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Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst

Author

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  • Qinggang Liu

    (Dalian University of Technology
    Chinese Academy of Sciences)

  • Xiaofeng Yang

    (Chinese Academy of Sciences)

  • Lin Li

    (Chinese Academy of Sciences)

  • Shu Miao

    (Chinese Academy of Sciences)

  • Yong Li

    (University of Bremen)

  • Yanqin Li

    (Dalian University of Technology)

  • Xinkui Wang

    (Dalian University of Technology)

  • Yanqiang Huang

    (Chinese Academy of Sciences)

  • Tao Zhang

    (Chinese Academy of Sciences)

Abstract

Catalytic transformation of CO2 to formate is generally realized through bicarbonate hydrogenation in an alkaline environment, while it suffers from a thermodynamic sink due to the considerable thermodynamic stability of the bicarbonate intermediate. Here, we devise a route for the direct catalytic conversion of CO2 over a Schiff-base-modified gold nanocatalyst that is comparable to the fastest known nanocatalysts, with a turnover number (TON) of up to 14,470 over 12 h at 90 °C. Theoretical calculations and spectral analysis results demonstrate that the activation of CO2 can be achieved through a weakly bonded carbamate zwitterion intermediate derived from a simple Lewis base adduct of CO2. However, this can only occur with a hydrogen lacking Lewis base center in a polar solvent. This finding offers a promising avenue for the direct activation of CO2 and is likely to have considerable implications in the fields of CO2 conversion and gold catalytic chemistry.

Suggested Citation

  • Qinggang Liu & Xiaofeng Yang & Lin Li & Shu Miao & Yong Li & Yanqin Li & Xinkui Wang & Yanqiang Huang & Tao Zhang, 2017. "Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-01673-3
    DOI: 10.1038/s41467-017-01673-3
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    Cited by:

    1. Wenqing Zhang & Dawei Xi & Yihong Chen & Aobo Chen & Yawen Jiang & Hengjie Liu & Zeyu Zhou & Hui Zhang & Zhi Liu & Ran Long & Yujie Xiong, 2023. "Light-driven flow synthesis of acetic acid from methane with chemical looping," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Jikai Sun & Rui Tu & Yuchun Xu & Hongyan Yang & Tie Yu & Dong Zhai & Xiuqin Ci & Weiqiao Deng, 2024. "Machine learning aided design of single-atom alloy catalysts for methane cracking," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. An, Xiaowei & Li, Shasha & Hao, Xiaoqiong & Xie, Zhengkun & Du, Xiao & Wang, Zhongde & Hao, Xiaogang & Abudula, Abuliti & Guan, Guoqing, 2021. "Common strategies for improving the performances of tin and bismuth-based catalysts in the electrocatalytic reduction of CO2 to formic acid/formate," Renewable and Sustainable Energy Reviews, Elsevier, vol. 143(C).

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