Electrocatalytic upgrading of biomass-derived platform molecules has emerged as a sustainable and environmentally benign route to produce high-value chemicals.The main challenge lies in developing efficient catalysts ...Electrocatalytic upgrading of biomass-derived platform molecules has emerged as a sustainable and environmentally benign route to produce high-value chemicals.The main challenge lies in developing efficient catalysts for the selective activation of designated chemical bonds in the presence of various reducible groups.This work demonstrated a high-efficiency electrochemical conversion of 5-hydroxymethylfurfural(HMF)to 2,5-bis(hydroxymethyl)furan(BHMF),an important industrial synthetic reagent.A highly porous Cu-based catalyst was developed that achieved nearly 100%BHMF selectivity and long-term stability.Through comprehensive operando and ex-situ structural characterizations,an electrochemically generated catalyst with abundant Cu/Cu2O interfaces was identified as a catalytically active phase for HMF conversion.Deuterated BHMF,with the potential to produce deuterated drugs,was also synthesized using D2O as the deuterium source.Density functional theory calculations show that the Cu/Cu2O interface structure exhibits relatively low energy barriers for the hydrogenation of HMF to BHMF.This work provides insights into the origin of electrocatalytic hydrogenation activity and highlights the promising potential of the electrocatalytic synthesis of high-value chemicals.展开更多
基金the National Natural Science Foundation of China(21838003,91834301 and 21978278)the Shanghai Scientific and Technological Innovation Project(18JC1410500 and 19JC1410400)the Fundamental Research Funds for the Central Universities(222201718002).
文摘Electrocatalytic upgrading of biomass-derived platform molecules has emerged as a sustainable and environmentally benign route to produce high-value chemicals.The main challenge lies in developing efficient catalysts for the selective activation of designated chemical bonds in the presence of various reducible groups.This work demonstrated a high-efficiency electrochemical conversion of 5-hydroxymethylfurfural(HMF)to 2,5-bis(hydroxymethyl)furan(BHMF),an important industrial synthetic reagent.A highly porous Cu-based catalyst was developed that achieved nearly 100%BHMF selectivity and long-term stability.Through comprehensive operando and ex-situ structural characterizations,an electrochemically generated catalyst with abundant Cu/Cu2O interfaces was identified as a catalytically active phase for HMF conversion.Deuterated BHMF,with the potential to produce deuterated drugs,was also synthesized using D2O as the deuterium source.Density functional theory calculations show that the Cu/Cu2O interface structure exhibits relatively low energy barriers for the hydrogenation of HMF to BHMF.This work provides insights into the origin of electrocatalytic hydrogenation activity and highlights the promising potential of the electrocatalytic synthesis of high-value chemicals.
基金the National Key R&D Program of China(2022YFB3808400)the National Natural Science Foundation of China(22222804 and U22B20143)+1 种基金the Science and Technology Commission of Shanghai Municipality(22dz1205900)the Shanghai Municipal Science and Technology Major Project。
