Abstract
AbstractControlling the metal geometric and electronic structure is of significance in developing efficient catalysts for heterogeneous hydroformylation. This study examines the structural sizes of Rh and Rh+‐Rh0 distribution to construct a highly active catalyst for formaldehyde hydroformylation. The active sites for hydroformylation require several Rhn atoms, while single‐atom Rh can solely catalyze hydrogenation. The highest activity was achieved on Rh nanoclusters (0.95 nm), giving a TOF of 191 h−1 and selectivity of 82% for glycolaldehyde formation. The tunability of the electronic properties of Rh nanoclusters and the synergistic interaction between Rh+ and Rh0 are essential for enhanced activity. Pseudo‐in situ FT‐IR analysis elucidated that formaldehyde adsorbed on Rh nanocluster prefers to produce glycolaldehyde via hydroformylation, while formaldehyde adsorbed on isolated Rhδ+ sites tends to form methanol via hydrogenation. This study provides a new insight into the design of heterogeneous catalysts and guidance for understanding the reaction mechanism for aldehydes/olefins hydroformylation.
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