Efficient full-spectrum-light-driven photocatalytic CO2 reduction boosted by synergetic electronic interactions 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–N 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 achieved 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 exhibited excellent stability. This work provides a new strategy for designing high-performance photocatalysts by tuning the electron push–pull effect.