Metal-free 2D/2D heterojunction of covalent triazine-based frameworks/graphitic carbon nitride with enhanced interfacial charge separation for highly efficient photocatalytic elimination of antibiotic pollutants

Metal-free 2D/2D heterojunction of covalent triazine-based frameworks/graphitic carbon nitride with enhanced interfacial charge separation for highly efficient photocatalytic elimination of antibiotic pollutants
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共价三嗪基框架/石墨碳氮化物的无金属二维/二维异质结,具有增强的界面电荷分离,可高效光催化消除抗生素污染物

DOI:
10.1016/j.jhazmat.2020.122204
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发表时间:
2020
影响因子:
13.6
通讯作者:
Jiang Fang
Jiang Fang
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Cao Shihai;Zhang Yu;He Nannan;Wang Jing;Chen Huan;Jiang Fang

文献摘要

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采用静电自组装方法,将胺基碳氮纳米管(CNNS)和羧基碳氮纳米管(CTFNS)分别组装在一起,成功制备了一种新型的聚合物基2D/2D异质结光催化剂--三嗪基共价骨架/石墨碳氮纳米片(CTFNS/CNNS)异质结。CNNS和CTFNS之间的这种大的接触表面和适当的界面接触在电荷载流子的转移和分离中起着关键作用。在模拟太阳光照射下,CTFNS/CNNS异质结对10 ppm磺胺二甲嘧啶(SMT)的光催化降解效率可达95.8%。在CTFNS/CNNS异质结上,由于氯离子产生更多的自由基物种,从而极大地促进了SMT的光催化降解,自由基dotO 2 −是SMT降解的主要活性物种。采用高效液相色谱-质谱联用仪对SMT的降解中间体进行了鉴定,并提出了SMT的降解途径。该研究为利用碳基纳米材料设计2D/2D异质结提供了新的见解,该异质结在废水中磺胺类抗生素的降解方面具有巨大的潜力。
A novel polymer-based 2D/2D heterojunction photocatalysts of covalent triazine-based frameworks/graphitic carbon nitride nanosheets (CTFNS/CNNS) heterojunction are successfully obtained by an electrostatic self-assembly method using amine-functionalized CNNS and carboxyl-rich CTFNS. Such large contact surface and appropriate interfacial contact between CNNS and CTFNS plays a critical role in transfer and separation of charge-carriers. The resulting CTFNS/CNNS heterojunction showed significantly enhanced photocatalytic activity under the irradiation of simulated solar light, which could decompose 10 ppm sulfamethazine (SMT) within 180 min with a high degradation efficiency of 95.8 %. Chloride ions can greatly promote the photocatalytic degradation of SMT due to the production of more radical species.radical dotO2−is the dominant active species for SMT decomposition over CTFNS/CNNS heterojunction. Moreover, the degradation intermediates of SMT were identified using high performance liquid chromatography-mass spectrometer and the degradation pathway was proposed. This study provides a new insight into the design of 2D/2D heterojunctions using carbon-based nanomaterials, which exhibits great potential in the degradation of sulfonamide antibiotics in wastewaters.