Strong Oxide‐Support Interaction Induced Thermal Stabilization of Pt Single Atoms for Durable Catalytic CO Oxidation

Abstract Supported metal nanoparticle catalysts often suffer from sintering‐induced size‐dependent deactivation, limiting their high‐temperature applications. Although high‐temperature redispersion offers a potential solution, this strategy remains restricted to reducible support materials, severely limiting the selection of catalyst supports with versatile compositions and tunable functionalities. Here, we engineer cationic vacancies at Al 2 O 3 ‐La 2 O 3 interface via strong oxide‐support interaction (SOSI)—driven interfacial reconstruction during calcination. The vacancy‐mediated confinement effect dynamically intercepts migrating Pt species, enabling the construction of Al 2 O 3 ‐Pt 1 ‐La 2 O 3 structure with precisely defined coordination environments. The resulting catalyst achieves complete CO conversion at 145 °C and maintains stability with minimal decline after a 6‐h treatment at 1100 °C in air with 10% steam. This interfacial engineering strategy proves universal, as demonstrated by ZrO 2 ‐La 2 O 3 counterparts. Our findings break the reducibility dependency in traditional single‐atom catalysts (SACs) stabilization by establishing oxide–oxide interface as universal anchoring platforms, which expands the design space of industrial‐grade SACs beyond conventional reducible oxides.