光催化
石墨氮化碳
氮化碳
材料科学
吸收(声学)
光化学
氮化物
电子结构
兴奋剂
氢
半导体
载流子
碳纤维
可见光谱
纳米技术
光电子学
化学
催化作用
计算化学
有机化学
复合材料
复合数
图层(电子)
作者
Yongkang Quan,Ruidong Li,Xingzhou Li,Rongxing Chen,Yun Hau Ng,Jianying Huang,Jun Hu,Yuekun Lai
出处
期刊:Small
[Wiley]
日期:2024-10-03
标识
DOI:10.1002/smll.202406576
摘要
Abstract Graphitic carbon nitride (gC 3 N 4 ) is an attractive photocatalyst for solar energy conversion due to its unique electronic structure and chemical stability. However, gC 3 N 4 generally suffers from insufficient light absorption and rapid compounding of photogenerated charges. The introduction of defects and atomic doping can optimize the electronic structure of gC 3 N 4 and improve the light absorption and carrier separation efficiency. Herein, the high efficiency of carbon nitride photocatalysis for hydrogen evolution in visible light is achieved by an S‐modified double‐deficient site strategy. Defect engineering forms abundant unsaturated sites and cyano (─C≡N), which promotes strong interlayer C─N bonding interactions and accelerates charge transport in gC 3 N 4 . S doping tunes the electronic structure of the semiconductors, and the formation of C─S─C bonds optimizes the electron‐transfer paths of the C─N bonding, which enhances the absorption of visible light. Meanwhile,C≡N acts as an electron trap to capture photoexcited electrons, providing the active site for the reduction of H + to hydrogen. The photocatalytic hydrogen evolution efficiency of SDCN (1613.5 µmol g −1 h −1 ) is 31.5 times higher than that of pristine MCN (51.2 µmol g −1 h −1 ). The charge separation situation and charge transfer mechanism of the photocatalysts are investigated in detail by a combination of experimental and theoretical calculations.
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