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NiCoO修饰的膨胀石墨活化过一硫酸盐高效降解磺胺甲恶唑:表征、机理及降解中间体

Efficient degradation of sulfamethoxazole by NiCoO modified expanded graphite activated peroxymonosulfate: Characterization, mechanism and degradation intermediates.

作者信息

Xu Mengjuan, Zhou Hongyu, Wu Zelin, Li Naiwen, Xiong Zhaokun, Yao Gang, Lai Bo

机构信息

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; College of Hydraulic and Hydroelectric Engineering, Sichuan University, Chengdu 610065, China.

出版信息

J Hazard Mater. 2020 Nov 15;399:123103. doi: 10.1016/j.jhazmat.2020.123103. Epub 2020 Jun 5.

DOI:10.1016/j.jhazmat.2020.123103
PMID:32937720
Abstract

Expanded graphite (EG) immobilized nickel ferrite (NiCoO) was successfully constructed by a simple hydrothermal approach and applied for the degradation of sulfamethoxazole (SMX) in model wastewater by peroxymonosulfate (PMS) activation. The features of prepared catalysts were characterized by SEM, TEM, EDS, XRD, BET, TPD and XPS techniques. The influences of several critical parameters including the prepared NiCoO-EG dosages, PMS concentrations, temperature, initial solution pH and inorganic ions on SMX removal were studied in details. In particular, the synthesized NiCoO-EG exhibits excellent catalytic performances for SMX depredation over a wide pH range (pH 3.0-11.0). Besides, the transformation of various reactive oxygen species (SO, HO, O and O) with the change of initial pH was investigated by the electron paramagnetic resonance (EPR) and quenching tests. In addition, twelve major degradation intermediates of SMX were detected by UPLC-QTOF-MS/MS. Finally, the PMS activation mechanism in NiCoO-EG/PMS system by the synergistic coupling of EG and NiCoO were put forward. In brief, this work provided a promising and potential catalyst for PMS activation to remove SMX from wastewater.

摘要

通过一种简单的水热法成功构建了膨胀石墨(EG)负载的镍铁氧体(NiCoO),并将其应用于通过过一硫酸盐(PMS)活化降解模拟废水中的磺胺甲恶唑(SMX)。采用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、能谱仪(EDS)、X射线衍射仪(XRD)、比表面积分析仪(BET)、程序升温脱附仪(TPD)和X射线光电子能谱仪(XPS)技术对制备的催化剂进行了表征。详细研究了制备的NiCoO-EG用量、PMS浓度、温度、初始溶液pH值和无机离子等几个关键参数对SMX去除的影响。特别是,合成的NiCoO-EG在较宽的pH范围(pH 3.0-11.0)内对SMX降解表现出优异的催化性能。此外,通过电子顺磁共振(EPR)和猝灭试验研究了各种活性氧物种(SO、HO、O和O)随初始pH值的变化。另外,通过超高效液相色谱-四极杆飞行时间串联质谱(UPLC-QTOF-MS/MS)检测了SMX的12种主要降解中间体。最后,提出了EG和NiCoO协同耦合作用下NiCoO-EG/PMS体系中PMS的活化机制。简而言之,这项工作为PMS活化从废水中去除SMX提供了一种有前景和潜力的催化剂。

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