Lattice Oxygen Activation Through Redox-Induced δ-MnO₂/Co_3-xMn_xO₄ Interfaces for Enhanced N₂O Decomposition

N₂O decomposition over spinel catalysts suffers from a spin-forbidden oxygen recombination step, resulting in substantial kinetic barriers of O₂ formation. Herein, we present a redox-induced interfacial engineering strategy to activate lattice oxygen in spinel oxides, thereby effectively overcoming the kinetic constraints associated with oxygen recombination. In a Co₃O₄-based model system, controlled permanganate etching partially substitutes Mn into octahedral Co³⁺ sites, while simultaneously generating heterointerfaces. The enhanced hybridization between Co 3d and O 2p orbitals and high Co-O-Mn covalency induced by the interface between δ-MnO₂ and Co_3-xMn_xO₄, lead to the formation of highly active lattice oxygen species adjacent to the interface. ¹⁸O isotope labeling experiment further confirms a dominant lattice-oxygen-mediated Mars-van Krevelen mechanism for N₂O decomposition, whereas pristine Co₃O₄ predominantly follows the Langmuir-Hinshelwood mechanism. Therefore, the optimized catalyst exhibits enhanced N₂O decomposition activities, maintaining stability under impurity-rich conditions. This work offers a promising approach for the rational design of efficient catalysts for N₂O abatement and provides mechanistic insights into redox-induced lattice oxygen activation.