Amide is essential in biologically active compounds,synthetic materials,and building blocks.However,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to ...Amide is essential in biologically active compounds,synthetic materials,and building blocks.However,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to construct the C–N bond.Herein,for the first time,we have successfully realized the formation of amides at industrial current density via the anodic coelectrolysis of alcohol and ammonia under ambient conditions.We have proved thatmodulation of the interface microenvironment concentration of nucleophile by electrolyte engineering can regulate the reaction pathways of amides rather than acetic acids.The C-N coupling strategy can be further extended to the electrosynthesis of the long-chain and aryl-ring amide with high selectivity by replacing ammonia with amine.Our work opens up a vast store of information on the utilization of biomass alcohol for high-value N-containing chemicals via an electrocatalytic C-N coupling reaction.展开更多
基金supported by the National Key R&D Program of China(grant no.2020YFA0710000)the National Natural Science Foundation of China(grant no.22122901)+1 种基金the Provincial Natural Science Foundation of Hunan(grant nos.2021JJ0008,2021JJ20024,2021RC3054,and 2020JJ5045)the Shenzhen Science and Technology Program(grant no.JCYJ20210324140610028).
文摘Amide is essential in biologically active compounds,synthetic materials,and building blocks.However,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to construct the C–N bond.Herein,for the first time,we have successfully realized the formation of amides at industrial current density via the anodic coelectrolysis of alcohol and ammonia under ambient conditions.We have proved thatmodulation of the interface microenvironment concentration of nucleophile by electrolyte engineering can regulate the reaction pathways of amides rather than acetic acids.The C-N coupling strategy can be further extended to the electrosynthesis of the long-chain and aryl-ring amide with high selectivity by replacing ammonia with amine.Our work opens up a vast store of information on the utilization of biomass alcohol for high-value N-containing chemicals via an electrocatalytic C-N coupling reaction.