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

G. sulfurreducens PCA cells have been shown to reduce, sorb, and methylate Hg(II) species, but it is unclear whether this organism can oxidize and methylate dissolved elemental Hg(0) as shown for Desulfovibrio desulfuricans ND132. Using Hg(II) and Hg(0) separately as Hg sources in washed cell assays...

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Published in:Environmental science & technology 2014-10, Vol.48 (20), p.11969-11976
Main Authors: Lin, Hui, Morrell-Falvey, Jennifer L, Rao, Balaji, Liang, Liyuan, Gu, Baohua
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container_issue 20
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description G. sulfurreducens PCA cells have been shown to reduce, sorb, and methylate Hg(II) species, but it is unclear whether this organism can oxidize and methylate dissolved elemental Hg(0) as shown for Desulfovibrio desulfuricans ND132. Using Hg(II) and Hg(0) separately as Hg sources in washed cell assays in phosphate buffered saline (pH 7.4), we report how cell-mediated Hg reduction and oxidation compete or synergize with sorption, thus affecting the production of toxic methylmercury by PCA cells. Methylation is found to be positively correlated to Hg sorption (r = 0.73) but negatively correlated to Hg reduction (r = −0.62). These reactions depend on the Hg and cell concentrations or the ratio of Hg to cellular thiols (−SH). Oxidation and methylation of Hg(0) are favored at relatively low Hg to cell–SH molar ratios (e.g.,
doi_str_mv 10.1021/es502537a
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(ORNL), Oak Ridge, TN (United States)</creatorcontrib><description>G. sulfurreducens PCA cells have been shown to reduce, sorb, and methylate Hg(II) species, but it is unclear whether this organism can oxidize and methylate dissolved elemental Hg(0) as shown for Desulfovibrio desulfuricans ND132. Using Hg(II) and Hg(0) separately as Hg sources in washed cell assays in phosphate buffered saline (pH 7.4), we report how cell-mediated Hg reduction and oxidation compete or synergize with sorption, thus affecting the production of toxic methylmercury by PCA cells. Methylation is found to be positively correlated to Hg sorption (r = 0.73) but negatively correlated to Hg reduction (r = −0.62). These reactions depend on the Hg and cell concentrations or the ratio of Hg to cellular thiols (−SH). Oxidation and methylation of Hg(0) are favored at relatively low Hg to cell–SH molar ratios (e.g., &lt;1). Increasing Hg to cell ratios from 0.25 × 10–19 to 25 × 10–19 moles-Hg/cell (equivalent to Hg/cell–SH of 0.71 to 71) shifts the major reaction from oxidation to reduction. In the absence of five outer membrane c-type cytochromes, mutant ΔomcBESTZ also shows decreases in Hg reduction and increases in methylation. However, the presence of competing thiol-binding ions such as Zn2+ leads to increased Hg reduction and decreased methylation. These results suggest that the coupled cell-Hg sorption and redox transformations are important in controlling the rates of Hg uptake and methylation by G. sulfurreducens PCA in anoxic environments.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/es502537a</identifier><identifier>PMID: 25268220</identifier><identifier>CODEN: ESTHAG</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Adsorption ; Anaerobiosis ; Bacteriology ; BASIC BIOLOGICAL SCIENCES ; Bioassays ; Biological and medical sciences ; Cellular biology ; Cytochrome c Group - genetics ; Cytochrome c Group - metabolism ; Cytotoxicity ; Desulfovibrio desulfuricans ; Fundamental and applied biological sciences. 