Intensifying the Oxide–Support Electronic Interaction via Zinc Doping to Boost Catalytic N <sub>2</sub> O Decomposition in the Presence of O <sub>2</sub> for Co <sub>3</sub> O <sub>4</sub> /CeO <sub>2</sub> Catalysts
Hao Liu, Siqing Cheng, Jianjun Chen, Xiaoping Chen, Shangchao Xiong, Fang Huang, Houfeng Liu, Junhua Li, Chuanzhi Sun
Abstract
Mitigating industrial nitrous oxide (N 2 O) emissions is critical for climate action, yet developing efficient low-temperature N 2 O decomposition catalysts under O 2 -containing conditions remains challenging. The weak oxygen–support interaction leads to unsatisfactory N 2 O decomposition performance in the supported Co 3 O 4 /CeO 2 catalyst. This study aims to enhance the electronic oxide–support interaction in the Co 3 O 4 /CeO 2 catalyst through Zn doping, thereby improving its catalytic performance for N 2 O decomposition under O 2 -rich conditions. The results demonstrate that, in the presence of 5% O 2, the activation energy of the catalyst sharply decreases from 117.5 to 60.4 kJ·mol –1 after Zn doping (Co 2.4 Zn 0.6 O 4 /CeO 2 ). Additionally, the doped catalyst exhibits strong durability to the O 2 + H 2 O + NO x 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 N 2 O molecules. This study elucidates the mechanism of N 2 O 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 N 2 O decomposition catalysts.