Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst
Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable...
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Veröffentlicht in: | Nature communications 2016-12, Vol.7 (1), p.14036-14036, Article 14036 |
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Sprache: | eng |
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Zusammenfassung: | Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable activity and selectivity towards propene hydroformylation. By increasing Rh mass loading, isolated Rh atoms switch to aggregated clusters of different atomicity. During the hydroformylation, Rh/CoO achieves the optimal selectivity of 94.4% for butyraldehyde and the highest turnover frequency number of 2,065 h
−1
among the obtained atomic-scale Rh-based catalysts. Mechanistic studies reveal that a structural reconstruction of Rh single atoms in Rh/CoO occurs during the catalytic process, facilitating the adsorption and activation of reactants. In kinetic view, linear products are determined as the dominating products by analysing reaction paths deriving from the two most stable co-adsorbed configurations. As a bridge of homogeneous and heterogeneous catalysis, single-atom catalysts can be potentially applied in other industrial reactions.
Despite the advantages of using heterogeneous catalysts, most successful rhodium hydrogenations are carried out with homogeneous catalysts. Here the authors report a supported single atom rhodium catalyst providing high activities and selectivities for propene hydroformylation. |
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ISSN: | 2041-1723 2041-1723 |
DOI: | 10.1038/ncomms14036 |