期刊
ACS CATALYSIS
卷 12, 期 2, 页码 1004-1011出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c04714
关键词
CO2 electroreduction; selectivity; Cu/CeO2 interface; in situ ATR-SEIRAS; prelithiation
资金
- National Natural Science Foundation of China [21991154, 21991150, 92045302, 22172115, 21902120]
- Fundamental Research Funds for the Central Universities [2042021kf1064]
This study achieved efficient electroreduction of CO2 by decorating Cu on CeO2 and controlling the selectivity of products. The dependence of reduction pathway on the relative ratio of the low-frequency band *COLFB to the high-frequency band *COHFB was revealed using in situ infrared and Raman spectroscopy, providing a theoretical basis for the design of heterostructured catalysts for CO2 electroreduction.
Cu-catalyzed CO2 electroreduction can produce various hydrocarbons and oxygenates. However, it suffers from low activity and poor selectivity. Herein, Cu-decorated CeO2 composites (Cu-y/CeO2) with distinct interfacial characteristics were fabricated through a highly controllable synthesis, based on chemical prelithiation of CeO2 and then galvanic displacement with Cu. The Cu decoration induced a strong-binding site for CO2 adsorption at the Cu and CeO2 interface, facilitating the CO2 activation and conversion to the *CO intermediate on the nearby Cu surface. Selective CO2 conversion to C-1 or C2+ products was customized by adjusting the Cu decoration amount. With the increase in the Cu loading, the C-1 and C2+ products exhibited a declining and volcano-shaped trend, showing a maximum faradaic efficiency of 70 and 63%, respectively. In situ infrared and Raman spectroscopy revealed that the reduction pathway depended on the relative ratio of the low-frequency band *COLFB to the high-frequency band *COHFB. Our findings may contribute to the rational design of heterostructured catalysts toward CO2 electroreduction.
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