期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 72, 期 3-4, 页码 373-381出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2006.12.002
关键词
boron-doped diamond anode; catalysis; electro-Fenton; photoelectro-fenton; drug mineralization
This work shows that aqueous solutions of clofibric acid (2-(4-chlorophenoxy)-2-methylpropionic acid), the bioactive metabolite of various lipid-regulating drugs, up to saturation at pH 3.0 are efficiently and completely degraded by electrochemical advanced oxidation processes such as electro-Fenton and photoelectro-Fenton with Fe2+ and UVA light as catalysts using an undivided electrolytic cell with a boron-doped diamond (BDD) anode and an O-2-diffusion cathode able to electrogenerate H2O2. This is feasible in these environmentally friendly methods by the production of oxidant hydroxyl radical at the BDD surface from water oxidation and in the medium from Fenton's reaction between Fe2+ and electrogenerated H2O2. The degradation process is accelerated in photoelectro-Fenton by additional photolysis of Fe3+ complexes under UVA irradiation. Comparative treatments by anodic oxidation with electrogenerated H2O2, but without Fe2+, yield much slower decontamination. Chloride ion is released and totally oxidized to chlorine at the BDD surface in all treatments. The decay kinetics of clofibric acid always follows a pseudo-first-order reaction. 4-Chlorophenol, 4-chlorocatechol, hydroquinone, p-benzoquinone and 2-hydroxyisobutyric, tartronic, maleic, fumaric, formic and oxalic acids, are detected as intermediates. The ultimate product is oxalic acid, which is slowly but progressively oxidized on BDD in anodic oxidation. In electro-Fenton this acid forms Fe3+-oxalato complexes that can also be totally destroyed at the BDD anode, whereas in photoelectro-Fenton the mineralization rate of these complexes is enhanced by its parallel photodecarboxylation with UVA light. (c) 2006 Elsevier B.V. All rights reserved.
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