1. Molecular-level insights on NIR-driven photocatalytic H2 generation with ultrathin porous S-doped g-C3N4 nanosheets.
- Author
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Wu, Xiaojie, Li, Di, Luo, Bifu, Chen, Biyi, Huang, Yuanyong, Yu, Tingting, Shen, Nanjun, Li, Longhua, and Shi, Weidong
- Subjects
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DOPING agents (Chemistry) , *NANOSTRUCTURED materials , *BAND gaps , *ENERGY conversion , *PHOTOCATALYSTS , *NITRIDES , *INTERSTITIAL hydrogen generation - Abstract
Unraveling how mid-gap state energy level of graphitic carbon nitride (g-C 3 N 4) promote near-infrared (NIR) driven photochemical energy conversion at the molecular level remains a grand challenge. Here, we report a series of S double-site-doped ultrathin g-C 3 N 4 nanosheets (SUCN) with adjustable intermediate band gap benefits from light response over NIR region. The SUCN produced after optimizing S double-site doping can effectively generate hydrogen (H 2) under NIR-light irradiation. The highest H 2 generation rate achieved was respectively 9.35 and 17.46 μmol g−1 h−1 under λ = 765 and λ > 800 nm, which is firstly expended photocatalytic activity of S-doped g-C 3 N 4 to NIR region beyond λ > 765 nm. We proposed a molecular-level method, i.e., the localized oxidation state of proton acceptor triethanolamine (TEOA) in the mid-gap state to ensure the NIR-driven H 2 generating behavior. [Display omitted] • g-C 3 N 4 was doped with S atoms at a specific site of the triazine skeleton. • S doping provides an adjustable intermediate band gap of g-C 3 N 4. • The 0.36-SUCN obtained 43 times higher PHE than g-C 3 N 4. • The S-doped g-C 3 N 4 firstly realized PHE in the near-infrared region. • The NIR-driven H 2 generation was firstly demonstrated by a molecular-level method. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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