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首页> 外文期刊>Environmental Science & Technology >Microbial Biosynthesis of Thiol Compounds: Implications for Speciation, Cellular Uptake, and Methylation of Hg(Ⅱ)
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Microbial Biosynthesis of Thiol Compounds: Implications for Speciation, Cellular Uptake, and Methylation of Hg(Ⅱ)

机译:硫醇化合物的微生物合成:对汞的形态,细胞吸收和甲基化的影响

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摘要

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)INFINFINF2/INF/INF /INFcomplexes (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, OHSUP-/SUP, and ClSUP-/SUP are methylated at higher rates than the more stable Hg(LMM-RS)INF2/INF complexes. The Hg(II) methylation rate across different Hg(LMM-RS)INF2/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.
机译:细胞对无机二价汞(Hg(II))的吸收是微生物形成神经毒性甲基汞(MeHg)的关键步骤,但机理尚不清楚。我们表明,铁还原细菌Geobacter sulfreducens产生并输出相当数量的低分子量硫醇(LMM-RSH)化合物,在分析培养基中的浓度达到约100 nM。这些化合物通过形成Hg(LMM-RS) 2 复合物(主要与Hg(LMM-RS))而在很大程度上控制Hg(II)的化学形态和生物利用度。半胱氨酸),而无需添加硫醇。通过表征这些作用,我们表明,Hg(II)配合物的热力学稳定性是该细菌对Hg(II)甲基化的主要控制因素,因此与LMM-RSH,OH - 和Cl -的甲基化速率比更稳定的Hg(LMM-RS) 2 复合物高。不同Hg(LMM-RS) 2 化合物的Hg(II)甲基化率也受配合物化学结构的影响。与目前对微生物吸收汞的看法相反,我们的研究结果坚持了基于金属与细胞表面配体络合的金属生物吸收的通用理论,并完善了对微生物甲基化可利用的Hg(II)的机理的理解。

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  • 来源
    《Environmental Science & Technology》 |2019年第14期|8187-8196|共10页
  • 作者单位

    Umea Univ, Dept Chem, SE-90187 Umea, Sweden;

    Umea Univ, Dept Chem, SE-90187 Umea, Sweden|Orebro Univ, Sch Sci & Technol, SE-70182 Orebro, Sweden;

    Swedish Univ Agr Sci, Dept Forest Ecol & Management, SE-90183 Umea, Sweden;

    Rutgers State Univ, Dept Environm Sci, 14 Coll Farm Rd, New Brunswick, NJ 08901 USA;

    Swedish Univ Agr Sci, Dept Forest Ecol & Management, SE-90183 Umea, Sweden;

    Umea Univ, Dept Chem, SE-90187 Umea, Sweden;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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