Efficient Full-spectrum-Light-Driven Photocatalytic CO2 Reduction Boosted by Synergetic Electronic Interaction in S-Ga Codoped Carbon Nitride

Abstract

To address the energy crisis and global warming, utilizing solar energy for photocatalytic reduction of CO₂ into fuels represents an ideal solution. This study addresses the core issue of low charge separation efficiency in traditional graphitic carbon nitride (g-C₃N₄) photocatalysts by successfully synthesizing sulfur (S) and gallium (Ga) co-doped bundled carbon nitride (SBCN-Ga) using a "solvothermal-copolymerization-impregnation" strategy. Characterization and theoretical calculations reveal that the synergistic effect of S and Ga constructs an efficient donor-acceptor (D-A) structure within the material, inducing a strong electron push-pull effect from "Ga-N sites" to "C-C triazine rings." This significantly promotes the separation and migration of photogenerated charges and broadens the light response range to the near-infrared region. The obtained SBCN-Ga catalyst achieves a high CO yield of up to 638 μmol·g⁻¹·h⁻¹ in the photocatalytic CO₂ reduction reaction, 49 times higher than that of pristine g-C₃N₄ and exhibits excellent stability. This work provides a new strategy for designing high-performance photocatalysts by tuning the electron push-pull effect.