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

Cong Wei, Yanyan Fang, Bo Liu, Chongyang Tang, Bin Dong, Xuanwei Yin, Zenan Bian, Zhandong Wang, Jun Liu, Yitai Qian and Gongming Wang ()
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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

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-39558-3

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