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Title: Intracellular Hg(0) Oxidation in Desulfovibrio desulfuricans ND132

Abstract

The disposal of elemental mercury (Hg(0)) wastes in mining and manufacturing areas has caused serious soil and groundwater contamination issues. Under anoxic conditions, certain anaerobic bacteria can oxidize dissolved elemental mercury and convert the oxidized Hg to neurotoxic methylmercury. In this study, we conducted experiments with the Hg-methylating bacterium Desulfovibrio desulfuricans ND132 to elucidate the role of cellular thiols in anaerobic Hg(0) oxidation. The concentrations of cell-surface and intracellular thiols were measured, and specific fractions of D. desulfuricans ND132 were examined for Hg(0) oxidation activity and analyzed with extended X-ray absorption fine structure (EXAFS) spectroscopy. The experimental data indicate that intracellular thiol concentrations are approximately six times higher than those of the cell wall. Cells reacted with a thiol-blocking reagent were severely impaired in Hg(0) oxidation activity. Spheroplasts lacking cell walls rapidly oxidized Hg(0) to Hg(II), while cell wall fragments exhibited low reactivity toward Hg(0). EXAFS analysis of spheroplast samples revealed that multiple different forms of Hg-thiols are produced by the Hg(0) oxidation reaction and that the local coordination environment of the oxidized Hg changes with reaction time. Here, the results of this study indicate that Hg(0) oxidation in D. desulfuricans ND132 is an intracellular process that occurs by reactionmore » with thiol-containing molecules.« less

Authors:
 [1];  [1];  [2];  [1]
  1. Rutgers Univ., New Brunswick, NJ (United States)
  2. Illinois Inst. of Technology, Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1331675
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 50; Journal Issue: 20; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
54 ENVIRONMENTAL SCIENCES; thiols; extended X-ray absorption fine structure; cells; mercury; oxidation

Citation Formats

Wang, Yuwei, Schaefer, Jeffra K., Mishra, Bhoopesh, and Yee, Nathan. Intracellular Hg(0) Oxidation in Desulfovibrio desulfuricans ND132. United States: N. p., 2016. Web. doi:10.1021/acs.est.6b03299.
Wang, Yuwei, Schaefer, Jeffra K., Mishra, Bhoopesh, & Yee, Nathan. Intracellular Hg(0) Oxidation in Desulfovibrio desulfuricans ND132. United States. https://doi.org/10.1021/acs.est.6b03299
Wang, Yuwei, Schaefer, Jeffra K., Mishra, Bhoopesh, and Yee, Nathan. Wed . "Intracellular Hg(0) Oxidation in Desulfovibrio desulfuricans ND132". United States. https://doi.org/10.1021/acs.est.6b03299. https://www.osti.gov/servlets/purl/1331675.
@article{osti_1331675,
title = {Intracellular Hg(0) Oxidation in Desulfovibrio desulfuricans ND132},
author = {Wang, Yuwei and Schaefer, Jeffra K. and Mishra, Bhoopesh and Yee, Nathan},
abstractNote = {The disposal of elemental mercury (Hg(0)) wastes in mining and manufacturing areas has caused serious soil and groundwater contamination issues. Under anoxic conditions, certain anaerobic bacteria can oxidize dissolved elemental mercury and convert the oxidized Hg to neurotoxic methylmercury. In this study, we conducted experiments with the Hg-methylating bacterium Desulfovibrio desulfuricans ND132 to elucidate the role of cellular thiols in anaerobic Hg(0) oxidation. The concentrations of cell-surface and intracellular thiols were measured, and specific fractions of D. desulfuricans ND132 were examined for Hg(0) oxidation activity and analyzed with extended X-ray absorption fine structure (EXAFS) spectroscopy. The experimental data indicate that intracellular thiol concentrations are approximately six times higher than those of the cell wall. Cells reacted with a thiol-blocking reagent were severely impaired in Hg(0) oxidation activity. Spheroplasts lacking cell walls rapidly oxidized Hg(0) to Hg(II), while cell wall fragments exhibited low reactivity toward Hg(0). EXAFS analysis of spheroplast samples revealed that multiple different forms of Hg-thiols are produced by the Hg(0) oxidation reaction and that the local coordination environment of the oxidized Hg changes with reaction time. Here, the results of this study indicate that Hg(0) oxidation in D. desulfuricans ND132 is an intracellular process that occurs by reaction with thiol-containing molecules.},
doi = {10.1021/acs.est.6b03299},
journal = {Environmental Science and Technology},
number = 20,
volume = 50,
place = {United States},
year = {Wed Sep 21 00:00:00 EDT 2016},
month = {Wed Sep 21 00:00:00 EDT 2016}
}

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Works referenced in this record:

Mercury Speciation and Mobilization in a Wastewater-Contaminated Groundwater Plume
journal, November 2013

  • Lamborg, Carl H.; Kent, Doug B.; Swarr, Gretchen J.
  • Environmental Science & Technology, Vol. 47, Issue 23
  • DOI: 10.1021/es402441d

