Synergistic modulation of valence state and oxygen vacancy induced by surface reconstruction of the CeO2/CuO catalyst toward enhanced electrochemical CO2 reduction
Fangfang Chang,
Zhenmao Zhang,
Yan Zhang,
Yongpeng Liu,
Lin Yang,
Xiaolei Wang,
Zhengyu Bai,
Qing Zhang
Affiliations
Fangfang Chang
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Zhenmao Zhang
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Yan Zhang
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Yongpeng Liu
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Lin Yang
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Xiaolei Wang
Department of Chemical and Materials Engineering University of Alberta Edmonton Alberta Canada
Zhengyu Bai
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Qing Zhang
Key Laboratory of Green Chemical Media and Reactions, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Ministry of Education Henan Normal University Xinxiang Henan China
Abstract Electrochemical CO2 reduction reaction (CO2RR) offers a promising strategy for CO2 conversion into value‐added C2+ products and facilitates the storage of renewable resources under comparatively mild conditions, but still remains a challenge. Herein, we propose the strategy of surface reconstruction and interface integration engineering to construct tuneable Cu0–Cu+–Cu2+ sites and oxygen vacancy oxide derived from CeO2/CuO nanosheets (OD‐CeO2/CuO NSs) heterojunction catalysts and promote the activity and selectivity of CO2RR. The optimized OD‐CeO2/CuO electrocatalyst shows the maximum Faradic efficiencies for C2+ products in the H‐type cell, which reaches 69.8% at −1.25 V versus a reversible hydrogen electrode (RHE). Advanced characterization analysis and density functional theory (DFT) calculations further confirm the fact that the existence of oxygen vacancies and Cu0–Cu+–Cu2+ sites modified with CeO2 is conducive to CO2 adsorption and activation, enhances the hydrogenation of *CO to *CHO, and further promotes the dimerization of *CHO, thus promoting the selectivity of C2+ generation. This facile interface integration and surface reconstruction strategy provides an ideal strategy to guide the design of CO2RR electrocatalysts.