Oxide Interface-Stabilized Superoxo Species for High-Temperature Catalysis

作者：Zhongsen Wang, Fanyu Wang, Jiamin Zheng, Liu Yi, Jintong Lan, Zewei Wu, Jun Wang, Fangfang Pan, Xiao Liu, Rentao Mu · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c08963 · 被引用次数：20 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Catalysis and Hydrodesulfurization Studies

High-temperature oxidation reactions catalyzed by earth–abundant transition metal oxides are vital for numerous industrial and environmental processes. However, their performance is often limited by the rapid desorption of active oxygen species at high temperatures. Here, we describe a straightforward approach to constructing a CuMn spinel/Mn 2 O 3 composite oxide catalyst that addresses this limitation and demonstrate that lattice oxygen can spontaneously migrate to form interface-stabilized superoxo species under high-temperature reaction conditions. This catalyst exhibits a 14-fold enhancement in the CH 4 oxidation reaction compared to Mn 2 O 3, with activity and stability even better than those of many reported noble-metal supported catalysts. In situ characterizations and theoretical calculations reveal that the superoxo species accept electrons from the neighboring Cu and Mn atoms, exhibiting enhanced ability for C–H activation. This work illustrates the critical role of interface-stabilized superoxo species in CH 4 oxidation and establishes a promising route for promoting high-temperature catalytic processes through interface engineering.