American Chemical Society

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Surface Lattice-Embedded Pt Single-Atom Catalyst on Ceria-Zirconia with Superior Catalytic Performance for Propane Oxidation

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journal contribution
posted on 2023-08-11, 07:03 authored by Wei Tan, Shaohua Xie, Yandi Cai, Haowei Yu, Kailong Ye, Meiyu Wang, Weijian Diao, Lu Ma, Steven N. Ehrlich, Fei Gao, Lin Dong, Fudong Liu
Tuning the metal–support interaction and coordination environment of single-atom catalysts can help achieve satisfactory catalytic performance for targeted reactions. Herein, via the facile control of calcination temperatures for Pt catalysts on pre-stabilized Ce0.9Zr0.1O2 (CZO) support, Pt single atoms (Pt1) with different strengths of Pt–CeO2 interaction and coordination environment were successfully constructed. With the increase in calcination temperature from 350 to 750 °C, a stronger Pt–CeO2 interaction and higher Pt-O-Ce coordination number were achieved due to the reaction between PtOx and surface Ce3+ species as well as the migration of Pt1 into the surface lattice of CZO. The Pt/CZO catalyst calcined at 750 °C (Pt/CZO-750) exhibited a surprisingly higher C3H8 oxidation activity than that calcined at 550 °C (Pt/CZO-550). Through systematic characterizations and reaction mechanism study, it was revealed that the higher concentration of surface Ce3+ species/oxygen vacancies and the stronger Pt–CeO2 interaction on Pt/CZO-750 could better facilitate the activation of oxygen to oxidize C3H8 into reactive carbonate/carboxyl species and further promote the transformation of these intermediates into gaseous CO2. The Pt/CZO-750 catalyst can be a potential candidate for the catalytic removal of hydrocarbons from vehicle exhaust.