The development of stable, highly active, and inexpensive catalysts for the ozone catalytic oxidation of volatile organic compounds (VOCs) is challenging but of great significance. Herein, the micro-coordination environment of Al in commercial Y zeolite was regulated by a specific dealumination method and then the dealuminated Y zeolite was used as the support of Cu–Mn oxides. The optimized catalyst Cu–Mn/DY exhibited excellent performance with around 95% of toluene removal at 30 °C. Besides, the catalyst delivered satisfactory stability in both high-humidity conditions and long-term reactions, which is attributed to more active oxygen vacancies and acidic sites, especially the strong Lewis acid sites newly formed in the catalyst. The decrease in the electron cloud density around aluminum species enhanced electron transfer at the interface between Cu–Mn oxides. Moreover, extra-framework octahedrally coordinated Al in the support promoted the electronic metal–support interaction (EMSI). Compared with single Mn catalysts, the incorporation of the Cu component changed the degradation pathway of toluene. Benzoic acid, as the intermediate of toluene oxidation, can directly ring-open on Cu-doped catalysts rather than being further oxidized to other byproducts, which increased the rate of the catalytic reaction. This work provides a new insight and theoretical guidance into the rational design of efficient catalysts for the catalytic ozonation of VOCs.

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