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

Author

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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)

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.

Suggested Citation

  • Shichuan Chen & Hui Wang & Zhixiong Kang & Sen Jin & Xiaodong Zhang & Xusheng Zheng & Zeming Qi & Junfa Zhu & Bicai Pan & Yi Xie, 2019. "Oxygen vacancy associated single-electron transfer for photofixation of CO2 to long-chain chemicals," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08697-x
    DOI: 10.1038/s41467-019-08697-x
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    Cited by:

    1. Shujuan Liu & Teng Li & Feng Shi & Haiying Ma & Bin Wang & Xingchao Dai & Xinjiang Cui, 2023. "Constructing multiple active sites in iron oxide catalysts for improving carbonylation reactions," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    2. Yanbiao Shi & Jie Li & Chengliang Mao & Song Liu & Xiaobing Wang & Xiufan Liu & Shengxi Zhao & Xiao Liu & Yanqiang Huang & Lizhi Zhang, 2021. "Van Der Waals gap-rich BiOCl atomic layers realizing efficient, pure-water CO2-to-CO photocatalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    3. Xin Chen & Junxiang Chen & Huayu Chen & Qiqi Zhang & Jiaxuan Li & Jiwei Cui & Yanhui Sun & Defa Wang & Jinhua Ye & Lequan Liu, 2023. "Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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