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Ultrathin Fe–Nx–C single-atom catalysts with bifunctional active site for simultaneous production of ethylene and aromatic chlorides
Nano Energy ( IF 16.8 ) Pub Date : 2020-10-23 , DOI: 10.1016/j.nanoen.2020.105532
Guoqiang Gan , Xinyong Li , Shiying Fan , Zhifan Yin , Liang Wang , Guohua Chen

Ethylene evolution reaction (EER) by electrochemical dechlorination of 1,2-dichloroethane is a promising and an economical strategy. The process is however severely impeded by the poor reactivity of catalysts, the accumulation of HCl in the electrolyte as well as low value-added by-products at anode. Herein, a bifunctional ultrathin Fe–Nx–C single-atom catalysts (SACs) has been successfully prepared and investigated as both cathode and anode material for EER and aromatic chlorination reaction (ACR), respectively. The generated HCl was recycled as a chlorinating reagent. The Fe–Nx–C SACs exhibited an excellent electrocatalytic performance simultaneously for both EER and ACR with high ethylene and para–chloroanisole selectivity obtained. The first-principles calculations indicated that Fe–N4 was the dominating catalytic active site for the generation of ethylene as well as para–chloroanisole. The coupling strategy of ACR at anode not only can accelerate the reaction rate of EER, but also provide a highly-efficient and atom-economical approach for the production of valuable ethylene and aromatic chlorides.



中文翻译:

具有双功能活性位的超薄Fe–N x –C单原子催化剂,可同时生产乙烯和芳族氯化物

通过1,2-二氯乙烷的电化学脱氯进行乙烯释放反应(EER)是一种有前途且经济的策略。然而,该方法由于催化剂的反应性差,电解质中HCl的积累以及阳极处的低附加值副产物而严重受到阻碍。在此,已经成功制备了双功能超薄Fe–N x –C单原子催化剂(SAC),并分别将其用作EER和芳族氯化反应(ACR)的正极和负极材料。产生的HCl作为氯化试剂循环使用。Fe–N x –C SAC对具有高乙烯和对位的EER和ACR同时显示出优异的电催化性能获得了–氯茴香醚的选择性。第一性原理计算表明,Fe–N 4是产生乙烯以及氯苯甲醚的主要催化活性中心。ACR在阳极的偶联策略不仅可以加快EER的反应速率,而且还为生产有价值的乙烯和芳族氯化物提供了一种高效且原子经济的方法。

更新日期:2020-11-12
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