doi.org/10.1016/j.scitotenv.2019.02.301
Xu, Xiaoyu, Bryan, Albert L., Mills, Gary L., and Korotasz, Alexis M. Wed . "Mercury speciation, bioavailability, and biomagnification in contaminated streams on the Savannah River Site (SC, USA)". United States. https://doi.org/10.1016/j.scitotenv.2019.02.301. https://www.osti.gov/servlets/purl/1819450.
@article{osti_1819450,
title = {Mercury speciation, bioavailability, and biomagnification in contaminated streams on the Savannah River Site (SC, USA)},
author = {Xu, Xiaoyu and Bryan, Albert L. and Mills, Gary L. and Korotasz, Alexis M.},
abstractNote = {Water, sediment, and biota from two streams on the Savannah River Site were sampled to study mercury (Hg) biogeochemistry. Total and methyl-Hg (MHg) concentrations were measured for all samples, speciation models were used to explore Hg speciation in the water, and Diffusive Gradients in Thin Films (DGT) were applied to indicate the vertical profiles of labile Hg (DGT-Hg). Trophic position (δ15N) was estimated for biota and used to establish MHg biomagnification model. Furthermore, the speciation model indicated Hg methylation in the water occurred on settling particles and the most bioavailable Hg species to bacteria were complexes of inorganic Hg and labile organic ligands. Correspondingly, dissolved organic carbon concentrations were positively related to MHg concentrations in the water. In the sediment, the sharp increase of DGT-Hg around the sediment water interface underscores the importance of this interface, which determines the differences in the accumulation and generation of labile Hg among different waterbodies. The positive correlation between sediment MHg and sulfate concentrations suggested possible methylation reaction by dissimilatory sulfate reducing bacteria in the sediment. The food web magnification factors of MHg were 9.6 (95% CI: 4.0 - 23.4) and 4.4 (95% 31 CI: 2.5 - 7.7) for the two streams established with trophic data of biofilm, invertebrates, and fish. Meanwhile, DGT-Hg concentrations in the water were positively correlated to biofilm Hg concentrations, which can be combined with the MHg biomagnification model to generate a modified biomagnification model that estimate MHg bioaccumulation with only labile Hg concentrations in the water. With this approach, Hg accumulation in abiotic and biotic environmental compartments were connected and the different bioaccumulation patterns of Hg in different waterbodies were explained with both geochemical and biological factors.},
doi = {10.1016/j.scitotenv.2019.02.301},
journal = {Science of the Total Environment},
number = ,
volume = 668,
place = {United States},
year = {Wed Feb 20 00:00:00 EST 2019},
month = {Wed Feb 20 00:00:00 EST 2019}
}

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Works referenced in this record:

In situ speciation measurements of trace components in natural waters using thin-film gels
journal, February 1994


Precipitation of Mercuric Sulfide Nanoparticles in NOM-Containing Water: Implications for the Natural Environment
journal, April 2009

  • Deonarine, Amrika; Hsu-Kim, Heileen
  • Environmental Science & Technology, Vol. 43, Issue 7
  • DOI: 10.1021/es803130h

Floodplain methylmercury biomagnification factor higher than that of the contiguous river (South River, Virginia USA)
journal, October 2011


Biogeochemical Cycling of Methylmercury in Lakes and Tundra Watersheds of Arctic Alaska
journal, February 2006

  • Hammerschmidt, Chad R.; Fitzgerald, William F.; Lamborg, Carl H.
  • Environmental Science & Technology, Vol. 40, Issue 4
  • DOI: 10.1021/es051322b

Biological Methylation of Mercury in Aquatic Organisms
journal, August 1969


Factors controlling the bioaccumulation of mercury and methylmercury by the estuarine amphipod Leptocheirus plumulosus
journal, February 2001


Complexation of Cu and Pb by DOC in polluted groundwater: a comparison of experimental data and predictions by computer speciation models (WHAM and MINTEQA2)
journal, October 1999


Formation of Nanocolloidal Metacinnabar in Mercury-DOM-Sulfide Systems
journal, November 2011

  • Gerbig, Chase A.; Kim, Christopher S.; Stegemeier, John P.
  • Environmental Science & Technology, Vol. 45, Issue 21
  • DOI: 10.1021/es201837h

Sulfide Controls on Mercury Speciation and Bioavailability to Methylating Bacteria in Sediment Pore Waters
journal, March 1999

  • Benoit, Janina M.; Gilmour, Cynthia C.; Mason, Robert P.
  • Environmental Science & Technology, Vol. 33, Issue 6
  • DOI: 10.1021/es9808200

Sulfate stimulation of mercury methylation in freshwater sediments
journal, November 1992

  • Gilmour, Cynthia C.; Henry, Elizabeth A.; Mitchell, Ralph
  • Environmental Science & Technology, Vol. 26, Issue 11
  • DOI: 10.1021/es00035a029

Cycling of mercury in the environment: Sources, fate, and human health implications: A review
journal, May 2017


