Intensifying the Oxide–Support Electronic Interaction via Zinc Doping to Boost Catalytic N2O Decomposition in the Presence of O2 for Co3O4/CeO2 Catalysts

Mitigating industrial nitrous oxide (N2O) emissions is critical for climate action, yet developing efficient low-temperature N2O decomposition catalysts under O2-containing conditions remains challenging. The weak oxygen–support interaction leads to unsatisfactory N2O decomposition performance in the supported Co3O4/CeO2 catalyst. This study aims to enhance the electronic oxide–support interaction in the Co3O4/CeO2 catalyst through Zn doping, thereby improving its catalytic performance for N2O decomposition under O2-rich conditions. The results demonstrate that, in the presence of 5% O2, the activation energy of the catalyst sharply decreases from 117.5 to 60.4 kJ·mol–1 after Zn doping (Co2.4Zn0.6O4/CeO2). Additionally, the doped catalyst exhibits strong durability to the O2 + H2O + NOx impurity gas components. Advanced spectral characterization and density functional theory calculations reveal that Zn doping modulates the geometry and electronic structure of active cobalt sites, optimizing the adsorption and activation capabilities of N2O molecules. This study elucidates the mechanism of N2O decomposition over the catalysts and establishes a clear structure–activity relationship between the atomic-scale configuration of active sites and their performance. These findings provide critical insights for designing efficient supported oxide catalysts through targeted doping strategies and offer new perspectives for developing highly efficient and low-energy N2O decomposition catalysts.