Citation: Yue Liu, Long Chen, Xiaona Liu, Tianwei Qian, Meng Yao, Wen Liu, Haodong Ji. Tuning band structure of graphitic carbon nitride for efficient degradation of sulfamethazine: Atmospheric condition and theoretical calculation[J]. Chinese Chemical Letters, ;2022, 33(3): 1385-1389. doi: 10.1016/j.cclet.2021.08.061 shu

Tuning band structure of graphitic carbon nitride for efficient degradation of sulfamethazine: Atmospheric condition and theoretical calculation

Yue Liu ^a ,
Long Chen ^b ,
Xiaona Liu ^a ,
Tianwei Qian ^a ,
Meng Yao ^a ,
Wen Liu ^{b, c} ,
Haodong Ji ^{b, c, *,}

a.
College of Environmental Science and Engineering, Taiyuan University of Technology, Jinzhong 030600, China
b.
The Key Laboratory of Water and Sediment Science, Ministry of Education; College of Environment Science and Engineering, Peking University, Beijing 100871, China
c.
State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems, Peking University, Beijing 100871, China

jihaodong@pku.edu.cn

Received Date: 17 June 2021
Revised Date: 12 July 2021
Accepted Date: 9 August 2021
Available Online: 17 August 2021

Figures(5)

Numerous approaches have been used to modify graphitic carbon nitride (g-C₃N₄) for improving its photocatalytic activity. In this study, we demonstrated a facial post-calcination method for modified graphitic carbon nitride (g-C₃N₄-Ar/Air) to direct tuning band structure, i.e., bandgap and positions of conduction band (CB)/valence band (VB), through the control of atmospheric condition without involving any additional elements or metals or semiconductors. The synthesized g-C₃N₄-Ar/Air could efficiently degrade sulfamethazine (SMT) under simulated solar light, i.e., 99.0% removal of SMT with rate constant k₁ = 2.696 h⁻¹ within 1.5 h (4.9 times than pristine g-C₃N₄). Material characterizations indicated that the damaged/partial-collapsed structure and decreased nanosheet-interlayer distance for g-C₃N₄-Ar/Air resulted in the shift of band structure due to the denser stacking of pristine g-C₃N₄ through oxidative exfoliation and planarization by air calcination. In addition, the bandgap of g-C₃N₄-Ar/Air was slightly shrunk from 2.82 eV (pristine g-C₃N₄) to 2.79 eV, and the CB was significantly upshifted from −0.44 eV (pristine g-C₃N₄) to −0.81 eV, suggesting the powerful ability for donating the electrons for O₂ to form ^•O₂⁻. Fukui index (f ^–) based on theoretical calculation indicated that the sites of SMT molecule with high values, i.e., N9, C4 and C6, preferred to be attacked by ^•O₂⁻ and ^•OH, which is confirmed by the intermediates' analysis. The tuning method for graphitic carbon nitride provides a simple approach to regulate the charge carrier lifetime then facilitate the utilization efficiency of solar light, which exhibits great potential in efficient removal of emerging organic contaminants from wastewater.
- Graphitic carbon nitride,
- Pharmaceuticals,
- Photocatalysis,
- Atmospheric condition,
- DFT calculation
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