Electrosynthesis of formamide from methanol and ammonia under ambient conditions

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 formami...

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Bibliographic Details
Published in:Nature communications 2022-09, Vol.13 (1), p.5452-8, Article 5452
Main Authors: Meng, Nannan, Shao, Jiang, Li, Hongjiao, Wang, Yuting, Fu, Xiaoli, Liu, Cuibo, Yu, Yifu, Zhang, Bin
Format: Article
Language:English
Subjects:
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Alcohol
Aldehydes
Ammonia
Aqueous solutions
Biomass
Carbon dioxide
Catalytic oxidation
Coupling (molecular)
Decay
Economic analysis
Efficiency
Electrocatalysts
Electrochemical oxidation
Electrochemistry
Humanities and Social Sciences
Laboratories
Manufacturing
Methanol
Methylamine
multidisciplinary
Nitrogen
NMR
Nuclear magnetic resonance
Oxidation
Production methods
Science
Science (multidisciplinary)
Selectivity
Sustainable production
Synthesis
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Summary: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 NH 3 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). Developing a sustainable manufacturing method using biomass-derived feedstock at ambient conditions is highly desirable. Here the authors report electrooxidation route for synthesis of formamide from methanol and ammonia in water
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-022-33232-w