Dual atomic catalysts from COF-derived carbon for CO_(2)RR by suppressing HER through synergistic effects  

作　　者：Minghao Liu Sijia Liu Qing Xu Qiyang Miao Shuai Yang Svenja Hanson George Zheng Chen Jun He Zheng Jiang Gaofeng Zeng 

机构地区：[1]CAS Key Laboratory of Low‐Carbon Conversion Science and Engineering,Shanghai Advanced Research Institute(SARI),Chinese Academy of Sciences(CAS),Shanghai,People's Republic of China [2]Department of Chemical and Environmental Engineering,University of Nottingham Ningbo China,Ningbo,People's Republic of China [3]School of Chemical Engineering,University of Chinese Academy of Sciences,Beijing,People's Republic of China [4]Shanghai Synchrotron Radiation Facility,Shanghai Advanced Research Institute,Chinese Academy of Science,Shanghai,People's Republic of China [5]Department of Chemical and Environmental Engineering,University of Nottingham,Nottingham,UK

出　　处：《Carbon Energy》2023年第6期92-103,共12页碳能源（英文）

基　　金：Q.Xu acknowledges financial support from the Natural Science Foundation of Shanghai(20ZR1464000);G.Zeng is grateful for the support from the National Natural Science Foundation of China(21878322,22075309);the Science and Technology Commission of Shanghai(19ZR1479200).The authors also thank the Shanghai Synchrotron Radiation Facility for XAFS measurements at Beamline BL14w1.

摘　　要：The electrochemical carbon dioxide reduction reaction(CO_(2)RR)for highvalue-added products is a promising strategy to tackle excessive CO_(2) emissions.However,the activity of and selectivity for catalysts for CO_(2)RR still need to be improved because of the competing reaction(hydrogen evolution reaction).In this study,for the first time,we have demonstrated dual atomic catalytic sites for CO_(2)RR from a core-shell hybrid of the covalent-organic framework and the metal-organic framework.Due to abundant dual atomic sites(with CoN_(4)O and ZnN_(4) of 2.47 and 11.05 wt.%,respectively)on hollow carbon,the catalyst promoted catalysis of CO_(2)RR,with the highest Faradic efficiency for CO of 92.6%at-0.8 V and a turnover frequency value of 1370.24 h^(-1) at-1.0 V.More importantly,the activity and selectivity of the catalyst were well retained for 30 h.The theoretical calculation further revealed that CoN_(4)O was the main site for CO_(2)RR,and the activity of and selectivity for Zn sites were also improved because of the synergetic roles.

关 键 词：carbon dioxide reduction reaction covalent-organic frameworks dual atomic catalysts metal-organic frameworks single-atom catalysts 

分 类 号：O64[理学—物理化学]