Active Interfacial Perimeter in Pt/CeO₂ Catalysts with Embedding Structure for Water-Tolerant Toluene Combustion

Abstract

Supported Pt catalysts are often subjected to severe deactivation under the conditions of high temperature and water vapor in catalytic oxidation; thus, the superior stability and water-resistant ability of catalysts have great significance for the effective degradation of volatile organic compounds (VOCs). Herein, we constructed a Pt/CeO₂-N catalyst with an active interfacial perimeter, in which Pt species were partially embedded in the defective CeO₂-N support to prevent the sintering. A significant charge transfer between Pt species and ceria in the embedding structure occurred via the Pt-CeO₂ interface, which induced the formation of a Pt⁴⁺-O_v-Ce³⁺ interfacial structure. Experimental research and theoretical calculations demonstrated that the active Pt⁴⁺-O_v-Ce³⁺ interface promoted the activation and migration of lattice oxygen, thus facilitating the participation of oxygen species in toluene oxidation. Consequently, Pt/CeO₂-N showed excellent catalytic performance for toluene degradation. <i>In situ</i> DRIFTS and DFT calculation proved that the Pt⁴⁺-Ov-Ce³⁺ interfacial sites served as the intrinsic active center in the dissociation of H₂O to generate ·OH, which contributed to the formation of benzaldehyde, thus remarkably improving the water-resistant property. This study provided a facile strategy for fabricating the interfacial embedding structure to enhance the catalytic activity and water tolerance for eliminating VOCs in practical application.