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具有增强可见光光催化活性用于降解甲氧苄啶的Ag-AgCl/WO/g-CN光催化剂中的双光电子转移机制

Double photoelectron-transfer mechanism in Ag-AgCl/WO/g-CN photocatalyst with enhanced visible-light photocatalytic activity for trimethoprim degradation.

作者信息

Fan Gongduan, Ning Rongsheng, Yan Zhongsen, Luo Jing, Du Banghao, Zhan Jiajun, Liu Lingshan, Zhang Jin

机构信息

College of Civil Engineering, Fuzhou University, 350116 Fujian, China; State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350002 Fujian, China; Fujian Provincial Key Laboratory of Electrochemical Energy Storage Materials, Fuzhou University, 350002 Fujian, China.

College of Civil Engineering, Fuzhou University, 350116 Fujian, China.

出版信息

J Hazard Mater. 2021 Feb 5;403:123964. doi: 10.1016/j.jhazmat.2020.123964. Epub 2020 Sep 14.

Abstract

Antibiotic contamination is increasing scrutinized recently. In this work, the Ag-AgCl/WO/g-CN (AWC) nanocomposites were successfully synthesized using a two-step process involving electrostatic self-assembly and in-situ deposition for trimethoprim (TMP) degradation. The as-prepared photocatalysts were investigated and characterized by XRD, FTIR, XPS, TGA, SEM, TEM, UV-vis, PL and EIS. The experimental results indicated that 99.9% of TMP (4 mg/L) was degraded within 60 min when the concentration of AWC was 0.5 g/L. Reactive species scavenging experiments and electron spin resonance (ESR) experiments illustrated that superoxide radical (•O) and photogenerated holes (h) were the main active species. The functional theory calculation and identification of intermediates via HPLC-MS revealed the possible degradation pathways of TMP. A double photoelectron-transfer mechanism in AWC photocatalyst was proposed. Five cycling photocatalytic tests and reactions under different solution matrix effects further supported that the AWC was a promising photocatalyst for the removal of TMP from the aquatic environment.

摘要

抗生素污染近来受到越来越多的审视。在这项工作中,通过涉及静电自组装和原位沉积的两步法成功合成了Ag-AgCl/WO/g-CN(AWC)纳米复合材料用于甲氧苄啶(TMP)的降解。通过XRD、FTIR、XPS、TGA、SEM、TEM、UV-vis、PL和EIS对所制备的光催化剂进行了研究和表征。实验结果表明,当AWC浓度为0.5 g/L时,4 mg/L的TMP在60分钟内99.9%被降解。活性物种清除实验和电子自旋共振(ESR)实验表明,超氧自由基(•O)和光生空穴(h)是主要的活性物种。通过HPLC-MS进行的功能理论计算和中间体鉴定揭示了TMP可能的降解途径。提出了AWC光催化剂中的双光电子转移机制。五次循环光催化测试以及在不同溶液基质效应下的反应进一步证明,AWC是一种从水环境中去除TMP的有前景的光催化剂。

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