American Chemical Society
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Tunable Interfacial Electronic Pd–Si Interaction Boosts Catalysis via Accelerating O2 and H2O Activation

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journal contribution
posted on 2023-04-03, 18:35 authored by Tao Dong, Jian Ji, Leyi Yu, Pingli Huang, Yiheng Li, Ziyi Suo, Biyuan Liu, Zhuofeng Hu, Haibao Huang
Engineering the interfacial structure between noble metals and oxides, particularly on the surface of non-reducible oxides, is a challenging yet promising approach to enhancing the performance of heterogeneous catalysts. The interface site can alter the electronic and d-band structure of the metal sites, facilitating the transition of energy levels between the reacting molecules and promoting the reaction to proceed in a favorable direction. Herein, we created an active Pd–Si interface with tunable electronic metal–support interaction (EMSI) by growing a thin permeable silica layer on a non-reducible oxide ZSM-5 surface (termed Pd@SiO2/ZSM-5). Our experimental results, combined with density functional theory calculations, revealed that the Pd–Si active interface enhanced the charge transfer from deposited Si to Pd, generating an electron-enriched Pd surface, which significantly lowered the activation barriers for O2 and H2O. The resulting reactive oxygen species, including O2, O22–, and −OH, synergistically facilitated formaldehyde oxidation. Additionally, moderate electronic metal–support interaction can promote the catalytic cycle of Pd0 ⇆ Pd2+, which is favorable for the adsorption and activation of reactants. This study provides a promising strategy for the design of high-performance noble metal catalysts for practical applications.