4.8 Article

Highly selective photocatalytic reduction of CO2 to ethane over Au-O-Ce sites at micro-interface

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APPLIED CATALYSIS B-ENVIRONMENTAL
卷 321, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.apcatb.2022.122020

关键词

CO 2 photoreduction; Au-CeO 2 micro -interface; Au-O-Ce active sites; C2 selectivity; Rare earth

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In this study, an Au-CeO2 nanocomposite with Au-O-Ce sites at the micro-interface was developed for the highly selective conversion of CO2 into C2H6. The formation of key intermediates COCO* was confirmed, indicating the role of the Au-CeO2 micro-interface in promoting the multi-electron reduction of CO* and facilitating the production of C2 species. Theoretical calculations suggested that Au-O-Ce sites at the micro-interface could lower the energy barriers for the formation of COOH* and COCO*, resulting in the production of C2H6. The Au-CeO2 nanocomposite exhibited a high C2H6 production rate and electron selectivity.
To date, the efficient photocatalytic conversion of CO2 into high-value C2 products remains a great challenge. Herein, the Au-CeO2 nanocomposite with Au-O-Ce sites at the micro-interface was developed to achieve a highly selective conversion of CO2 into C2H6. This can be partially ascribed to the formation of key intermediates of COCO* was confirmed via in-situ Fourier transform infrared (FTIR) spectroscopy, indicating that the Au-CeO2 micro-interface could prompt the multi-electron reduction of CO* before desorption, and enable the production of C2 species. Moreover, theoretical calculations suggested that Au-O-Ce sites at the micro-interface could reduce the energy barriers for the formation of COOH* and COCO*, facilitating the production of C2H6. Therefore, the Au-CeO2 nanocomposite exhibited a C2H6 production rate of 11.07 mu mol g-1 h-1 and high electron selectivity of 93.1 % (product selectivity: 65.3 %), which is comparable with most state-of-the-art photocatalysts.

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