Photoinduced Translocation‐Transformation Strategy for Vacancy Re‐Exposure and Synthesis of Stable Single Atoms

Abstract Single‐atom catalysts have attracted considerable attention owing to their unparalleled atomic‐level efficiencies and distinctive structural properties. However, traditional synthesis methods often lead to less‐than‐optimal catalytic performance, as single atoms may occupy and block surface vacancies beneficial for catalytic activity. Achieving single‐atom dispersion while retaining or reactivating vacancies remains challenging. This paper proposes a photoinduced translocation‐transformation strategy using anatase TiO 2 with high concentrations of surface oxygen vacancies as a support. Following N doping, Rh nanoparticles are loaded and subsequently disperse into single atoms through a photoinduced treatment accompanied by N translocation, ultimately restoring the oxygen vacancy concentrations to levels comparable to those of the original TiO 2 . This approach enhances the photocatalytic performance, yielding a hydrogen production rate twofold higher for the single‐atom catalyst Rh(SA)/N‐TiO 2 than for the nanoparticle catalyst Rh(NP)/N‐TiO 2 . This novel method is promising in organic synthesis, CO 2 reduction, and nitrogen fixation applications.