6533b82bfe1ef96bd128d924
RESEARCH PRODUCT
The MOF-driven synthesis of supported palladium clusters with catalytic activity for carbene-mediated chemistry
Emilio PardoJesús Ferrando-soriaJuan Manuel HerreraAvelino CormaAntonio Leyva-pérezDonatella ArmentanoMercedes BoronatJorge GasconFrancisco R. Fortea-pérezMarta MonDmitrii Osadchiisubject
Chemical processMechanical Engineeringchemistry.chemical_element02 engineering and technologyGeneral Chemistry010402 general chemistry021001 nanoscience & nanotechnologyCondensed Matter PhysicsHeterogeneous catalysis01 natural sciencesCombinatorial chemistry0104 chemical sciencesCatalysischemistry.chemical_compoundchemistryMechanics of MaterialsOrganic chemistryGeneral Materials ScienceMetal catalyst0210 nano-technologyCarbenePalladiumMetal clustersdescription
The development of catalysts able to assist industrially important chemical processes is a topic of high importance. In view of the catalytic capabilities of small metal clusters, research efforts are being focused on the synthesis of novel catalysts bearing such active sites. Here we report a heterogeneous catalyst consisting of Pd4 clusters with mixed-valence 0/+1 oxidation states, stabilized and homogeneously organized within the walls of a metal-organic framework (MOF). The resulting solid catalyst outperforms state-of-the-art metal catalysts in carbene-mediated reactions of diazoacetates, with high yields (>90%) and turnover numbers (up to 100,000). In addition, the MOF-supported Pd4 clusters retain their catalytic activity in repeated batch and flow reactions (>20 cycles). Our findings demonstrate how this synthetic approach may now instruct the future design of heterogeneous catalysts with advantageous reaction capabilities for other important processes.
year | journal | country | edition | language |
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2016-11-30 | Nature Materials |