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利用紫外光/过硫酸盐降解水中高氯农药林丹:动力学与机理、毒性评估及羟基自由基的协同作用

Degradation of highly chlorinated pesticide, lindane, in water using UV/persulfate: kinetics and mechanism, toxicity evaluation, and synergism by HO.

作者信息

Khan Sanaullah, Sohail M, Han Changseok, Khan Javed Ali, Khan Hasan M, Dionysiou Dionysios D

机构信息

Department of Chemistry, Women University, Swabi, 23430, Pakistan; Radiation Chemistry Laboratory, National Centre of Excellence in Physical Chemistry, University of Peshawar, Peshawar, 25120, Pakistan; Environmental Engineering and Science Program, University of Cincinnati, Cincinnati, Ohio, 45221-0012, USA.

Institute of Chemical Sciences, University of Swat, Swat, 19130, Pakistan.

出版信息

J Hazard Mater. 2021 Jan 15;402:123558. doi: 10.1016/j.jhazmat.2020.123558. Epub 2020 Jul 25.

Abstract

Sulfate radical-advanced oxidation processes (SR-AOPs) are emerging technologies for decomposing organic pollutants in water. This study investigated the efficiency of UV/persulfate (UV/SO) process to degrade lindane in water, showing 93.2% lindane removal ([lindane] = 3.43 μM, [SO] = 100 μM) at a UV fluence of 720 mJ/cm. The lindane degradation followed first order kinetics and mechanistic studies suggested H-abstraction by SO and Cl removal via C-Cl bond cleavage by UV-C light. Toxicity assessment using ECOSAR program showed toxicity gradually decreased and eventually no significant toxicity remained when all by-products vanished at high UV dose. Removal efficiency of lindane decreased from 93.2% to 38.4, 45.5, 56.0, 84.3 and 88.6%, by adding 1.0 mg/L humic acid or 1.0 mM CO, HCO, Cl or SO, respectively. Coupling of HO with UV/SO showed a significant synergistic effect with 99.0% lindane removal at a UV fluence of 600 mJ/cm, using [SO] = [HO] = 50 μM while UV/HO resulted in only 36.6% lindane removal ([lindane] = 3.43 μM, [HO] = 100 μM) at a UV fluence of 720 mJ/cm. The results indicate that SR-AOP has potential for consideration as a remedial technology to treat persistent chlorinated pesticides such as lindane in contaminated water.

摘要

硫酸根自由基高级氧化工艺(SR-AOPs)是用于分解水中有机污染物的新兴技术。本研究考察了紫外光/过硫酸盐(UV/S₂O₈)工艺降解水中林丹的效率,结果表明在紫外光通量为720 mJ/cm²时,林丹去除率达93.2%([林丹]=3.43 μM,[S₂O₈²⁻]=100 μM)。林丹降解遵循一级动力学,机理研究表明通过S₂O₈²⁻进行氢原子提取以及通过紫外C光使C-Cl键断裂来去除氯。使用ECOSAR程序进行的毒性评估表明,在高紫外剂量下所有副产物消失时,毒性逐渐降低,最终无显著毒性残留。分别添加1.0 mg/L腐殖酸或1.0 mM CO₃²⁻、HCO₃⁻、Cl⁻或SO₄²⁻后,林丹去除率从93.2%分别降至38.4%、45.5%、56.0%、84.3%和88.6%。HO·与UV/S₂O₈耦合显示出显著的协同效应,在紫外光通量为600 mJ/cm²、[S₂O₈²⁻]=[HO·]=50 μM时,林丹去除率达99.0%,而在紫外光通量为720 mJ/cm²、[林丹]=3.43 μM、[HO·]=100 μM时,UV/HO·工艺的林丹去除率仅为36.6%。结果表明,SR-AOP有潜力作为一种修复技术用于处理受污染水中的持久性氯化农药,如林丹。

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