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Lattice oxygen-mediated electron tuning promotes electrochemical hydrogenation of acetonitrile on copper catalysts

Author

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  • Cong Wei

    (University of Science and Technology of China)

  • Yanyan Fang

    (University of Science and Technology of China)

  • Bo Liu

    (University of Science and Technology of China)

  • Chongyang Tang

    (University of Science and Technology of China)

  • Bin Dong

    (University of Science and Technology of China)

  • Xuanwei Yin

    (University of Science and Technology of China)

  • Zenan Bian

    (University of Science and Technology of China)

  • Zhandong Wang

    (University of Science and Technology of China)

  • Jun Liu

    (Hefei Institutes of Physical Science, Chinese Academy of Sciences)

  • Yitai Qian

    (University of Science and Technology of China)

  • Gongming Wang

    (University of Science and Technology of China)

Abstract

Copper is well-known to be selective to primary amines via electrocatalytic nitriles hydrogenation. However, the correlation between the local fine structure and catalytic selectivity is still illusive. Herein, we find that residual lattice oxygen in oxide-derived Cu nanowires (OD-Cu NWs) plays vital roles in boosting the acetonitrile electroreduction efficiency. Especially at high current densities of more than 1.0 A cm−2, OD-Cu NWs exhibit relatively high Faradic efficiency. Meanwhile, a series of advanced in situ characterizations and theoretical calculations uncover that oxygen residues, in the form of Cu4-O configuration, act as electron acceptors to confine the free electron flow on the Cu surface, consequently improving the kinetics of nitriles hydrogenation catalysis. This work could provide new opportunities to further improve the hydrogenation performance of nitriles and beyond, by employing lattice oxygen-mediated electron tuning engineering.

Suggested Citation

  • Cong Wei & Yanyan Fang & Bo Liu & Chongyang Tang & Bin Dong & Xuanwei Yin & Zenan Bian & Zhandong Wang & Jun Liu & Yitai Qian & Gongming Wang, 2023. "Lattice oxygen-mediated electron tuning promotes electrochemical hydrogenation of acetonitrile on copper catalysts," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39558-3
    DOI: 10.1038/s41467-023-39558-3
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    References listed on IDEAS

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    1. Zhibo Liu & Fei Huang & Mi Peng & Yunlei Chen & Xiangbin Cai & Linlin Wang & Zenan Hu & Xiaodong Wen & Ning Wang & Dequan Xiao & Hong Jiang & Hongbin Sun & Hongyang Liu & Ding Ma, 2021. "Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    2. Geng Wu & Xiao Han & Jinyan Cai & Peiqun Yin & Peixin Cui & Xusheng Zheng & Hai Li & Cai Chen & Gongming Wang & Xun Hong, 2022. "In-plane strain engineering in ultrathin noble metal nanosheets boosts the intrinsic electrocatalytic hydrogen evolution activity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Sai Zhang & Zhaoming Xia & Yong Zou & Mingkai Zhang & Yongquan Qu, 2021. "Spatial intimacy of binary active-sites for selective sequential hydrogenation-condensation of nitriles into secondary imines," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
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