首页|Mechanistic investigation on Ag-Cu2O in electrocatalytic CO2 to CH4 by in situ/operando spectroscopic and theoretical analysis

Mechanistic investigation on Ag-Cu2O in electrocatalytic CO2 to CH4 by in situ/operando spectroscopic and theoretical analysis

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Silver-copper electrocatalysts have demonstrated effectively catalytic performance in electroreduction CO2 toward CH4,yet a revealing insight into the reaction pathway and mechanism has remained elusive.Herein,we construct chemically bonded Ag-Cu2O boundaries,in which the complete reduction of Cu2O to Cu has been strongly impeded owing to the presence of surface Ag shell.The interfacial confinement effect helps to maintain Cu+sites at the Ag-Cu2O boundaries.Using in situ/operando spectroscopy and theoretical simulations,it is revealed that CO2 is enriched at the Ag-Cu2O boundaries due to the enhanced physisorption and chemisorption to CO2,activating CO2 to form the stable intermediate*CO.The bound-aries between Ag shell and the Cu2O mediate local*CO coverage and promote*CHO intermediate forma-tion,consequently facilitating CO2-to-CH4 conversion.This work not only reveals the structure-activity relationships but also offers insights into the reaction mechanism on Ag-Cu catalysts for efficient electro-catalytic CO2 reduction.

Ag shellInterfacial confinement effectCu+Local*CO coverageCO2 reduction

Min Sun、Luxiao Zhang、Fuli Tian、Jiaxin Li、Yanqiu Lei、Heng Zhang、Lifeng Han、Zhihua Guo、Yonghui Gao、Fenrong Liu、Yan Wang、Luhui Wang、Shanghong Zeng

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School of Chemistry and Chemical Engineering,Inner Mongolia University,Hohhot 010021,Inner Mongolia,China

Key Laboratory of Medicinal and Edible Plants Resources of Hainan Province,Hainan Vocational University of Science and Technology,Haikou 571126,Hainan,China

State Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization,Baotou Research Institute of Rare Earths,Baotou 014030,Inner Mongolia,China

Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control,Zhejiang Ocean University,Zhoushan 316022,Zhejiang,China

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National Natural Science Foundation of ChinaNatural Science Foundation of Inner MongoliaNatural Science Foundation of Inner MongoliaScience and Technology Projects of China Northern Rare EarthOpen Research Subject of Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control

219680202022MS020112023MS02014BFXT-2022-D-00232021Z01

2024

10.1016/j.jechem.2023.10.004

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.88(1)
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