Efficient visible light driven degradation of sulfamethazine and tetracycline by salicylic acid modified polymeric carbon nitride via charge transfer

Efficient visible light driven degradation of sulfamethazine and tetracycline by salicylic acid modified polymeric carbon nitride via charge transfer
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水杨酸改性聚合氮化碳通过电荷转移有效可见光驱动降解磺胺二甲嘧啶和四环素

DOI:
10.1016/j.cej.2019.03.279
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发表时间:
2019-08
影响因子:
15.1
通讯作者:
Zhou Man
Zhou Man
中科院分区:
工程技术1区
文献类型:
--
作者:
Zhou Chengyun;Huang Danlian;Xu Piao;Zeng Guangming;Huang Jinhui;Shi Tianzhe;Lai Cui;Zhang Chen;Cheng Min;Lu Yue;Duan Abing;Xiong Weiping;Zhou Man

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光催化技术是一种很有前途的去除废水中有机污染物的技术。为此设计了一种改性的氮化碳。本研究探索了一种简单的尿素与水杨酸共聚合成畸变氮化碳的方法。SA的引入导致了结构从平面结构到扭曲卷曲结构的变化。与CN相比,CN-SA显示出宽的光吸收,这归因于氮原子与七嗪单元的孤对电子的n → π* 跃迁。CN-SA的光电极比CN电极具有更高的光电流和更低的充电电阻,表明CN-SA的光生载流子被更有效地分离。因此,最佳CN-SA显示与原始CN相比,四环素(TC)的降解提高了2倍。此外,我们发现,使用CN-SA光催化剂时,磺胺二甲嘧啶(SMZ)的降解速率为0.0823 min− 1,是原始CN(0.0293 min−1)的三倍。此外,CN-SA显示出良好的稳定性,在四个循环后没有结构变化或光催化性能的损失。根据自由基捕获实验和电子自旋共振分析,自由基dotO 2 −和h+是参与有机污染物降解的主要活性物种。该方法为设计可调能带结构的有机半导体材料提供了一种新的途径。
Photocatalysis has been widely studied as a promising technique for removal of organic pollutants in wastewater. A modified carbon nitride has been designed for this purpose. In this study, a facile method to synthesize distorted carbon nitride by simply copolymerizing urea and salicylic acid (SA) has been explored. The incorporation of SA induced the structure change from planar structure to distorted curls structure. Compared to pristine CN, the CN-SA shows wide light absorption, which is attributed to the n → π*transition at the nitrogen atoms with lone pair electrons of heptazine units. The photoelectrode of CN-SA exhibited higher photocurrent and lower charge resistance than that of pristine CN electrode, indicating that the photogenerated charge carriers of CN-SA are more efficiently separated. As a result, the optimal CN-SA shows 2-fold enhancement in degradation of tetracycline (TC) as compared to pristine CN. Furthermore, we found that the degradation rate of sulfamethazine (SMZ) was 0.0823 min−1using the CN-SA photocatalyst, which is three times higher than that of pristine CN (0.0293 min−1). In addition, the CN-SA shows good stability without structural change or loss of photocatalytic performance after four cycles. According to the radical species trapping experiments and electron spin resonance analyses, radical dotO2−and h+were the main active species involved in the degradation of organic pollutants. The developed strategy provides a novel approach to design the tunable band structure of organic semiconductor materials for various applications.
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