LAUSR

Ir-based materials are still the benchmark catalysts for various reactions in acidic environment, but the high loading and low atom utilization limit their large-scale deployment. Herein, we report an effective strategy for implanting fully dispersed iridium-oxide atomic clusters onto hematite for boosting photoelectrochemical water oxidation in acidic solution. The resulting photoanode achieves a record-high photocurrent of 1.35 mA cm-2 at 1.23 V, corresponding to a mass activity of 172.70 A g-1 (3 times higher than electrodeposited control sample) and demonstrating the merits from the high atomic utilization of Ir. The systematically experimental and theoretical results reveal that the performance improvement correlates with the modulated electronic structure including the adjusted Fermi level and d-band center, which significantly enhances charge separation efficiency and promotes the conversion from intermediate *O into *OOH.