Precisely Tailoring the First Coordination Shell of Metal Centers in Porous Nitrogen-Doped Carbon Promoting Electroreduction of CO^(2)Under Neutral Condition
作者机构：MOE Key Laboratory of Bioinorganic and Synthetic ChemistryGBRCE for Functional Molecular EngineeringSchool of ChemistrySun Yat-sen UniversityGuangzhouGuangdong 510275 Institute of High Energy PhysicsChinese Academy of Sciences(CAS)Beijing 100049
出 版 物：《CCS Chemistry》 (中国化学会会刊（英文）)
年 卷 期：2024年第6卷第8期
页 面：1978-1986页
核心收录：
学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学]
基 金：supported by the National Key Research and Development Program of China(grant no.2021YFA1500401) the National Natural Science Foundation of China(NSFC,grant nos.21890380,21821003,and 22371304) the Local Innovative and Research Teams Project of the Guangdong Pearl River Talents Program,China(grant no.2017BT01C161) Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province,China(grant no.STKJ2023078)
主 题：single-atom Ni catalysts first coordination shell porous nitrogen-doped carbon electrochemical CO_(2)reduction reaction coordination environment
摘 要：Precise regulation of the coordination environment of a metal active center is very important but remains a ***,single-atom Ni catalysts with a combined N-and C-coordination structure(Ni-NC_(3))and N-coordination structure(Ni-N4)were prepared by modulating the side groups of organic ligands in the corresponding precursor metal–azolate *** with the Ni-N4 site,the d-band center of 3d orbitals of the Ni atom in Ni-NC_(3)was more significantly shifted to the Fermi energy level;thus,the Ni-NC_(3)catalytic site was superior to activating CO_(2)molecule into the*COOH *** a result,Ni-NC_(3)exhibited an exceptionally high performance for CO_(2)-to-CO conversion with a Faradaic efficiency of 98.4%,an energy efficiency of50%,as well as an industrial current density of∼300 mA cm^(−2) in neutral *** high performance could be retained for at least 70 *** work reveals the importance of modulating the coordination environment in the electrochemical CO_(2)reduction reaction and provides a possible way to rational design of electrocatalysts for highly efficient conversion of CO_(2)to target products.
维普期刊数据库