Electronic and energy level structural engineering of graphitic carbon nitride nanotubes with B and S co-doping for...

The ideal photocatalyst used for photocatalytic water splitting requires strong light absorption, fast charge separation/transfer ability and abundant active sites. Heteroatom doping offers a promising and rational approach to optimize the photocatalytic activity. However, achieving high photocatalytic performance remains challenging if just relying on single-element doping. Herein, Boron (B) and sulfur (S) dopants are simultaneously introduced into graphitic carbon nitride (g-C₃N₄) nanotubes by supramolecular self-assembly strategy. The developed B and S co-doped g-C₃N₄ nanotubes (B,S-TCN) exhibited an outstanding photocatalytic performance in the conversion of H₂O into H₂ (9.321 mmol g^-1h^-1), and the corresponding external quantum efficiency (EQE) reached 5.3% under the irradiation of λ = 420 nm. It is well evidenced by the closely combined experimental and (density functional theory) DFT calculations: (1) the introduction of B dopants can facilitate H₂O adsorption and drive interatomic electron transfer, leading to efficient water splitting reaction. (2) S dopants can stretch the VB position to promote the oxidation ability of g-C₃N₄, which can accelerate the consumption of holes and thus inhibit the recombination with electrons. (3) the simultaneous introduction of B and S can engineer the electronic and energy level structural of g-C₃N₄ for optimizing interior charge transfer. Finally, the purpose of maximizing photocatalytic performance is achieved.