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Post-synthetic modification of covalent organic frameworks for CO2 electroreduction

Author

Listed:
  • Minghao Liu

    (Chinese Academy of Sciences
    University of Nottingham Ningbo China)

  • Shuai Yang

    (Chinese Academy of Sciences
    ShanghaiTech University)

  • Xiubei Yang

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Cheng-Xing Cui

    (Henan Institute of Science and Technology
    ZhengZhou JiShu Institute of AI Science)

  • Guojuan Liu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Xuewen Li

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Jun He

    (University of Nottingham Ningbo China)

  • George Zheng Chen

    (University of Nottingham)

  • Qing Xu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Gaofeng Zeng

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

Abstract

To achieve high-efficiency catalysts for CO2 reduction reaction, various catalytic metal centres and linker molecules have been assembled into covalent organic frameworks. The amine-linkages enhance the binding ability of CO2 molecules, and the ionic frameworks enable to improve the electronic conductivity and the charge transfer along the frameworks. However, directly synthesis of covalent organic frameworks with amine-linkages and ionic frameworks is hardly achieved due to the electrostatic repulsion and predicament for the strength of the linkage. Herein, we demonstrate covalent organic frameworks for CO2 reduction reaction by modulating the linkers and linkages of the template covalent organic framework to build the correlation between the catalytic performance and the structures of covalent organic frameworks. Through the double modifications, the CO2 binding ability and the electronic states are well tuned, resulting in controllable activity and selectivity for CO2 reduction reaction. Notably, the dual-functional covalent organic framework achieves high selectivity with a maximum CO Faradaic efficiency of 97.32% and the turnover frequencies value of 9922.68 h−1, which are higher than those of the base covalent organic framework and the single-modified covalent organic frameworks. Moreover, the theoretical calculations further reveal that the higher activity is attributed to the easier formation of immediate *CO from COOH*. This study provides insights into developing covalent organic frameworks for CO2 reduction reaction.

Suggested Citation

  • Minghao Liu & Shuai Yang & Xiubei Yang & Cheng-Xing Cui & Guojuan Liu & Xuewen Li & Jun He & George Zheng Chen & Qing Xu & Gaofeng Zeng, 2023. "Post-synthetic modification of covalent organic frameworks for CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39544-9
    DOI: 10.1038/s41467-023-39544-9
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    References listed on IDEAS

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    1. Ting Zhou & Lei Wang & Xingye Huang & Junjuda Unruangsri & Hualei Zhang & Rong Wang & Qingliang Song & Qingyuan Yang & Weihua Li & Changchun Wang & Kaito Takahashi & Hangxun Xu & Jia Guo, 2021. "PEG-stabilized coaxial stacking of two-dimensional covalent organic frameworks for enhanced photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    2. Rong-Ran Liang & Shun-Qi Xu & Lei Zhang & Ru-Han A & Pohua Chen & Fu-Zhi Cui & Qiao-Yan Qi & Junliang Sun & Xin Zhao, 2019. "Rational design of crystalline two-dimensional frameworks with highly complicated topological structures," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    3. Hong-Jing Zhu & Meng Lu & Yi-Rong Wang & Su-Juan Yao & Mi Zhang & Yu-He Kan & Jiang Liu & Yifa Chen & Shun-Li Li & Ya-Qian Lan, 2020. "Efficient electron transmission in covalent organic framework nanosheets for highly active electrocatalytic carbon dioxide reduction," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    4. Zhendong Lei & Qinsi Yang & Yi Xu & Siyu Guo & Weiwei Sun & Hao Liu & Li-Ping Lv & Yong Zhang & Yong Wang, 2018. "Boosting lithium storage in covalent organic framework via activation of 14-electron redox chemistry," Nature Communications, Nature, vol. 9(1), pages 1-13, December.
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