Sulfate-Reducing Bacteria Mobilize Adsorbed Antimonate by Thioantimonate Formation
Sulfate-Reducing Bacteria Mobilize Adsorbed Antimonate by Thioantimonate Formation
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硫酸盐还原菌通过形成硫代锑酸盐来动员吸附的锑酸盐
DOI：
10.1021/acs.estlett.9b00353
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发表时间：
2019-07-01
影响因子：
10.9
通讯作者：
Jing, Chuanyong
中科院分区：
文献类型：
--
作者：
Ye, Li;Chen, Haoze;Jing, Chuanyong
锑(SB)的生物地球化学循环往往与硫磺和硫酸盐还原细菌(SRB)相耦合。生物硫化物通常被认为通过Sb_2S_3沉淀促进了Sb的固定。相反，我们发现SRB动员吸附了Sb(V)。当含SbV(OH)6的针铁矿与普通硫化弧菌DP4厌氧培养时，由于溶液中主要的Sb形态--硫代锑酸盐的形成，释放出较高水平的Sb。我们的傅里叶变换离子回旋共振质谱学分析发现了多个六配位或五配位的硫代锑中间体，这表明生物成因的硫化物在SBV(OH)6-上逐步地进行了羟基的配体交换。直接的H_2S消除反应生成了稳定的四配位硫代锑酸盐物种，密度泛函理论计算证实了这一点。锑的硫代化反应是pH依赖的，发生在中性环境中。硫代化反应改变了Sb(V)。
The biogeochemical cycling of antimony (Sb) is often coupled with sulfur and sulfate-reducing bacteria (SRB). The biogenic sulfide is usually assumed to facilitate Sb immobilization via Sb2S3 precipitation. Here, on the contrary, we discovered that SRB mobilize adsorbed Sb(V). When SbV(OH)6–-bearing goethite was incubated anaerobically with Desulfovibrio vulgaris DP4, an elevated level of antimony was released due to the formation of thioantimonate, which is the dominant Sb species in solution. Our Fourier transform ion cyclotron resonance mass spectrometry analysis revealed multiple six- or five-coordinate thioantimonate intermediates, suggesting stepwise ligand exchange of hydroxyl groups on SbV(OH)6– by biogenic sulfide. Direct H2S elimination reactions resulted in four-coordinate thioantimonate species as the stable end product, which was confirmed by our density functional theory calculations. The thiolation of antimonate is pH-dependent and occurs in neutral environments. The thiolation changed Sb(V...