Electrosynthesis of formamide from methanol and ammonia under ambient conditions

Nannan Meng, Jiang Shao, Hongjiao Li, Yuting Wang, Xiaoli Fu, Cuibo Liu, Yifu Yu () and Bin Zhang ()
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Nannan Meng: Tianjin University
Jiang Shao: Tianjin University
Hongjiao Li: Sichuan University
Yuting Wang: Tianjin University
Xiaoli Fu: Tianjin University
Cuibo Liu: Tianjin University
Yifu Yu: Tianjin University
Bin Zhang: Tianjin University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Electrochemical conversion of abundant carbon- and nitrogen-containing small molecules into high-valued organonitrogen compounds is alluring to reducing current dependence on fossil energy. Here we report a single-cell electrochemical oxidation approach to transform methanol and ammonia into formamide under ambient conditions over Pt electrocatalyst that provides 74.26% selectivity from methanol to formamide and a Faradaic efficiency of 40.39% at 100 mA cm−2 current density, gaining an economic advantage over conventional manufacturing based on techno-economic analysis. A 46-h continuous test performed in the flow cell shows no performance decay. The combined results of in situ experiments and theoretical simulations unveil the C–N bond formation mechanism via nucleophilic attack of NH3 on an aldehyde-like intermediate derived from methanol electrooxidation. This work offers a way to synthesize formamide via C–N coupling and can be extended to substantially synthesize other value-added organonitrogen chemicals (e.g., acetamide, propenamide, formyl methylamine).

Date: 2022
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DOI: 10.1038/s41467-022-33232-w

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