Promoting Catalytic Performance Involving Hydrogen Spillover by Ion Exchange of Pt@A Catalysts to Regulate Reactant Adsorption.

Abstract

Zeolite-encapsulated metal nanoparticle systems have exhibited interesting catalytic performances via the hydrogen spillover process, yet how to further utilize the function of zeolite supports to promote catalytic properties in such a process is still challenging and has rarely been investigated. Herein, to address this issue, the strategy to strengthen the adsorption energy of reactant onto the zeolite surface via a simple ion exchange method has been implemented. Ion-exchanged linde type A (LTA) zeolite-encapsulated platinum nanoclusters (Pt@NaA, Pt@HA, Pt@KA, and Pt@CaA) were prepared to study the influence of ion exchange on the catalytic performance in the model reaction of hydrogenation of acetophenone to 1-phenylethanol. The reaction results showed that the Pt@CaA catalyst exhibited the best catalytic activity in the series of encapsulated catalysts, and the selectivity of 1-phenylethanol approached 100%. As revealed by density functional theory (DFT) calculations and acetophenone temperature-programmed desorption (acetophenone-TPD) experiments, in comparison with introduced cations of Na+, H+, and K+, ion-exchanged Ca2+ on the zeolite maximumly enhanced the adsorption of carbonyl groups in acetophenone, playing a critical role in achieving the highest activity and excellent catalytic selectivity among the Pt@A catalysts.