Highly Efficient Photocatalytic Reduction of CO2 to CO by In Situ Formation of a Hybrid Catalytic System Based on Molecular Iron Quaterpyridine Covalently Linked to Carbon Nitride

Abstract Efficient and selective photocatalytic CO 2 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 CH 3 CN solution containing 1,3‐dimethyl‐2‐phenyl‐2,3‐dihydro‐1 H ‐benzo[d]imidazole (BIH), triethylamine (TEA), Feqpy‐BA (qpy‐BA=4‐([2,2′:6′,2′′:6′′,2′′′‐quaterpyridin]‐4‐yl)benzaldehyde) and C 3 N 4 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 CO 2 , opening a pathway for diverse photocatalysis.