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首页> 外文期刊>Environmental Science & Technology >Antimonite Complexation with Thiol and Carboxyl/Phenol Groups of Peat Organic Matter
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Antimonite Complexation with Thiol and Carboxyl/Phenol Groups of Peat Organic Matter

机译:硫胺素和泥炭有机物的羧基/苯酚基团的锑酸盐络合

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摘要

Peatlands and other wetlands with abundant natural organic matter (NOM) are important sinks for antimony (Sb). While formation of Sb (III) sulfide phases or Sb(III) binding to NOM are discussed to decrease Sb mobility, the exact binding mechanisms remain elusive. Here, we reacted increasing sulfide concentrations with purified model peat at pH 6, forming reduced organic sulfur species, and subsequently equilibrated the reaction products with 50 mu M of antimonite under anoxic conditions. Sulfur solid-phase speciation and the local binding environment of Sb were analyzed using X-ray absorption spectroscopy. We found that 85% of antimonite was sorbed by untreated peat. Sulfide-reacted peat increased sorption to 98%. Shell-by-shell fitting of Sb K-edge X-ray absorption fine structure spectra revealed Sb in untreated peat bound to carboxyl or phenol groups with average Sb-carbon distances of similar to 2.90 angstrom. With increasing content of reduced organic sulfur, Sb was progressively coordinated to S atoms at distances of similar to 2.45 angstrom and Sb-carbon distances of similar to 3.33 angstrom, suggesting increasing Sb-thiol binding. Iterative target factor analysis allowed exclusion of reduced inorganic Sb-sulfur phases with similar Sb-sulfur distances. In conclusion, even when free sulfide concentrations are too low for formation of Sb-sulfur precipitates, peat NOM can sequester Sb in anoxic, sulfur-enriched environments.
机译:泥炭地和其他自然有机物含量丰富的湿地是锑(Sb)的重要汇。虽然讨论了形成Sb(III)硫化物相或与NOM结合的Sb(III)以降低Sb迁移率,但确切的结合机理仍然难以捉摸。在这里,我们将增加的硫化物浓度与纯模型泥炭在pH 6下反应,形成还原的有机硫,然后在缺氧条件下用50μM的锑矿平衡反应产物。使用X射线吸收光谱法分析了硫的固相形态和Sb的局部结合环境。我们发现未经处理的泥炭吸附了85%的锑矿。硫化物反应的泥炭将吸附提高到98%。 Sb K边缘X射线吸收精细结构光谱的逐壳拟合显示,未处理泥炭中的Sb与羧基或酚基键合,平均Sb-碳距离约为2.90埃。随着还原性有机硫含量的增加,Sb在接近2.45埃的距离处逐渐与S原子配位,而Sb-碳的距离类似于3.33埃的距离逐渐变位,表明Sb-硫醇结合增加。迭代目标因子分析可以排除具有相似Sb-硫距离的还原性无机Sb-硫相。总之,即使游离硫化物的浓度过低而无法形成Sb-硫沉淀,泥炭NOM仍可以在缺氧,富硫的环境中螯合Sb。

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  • 来源
    《Environmental Science & Technology》 |2019年第9期|5005-5015|共11页
  • 作者单位

    Bayreuth Univ, Bayreuth Ctr Ecol & Environm Res BAYCEER, Dept Environm Geochem, D-95440 Bayreuth, Germany;

    Stanford Univ, Sch Earth Energy & Environm Sci, Dept Geol Sci, Stanford, CA 94305 USA|Univ Vienna, Dept Environm Geosci, A-1090 Vienna, Austria;

    ESRF, Rossendorf Beamline ROBL, F-38043 Grenoble, France|HZDR, Inst Resource Ecol, D-01328 Dresden, Germany;

    Stanford Univ, Dept Earth Syst Sci, Sch Earth Energy & Environm Sci, Stanford, CA 94305 USA;

    Stanford Univ, Dept Earth Syst Sci, Sch Earth Energy & Environm Sci, Stanford, CA 94305 USA;

    Bayreuth Univ, Bayreuth Ctr Ecol & Environm Res BAYCEER, Dept Environm Geochem, D-95440 Bayreuth, Germany;

  • 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);
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