Abstract
The size and geometry of supported metal ensembles have a substantial influence on their catalytic efficacy and are pivotal in the design of effective heterogeneous catalysts. Here we developed a straightforward electronic and structural engineering strategy to create supported single atomic-layered, low-nuclearity palladium catalysts. This atomically dispersed Pd catalyst possesses unique synergistic geometric and electronic effects and nearly full metal availability to the reactant, exhibiting excellent catalytic activity (turnover frequency of 12480 h−1) and yield (>99%) in the hydrogenation of levulinic acid to 1,4-pentanediol under mild conditions, a reaction of importance for conversion of biomass to renewable chemicals. Theoretical calculations reveal that the high catalytic activity results from the cooperation of adjacent Pd atoms, high d-band center, and strong electronic metal-support interactions, thus guaranteeing efficient activation of reactant and facilitating the subsequent ring-opening step. The present work sheds light on the elegant design of low-nuclearity metal cluster catalysts with structure sensitivity to maximize the catalytic efficiency at the atomic scale.
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