Tailoring Advanced N‐Defective and S‐Doped g‐C<sub>3</sub>N<sub>4</sub> for Photocatalytic H<sub>2</sub> Evolution
Haitao Wang, Jizhou Jiang, Lianglang Yu, Jiahe Peng, Zhou Song, Zhiguo Xiong, Neng Li, Kun Xiang, Jing Zou, Jyh‐Ping Hsu, Tianyou Zhai
Abstract
Abstract Although challenges remain, synergistic adjusting various microstructures and photo/electrochemical parameters of graphitic carbon nitride (g‐C 3 N 4 ) in photocatalytic hydrogen evolution reaction (HER) are the keys to alleviating the energy crisis and environmental pollution. In this work, a novel nitrogen‐defective and sulfur‐doped g‐C 3 N 4 (S‐g‐C 3 N 4 ‐D) is designed elaborately. Subsequent physical and chemical characterization proved that the developed S‐g‐C 3 N 4 ‐D not only displays well‐defined 2D lamellar morphology with a large porosity and a high specific surface area but also has an efficient light utilization and carriers‐separation and transfer. Moreover, the calculated optimal Gibbs free energy of adsorbed hydrogen (ΔG H* ) for S‐g‐C 3 N 4 ‐D at the S active sites is close to zero (≈0.24 eV) on the basis of first‐principle density functional theory (DFT). Accordingly, the developed S‐g‐C 3 N 4 ‐D catalyst shows a high H 2 evolution rate of 5651.5 µmol g −1 h −1 . Both DFT calculations and experimental results reveal that a memorable defective g‐C 3 N 4 /S‐doped g‐C 3 N 4 step‐scheme heterojunction is constructed between S‐doped domains and N‐defective domains in the structural configuration of S‐g‐C 3 N 4 ‐D. This work exhibits a significant guidance for the design and fabrication of high‐efficiency photocatalysts.