Electrocatalytic hydrogenation of acetonitrile to ethylamine in acid

Chongyang Tang, Cong Wei, Yanyan Fang, Bo Liu, Xianyin Song, Zenan Bian, Xuanwei Yin, Hongbo Wang, Zhaohui Liu, Gongming Wang (), Xiangheng Xiao () and Xiangfeng Duan ()
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Chongyang Tang: Wuhan University
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
Xianyin Song: Wuhan University
Zenan Bian: University of Science and Technology of China
Xuanwei Yin: University of Science and Technology of China
Hongbo Wang: Wuhan University
Zhaohui Liu: University of Science and Technology of China
Gongming Wang: University of Science and Technology of China
Xiangheng Xiao: Wuhan University
Xiangfeng Duan: University of California, Los Angeles

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Electrochemical hydrogenation of acetonitrile based on well-developed proton exchange membrane electrolyzers holds great promise for practical production of ethylamine. However, the local acidic condition of proton exchange membrane results in severe competitive proton reduction reaction and poor selection toward acetonitrile hydrogenation. Herein, we conduct a systematic study to screen various metallic catalysts and discover Pd/C exhibits a 43.8% ethylamine Faradaic efficiency at the current density of 200 mA cm−2 with a specific production rate of 2912.5 mmol g−1 h−1, which is about an order of magnitude higher than the other screened metal catalysts. Operando characterizations indicate the in-situ formed PdHx is the active centers for catalytic reaction and the adsorption strength of the *MeCH2NH2 intermediate dictates the catalytic selectivity. More importantly, the theoretical analysis reveals a classic d-band mediated volcano curve to describe the relation between the electronic structures of catalysts and activity, which could provide valuable insights for designing more effective catalysts for electrochemical hydrogenation reactions and beyond.

Date: 2024
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DOI: 10.1038/s41467-024-47622-9

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