Oxygen vacancy associated single-electron transfer for photofixation of CO2 to long-chain chemicals

Shichuan Chen, Hui Wang, Zhixiong Kang, Sen Jin, Xiaodong Zhang (), Xusheng Zheng, Zeming Qi, Junfa Zhu, Bicai Pan and Yi Xie ()
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Shichuan Chen: University of Science and Technology of China
Hui Wang: University of Science and Technology of China
Zhixiong Kang: University of Science and Technology of China
Sen Jin: University of Science and Technology of China
Xiaodong Zhang: University of Science and Technology of China
Xusheng Zheng: University of Science and Technology of China
Zeming Qi: University of Science and Technology of China
Junfa Zhu: University of Science and Technology of China
Bicai Pan: University of Science and Technology of China
Yi Xie: University of Science and Technology of China

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract The photofixation and utilization of CO2 via single-electron mechanism is considered to be a clean and green way to produce high-value-added commodity chemicals with long carbon chains. However, this topic has not been fully explored for the highly negative reduction potential in the formation of reactive carbonate radical. Herein, by taking Bi2O3 nanosheets as a model system, we illustrate that oxygen vacancies confined in atomic layers can lower the adsorption energy of CO2 on the reactive sites, and thus activate CO2 by single-electron transfer in mild conditions. As demonstrated, Bi2O3 nanosheets with rich oxygen vacancies show enhanced generation of •CO2– species during the reaction process and achieve a high conversion yield of dimethyl carbonate (DMC) with nearly 100% selectivity in the presence of methanol. This study establishes a practical way for the photofixation of CO2 to long-chain chemicals via defect engineering.

Date: 2019
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DOI: 10.1038/s41467-019-08697-x

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