Amorphous Aluminum Oxide Clusters Regulating Oxygen Reduction for Photocatalytic H2 O2 Production over Carbon Nitride

The rational design of catalysts for photocatalytic H ₂ O ₂ production remains a major challenge, as most photocatalysts for H ₂ O ₂ production also tend to decompose H ₂ O ₂ . Here, density functional theory (DFT) calculations reveal that amorphous Al ₂ O ₃ clusters anchored on crystalline carbon nitride (CCN) provide efficient oxygen adsorption sites, facilitate electron transfer, and stabilize key *OOH intermediates. Guided by these insights, CCN composites loaded with Al ₂ O ₃ clusters (CCN-Al-x) were synthesized using an ionothermal treatment strategy. Experimental studies confirm that the introduction of Al ₂ O ₃ clusters enhances charge separation, suppresses H ₂ O ₂ decomposition and improves the selectivity of the 2e ⁻ oxygen reduction reaction (ORR). The optimized CCN-Al-2 achieves an H ₂ O ₂ production rate of 50.2 mmol g ^− 1 h ^− 1 , with an apparent quantum yield (AQY) of 21.6% under 420 nm irradiation. This work highlights the critical impact of Al ₂ O ₃ clusters modification on CCN, providing new opportunities for efficient and selective photocatalytic H ₂ O ₂ production.