Wang Yuwei, Schaefer Jeffra K, Mishra Bhoopesh, Yee Nathan
Department of Environmental Sciences, Rutgers University , New Brunswick, New Jersey 08901, United States.
Department of Physics, Illinois Institute of Technology , Chicago, Illinois 60616, United States.
Environ Sci Technol. 2016 Oct 18;50(20):11049-11056. doi: 10.1021/acs.est.6b03299. Epub 2016 Oct 3.
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. 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.
在采矿和制造区域,元素汞(Hg(0))废物的处置已引发了严重的土壤和地下水污染问题。在缺氧条件下,某些厌氧细菌能够氧化溶解的元素汞,并将氧化态的汞转化为具有神经毒性的甲基汞。在本研究中,我们利用汞甲基化细菌脱硫脱硫弧菌ND132进行实验,以阐明细胞硫醇在厌氧Hg(0)氧化中的作用。我们测量了细胞表面和细胞内硫醇的浓度,并检测了脱硫脱硫弧菌ND132的特定组分的Hg(0)氧化活性,并用扩展X射线吸收精细结构(EXAFS)光谱进行分析。实验数据表明,细胞内硫醇浓度大约是细胞壁硫醇浓度的六倍。与硫醇阻断试剂反应的细胞,其Hg(0)氧化活性严重受损。缺乏细胞壁的原生质体能够迅速将Hg(0)氧化为Hg(II),而细胞壁碎片对Hg(0)的反应性较低。对原生质体样品的EXAFS分析表明,Hg(0)氧化反应会产生多种不同形式的汞硫醇,并且氧化态汞的局部配位环境会随反应时间而变化。本研究结果表明,脱硫脱硫弧菌ND132中的Hg(0)氧化是一个通过与含硫醇分子反应而发生的细胞内过程。