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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 |
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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., <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. 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</subject><ispartof>Environmental science & technology, 2014-10, Vol.48 (20), p.11969-11976</ispartof><rights>2015 INIST-CNRS</rights><rights>Copyright American Chemical Society Oct 21, 2014</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a468t-4eba834e2c27c43f4cebd4418dee1313c59e58fea87a4463aeda4d5345ab12a83</citedby><cites>FETCH-LOGICAL-a468t-4eba834e2c27c43f4cebd4418dee1313c59e58fea87a4463aeda4d5345ab12a83</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,776,780,881,27901,27902</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=28992643$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/25268220$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/servlets/purl/1286719$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><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. (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 & 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., <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. (ORNL), Oak Ridge, TN (United States)</creatorcontrib><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lin, Hui</au><au>Morrell-Falvey, Jennifer L</au><au>Rao, Balaji</au><au>Liang, Liyuan</au><au>Gu, Baohua</au><aucorp>Oak Ridge National Lab. (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 & 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., <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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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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