期刊
JOURNAL OF HAZARDOUS MATERIALS
卷 386, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.jhazmat.2019.121947
关键词
Polymeric carbon nitride; 2,5-dibromopyrazine; Carrier channel; Photocatalytic H-2 evolution; Sulfamethazine degradation
资金
- Program for the National Natural Science Foundation of China [81773333, 51879101, 51809090, 51579098, 51779090, 51709101, 51709100, 51278176, 51521006, 51378190]
- National Program for Support of Top-Notch Young Professionals of China (2014)
- Hunan Provincial Science and Technology Plan Project [2016RS3026, 2017SK2243, 2018SK20410]
- Program for New Century Excellent Talents in University [NCET-13-0186]
- Fundamental Research Funds for the Central Universities [531109200027, 531107051080, 531107050978, 531107051205]
- Shanghai Tongji Gao Tingyao Environmental Science and Technology Development Foundation
- Program for Changjiang Scholars and Innovative Research Team in University [IRT-13R17]
Polymeric carbon nitride (PCN) has become the most promising metal-free photocatalysts but its activity is low. Molecule doping of PCN has been proved to be an effective strategy to achieve high photocatalytic performance. Herein, we report a bottom-up method to synthesize modified PCN, which includes 2,5-dibromopyrazine doping, thermal-induced exfoliation and condensation/polymerization. The incorporation of electron-deficiency 2,5-dibromopyrazine into the PCN framework can effectively tune the electronic structures and improve the charge-carrier separation. In addition, the incorporation of 2,5-dibromopyrazine induced significant structural changes from planar symmetric to distortion. The optimized pyrazine doped PCN showed a reaction rate enhancement of 4-fold for the degradation of sulfamethazine compared to that of conventional urea-based PCN. Further reactive species and degradation intermediate detection studies, indicated that O-center dot(2)- was generated during the photocatalytic process, which could lead to the decomposition, and finally mineralization of sulfamethazine. 2,5-Dibromopyrazine doped PCN also leads to a 6.3-fold improvement in H-2 generation with the visible light. Especially, phytotoxicity experiments showed that the toxicity of sulfamethazine after degradation is greatly reduced, and the as-prepared photocatalyst is environmentally friendly.
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