Mesoporous Polymeric Cyanamide-Triazole-Heptazine Photocatalysts for Highly-Efficient Water Splitting

Conjugated polymers are promising light harvesters for water reduction/oxidation due to their simple synthesis and adjustable bandgap. Herein, both cyanamide and triazole functional groups are first incorporated into a heptazine-based carbon nitride (CN) polymer, resulting in a mesoporous conjugated cyanamide-triazole-heptazine polymer (CTHP) with different compositions by increasing the quantity of cyanamide/triazole units in the CN backbone. Varying the compositions of CTHP modulates its electronic structures, mesoporous morphologies, and redox energies, resulting in a significantly improved photocatalytic performance for both H(2)and O(2)evolution under visible light irradiation. A remarkable H(2)evolution rate of 12723 mu mol h(-1)g(-1)is observed, resulting in a high apparent quantum yield of 11.97% at 400 nm. In parallel, the optimized photocatalyst also exhibits an O(2)evolution rate of 221 mu mol h(-1) g(-1), 9.6 times higher than the CN counterpart, with the value being the highest among the reported CN-based bifunctional photocatalysts. This work provides an efficient molecular engineering approach for the rational design of functional polymeric photocatalysts.