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利用 ZnO 修饰的磁性核/壳结构光解过一硫酸盐实现对水中敌敌畏农药的高效净化。

Efficient clean-up of waters contaminated with diazinon pesticide using photo-decomposition of peroxymonosulfate by ZnO decorated on a magnetic core/shell structure.

机构信息

Student Research Committee, Alborz University of Medical Sciences, Karaj, Iran.

Research Center for Health, Safety and Environment, Alborz University of Medical Sciences, Karaj, Iran; Department of Environmental Health Engineering, Alborz University of Medical Sciences, Karaj, Iran.

出版信息

J Environ Manage. 2019 Nov 15;250:109472. doi: 10.1016/j.jenvman.2019.109472. Epub 2019 Sep 11.

Abstract

In the present study, ZnO nanoparticles were anchored on a magnetic core/shell structure (SiO@FeO) to perpetrate ZnO@SiO@FeO and then coupled with UV light as a heterogeneous nanocatalyst for activating peroxymonosulfate (PMS) into diazinon (DZ) degradation. Several techniques like XRD (X-ray diffraction), BET (Brunaeur, Emmett and Teller), TEM (Transmission electron microscope), FESEM (Field emission-scanning electron microscope) coupled with EDS (Energy Dispersive X-ray Spectrometer), PL (photoluminescence), VSM (Vibrating Sample Magnetometer) and UV-vis diffuse reflectance spectroscopy (DRS) were applied for identification of catalyst features. A possible mechanism for PMS activation and DZ degradation was proposed in details. The effect of solution pH, various concentrations of catalyst, PMS and DZ, quenching agents, different chemical oxidants and co-existing anions was assessed as operating factors to determine the optimum conditions. PMS decomposed effectively in coupling with ZnO@SiO@FeO and UV. At optimal conditions, over 95 and 56% of DZ and TOC were removed during 60 min reaction, respectively. The complete degradation of DZ was confirmed using its absorption peak in UV-vis spectra analysis over 60 min treatment. A wide variety of free radicals was identified during quenching tests. HO and h played a pivotal role in the degradation process of DZ. Decreasing the degradation efficiency in the presence of anions was as Cl > CO > NO > PO > SO > HCO. A negligible amount of leaching Fe (<0.2 mg/L) was found for ZnO@SiO@FeO, indicating that the catalyst possesses a high stability in oxidation systems. In addition, a significant potential was achieved in reusing of catalyst within five consecutive runs. In conclusion, ZnO@SiO@FeO/PMS/UV hybrid system can be utilized as a promising advanced oxidation process into efficient degradation of pesticides, thanks to easy recovery, high catalytic activity, co-production of different reactive species and high durability and recyclability potential.

摘要

在本研究中,将氧化锌纳米粒子锚定在磁性核/壳结构(SiO@FeO)上,形成 ZnO@SiO@FeO,并与紫外光耦合作为非均相纳米催化剂,用于将过一硫酸盐(PMS)激活为敌敌畏(DZ)降解。应用了多种技术,如 X 射线衍射(XRD)、BET(Brunaeur、Emmett 和 Teller)、透射电子显微镜(TEM)、场发射扫描电子显微镜(FESEM)耦合能谱仪(EDS)、光致发光(PL)、振动样品磁强计(VSM)和紫外-可见漫反射光谱(DRS)来鉴定催化剂的特征。详细提出了一种 PMS 激活和 DZ 降解的可能机制。评估了溶液 pH 值、催化剂、PMS 和 DZ 的各种浓度、猝灭剂、不同的化学氧化剂和共存阴离子等操作因素的影响,以确定最佳条件。在 ZnO@SiO@FeO 和 UV 的耦合作用下,PMS 有效地分解。在最佳条件下,反应 60 分钟后,DZ 和总有机碳(TOC)的去除率分别超过 95%和 56%。通过在 60 分钟处理过程中分析其在紫外-可见光谱中的吸收峰,确认了 DZ 的完全降解。在猝灭试验中鉴定了多种自由基。HO 和 h 在 DZ 的降解过程中发挥了关键作用。在阴离子存在下,降解效率降低的顺序为 Cl⁃>CO₃²⁻>NO₃⁻>PO₄³⁻>SO₄²⁻>HCO₃⁻。在 ZnO@SiO@FeO 中发现了可忽略的溶出铁量(<0.2 mg/L),表明催化剂在氧化体系中具有高稳定性。此外,在五个连续运行中实现了催化剂的显著再利用潜力。总之,由于易于回收、高催化活性、同时产生不同的活性物质以及高耐久性和可回收性潜力,ZnO@SiO@FeO/PMS/UV 杂化系统可用于有效降解农药的有前途的高级氧化工艺。

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