Developing an efficient and selective catalyst for the dehydration of fructose to 5-hydroxymethylfurfural(HMF)is significant for biomass conversion.Herein,a metal-organic framework(MOF)with acidity and strong hydropho...Developing an efficient and selective catalyst for the dehydration of fructose to 5-hydroxymethylfurfural(HMF)is significant for biomass conversion.Herein,a metal-organic framework(MOF)with acidity and strong hydrophobicity is first reported by the condensation of amino-tagged MOFs with mercapto carboxylic acids and subsequent oxidation.The hydrophobic acidic MOFs possess acid densities ranging from 0.2-1.0 mmol·g^(-1),H_(2)O contact angles of 114°-125°,and specific surface areas above260 m^(2)·g^(-1).Compared to the methyl sulfo-functionalized MOF,the benzene sulfo-functionalized MOF with a strong hydrophobicity shows much higher activity and selectivity for the conversion of fructose to 5-hydroxymethylfurfural.In particular,2.99%(mass)UiO-PhSO_(3)H shows the best catalytic performance with a 90.4%HMF yield due to its suitable hydrophobicity and abundant acidic sites.Moreover,the catalyst shows great stability after recycling for 5 runs.This work provides an interesting design strategy for the preparation of hydrophobic acidic MOFs and shows the powerful synergistic effect of acidity and hydrophobicity.展开更多
基金support from the National Natural Science Foundation of China(21878138,21666021,and 21706112)the Postdoctoral Science Foundation of China(2017M622104,2018T110660)。
文摘Developing an efficient and selective catalyst for the dehydration of fructose to 5-hydroxymethylfurfural(HMF)is significant for biomass conversion.Herein,a metal-organic framework(MOF)with acidity and strong hydrophobicity is first reported by the condensation of amino-tagged MOFs with mercapto carboxylic acids and subsequent oxidation.The hydrophobic acidic MOFs possess acid densities ranging from 0.2-1.0 mmol·g^(-1),H_(2)O contact angles of 114°-125°,and specific surface areas above260 m^(2)·g^(-1).Compared to the methyl sulfo-functionalized MOF,the benzene sulfo-functionalized MOF with a strong hydrophobicity shows much higher activity and selectivity for the conversion of fructose to 5-hydroxymethylfurfural.In particular,2.99%(mass)UiO-PhSO_(3)H shows the best catalytic performance with a 90.4%HMF yield due to its suitable hydrophobicity and abundant acidic sites.Moreover,the catalyst shows great stability after recycling for 5 runs.This work provides an interesting design strategy for the preparation of hydrophobic acidic MOFs and shows the powerful synergistic effect of acidity and hydrophobicity.
