Tailoring a sulfur doped carbon nitride skeleton to enhance the photocatalytic hydrogen evolution activity

Abstract

Although graphite phase carbon nitride (CN) photocatalysts possess great potential in solving the global energy crisis, their photocatalytic activity is severely affected by sluggish charge dissociation/migration efficiency, a high carrier recombination rate, low active site exposure, and limited visible-light harvesting. Herein, a sulfur doped CN (x-DZCN) was tailored via one-step thermally-induced polymerization of urea with dithizone, which could evolve hydrogen at a rate of 1930 μmol g⁻¹ h⁻¹ (7.1 times higher than that of a single CN). The characterization of the catalyst confirmed that the boosted photocatalytic activity originated from the improved specific surface area from 46 to 61 m² g⁻¹, broadened visible light harvesting from 470 nm to over 600 nm, more negative conduction band (shift up of 0.54 eV), and promoted charge behavior (improved exciton dissociation and carrier migration efficiency, as well as suppressed carrier recombination capacity). The stable and efficient photocatalytic hydrogen evolution performance verifies the feasibility and potential of this photocatalyst in clean energy production.