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Nitrogen-Doped Carbon Materials as Metal-Free Catalyst for the Dechlorination of Trichloroethylene by Sulfide

机译:氮掺杂碳材料作为无金属催化剂硫化三氯乙烯脱氯

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摘要

A new method for trichloroethylene (TCE) dechlorination is proposed using sulfide (HS- and S2-) as reductant under the mediation of nitrogen-doped carbon materials (NCMs). About 99% of the TCE was converted to acetylene after 200 h using this method. Dechlorination of TCE in the NCMs-sulfide system (NCSS) followed pseudo-first-order kinetics. Pyridinic N (N6) on surface of the NCMs appeared to play a critical role in NCSS as shown by the good linear relationship between the surface content of N6 and k(obs). Nucleophilic substitution was suggested as the first step in TCE dechlorination, and the nucleophilic reagent was identified as a sulfur intermediate with C-S-S-H as the functional group. The generation of C-S-S-H could be ascribed to the interaction between positively charged carbon atoms in N6 and negative charged sulfide. This work is the first to demonstrate that sulfide combined with NCMs can produce active substances that are effective in TCE dechlorination and the findings will assist in the development of strategies that use natural sulfide as reductant for detoxicating organic chloroethene contaminants.
机译:提出了一种新的三氯乙烯(TCE)脱氯方法,该方法以硫化物(HS-和S2-)为还原剂,在氮掺杂碳材料(NCM)的介导下进行。使用此方法,200小时后约有99%的TCE转化为乙炔。在NCMs-硫化物系统(NCSS)中TCE的脱氯遵循伪一级动力学。 NCM表面上的吡啶N(N6)似乎在NCSS中起着关键作用,这由N6表面含量与k(obs)之间的良好线性关系表明。 TCE脱氯的第一步建议是亲核取代,亲核试剂被鉴定为以C-S-S-H为官能团的硫中间体。 C-S-S-H的产生可归因于N6中带正电的碳原子与带负电的硫化物之间的相互作用。这项工作是第一个证明硫化物与NCM结合可以产生对TCE脱氯有效的活性物质,这项发现将有助于开发使用天然硫化物作为还原剂对有机氯乙烯污染物进行除毒的策略。

著录项

  • 来源
    《Environmental Science & Technology》 |2018年第24期|14286-14293|共8页
  • 作者单位

    Jilin Univ, Minist Educ, Key Lab Groundwater Resources & Environm, Changchun 130021, Jilin, Peoples R China;

    Jilin Univ, Minist Educ, Key Lab Groundwater Resources & Environm, Changchun 130021, Jilin, Peoples R China;

    Chevron Energy Technol Co, Houston, TX 77002 USA;

    Canadian Light Source, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada;

    Univ Western Ontario, Dept Mech & Mat Engn, London, ON N6A 5B8, Canada;

    Jilin Univ, Coll Chem, Changchun 130021, Jilin, Peoples R China;

    Jilin Univ, Minist Educ, Key Lab Groundwater Resources & Environm, Changchun 130021, Jilin, Peoples R China;

  • 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
  • 中图分类
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  • 入库时间 2022-08-18 03:58:35

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