Wang, HaitaoHaitaoWangJiang, JizhouJizhouJiangYu, LianglangLianglangYuPeng, JiaheJiahePengSong, ZhouZhouSongXiong, ZhiguoZhiguoXiongLi, NengNengLiXiang, KunKunXiangZou, JingJingZouJYH-PING HSUZhai, TianyouTianyouZhai2023-06-092023-06-092023-01-0116136810https://scholars.lib.ntu.edu.tw/handle/123456789/632025Although challenges remain, synergistic adjusting various microstructures and photo/electrochemical parameters of graphitic carbon nitride (g-C3N4) 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-C3N4 (S-g-C3N4-D) is designed elaborately. Subsequent physical and chemical characterization proved that the developed S-g-C3N4-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 (ΔGH*) for S-g-C3N4-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-C3N4-D catalyst shows a high H2 evolution rate of 5651.5 µmol g−1 h−1. Both DFT calculations and experimental results reveal that a memorable defective g-C3N4/S-doped g-C3N4 step-scheme heterojunction is constructed between S-doped domains and N-defective domains in the structural configuration of S-g-C3N4-D. This work exhibits a significant guidance for the design and fabrication of high-efficiency photocatalysts.eng-C N 3 4 | N-defects | photocatalytic H evolution 2 | S-doping | theoretical analysis[SDGs]SDG7journal article10.1002/smll.202301116371913262-s2.0-85159327181WOS:000987156000001https://api.elsevier.com/content/abstract/scopus_id/85159327181