As a reproducible intermediate for hydrogen (H) and carbon cycling, methanol mixed with water (HO) in a ratio of 1 : 1 can multiply the outcome of green H generation via Photocatalytic reforming of methanol-HO (PRMW). Hitherto, low-energy and mild-condition PRMW remains a serious challenge. Here, the amino acid-derived carbon nitrides (ACN) were synthesized supramolecular precursor strategy for PRMW and achieved excellent performance (H, 35.6 mmol h g; CO, 11.5 mmol h g) under sunlight at 35 °C. It was revealed that the surface-terminating carboxyl groups (-COOH) promote the dark dehydrogenation of methanol on MetCNx to form methoxy (*OCH) and methylol (*CHOH) simultaneously, with the hydroxyl (*OH) generated by photostimulated HO oxidation promotes the C-H activation of formaldehyde, then leads the whole reaction into the formation of CO and three H. The extended light absorption, enhanced charge separation and transport, and efficient surface reaction improve photocatalytic efficiency.
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