Exsolution of Iron Oxide on LaFeO₃ Perovskite: A Robust Heterostructured Support for Constructing Self-Adjustable Pt-Based Room-Temperature CO Oxidation Catalysts

Constructing highly active and stable surface sites for O2 activation is essential to lower the barrier of Pt-based catalysts for CO oxidation. Although a few active Pt–metal oxide interfaces have been reported, questions about the stability of these sites under the long-term storage and operation remain unresolved. Here, based on developing a robust FeOx/LaFeO3 heterostructure as a support, we constructed stable Pt–support interfaces to achieve highly active CO oxidation at room temperature. Even after it is kept in the air for more than 6 months, the catalyst (without pretreatment) still maintains the high activity like a fresh one, which is superior to metal hydroxide–Pt interfaces, and meets the requirements of long-term storage for emergency use. In situ characterizations and systematic reaction results showed that CO oxidation occurs through an alternative mechanism, which is triggered by intrinsic reactants and self-adjusted to a more active interface in the reaction process. Theoretical calculations and 57Fe Mössbauer spectra revealed that abundant cation vacancies significantly increase the activity of surface oxygen species and should be responsible for this unique process. This work demonstrates an alternative concept to fabricate robust and highly active Pt-based catalysts for catalytic oxidation.