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(ORNL), Oak Ridge, TN (United States)</creatorcontrib><title>Coupled Mercury–Cell Sorption, Reduction, and Oxidation on Methylmercury Production by Geobacter sulfurreducens PCA</title><title>Environmental science &amp; technology</title><addtitle>Environ. Sci. Technol</addtitle><description>G. sulfurreducens PCA cells have been shown to reduce, sorb, and methylate Hg(II) species, but it is unclear whether this organism can oxidize and methylate dissolved elemental Hg(0) as shown for Desulfovibrio desulfuricans ND132. Using Hg(II) and Hg(0) separately as Hg sources in washed cell assays in phosphate buffered saline (pH 7.4), we report how cell-mediated Hg reduction and oxidation compete or synergize with sorption, thus affecting the production of toxic methylmercury by PCA cells. Methylation is found to be positively correlated to Hg sorption (r = 0.73) but negatively correlated to Hg reduction (r = −0.62). These reactions depend on the Hg and cell concentrations or the ratio of Hg to cellular thiols (−SH). Oxidation and methylation of Hg(0) are favored at relatively low Hg to cell–SH molar ratios (e.g., &lt;1). Increasing Hg to cell ratios from 0.25 × 10–19 to 25 × 10–19 moles-Hg/cell (equivalent to Hg/cell–SH of 0.71 to 71) shifts the major reaction from oxidation to reduction. In the absence of five outer membrane c-type cytochromes, mutant ΔomcBESTZ also shows decreases in Hg reduction and increases in methylation. However, the presence of competing thiol-binding ions such as Zn2+ leads to increased Hg reduction and decreased methylation. These results suggest that the coupled cell-Hg sorption and redox transformations are important in controlling the rates of Hg uptake and methylation by G. sulfurreducens PCA in anoxic environments.</description><subject>Adsorption</subject><subject>Anaerobiosis</subject><subject>Bacteriology</subject><subject>BASIC BIOLOGICAL SCIENCES</subject><subject>Bioassays</subject><subject>Biological and medical sciences</subject><subject>Cellular biology</subject><subject>Cytochrome c Group - genetics</subject><subject>Cytochrome c Group - metabolism</subject><subject>Cytotoxicity</subject><subject>Desulfovibrio desulfuricans</subject><subject>Fundamental and applied biological sciences. Psychology</subject><subject>Geobacter - drug effects</subject><subject>Geobacter - genetics</subject><subject>Geobacter - metabolism</subject><subject>Geobacter sulfurreducens</subject><subject>Gram-negative bacteria</subject><subject>Mercury - chemistry</subject><subject>Mercury - metabolism</subject><subject>Metabolism. Enzymes</subject><subject>Methylation</subject><subject>Methylmercury Compounds - metabolism</subject><subject>Microbiology</subject><subject>Oxidation</subject><subject>Oxidation-Reduction</subject><subject>Sorption</subject><subject>Sulfhydryl Compounds - metabolism</subject><subject>Zinc - metabolism</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><recordid>eNpl0d1qFDEUB_AgFrtWL3wBCYpgwdF8zmQuy2Cr0NLiB3g3nEnO0CmzkzWZgHvnO_iGfRKzzNqKQiAJ_M4_H4eQZ5y95Uzwdxg1E1pW8ICsuBas0Ebzh2TFGJdFLctvh-RxjDeMMSGZeUQOhRalEYKtSGp82ozo6AUGm8L29uevBseRfvZhMw9-ekM_oUt2WcLk6OWPwcFuS_O4wPl6O66XUnoV_J7SbkvP0HdgZww0prFPIexycIr0qjl5Qg56GCM-3c9H5Ovp-y_Nh-L88uxjc3JegCrNXCjswEiFworKKtkri51TihuHyCWXVteoTY9gKlCqlIAOlNNSaei4yKVH5MWS6-M8tNEOM9pr66cJ7dxyYcqK1xm9XtAm-O8J49yuh2jzJ8CEPsWWl6Kqq9IYlunLf-iNT2HKT9gpboTSSmV1vCgbfIwB-3YThjWEbctZu2tYe9ewbJ_vE1O3Rncn_3Qog1d7ANHC2AeY7BDvnalrUSp578DGv27134G_AWBmqps</recordid><startdate>20141021</startdate><enddate>20141021</enddate><creator>Lin, Hui</creator><creator>Morrell-Falvey, Jennifer L</creator><creator>Rao, Balaji</creator><creator>Liang, Liyuan</creator><creator>Gu, Baohua</creator><general>American Chemical Society</general><general>American Chemical Society (ACS)</general><scope>IQODW</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><scope>OIOZB</scope><scope>OTOTI</scope></search><sort><creationdate>20141021</creationdate><title>Coupled Mercury–Cell Sorption, Reduction, and Oxidation on Methylmercury Production by Geobacter sulfurreducens PCA</title><author>Lin, Hui ; Morrell-Falvey, Jennifer L ; Rao, Balaji ; Liang, Liyuan ; Gu, Baohua</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a468t-4eba834e2c27c43f4cebd4418dee1313c59e58fea87a4463aeda4d5345ab12a83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Adsorption</topic><topic>Anaerobiosis</topic><topic>Bacteriology</topic><topic>BASIC BIOLOGICAL SCIENCES</topic><topic>Bioassays</topic><topic>Biological and medical sciences</topic><topic>Cellular biology</topic><topic>Cytochrome c Group - genetics</topic><topic>Cytochrome c Group - metabolism</topic><topic>Cytotoxicity</topic><topic>Desulfovibrio desulfuricans</topic><topic>Fundamental and applied biological sciences. Psychology</topic><topic>Geobacter - drug effects</topic><topic>Geobacter - genetics</topic><topic>Geobacter - metabolism</topic><topic>Geobacter sulfurreducens</topic><topic>Gram-negative bacteria</topic><topic>Mercury - chemistry</topic><topic>Mercury - metabolism</topic><topic>Metabolism. Enzymes</topic><topic>Methylation</topic><topic>Methylmercury Compounds - metabolism</topic><topic>Microbiology</topic><topic>Oxidation</topic><topic>Oxidation-Reduction</topic><topic>Sorption</topic><topic>Sulfhydryl Compounds - metabolism</topic><topic>Zinc - metabolism</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lin, Hui</creatorcontrib><creatorcontrib>Morrell-Falvey, Jennifer L</creatorcontrib><creatorcontrib>Rao, Balaji</creatorcontrib><creatorcontrib>Liang, Liyuan</creatorcontrib><creatorcontrib>Gu, Baohua</creatorcontrib><creatorcontrib>Oak Ridge National Lab. 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(ORNL), Oak Ridge, TN (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Coupled Mercury–Cell Sorption, Reduction, and Oxidation on Methylmercury Production by Geobacter sulfurreducens PCA</atitle><jtitle>Environmental science &amp; technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2014-10-21</date><risdate>2014</risdate><volume>48</volume><issue>20</issue><spage>11969</spage><epage>11976</epage><pages>11969-11976</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><coden>ESTHAG</coden><abstract>G. sulfurreducens PCA cells have been shown to reduce, sorb, and methylate Hg(II) species, but it is unclear whether this organism can oxidize and methylate dissolved elemental Hg(0) as shown for Desulfovibrio desulfuricans ND132. Using Hg(II) and Hg(0) separately as Hg sources in washed cell assays in phosphate buffered saline (pH 7.4), we report how cell-mediated Hg reduction and oxidation compete or synergize with sorption, thus affecting the production of toxic methylmercury by PCA cells. Methylation is found to be positively correlated to Hg sorption (r = 0.73) but negatively correlated to Hg reduction (r = −0.62). These reactions depend on the Hg and cell concentrations or the ratio of Hg to cellular thiols (−SH). Oxidation and methylation of Hg(0) are favored at relatively low Hg to cell–SH molar ratios (e.g., &lt;1). Increasing Hg to cell ratios from 0.25 × 10–19 to 25 × 10–19 moles-Hg/cell (equivalent to Hg/cell–SH of 0.71 to 71) shifts the major reaction from oxidation to reduction. In the absence of five outer membrane c-type cytochromes, mutant ΔomcBESTZ also shows decreases in Hg reduction and increases in methylation. However, the presence of competing thiol-binding ions such as Zn2+ leads to increased Hg reduction and decreased methylation. These results suggest that the coupled cell-Hg sorption and redox transformations are important in controlling the rates of Hg uptake and methylation by G. sulfurreducens PCA in anoxic environments.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>25268220</pmid><doi>10.1021/es502537a</doi><tpages>8</tpages><oa>free_for_read</oa></addata></record>
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source American Chemical Society:Jisc Collections:American Chemical Society Read & Publish Agreement 2022-2024 (Reading list)
subjects Adsorption
Anaerobiosis
Bacteriology
BASIC BIOLOGICAL SCIENCES
Bioassays
Biological and medical sciences
Cellular biology
Cytochrome c Group - genetics
Cytochrome c Group - metabolism
Cytotoxicity
Desulfovibrio desulfuricans
Fundamental and applied biological sciences. Psychology
Geobacter - drug effects
Geobacter - genetics
Geobacter - metabolism
Geobacter sulfurreducens
Gram-negative bacteria
Mercury - chemistry
Mercury - metabolism
Metabolism. Enzymes
Methylation
Methylmercury Compounds - metabolism
Microbiology
Oxidation
Oxidation-Reduction
Sorption
Sulfhydryl Compounds - metabolism
Zinc - metabolism
title Coupled Mercury–Cell Sorption, Reduction, and Oxidation on Methylmercury Production by Geobacter sulfurreducens PCA
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