One-step synthesis of S-doped C-vacancy g-C3N4 with honeycomb porous nanosheets structure for efficient visible-light-driven hydrogen evolution

Abstract

A defective construction method was applied to design the molecular framework from the source and use the intermolecular forces of the raw materials to connect the long chains. The S-doped honeycomb g-C3N4 nanosheets were prepared by selective volatilization at elevated temperatures using melamine-tricyanuric acid-thiourea supramolecular liquid as precursor and template. In addition to significantly increasing the high surface area, the S-doped honeycomb g-C3N4 nanosheets also modify the band gap structure and shape. The introduction of the C defect also increased the number of reaction sites, improved visible light responsiveness, broadened the photoresponse range, and accelerated the segregated transfer of photogenerated carriers. The experimental results showed that the hydrogen production efficiency of S-PDCN-3 (The best sample of S-doped C-vacancy g-C3N4) is 23.78 mmol‧g−1‧h−1, which was 21.8 times that of BCN, namely Bulk g-C3N4 (1.1 mmol‧g−1‧h−1). After adding the photosensitizer (Erythrosin B) to the photocatalytic reaction system, EB + S-PDCN-3 (the best sample of S-doped honeycomb g-C3N4 nanosheets with the sensitizer) precipitated hydrogen up to 63.8 mmol‧g−1‧h−1, which was 17.78 times greater than the hydrogen production of the EB + BCN sample (3.59 mmol‧g−1‧h−1). Furthermore, the sample was observed to experience a reduction in band gap energy, an increase in electron density near VB and a reduction of H* adsorption–desorption barrier, all of which are essential for the enhancement of the hydrogen evolution reaction. Successful preparation of S-doped honeycomb g-C3N4 nanosheets provides a simple and efficient method for developing efficient g-C3N4 photocatalysts—potential applications in the development process of hydrogen energy and pollutant degradation.