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氮掺杂碳材料作为无金属催化剂用于通过硫化物脱除三氯乙烯。

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

机构信息

Key Laboratory of Groundwater Resources and Environment (Jilin University) , Ministry of Education , Changchun 130021 , China.

Chevron Energy Technology Company, Houston , Texas 77002 , United States.

出版信息

Environ Sci Technol. 2018 Dec 18;52(24):14286-14293. doi: 10.1021/acs.est.8b03565. Epub 2018 Nov 30.

Abstract

A new method for trichloroethylene (TCE) dechlorination is proposed using sulfide (HS and S) 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. 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.

摘要

提出了一种使用硫化物(HS 和 S)作为还原剂,在氮掺杂碳材料(NCMs)介导下进行三氯乙烯(TCE)脱氯的新方法。使用该方法,TCE 在 200 小时后转化为乙炔的转化率约为 99%。TCE 在 NCMs-硫化物体系(NCSS)中的脱氯遵循准一级动力学。NCMs 表面的吡啶 N(N6)似乎在 NCSS 中起着关键作用,因为 N6 的表面含量与 k 之间存在良好的线性关系。亲核取代被认为是 TCE 脱氯的第一步,亲核试剂被鉴定为具有 C-S-S-H 官能团的硫中间体。C-S-S-H 的生成可归因于 N6 中带正电荷的碳原子与带负电荷的硫化物之间的相互作用。这项工作首次证明,硫化物与 NCMs 结合可以产生有效脱除 TCE 的活性物质,这一发现将有助于开发利用天然硫化物作为还原剂去除有机氯代烯烃污染物的策略。

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