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Microbial Biosynthesis of Thiol Compounds: Implications for Speciation, Cellular Uptake, and Methylation of Hg(II)
Department of Chemistry, Umeå University, Umeå, Sweden.
Örebro universitet, Institutionen för naturvetenskap och teknik. Department of Chemistry, Umeå University, Umeå, Sweden.ORCID-id: 0000-0001-6056-7613
Department of Forest Ecology and Management, Swedish University of Agricultural Sciences, Umeå, Sweden.ORCID-id: 0000-0002-8610-0525
Department of Environmental Sciences, Rutgers University, New Brunswick, New Jersey, United States.
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2019 (engelsk)Inngår i: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 53, nr 14, s. 8187-8196Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

Cellular uptake of inorganic divalent mercury (Hg(II)) is a key step in microbial formation of neurotoxic methylmercury (MeHg), but the mechanisms remain largely unidentified. We show that the iron reducing bacterium Geobacter sulfurreducens produces and exports appreciable amounts of low molecular mass thiol (LMM-RSH) compounds reaching concentrations of about 100 nM in the assay medium. These compounds largely control the chemical speciation and bioavailability of Hg(II) by the formation of Hg(LMM-RS)<INF><INF><INF>2</INF></INF> </INF>complexes (primarily with cysteine) in assays without added thiols. By characterizing these effects, we show that the thermodynamic stability of Hg(II)-complexes is a principal controlling factor for Hg(II) methylation by this bacterium such that less stable complexes with mixed ligation involving LMM-RSH, OH<SUP>-</SUP>, and Cl<SUP>-</SUP> are methylated at higher rates than the more stable Hg(LMM-RS)<INF>2</INF> complexes. The Hg(II) methylation rate across different Hg(LMM-RS)<INF>2</INF> compounds is also influenced by the chemical structure of the complexes. In contrast to the current perception of microbial uptake of Hg, our results adhere to generalized theories for metal biouptake based on metal complexation with cell surface ligands and refine the mechanistic understanding of Hg(II) availability for microbial methylation.

sted, utgiver, år, opplag, sider
American Chemical Society (ACS), 2019. Vol. 53, nr 14, s. 8187-8196
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Identifikatorer
URN: urn:nbn:se:oru:diva-75727DOI: 10.1021/acs.est.9b01502ISI: 000476685500028PubMedID: 31257868Scopus ID: 2-s2.0-85069948405OAI: oai:DiVA.org:oru-75727DiVA, id: diva2:1342493
Forskningsfinansiär
The Kempe Foundations, JCK-1501 SMK-2745 SMK-1243
Merknad

Funding Agency:

Swedish Research Council via the project Sino-Swedish Mercury Management Research Framework-SMaReF  2013-6978

Tilgjengelig fra: 2019-08-13 Laget: 2019-08-13 Sist oppdatert: 2019-08-13bibliografisk kontrollert

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