In this work,we report that high catalytic performance of metal–organic frameworks(MOFs)can be obtained through a synergistic effect of postsynthetic modification of MOF nanoparticles and liquid superwetting and conf...In this work,we report that high catalytic performance of metal–organic frameworks(MOFs)can be obtained through a synergistic effect of postsynthetic modification of MOF nanoparticles and liquid superwetting and confinement in the MOF coating.Specifically,2-ureido-4[1H]pyrimidinone(UPy)functionalized polysiloxanes were covalently appended onto the UiO-66 nanoparticles via a postsynthetic approach,which were further anchored onto different porous films through multivalent hydrogen bonding of the UPy motifs.The hydrophobic MOF coating can preserve the porosity of the solid substrates,enable rapid liquid superwetting and confinement within the porous substrates.Using the Knoevenagel condensation as a modeled system,robust and highly catalytic performances of the MOF coating were observed on a range of aldehyde substrates.Gram-scale production of chromene,a pharmaceutical which is typically synthesized via expensive catalysis,was successfully demonstrated on the MOF coating with high yielding rates,demonstrating the great potential of the MOF coating in pharmaceutical synthesis.展开更多
基金X.Y.acknowledges the Research Grant Council of Hong Kong(Nos.11305219 and 11307220)CityU Applied Research Grant(ARG,No.9667203)+2 种基金Shenzhen Basic Research Program(No.JCYJ20210324134009024)Z.X.acknowledges a Shenzhen-HKMacao Science and Technology Grant(type CNo.SGDX2020110309300301)from the Science,Technology,and Innovation Commission of Shenzhen Municipality.
文摘In this work,we report that high catalytic performance of metal–organic frameworks(MOFs)can be obtained through a synergistic effect of postsynthetic modification of MOF nanoparticles and liquid superwetting and confinement in the MOF coating.Specifically,2-ureido-4[1H]pyrimidinone(UPy)functionalized polysiloxanes were covalently appended onto the UiO-66 nanoparticles via a postsynthetic approach,which were further anchored onto different porous films through multivalent hydrogen bonding of the UPy motifs.The hydrophobic MOF coating can preserve the porosity of the solid substrates,enable rapid liquid superwetting and confinement within the porous substrates.Using the Knoevenagel condensation as a modeled system,robust and highly catalytic performances of the MOF coating were observed on a range of aldehyde substrates.Gram-scale production of chromene,a pharmaceutical which is typically synthesized via expensive catalysis,was successfully demonstrated on the MOF coating with high yielding rates,demonstrating the great potential of the MOF coating in pharmaceutical synthesis.
