南方科技大学知识苑(SUSTech KC): Electronic Perturbation of Copper Single-Atom CO<inf>2</inf> Reduction Catalysts in a Molecular Way

题名	Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way
作者	Zou, Haiyuan1 ; Zhao, Gang 2; Dai, Hao1 ; Dong, Hongliang 3; Luo, Wen4 ; Wang, Lei 5; Lu, Zhouguang4 ; Luo, Yi 2; Zhang, Guozhen 2; Duan, Lele1
通讯作者	Zhang, Guozhen; Duan, Lele
发表日期	2023-02-01
DOI	10.1002/anie.202217220
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 影响因子和分区
ISSN	1433-7851
EISSN	1521-3773
卷号	62 期号:6
摘要	Fine-tuning electronic structures of single-atom catalysts (SACs) plays a crucial role in harnessing their catalytic activities, yet challenges remain at a molecular scale in a controlled fashion. By tailoring the structure of graphdiyne (GDY) with electron-withdrawing/-donating groups, we show herein the electronic perturbation of Cu single-atom CO2 reduction catalysts in a molecular way. The elaborately introduced functional groups (−F, −H and −OMe) can regulate the valance state of Cu^δ+, which is found to be directly scaled with the selectivity of the electrochemical CO2-to-CH4 conversion. An optimum CH4 Faradaic efficiency of 72.3 % was achieved over the Cu SAC on the F-substituted GDY. In situ spectroscopic studies and theoretical calculations revealed that the positive Cu^δ+ centers adjusted by the electron-withdrawing group decrease the pKa of adsorbed H2O, promoting the hydrogenation of intermediates toward the CH4 production. Our strategy paves the way for precise electronic perturbation of SACs toward efficient electrocatalysis. © 2022 Wiley-VCH GmbH.
关键词	CO2 Reduction Reaction Copper Electrochemistry Electronic Perturbation Single-Atom Catalysts
相关链接	[来源记录]
收录类别	EI ; SCI ; IC
语种	英语
重要成果	NI论文
学校署名	第一 ; 通讯
资助项目	This work is supported by the National Natural Science Foundation of China (22179057, 21790351, 22273093, U22A20439), Stable Support Plan Program of Shenzhen Natural Science Fund (20200925152742003), Educational Commission of Guangdong Province (2020KTSCX121) and the CAS Project for Young Scientists in Basic Research (YSBR-005). We thank the staff at the 4B9A beamline of Beijing Synchrotron Radiation Facility(BSRF) for assistance with the XAFS measurement. G.Z.Z. is grateful for the start-up funding of University of Science and Technology of China. The Supercomputing Center of University of Science and Technology of China and Hefei Advanced Computing Center are acknowledged for the computing resource.This work is supported by the National Natural Science Foundation of China (22179057, 21790351, 22273093, U22A20439), Stable Support Plan Program of Shenzhen Natural Science Fund (20200925152742003), Educational Commission of Guangdong Province (2020KTSCX121) and the CAS Project for Young Scientists in Basic Research (YSBR‐005). We thank the staff at the 4B9A beamline of Beijing Synchrotron Radiation Facility(BSRF) for assistance with the XAFS measurement. G.Z.Z. is grateful for the start‐up funding of University of Science and Technology of China. The Supercomputing Center of University of Science and Technology of China and Hefei Advanced Computing Center are acknowledged for the computing resource.
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:000905253400001
出版者	John Wiley and Sons Inc
EI入藏号	20225313322916
EI主题词	Atoms ; Carbon dioxide ; Catalyst activity ; Electrocatalysis ; Electronic structure ; Reduction ; Spectroscopic analysis
EI分类号	Copper:544.1 ; Chemistry:801 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3
ESI学科分类	CHEMISTRY
来源库	EV Compendex
引用统计	被引频次[WOS]：36
成果类型	期刊论文
条目标识符	http://sustech.caswiz.com/handle/2SGJ60CL/519669
专题	理学院_化学系深圳格拉布斯研究院工学院_材料科学与工程系
作者单位	1.Department of Chemistry and Shenzhen Grubbs Institute, Southern University of Science and Technology, Shenzhen; 518055, China 2.Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei; 230026, China 3.Center for High Pressure Science and Technology Advanced Research Pudong, Shanghai; 201203, China 4.Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen; 518055, China 5.Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore; 117585, Singapore
第一作者单位	化学系; 深圳格拉布斯研究院
通讯作者单位	化学系; 深圳格拉布斯研究院
第一作者的第一单位	化学系; 深圳格拉布斯研究院
推荐引用方式 GB/T 7714	Zou, Haiyuan,Zhao, Gang,Dai, Hao,et al. Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023,62(6).
APA	Zou, Haiyuan.,Zhao, Gang.,Dai, Hao.,Dong, Hongliang.,Luo, Wen.,...&Duan, Lele.(2023).Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,62(6).
MLA	Zou, Haiyuan,et al."Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62.6(2023).