Abstract
This article reports the complete mineralization of atrazine. Atrazine has been the most widely used s-triazine herbicide. Atrazine occurs in natural waters and presents a potential danger for public health because atrazine is considered as an endocrine disruptor. The use of chemical, photochemical and photocatalytic advanced oxidation processes (AOPs) to decontaminate waters containing atrazine only allowed its conversion into the cyanuric acid as ultimate end products, since it cannot be completely degraded by hydroxyl radicals (•OH) produced by these techniques. The same behavior was previously reported for anodic oxidation and electro-Fenton with Pt anode, although better performances were found using boron-doped diamond (BDD) anode but without explaining the role of generated •OH. Here, the oxidative action of these radicals in such electrochemical AOPs has been clarified by studying the mineralization process and decay kinetics of atrazine and cyanuric acid in separated solutions by anodic oxidation with BDD and electro-Fenton with Pt or BDD anode using an undivided cell with a carbon-felt cathode under galvanostatic conditions. Results showed that electro-Fenton with BDD anode was the more powerful treatment to degrade both compounds. Almost total mineralization, 97% total organic carbon (COT) removal, of atrazine was only feasible by this method with a faster removal of its oxidation intermediates by •OH formed at the BDD surface than that formed in the bulk from Fenton reaction, although the latter process caused a more rapid decay of the herbicide. Cyanuric acid was much slowly mineralized mainly with •OH produced at the BDD surface, and it was not degraded by electro-Fenton with Pt anode. These results highlight that electrochemical advanced oxidation processes (EAOPs) using a BDD anode are more powerful than the classical electro-Fenton process with Pt or PbO2 anodes.
Similar content being viewed by others
References
Balci B, Oturan N, Cherrier R, Oturan MA (2009) Degradation of atrazine in aqueous medium by electrocatalytically generated hydroxyl radicals. A kinetic and mechanistic study. Water Res 43:1924–1934. doi:10.1016/j.watres.2009.01.021
Borràs N, Oliver R, Arias C, Brillas E (2010) Degradation of atrazine by electrochemical advanced oxidation processes using a boron-doped diamond anode. J Phys Chem A 114:6613–6621. doi:10.1021/jp1035647
Brillas E, Sirés I, Oturan MA (2009) Electro-Fenton process and related electrochemical technologies based on Fenton’s reaction chemistry. Chem Rev 109:6570–6631. doi:10.1021/cr900136g
Buxton GU, Greenstock CL, Helman WP, Ross AB (1988) Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (•OH/O•−) in aqueous solution. J Phys Chem Ref Data 17:513–886. doi:10.1063/1.555805
Chan KH, Chu W (2003) Modeling the reaction kinetics of Fenton’s process on the removal of atrazine. Chemosphere 51:305–311. doi:10.1016/S0045-6536(02)00812-3
De Laat J, Gallard H, Ancelin A, Legube B (1999) Comparative study of the oxidation of atrazine and acetone by H2O2/UV, Fe(III)/UV, Fe(III)/H2O2/UV and Fe(II) or Fe(III)/H2O2. Chemosphere 39:2693–2706. doi:10.1016/S0045-6535(99)00204-0
Dirany A, Sirés I, Oturan N, Oturan MA (2010) Electrochemical abatement of the antibiotic sulfamethoxazole from water. Chemosphere 81:594–602. doi:10.1016/j.chemosphere.2010.08.032
Farré MJ, Franch MI, Malato S, Ayllón JA, Peral J, Domènech X (2005) Degradation of some biorecalcitrant pesticides by homogeneous and heterogeneous photocatalytic ozonation. Chemosphere 58:1127–1133. doi:10.1016/j.chemosphere.2004.09.064
Huston PL, Pignatello JJ (1999) Degradation of selected pesticide active ingredients and commercial formulations in water by photo-assisted Fenton reaction. Water Res 33:1238–1246. doi:10.1016/S0043-1354(98)00330-3
Lawton JC, Pennington PL, Chung KW, Geoffrey IS (2006) Toxicity of atrazine to the juvenile hard clam, Mercenaria mercenaria. Ecotoxicol Environ Saf 65:388–394. doi:10.1016/j.ecoenv.2005.08.001
Malpass GRP, Miwa DW, Machado SAS, Olivi P, Motheo AJ (2006) Oxidation of the pesticide atrazine at DSA electrode. J Hazard Mater B137:565–572. doi:10.1016/j.hazmat.2006.02.045
Mamián M, Torres W, Larmat FE (2009) Electrochemical degradation of atrazine in aqueous solution at a platinum electrode. Port Electrochim Acta 27:371–379. doi:10.4152/pea.200903371
McMurray TA, Dunlp PSM, Byrne JA (2006) The photocatalytic degradation of atrazine on nanoparticulate TiO2 films. J Photochem Photobio A Chem 182:43–51. doi:10.1016/j.photochem.2006.01.010
Nélieu S, Kerhoas L, Einhor J (2000) Degradation of atrazine into ammeline by combined ozone/hydrogen peroxide treatment in water. Environ Sci Technol 34:430–437. doi:10.1021/es980540k
Panizza M, Cerisola G (2009) Direct and mediated anodic oxidation of organic pollutants. Chem Rev 109:6541–6569. doi:10.1021/cr9001319
Polcaro AM, Vacca A, Mascia M, Palmas S (2005) Oxidation at boron doped diamond electrodes: an effective method to mineralise triazines. Electrochim Acta 50:1841–1847. doi:10.1016/j.electacta.2004.08.037
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Oturan, N., Brillas, E. & Oturan, M.A. Unprecedented total mineralization of atrazine and cyanuric acid by anodic oxidation and electro-Fenton with a boron-doped diamond anode. Environ Chem Lett 10, 165–170 (2012). https://doi.org/10.1007/s10311-011-0337-z
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10311-011-0337-z