Abstract
AbstractPrecisely tailoring the distance between adjacent metal sites to match adsorption configurations of key species for the targeted reaction pathway is a great challenge in heterogeneous catalysis. Here, we report a proof‐of‐concept study on the atomically sites‐tailored pathway in Pd‐catalyzed acetylene hydrogenation, i.e., increasing the distance of adjacent Pd atoms (dPd‐a‐Pd) for configuration matching in acetylene semi‐hydrogenation against coupling.dPd‐a‐Pdis identified as a structural descriptor for describing the competitiveness for reaction pathways, and the increaseddPd‐a‐Pdprefers the semi‐hydrogenation pathway due to simultaneously promoted C2H4desorption and the destabilized transition state of the C2H3* coupling. Spectroscopic, kinetics and electronic structure studies reveal that increasingdPd‐a‐Pdto 3.31 Å delivers superior selectivity and stability due to energy matching and appropriate hybridization of Pd 4d with In 2s and, especially, 2p orbitals.
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