Tunable Interfacial Electronic Pd-Si Interaction Boosts Catalysis via Accelerating O 2 and H 2 O Activation

• Published in: JACS Au 2023-04, Vol.3 (4), p.1230-1240
• Main Authors: Dong, Tao, Ji, Jian, Yu, Leyi, Huang, Pingli, Li, Yiheng, Suo, Ziyi, Liu, Biyuan, Hu, Zhuofeng, Huang, Haibao
• Format: Article
• Language: English
• ISSN: 2691-3704; 2691-3704
• DOI: 10.1021/jacsau.3c00093

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 -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@SiO /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 O and H O. The resulting reactive oxygen species, including O , O , and -OH, synergistically facilitated formaldehyde oxidation. Additionally, moderate electronic metal-support interaction can promote the catalytic cycle of Pd ⇆ Pd , 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.