Active Sites in Single-Atom Fe–Nx–C Nanosheets for Selective Electrochemical Dechlorination of 1,2-Dichloroethane to Ethylene

IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ACS Nano Pub Date : 2020-07-16 DOI:10.1021/acsnano.0c02783
Guoqiang Gan, Xinyong Li*, Liang Wang, Shiying Fan, Jincheng Mu, Penglei Wang, Guohua Chen*
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引用次数: 67

Abstract

Electrochemical dechlorination of 1,2-dichloroethane (DCE) is one of the prospective and economic strategies for the preparation of high-value ethylene. However, the exploration of advanced electrocatalysts with high reactivity and selectivity and the identification of their active sites are still a challenge. Herein, a single-atom (SA) Fe–Nx–C nanosheet with the presence of a highly efficient Fe–N4 coordination pattern is reported. The as-prepared single-atom electrocatalyst exhibits a higher reactivity and ethylene selectivity for DCE dechlorination reaction than those of the commercially adopted 20% Pt–C catalyst. By a combination of experiments and theoretical calculations, the atomically dispersed Fe center in the Fe–N4 structure was unveiled to be the dominating active site for electrochemical production of ethylene. Our work would offer an approach for the rational development of SA materials and supply crucial insight into the mechanism of ethylene production through the DCE dechlorination reaction.

Abstract Image

单原子Fe-Nx-C纳米片选择性电化学脱氯制乙烯的活性位点研究
1,2-二氯乙烷(DCE)的电化学脱氯是制备高值乙烯的一种有前景且经济的方法。然而,探索具有高反应活性和选择性的先进电催化剂及其活性位点的确定仍然是一个挑战。本文报道了一种具有高效Fe-N4配位模式的单原子(SA) Fe-Nx-C纳米片。所制备的单原子电催化剂对DCE脱氯反应的反应活性和乙烯选择性高于工业上采用的20% Pt-C催化剂。通过实验和理论计算相结合,揭示了Fe - n4结构中原子分散的Fe中心是电化学生产乙烯的主要活性位点。我们的工作将为SA材料的合理开发提供途径,并为通过DCE脱氯反应产生乙烯的机理提供重要的见解。
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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