Mercury (II) reduction and co-precipitation of metallic mercury on hydrous ferric oxide in contaminated groundwater
journal, January 2016


X-ray Absorption Spectroscopic Evidence for the Complexation of Hg(II) by Reduced Sulfur in Soil Humic Substances
journal, January 1999

  • Xia, K.; Skyllberg, U. L.; Bleam, W. F.
  • Environmental Science & Technology, Vol. 33, Issue 2
  • DOI: 10.1021/es980433q

Interactions between mercury and dissolved organic matter––a review
journal, April 2004


Transport of elemental mercury in the unsaturated zone from a waste disposal site in an arid region
journal, March 2008


The Chemical Cycle and Bioaccumulation of Mercury
journal, November 1998


Mechanisms Regulating Mercury Bioavailability for Methylating Microorganisms in the Aquatic Environment: A Critical Review
journal, February 2013

  • Hsu-Kim, Heileen; Kucharzyk, Katarzyna H.; Zhang, Tong
  • Environmental Science & Technology, Vol. 47, Issue 6
  • DOI: 10.1021/es304370g

History of mercury use and environmental contamination at the Oak Ridge Y-12 Plant
journal, January 2011


Characterization of soils from an industrial complex contaminated with elemental mercury
journal, August 2013


Mercury mobility at the Carson River Superfund Site, west-central Nevada, USA: Interpretation of mercury speciation data in mill tailings, soils, and sediments
journal, April 1997


Speciation of Mercury and Mode of Transport from Placer Gold Mine Tailings
journal, January 2005

  • Slowey, Aaron J.; Rytuba, James J.; Brown, Gordon E.
  • Environmental Science & Technology, Vol. 39, Issue 6
  • DOI: 10.1021/es049113z

Anaerobic oxidation of Hg(0) and methylmercury formation by Desulfovibrio desulfuricans ND132
journal, July 2013

  • Colombo, Matthew J.; Ha, Juyoung; Reinfelder, John R.
  • Geochimica et Cosmochimica Acta, Vol. 112
  • DOI: 10.1016/j.gca.2013.03.001

Oxidation and methylation of dissolved elemental mercury by anaerobic bacteria
journal, August 2013

  • Hu, Haiyan; Lin, Hui; Zheng, Wang
  • Nature Geoscience, Vol. 6, Issue 9
  • DOI: 10.1038/ngeo1894

Unexpected Effects of Gene Deletion on Interactions of Mercury with the Methylation-Deficient Mutant Δ hgcAB
journal, April 2014

  • Lin, Hui; Hurt, Richard A.; Johs, Alexander
  • Environmental Science & Technology Letters, Vol. 1, Issue 5
  • DOI: 10.1021/ez500107r

Coupled Mercury–Cell Sorption, Reduction, and Oxidation on Methylmercury Production by Geobacter sulfurreducens PCA
journal, October 2014

  • Lin, Hui; Morrell-Falvey, Jennifer L.; Rao, Balaji
  • Environmental Science & Technology, Vol. 48, Issue 20
  • DOI: 10.1021/es502537a

Mercury reduction and complexation by natural organic matter in anoxic environments
journal, January 2011

  • Gu, B.; Bian, Y.; Miller, C. L.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 4
  • DOI: 10.1073/pnas.1008747108

Mercury Reduction and Oxidation by Reduced Natural Organic Matter in Anoxic Environments
journal, November 2011

  • Zheng, Wang; Liang, Liyuan; Gu, Baohua
  • Environmental Science & Technology, Vol. 46, Issue 1
  • DOI: 10.1021/es203402p

Sulfate-Reducing Bacterium Desulfovibrio desulfuricans ND132 as a Model for Understanding Bacterial Mercury Methylation
journal, April 2011

  • Gilmour, Cynthia C.; Elias, Dwayne A.; Kucken, Amy M.
  • Applied and Environmental Microbiology, Vol. 77, Issue 12, p. 3938-3951
  • DOI: 10.1128/AEM.02993-10

Sporulation and further nutritional characteristics of Desulfotomaculum acetoxidans
journal, July 1981

  • Widdel, Friedrich; Pfennig, Norbert
  • Archives of Microbiology, Vol. 129, Issue 5
  • DOI: 10.1007/BF00406471

A Highly Sensitive Fluorescence Probe for Fast Thiol-Quantification Assay of Glutathione Reductase
journal, May 2009

  • Yi, Long; Li, Heyang; Sun, Lu
  • Angewandte Chemie International Edition, Vol. 48, Issue 22
  • DOI: 10.1002/anie.200805693

High-Throughput Mass Spectrometric Analysis of Covalent Protein-Inhibitor Adducts for the Discovery of Irreversible Inhibitors: A Complete Workflow
journal, December 2015

  • Campuzano, Iain D. G.; San Miguel, Tisha; Rowe, Todd
  • Journal of Biomolecular Screening, Vol. 21, Issue 2
  • DOI: 10.1177/1087057115621288

The UWXAFS analysis package: philosophy and details
journal, March 1995


ATHENA and ARTEMIS Interactive Graphical Data Analysisusing IFEFFIT
journal, January 2005


