Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO_(2)reduction

查看全文 作　　者：Ming [1]Qu;Zhe [2]Chen;Zhiyi [3]Sun;Danni [3]Zhou;Wenjing [3]Xu;Hao [3]Tang;Hongfei [3]Gu;Tuo [1]Liang;Pengfei [4,5]Hu;Guangwen [6]Li;Yu [7]Wang;Zhuo [3]Chen;Tao [2]Wang;Binbin [4]Jia

机构地区：[1]Unconventional Petroleum Research Institute,China University of Petroleum(Beijing),Beijing 102249,China;[2]Center of Artificial Photosynthesis for Solar Fuels,School of Science,Westlake University,Hangzhou 310024,China;[3]Energy&Catalysis Center,School of Materials Science and Engineering,Beijing Institute of Technology,Beijing 100081,China;[4]School of Chemistry,Beihang University,Beijing 100191,China;[5]Research Institute of Aero-Engine,Beihang University,Beijing 102206,China;[6]Research Institude of Petroleum Processing,Sinopec Group(SINOPEC),Beijing 100083,China;[7]Shanghai Synchrotron Radiation Facilities,Shanghai Institute of Applied Physics,Chinese Academy of Science,Shanghai 201204,China

出　　处：《Nano Research》索引2023年第16卷第2期,共7页

基　　金：supported by the Beijing Natural Science Foundation(No.2212018);China National Petroleum Corporation(CNPC)Innovation Found(No.2021DQ02-0202);the National Natural Science Foundation of China(No.51902013). 摘　　要：The atomic-level interfacial regulation of single metal sites through heteroatom doping can significantly improve the characteristics of the catalyst and obtain surprising activity.Herein,nickel single-site catalysts(SSCs)with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed(denoted as Ni-PxNy,x=1,2 and y=3,2).In CO_(2)reduction reaction(CO_(2)RR),the CO current density on Ni-PxNy was significantly higher than that of Ni-N4 catalyst without phosphorus modification.Besides,Ni-P1N3 performed the highest CO Faradaic efficiency(FECO)of 85.0%–98.0%over a wide potential range of−0.65 to−0.95 V(vs.the reversible hydrogen electrode(RHE)).Experimental and theoretical results revealed that the asymmetric Ni-P1N3 site was beneficial to CO_(2)intermediate adsorption/desorption,thereby accelerating the reaction kinetics and boosting CO_(2)RR activity.This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance,targetting to CO_(2)RR applications. 关键词：nickel single-site catalysts asymmetric coordination CO_(2)reduction reaction atomic interface

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Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO_(2)reduction

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