Photocatalytic Hydrogen Production Coupled with Selective Benzylamine Oxidation over MOF Composites

Photocatalytic water splitting requires separation of the mixed H 2 and O 2 products and is often hampered by the sluggish O 2 ‐producing half reaction. An approach is now reported to address these issues by coupling the H 2 ‐producing half reaction with value‐added benzylamine oxidation reaction using metal–organic framework (MOF) composites. Upon MOF photoexcitation, the electrons rapidly reduce the protons to generate H 2 and the holes promote considerable benzylamine oxidation to N‐benzylbenzaldimine with high selectivity. Further experimental characterizations and theoretical calculation reveal that the highly conjugated s‐triazine strut in the MOF structure is crucial to the efficient charge separation and excellent photocatalytic activity.