The MOF-driven synthesis of supported palladium clusters with catalytic activity for carbene-mediated chemistry
Autor: | Emilio Pardo, Jesús Ferrando-Soria, Juan Manuel Herrera, Avelino Corma, Antonio Leyva-Pérez, Donatella Armentano, Mercedes Boronat, Jorge Gascon, Francisco R. Fortea-Pérez, Marta Mon, Dmitrii Osadchii |
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Rok vydání: | 2017 |
Předmět: |
Chemical process
Mechanical Engineering chemistry.chemical_element 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology Condensed Matter Physics Heterogeneous catalysis 01 natural sciences Combinatorial chemistry 0104 chemical sciences Catalysis chemistry.chemical_compound chemistry Mechanics of Materials Organic chemistry General Materials Science Metal catalyst 0210 nano-technology Carbene Palladium Metal clusters |
Zdroj: | Nature Materials. 16:760-766 |
ISSN: | 1476-4660 1476-1122 |
DOI: | 10.1038/nmat4910 |
Popis: | 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. |
Databáze: | OpenAIRE |
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