Electrocatalytic valorization of biomass derivatives can be powered by electricity generated from renewable sources such as solar and wind energy.A shift from centralized,high-temperature,and energy-intensive processe...Electrocatalytic valorization of biomass derivatives can be powered by electricity generated from renewable sources such as solar and wind energy.A shift from centralized,high-temperature,and energy-intensive processes to decentralized,low-temperature conversions is achieved,which meets the requirement of sustainable energy generation.This approach provides an efficient,green,and additive-free strategy for biomass derivative valorization,in which product selectivity could be easily regulated by the applied potential and electrocatalyst utilized.However,a scale-up application is still far from being completed due to the inability of conversion rates and selectivity to meet the industrialization requirements.A better understanding of the reaction mechanism and the development of highefficiency and high-selectivity electrocatalysts are required to pave the path toward larger industrialization applications.Herein,we summarize the recent research progress in the electrocatalytic oxidation and hydrogenation of platform compounds such as furanic compounds and glycerol.In the literature,these three research areas are integrated to realize the scale-up application of the processes as mentioned above.The investigations of the mechanism are based on in situ techniques,theoretical calculations,and advanced electrocatalyst studies.Finally,the challenges and prospects in this topic are described.We expect that this review will provide the fundamental understanding and design guidelines to achieve efficient and high-selectivity catalysts and further facilitate the scale-up application of the electrocatalytic conversion of biomass derivatives.展开更多
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(2020YFA0710000)the Fundamental Research Funds for the Central Universities(531118010127)+1 种基金the National Natural Science Foundation of China(22122901,21902047,21825201,and U19A2017)the Provincial Natural Science Foundation of Hunan(2020JJ5045,2021RC3054).
文摘Electrocatalytic valorization of biomass derivatives can be powered by electricity generated from renewable sources such as solar and wind energy.A shift from centralized,high-temperature,and energy-intensive processes to decentralized,low-temperature conversions is achieved,which meets the requirement of sustainable energy generation.This approach provides an efficient,green,and additive-free strategy for biomass derivative valorization,in which product selectivity could be easily regulated by the applied potential and electrocatalyst utilized.However,a scale-up application is still far from being completed due to the inability of conversion rates and selectivity to meet the industrialization requirements.A better understanding of the reaction mechanism and the development of highefficiency and high-selectivity electrocatalysts are required to pave the path toward larger industrialization applications.Herein,we summarize the recent research progress in the electrocatalytic oxidation and hydrogenation of platform compounds such as furanic compounds and glycerol.In the literature,these three research areas are integrated to realize the scale-up application of the processes as mentioned above.The investigations of the mechanism are based on in situ techniques,theoretical calculations,and advanced electrocatalyst studies.Finally,the challenges and prospects in this topic are described.We expect that this review will provide the fundamental understanding and design guidelines to achieve efficient and high-selectivity catalysts and further facilitate the scale-up application of the electrocatalytic conversion of biomass derivatives.
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.
