One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy,yet it is still challenging due to the lack of su...One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy,yet it is still challenging due to the lack of suitable catalysts with cascade conversion ability.In this work,we developed a porous hybrid catalyst (i.e.PMo_(10)V_(2)@2Br-PIL) based on the assembly of polyoxometalates and porous polyionic liquids that can be applied in the one-pot conversion of fructose to DFF.The integration of PMo_(10)V_(2) with 2Br-PIL can impart both Brønsted acid and oxidation sites in the porous structure,thereby enabling the one-pot cascade conversion.As a result,PMo_(10)V_(2)@2Br-PIL demonstrated a remarkable DFF yield (95% yield),satisfying stability,recyclability and scale-up production ability (≈12.3 g in a batch experiment),demonstrating great potential for industrial production of DFF from fructose.Theoretical calculations revealed a synergistic effect of Brønsted acid sites and oxidation sites in PMo_(10)V_(2)@2Br-PIL,which promoted the one-pot conversion of fructose to DFF.This study enhances the understanding of biomass transformation over hybrid catalysts through synergetic acidic/oxidative catalysis,contributing to the development of highly active,selective,and multifunctional catalysts for one-pot biomass conversion.展开更多
基金financially supported by the National Natural Science Foundation of China(No.21871125,22475074,22171139 and 22201116)Natural Science Foundation of Guangdong Province(No.2023B1515020076)+2 种基金Natural Science Foundation of Shandong Province(No.ZR2022QB066 and ZR2023MB018)Dongying City School Cooperation Fund Key Project(SXHZ-2023-02-15)college Student Innovation and Entrepreneurship Training Plan of Liaocheng University(cxcy089).
文摘One-pot direct conversion of cheap and abundant fructose to 2,5-diformylfuran (DFF) is highly desirable to achieve hundreds-fold value-increase and high atomic economy,yet it is still challenging due to the lack of suitable catalysts with cascade conversion ability.In this work,we developed a porous hybrid catalyst (i.e.PMo_(10)V_(2)@2Br-PIL) based on the assembly of polyoxometalates and porous polyionic liquids that can be applied in the one-pot conversion of fructose to DFF.The integration of PMo_(10)V_(2) with 2Br-PIL can impart both Brønsted acid and oxidation sites in the porous structure,thereby enabling the one-pot cascade conversion.As a result,PMo_(10)V_(2)@2Br-PIL demonstrated a remarkable DFF yield (95% yield),satisfying stability,recyclability and scale-up production ability (≈12.3 g in a batch experiment),demonstrating great potential for industrial production of DFF from fructose.Theoretical calculations revealed a synergistic effect of Brønsted acid sites and oxidation sites in PMo_(10)V_(2)@2Br-PIL,which promoted the one-pot conversion of fructose to DFF.This study enhances the understanding of biomass transformation over hybrid catalysts through synergetic acidic/oxidative catalysis,contributing to the development of highly active,selective,and multifunctional catalysts for one-pot biomass conversion.
