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

Title	Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way
Author	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
Corresponding Author	Zhang, Guozhen; Duan, Lele
Publication Years	2023-02-01
DOI	10.1002/anie.202217220
Source Title	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Impact Factor & Quartile
ISSN	1433-7851
EISSN	1521-3773
Volume	62
Abstract	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.
Indexed By	EI ; SCI
Language	English
Important Publications	NI Journal Papers
SUSTech Authorship	First ; Corresponding
Funding Project	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 Accession No	WOS:000905253400001
Publisher	John Wiley and Sons Inc
EI Accession Number	20225313322916
EI Keywords	Atoms ; Carbon dioxide ; Catalyst activity ; Electrocatalysis ; Electronic structure ; Reduction ; Spectroscopic analysis
ESI Classification Code	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 Research Field	CHEMISTRY
Data Source	EV Compendex
Citation statistics	Cited Times [WOS]:2
Document Type	Journal Article
Identifier	http://kc.sustech.edu.cn/handle/2SGJ60CL/519669
Department	Department of Chemistry 深圳格拉布斯研究院工学院_材料科学与工程系
Affiliation	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
First Author Affilication	Department of Chemistry; Shenzhen Grubbs Institute
Corresponding Author Affilication	Department of Chemistry; Shenzhen Grubbs Institute
First Author's First Affilication	Department of Chemistry; Shenzhen Grubbs Institute
Recommended Citation 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.
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.
MLA	Zou, Haiyuan,et al."Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62(2023).

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Electronic Perturbation of Copper Single-Atom CO2 Reduction Catalysts in a Molecular Way