Photocatalytic hydrogen peroxide (HO) production encounters a major impediment in its low solar-to-chemical conversion (SCC) efficiency due to undesired HO product decomposition. Herein, an isolated nickel (Ni) atom modification strategy is developed to adjust the thermodynamic process of HO production to address the challenge. Sacrificial experiments and in situ characterization reveal that HO generation occurs via a highly selective indirect two-electron oxygen reduction reaction. The optimized photocatalyst exhibits a remarkable HO production rate of 338.9 μmol g h in pure water, representing a 48-fold enhancement. Notably, it attains an impressive SCC efficiency of 1.05%, surpassing that of current state-of-the-art catalysts. Theoretical insights reveal the downshifted d-band center facilitates moderate O adsorption and barrier-free *OOH conversion, favoring HO release and preventing *HO decomposition. This work showcases efficient HO photosynthesis via d-band manipulation, presenting a fresh perspective for advancing high-efficiency SCC systems.
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