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无金属二维/二维共价三嗪骨架/石墨相氮化碳异质结,具有增强的界面电荷分离,用于高效光催化消除抗生素污染物。

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.

机构信息

Key Laboratory of Jiangsu Province for Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.

Institute of Chemistry, Henan Academy of Sciences, Zhengzhou 450002, China.

出版信息

J Hazard Mater. 2020 Jun 5;391:122204. doi: 10.1016/j.jhazmat.2020.122204. Epub 2020 Jan 30.

Abstract

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. O 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.

摘要

通过静电自组装法,成功地获得了基于共价三嗪框架/石墨相氮化碳纳米片(CTFNS/CNNS)的二维/二维异质结新型聚合物光催化剂,该方法使用胺功能化的 CNNS 和富含羧基的 CTFNS。CNNS 和 CTFNS 之间如此大的接触表面和适当的界面接触在载流子的转移和分离中起着关键作用。在模拟太阳光的照射下,所得的 CTFNS/CNNS 异质结表现出显著增强的光催化活性,可在 180 分钟内分解 10 ppm 的磺胺甲恶唑(SMT),降解效率高达 95.8%。由于生成了更多的自由基物种,氯离子可以极大地促进 SMT 的光催化降解。O 是 CTFNS/CNNS 异质结上 SMT 分解的主要活性物质。此外,使用高效液相色谱-质谱联用仪鉴定了 SMT 的降解中间产物,并提出了降解途径。本研究为使用碳基纳米材料设计二维/二维异质结提供了新的思路,在废水中磺胺类抗生素的降解方面表现出巨大的潜力。

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