Abstract
In this work, three MOF-based materials with highly dispersed Rh(I) were synthesized for hydroformylation of n-butene, namely Rh(I)/UiO-66, Rh(I)/MOF-5 and Rh(I)/MIL-101. The defect sites on the metal nodes of MOFs promoted the anchoring of Rh as a single active site. A high-performance Rh(I)/MOF-5 catalyst was obtained with the n-butene conversion and pentanal selectivity of 96.4% and 85.8%, respectively. In addition, it showed a good stability in the recycling tests after five runs. XRD, TEM, XPS, in situ DRIRTS confirmed that the metal nodes in MOFs modified the activity of the coordinated Rh catalyst by influencing the adsorption strength of CO. Combing the DFT results, we predicted that Rh(I)/MOF-5 catalyst with suitable CO adsorption energy could reduce the reaction energy barrier in CO insertion process, which was the rate-determining step of overall reaction, thus improving the selectivity of total aldehydes. This work broadened the application of MOFs as catalyst supports and provided assistance for the development of heterogeneous catalysts in hydroformylation of olefins.
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