Degradation of clofibric acid in acidic aqueous medium by electro-Fenton and photoelectro-Fenton

被引:132
作者
Sires, Ignasi [1 ]
Arias, Conchita [1 ]
Lluis Cabot, Pere [1 ]
Centellas, Francesc [1 ]
Antonio Garrido, Jose [1 ]
Maria Rodriguez, Rosa [1 ]
Brillas, Enric [1 ]
机构
[1] Univ Barcelona, Fac Quim, Dept Quim Fis, Lab Electroquim Mat & Medi Ambienti, Barcelona 08028, Spain
关键词
drug mineralization; electro-Fenton; photoelectro-Fenton; catalysis; water treatment;
D O I
10.1016/j.chemosphere.2006.07.039
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Acidic aqueous solutions of clofibric acid (2-(4-chlorophenoxy)-2-methylpropionic acid), the bioactive metabolite of various lipid-regulating drugs, have been degraded by indirect electrooxidation methods such as electro-Fenton and photoelectro-Fenton with Fe2+ as catalyst using an undivided electrolytic cell with a Pt anode and an O-2-diffusion cathode able to electrogenerate H2O2. At pH 3.0 about 80% of mineralization is achieved with the electro-Fenton method due to the efficient production of oxidant hydroxyl radical from Fenton's reaction between Fe2+ and H2O2, but stable Fe3+ complexes are formed. The photoelectro-Fenton method favors the photodecomposition of these species under UVA irradiation, reaching more than 96% of decontamination. The mineralization current efficiency increases with rising metabolite concentration up to saturation and with decreasing current density. The photoelectro-Fenton method is then viable for treating acidic wastewaters containing this pollutant. Comparative degradation by anodic oxidation (without Fe2+) yields poor decontamination. Chloride ion is released during all degradation processes. The decay kinetics of clofibric acid always follows a pseudo-first-order reaction, with a similar rate constant in electro-Fenton and photoelectro-Fenton that increases with rising current density, but decreases at greater metabolite concentration. 4-Chlorophenol, 4-chlorocatechol, 4-chlororesorcinol, hydroquinone, p-benzoquinone and 1,2,4-benzenetriol, along with carboxylic acids such as 2-hydroxyisobutyric, tartronic, maleic, fumaric, formic and oxalic, are detected as intermediates. The ultimate product is oxalic acid, which forms very stable Fe3+-oxalato complexes under electro-Fenton conditions. These complexes are efficiently photodecarboxylated in photoclectro-Fenton under the action of UVA light. (c) 2006 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1660 / 1669
页数:10
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