Contributions of Schoenoplectus californicus in a Constructed Wetland System Receiving Copper Contaminated Wastewater
journal, May 2005

  • Murray-Gulde, Cynthia L.; Huddleston, George M.; Garber, Kristina V.
  • Water, Air, and Soil Pollution, Vol. 163, Issue 1-4
  • DOI: 10.1007/s11270-005-1297-3

Investigation of Mercury Methylation Pathways in Biofilm versus Planktonic Cultures of Desulfovibrio desulfuricans
journal, May 2013

  • Lin, Tiffany Y.; Kampalath, Rita A.; Lin, Chu-Ching
  • Environmental Science & Technology, Vol. 47, Issue 11
  • DOI: 10.1021/es400079n

Null Hypothesis Testing: Problems, Prevalence, and an Alternative
journal, October 2000

  • Anderson, David R.; Burnham, Kenneth P.; Thompson, William L.
  • The Journal of Wildlife Management, Vol. 64, Issue 4
  • DOI: 10.2307/3803199

Methylmercury speciation in the dissolved phase of a stratified lake using the diffusive gradient in thin film technique
journal, March 2009


Appropriateness of Aufwuchs as a monitor of bioaccumulation
journal, January 1989


A unifying model of cation binding by humic substances
journal, October 1992


Limnological investigation methods for the periphyton (“Aufwuchs”) Community
journal, April 1962


The Estimated Six-Year Mercury Dry Deposition Across North America
journal, November 2016

  • Zhang, Leiming; Wu, Zhiyong; Cheng, Irene
  • Environmental Science & Technology, Vol. 50, Issue 23
  • DOI: 10.1021/acs.est.6b04276

Environmental factors affecting the formation of methylmercury in low pH lakes
journal, July 1990

  • Winfrey, Michael R.; Rudd, John W. M.
  • Environmental Toxicology and Chemistry, Vol. 9, Issue 7
  • DOI: 10.1002/etc.5620090705

Mercury Exposure as a Function of Fish Consumption in Two Asian Communities in Coastal Virginia, USA
journal, November 2014

  • Xu, Xiaoyu; Newman, Michael C.
  • Archives of Environmental Contamination and Toxicology, Vol. 68, Issue 3
  • DOI: 10.1007/s00244-014-0102-y

Effects of dissolved organic carbon and salinity on bioavailability of mercury.
journal, January 1997


Kinetics of metal exchange between solids and solutions in sediments and soils interpreted from DGT measured fluxes
journal, August 1998


Biotic ligand model of the acute toxicity of metals. 1. Technical Basis
journal, October 2001

  • Di Toro, Dominic M.; Allen, Herbert E.; Bergman, Harold L.
  • Environmental Toxicology and Chemistry, Vol. 20, Issue 10
  • DOI: 10.1002/etc.5620201034

Mercury sources and cycling in the Connecticut River and Long Island Sound
journal, November 2004


Performance of Diffusion Gradient in thin Films to Evaluate the Toxic Fraction of Copper to Daphnia Magna
journal, January 2004

  • Tusseau-Vuillemin, Marie-Hélène; Gilbin, Rodolphe; Bakkaus, Estelle
  • Environmental Toxicology and Chemistry, Vol. 23, Issue 9
  • DOI: 10.1897/03-202a

Intestinal Solubilization of Particle-Associated Organic and Inorganic Mercury as a Measure of Bioavailability to Benthic Invertebrates
journal, June 1999

  • Lawrence, Angie L.; McAloon, Kelly M.; Mason, Robert P.
  • Environmental Science & Technology, Vol. 33, Issue 11
  • DOI: 10.1021/es981328j

Geochemical factors complicating the use of aufwuchs to monitor bioaccumulation of arsenic, cadmium, chromium, copper and zinc
journal, January 1985


An Ecologically Framed Mercury Survey of Finfish of the Lower Chesapeake Bay
journal, May 2013

  • Xu, Xiaoyu; Newman, Michael C.; Fabrizio, Mary C.
  • Archives of Environmental Contamination and Toxicology, Vol. 65, Issue 3
  • DOI: 10.1007/s00244-013-9917-1

Stepwise enrichment of 15N along food chains: Further evidence and the relation between δ15N and animal age
journal, May 1984


Influences of Zero-Valent Sulfur on Mercury Methylation in Bacterial Cocultures
journal, January 2013

  • Kampalath, Rita A.; Lin, Chu-Ching; Jay, Jennifer A.
  • Water, Air, & Soil Pollution, Vol. 224, Issue 2
  • DOI: 10.1007/s11270-012-1399-7

Higher and more variable methylmercury biomagnification factors for floodplain than the contiguous river (South River, Virginia USA)
journal, June 2013


Role of the ocean in the global mercury cycle: ROLE OF OCEAN IN GLOBAL HG CYCLE
journal, November 2002

