Construction of Spatially Adjacent Ni and Co‐Based Spinel Frustrated Lewis Pair Sites for Efficient Catalytic Ozonation

Abstract Frustrated Lewis pairs (FLPs) present new opportunities for the development of highly active spinel materials for the activation of stable molecules. Herein, a Ni and Co‐based spinel with abundant FLPs sites (NiCo 2 O 4 ‐F) is synthesized through morphologic defect engineering and used for efficient catalytic ozonation CH 3 SH elimination. Characterization results reveal that the NiCo 2 O 4 ‐F with nanoflower structure exposes more surface oxygen vacancies (Ov), inducing local charge redistribution and forming active regions. Ov acts as Lewis basic sites, while the unsaturated coordinated Ni atoms (Ni uc ) act as Lewis acidic sites, and spatially ≈4.08 Å. The Ov···Ni uc FLPs function as “electron shuttles” in the reaction, facilitating specific adsorption of reactants via the dual acidic–basic reaction sites, thereby activating O 3 to generate ·O 2 − and 1 O 2 species to achieve deep oxidation of CH 3 SH. The resulting NiCo 2 O 4 ‐F catalyst exhibits an outstanding CH 3 SH removal efficiency of 94.4%, achieving a high mass activity (5.6 ppm mg −1 ), which is 70 times greater than that of commercial MnO 2 (0.08 ppm mg −1 ). This work presents a promising approach to developing sophisticated ozone catalysts by controllable construction of acid–base sites on spinel surface, enhancing the understanding of the role of FLPs structure in molecular activation.