Efficient Photoreduction of CO2 to CO with 100% Selectivity by Slowing Down Electron Transport

Cheng Chen; Mingge Wu; Yifan Xu; Chunyan Ma; Maoyong Song; Guibin Jiang

doi:10.1021/jacs.3c14590

Efficient Photoreduction of CO₂ to CO with 100% Selectivity by Slowing Down Electron Transport

J Am Chem Soc. 2024 Apr 3;146(13):9163-9171. doi: 10.1021/jacs.3c14590. Epub 2024 Mar 21.

Authors

Cheng Chen^{1

2

3}, Mingge Wu^{1

3}, Yifan Xu⁴, Chunyan Ma^{1

2}, Maoyong Song^{1

2

3}, Guibin Jiang^{2

3}

Affiliations

¹ Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
² State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
³ University of Chinese Academy of Sciences, Beijing 100049, China.
⁴ Nanjing Institute of Environmental Sciences, Ministry of Ecology and Environment of China, Nanjing 210042, China.

PMID: 38515295
DOI: 10.1021/jacs.3c14590

Abstract

It remains challenging to obtain a single product in the gas-solid photocatalytic reduction of CO₂ because CO and CH₄ are usually produced simultaneously. This study presents the design of the I-type nested heterojunction TiO₂/BiVO₄ with controllable electron transport by modulating the TiO₂ component. This study demonstrates that slowing electron transport could enable TiO₂/BiVO₄-4 to generate CO with 100% selectivity. In addition, modifying TiO₂/BiVO₄-4 by loading a Cu single atom further increased the CO product yield by 3.83 times (17.33 μmol·g_cat^-1·h^-1), while maintaining 100% selectivity for CO. Characterization and density functional theory (DFT) calculations revealed that the selectivity was mainly determined by the electron transport of the support, whereas CO₂ was efficiently adsorbed and activated by the Cu single atom. Such a two-step regulation strategy of combining heterojunction with single atom enhances the possibility of simultaneously obtaining high selectivity and high yield in the photocatalytic reduction of CO₂.