{"title":"Active Sites in Single-Atom Fe–Nx–C Nanosheets for Selective Electrochemical Dechlorination of 1,2-Dichloroethane to Ethylene","authors":"Guoqiang Gan, Xinyong Li*, Liang Wang, Shiying Fan, Jincheng Mu, Penglei Wang, Guohua Chen*","doi":"10.1021/acsnano.0c02783","DOIUrl":null,"url":null,"abstract":"<p >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–N<sub><i>x</i></sub>–C nanosheet with the presence of a highly efficient Fe–N<sub>4</sub> 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–N<sub>4</sub> 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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"14 8","pages":"9929–9937"},"PeriodicalIF":16.0000,"publicationDate":"2020-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1021/acsnano.0c02783","citationCount":"67","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Nano","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsnano.0c02783","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
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.
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.