Promoting Electrocatalytic CO_(2) Reduction to CO via Sulfur-Doped Co-N-C Single-Atom Catalyst  

作　　者：Zhiming Wei Yuhang Liu Jie Ding Qinye He Qiao Zhang Yueming Zhai 

机构地区：[1]The Institute for Advanced Studies,Wuhan University,Wuhan,Hubei,430072 China [2]School of Materials Science and Engineering,Suzhou University of Science and Technology,Suzhou,Jiangsu,215009 China

出　　处：《Chinese Journal of Chemistry》2023年第24期3553-3559,共7页中国化学（英文版）

基　　金：financially supported by National Natural Science Foundation of China(No.21974103);the start-up funds of Wuhan University and the Experimental Supporting System at Shanghai Synchrotron Radiation Facility.

摘　　要：Electrocatalytic reduction of CO_(2) to fuels and chemicals possesses huge potential to alleviate current environmental crisis.Heteroatom doping in metal-nitrogen-carbon(M-N-C)single-atom catalysts(SACs)has been found to be capable to promote the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).However,the origin of the enhanced activity is still elusive.Here,we report that sulfur-doped cobalt-nitrogen-carbon single-atom catalyst(Co1-SNC)exhibits superior CO_(2)RR performance compared to sulfur-free counterpart(Co1-NC).On the basis of in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),kinetic isotope effect(KIE)and theoretical calculation,it is demonstrated that sulfur doping can promote water activation,elevate the d-band center of Co active site,and reduce the free energy of*COOH intermediate formation.This work deepens the understanding of the CO_(2)RR chemistry over heteroatom-doped SACs for designing efficient CO_(2)RR processes.

关 键 词：ELECTROCATALYTIC CO_(2)reduction Doping Heterogeneous catalysis Single-atom catalysts ATR-SEIRAS 

分 类 号：O64[理学—物理化学]