High- and low-affinity binding sites for Cd on the bacterial cell walls of Bacillus subtilis and Shewanella oneidensis
journal, August 2010

  • Mishra, Bhoopesh; Boyanov, Maxim; Bunker, Bruce A.
  • Geochimica et Cosmochimica Acta, Vol. 74, Issue 15
  • DOI: 10.1016/j.gca.2010.02.019

Thiol self-assembled monolayers on mercury surfaces: the adsorption and electrochemistry of ω-mercaptoalkanoic acids
journal, November 1999


Studying thiol adsorption on Au, Ag and Hg surfaces by potentiometric measurements
journal, July 2003


Self-assembled monolayers (SAMs) for electrochemical sensing
journal, July 2011

  • Mandler, Daniel; Kraus-Ophir, Shlomit
  • Journal of Solid State Electrochemistry, Vol. 15, Issue 7-8
  • DOI: 10.1007/s10008-011-1493-6

Oxidation of Dissolved Elemental Mercury by Thiol Compounds under Anoxic Conditions
journal, November 2013

  • Zheng, Wang; Lin, Hui; Mann, Benjamin F.
  • Environmental Science & Technology, Vol. 47, Issue 22
  • DOI: 10.1021/es402697u

Mercury Reduction and Cell-Surface Adsorption by Geobacter sulfurreducens PCA
journal, September 2013

  • Hu, Haiyan; Lin, Hui; Zheng, Wang
  • Environmental Science & Technology, Vol. 47, Issue 19
  • DOI: 10.1021/es400527m

The effect of natural organic matter on the adsorption of mercury to bacterial cells
journal, February 2015

  • Dunham-Cheatham, Sarrah; Mishra, Bhoopesh; Myneni, Satish
  • Geochimica et Cosmochimica Acta, Vol. 150
  • DOI: 10.1016/j.gca.2014.11.018

Binding of Hg II to High-Affinity Sites on Bacteria Inhibits Reduction to Hg 0 by Mixed Fe II/III Phases
journal, November 2011

  • Mishra, Bhoopesh; O’Loughlin, Edward J.; Boyanov, Maxim I.
  • Environmental Science & Technology, Vol. 45, Issue 22
  • DOI: 10.1021/es201820c

Bacterial mercury resistance from atoms to ecosystems
journal, June 2003


Determination of thiol functional groups on bacteria and natural organic matter in environmental systems
journal, February 2014


The impact of ionic mercury on antioxidant defenses in two mercury-sensitive anaerobic bacteria
journal, October 2013


Response of the anaerobe Desulfovibrio vulgaris Hildenborough to oxidative conditions: proteome and transcript analysis
journal, January 2006


Occurrence of glutathione in bacteria
journal, March 1978


Relationships between Hg(ii)–S bond distance and Hg(ii) coordination in thiolates
journal, January 2008

  • Manceau, Alain; Nagy, Kathryn L.
  • Dalton Transactions, Issue 11
  • DOI: 10.1039/b718372k

Metallothionein-Like Multinuclear Clusters of Mercury(II) and Sulfur in Peat
journal, September 2011

  • Nagy, Kathryn L.; Manceau, Alain; Gasper, Jarrod D.
  • Environmental Science & Technology, Vol. 45, Issue 17
  • DOI: 10.1021/es201025v

Nuclear magnetic resonance studies of the solution chemistry of metal complexes. 25. Hg(thiol)3 complexes and HG(II)-thiol ligand exchange kinetics
journal, September 1988

  • Cheesman, Bruce V.; Arnold, Alan P.; Rabenstein, Dallas L.
  • Journal of the American Chemical Society, Vol. 110, Issue 19
  • DOI: 10.1021/ja00227a014

Mercury(II) Cysteine Complexes in Alkaline Aqueous Solution
journal, January 2006

  • Jalilehvand, Farideh; Leung, Bonnie O.; Izadifard, Maryam
  • Inorganic Chemistry, Vol. 45, Issue 1
  • DOI: 10.1021/ic0508932

Bacterial community succession during in situ uranium bioremediation: spatial similarities along controlled flow paths
journal, September 2008

  • Hwang, Chiachi; Wu, Weimin; Gentry, Terry J.
  • The ISME Journal, Vol. 3, Issue 1
  • DOI: 10.1038/ismej.2008.77

A Limited Microbial Consortium Is Responsible for Extended Bioreduction of Uranium in a Contaminated Aquifer
journal, July 2011

  • Gihring, Thomas M.; Zhang, Gengxin; Brandt, Craig C.
  • Applied and Environmental Microbiology, Vol. 77, Issue 17
  • DOI: 10.1128/AEM.00220-11

XANES Studies of Oxidation States of Sulfur in Aquatic and Soil Humic Substances
journal, January 1998


Works referencing / citing this record:

Mercury isotope signatures record photic zone euxinia in the Mesoproterozoic ocean
journal, October 2018

  • Zheng, Wang; Gilleaudeau, Geoffrey J.; Kah, Linda C.
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 42
  • DOI: 10.1073/pnas.1721733115