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A covalent-linked C₃N₄-aldehyde-decorated iron quaterpyridine hybrid catalyst was initially developed by in situ Schiff base reaction, achieving high CO generation and selectivity for photocatalytic CO₂ reduction. The enhanced catalytic performance is mainly attributed to the accelerated photoinduced electron transfer and utilization via the formed covalent linkage.

Abstract

Efficient and selective photocatalytic CO₂ reduction was obtained within a hybrid system that is formed in situ via a Schiff base condensation between a molecular iron quaterpyridine complex bearing an aldehyde function and carbon nitride. Irradiation (blue LED) of an CH₃CN solution containing 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH), triethylamine (TEA), Feqpy-BA (qpy-BA=4-([2,2′:6′,2′′:6′′,2′′′-quaterpyridin]-4-yl)benzaldehyde) and C₃N₄ resulted in CO evolution with a turnover number of 2554 and 95 % selectivity. This hybrid catalytic system unlocks covalent linkage of molecular catalysts with semiconductor photosensitizers via Schiff base reaction for high-efficiency photocatalytic reduction of CO₂, opening a pathway for diverse photocatalysis.