  • Mason, R. P.; Sheu, G. -R.
  • Global Biogeochemical Cycles, Vol. 16, Issue 4
  • DOI: 10.1029/2001GB001440

Inference by Eye: Confidence Intervals and How to Read Pictures of Data.
journal, January 2005


Uptake, Toxicity, and Trophic Transfer of Mercury in a Coastal Diatom
journal, January 1996

  • Mason, Robert P.; Reinfelder, John R.; Morel, François M. M.
  • Environmental Science & Technology, Vol. 30, Issue 6
  • DOI: 10.1021/es950373d

Dissolved Organic Matter Enhances Microbial Mercury Methylation Under Sulfidic Conditions
journal, February 2012

  • Graham, Andrew M.; Aiken, George R.; Gilmour, Cynthia C.
  • Environmental Science & Technology, Vol. 46, Issue 5
  • DOI: 10.1021/es203658f

Distribution of dissolved iron in sediment pore waters at submillimetre resolution
journal, July 1991

  • Davison, W.; Grime, G. W.; Morgan, J. A. W.
  • Nature, Vol. 352, Issue 6333
  • DOI: 10.1038/352323a0

Influence of natural dissolved organic carbon on the bioavailability of mercury to a freshwater alga
journal, July 2008


Geochemical factors complicating the use of aufwuchs as a biomonitor for lead levels in two New Jersey reservoirs
journal, January 1983


Modelling ion binding by humic acids
journal, June 1993


Do constructed wetlands remove metals or increase metal bioavailability?
journal, July 2018


The mercury cycle and fish in the Adirondack lakes
journal, March 1994

  • Driscoll, Charles T.; Yan, Cheng; Schofield, Carl L.
  • Environmental Science & Technology, Vol. 28, Issue 3
  • DOI: 10.1021/es00052a003

Influence of Natural Organic Matter Source on Copper Speciation As Demonstrated by Cu Binding to Fish Gills, by Ion Selective Electrode, and by DGT Gel Sampler
journal, May 2004

  • Luider, Chad D.; Crusius, John; Playle, Richard C.
  • Environmental Science & Technology, Vol. 38, Issue 10
  • DOI: 10.1021/es030566y

Isotopic fractionation during the uptake and elimination of inorganic mercury by a marine fish
journal, November 2015


The Seasonal Dynamics of The Chesapeake Bay Ecosystem
journal, December 1989

  • Baird, Daniel; Ulanowicz, Robert E.
  • Ecological Monographs, Vol. 59, Issue 4
  • DOI: 10.2307/1943071

Geochemical Controls on the Production and Distribution of Methylmercury in Near-Shore Marine Sediments
journal, March 2004

  • Hammerschmidt, Chad R.; Fitzgerald, William F.
  • Environmental Science & Technology, Vol. 38, Issue 5
  • DOI: 10.1021/es034528q

Gill surface interaction model for trace-metal toxicity to fishes: role of complexation, pH, and water hardness
journal, June 1983

  • Pagenkopf, Gordon K.
  • Environmental Science & Technology, Vol. 17, Issue 6
  • DOI: 10.1021/es00112a007

Comparison of Analytical Techniques for Dynamic Trace Metal Speciation in Natural Freshwaters
journal, March 2006

  • Sigg, Laura; Black, Frank; Buffle, Jacques
  • Environmental Science & Technology, Vol. 40, Issue 6
  • DOI: 10.1021/es051245k

Predicting Net Mercury Methylation in Sediments Using Diffusive Gradient in Thin Films Measurements
journal, February 2011

  • Clarisse, Olivier; Dimock, Brian; Hintelmann, Holger
  • Environmental Science & Technology, Vol. 45, Issue 4
  • DOI: 10.1021/es102730n

Impact of Criticism of Null-Hypothesis Significance Testing on Statistical Reporting Practices in Conservation Biology
journal, October 2006


Mercury methylation in aquatic systems affected by acid deposition
journal, January 1991


Performance Characteristics of Diffusion Gradients in Thin Films for the in Situ Measurement of Trace Metals in Aqueous Solution
journal, October 1995

  • Zhang, Hao.; Davison, William.
  • Analytical Chemistry, Vol. 67, Issue 19
  • DOI: 10.1021/ac00115a005

Biomonitoring and assessment of monomethylmercury exposure in aqueous systems using the DGT technique
journal, February 2012


Sulfate-Reducing Bacteria: Principal Methylators of Mercury in Anoxic Estuarine Sediment †
journal, January 1985


In situ high resolution measurements of fluxes of Ni, Cu, Fe, and Mn and concentrations of Zn and Cd in porewaters by DGT
journal, October 1995


Re-evaluation of distillation and comparison with HNO3 leaching/solvent extraction for isolation of methylmercury compounds from sediment/soil samples
journal, May 2004

  • Liang, Lian; Horvat, Milena; Feng, Xinbin
  • Applied Organometallic Chemistry, Vol. 18, Issue 6
  • DOI: 10.1002/aoc.617