A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N_4 Sites for CO_2 Electroreduction

作     者：Wanzhen Zheng Feng Chen Qi Zeng Zhongjian Li Bin Yang Lecheng Lei Qinghua Zhang Feng He Xilin Wu Yang Hou Wanzhen Zheng;Feng Chen;Qi Zeng;Zhongjian Li;Bin Yang;Lecheng Lei;Qinghua Zhang;Feng He;Xilin Wu;Yang Hou

作者机构：Key Laboratory of Biomass Chemical Engineering of Ministry of EducationCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China College of Geography and Environmental ScienceZhejiang Normal UniversityJinhua 321004People’s Republic of China College of EnvironmentZhejiang University of TechnologyHangzhou 310014People’s Republic of China Institute of Zhejiang University-QuzhouQuzhou 324000People’s Republic of China Ningbo Research InstituteZhejiang UniversityNingbo 315100People’s Republic of China Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture TechnologyCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China 

出 版 物：《Nano-Micro Letters》 (纳微快报（英文版）)

年 卷 期：2020年第12卷第9期

页      面：14-25页

核心收录：

学科分类：0808[工学-电气工程] 081704[工学-应用化学] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：financial support from Zhejiang Province Basic Public Welfare Research Project(LGF19B070006) financial supports from National Natural Science Foundation of China(21922811,21878270,51702284,21961160742) Zhejiang Provincial Natural Science Foundation of China(LR19B060002) supported by the Fundamental Research Funds for the Central Universities the Startup Foundation for Hundred-Talent Program of Zhejiang University 

主　　题：Atomic dispersion Pyrrole-type metal–N4 structure Catalytic site CO2 electroreduction Zn–CO2 battery 

摘      要：Atomically dispersed metal-nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction(CO2 ER),but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central ***,we develop a family of single metal atom bonded by N atoms anchored on carbons(SAs-M-N-C,M=Fe,Co,Ni,Cu)for CO2 ER,which composed of accurate pyrrole-type M-N4 structures with isolated metal atom coordinated by four pyrrolic N *** from atomically coordinated environment and specific selectivity of M-N4 centers,SAs-Ni-N-C exhibits superior CO2 ER performance with onset potential of-0.3 V,CO Faradaic efficiency(F.E.) of 98.5%at-0.7 V,along with low Tafel slope of 115 mV dec-1 and superior stability of 50 h,exceeding all the previously reported M-N-C electrocatalysts for CO2-to-CO *** results manifest that the different intrinsic activities of M-N4 structures in SAs-M-N-C result in the corresponding sequence of Ni Fe Cu Co for CO2 ER *** integrated Zn-CO2 battery with Zn foil and SAs-Ni-N-C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output,which delivers a peak power density of 1.4 mW cm-2 and maximum CO *** 93.3%.