Unprecedented total mineralization of atrazine and cyanuric acid by anodic oxidation and electro-Fenton with a boron-doped diamond anode

被引:234
作者
Oturan, Nihal [1 ]
Brillas, Enric [2 ]
Oturan, Mehmet A. [1 ]
机构
[1] Univ Paris Est, Lab Geomat & Environm LGE, F-77454 Marne La Vallee 2, France
[2] Univ Barcelona, Lab Electroquim Dels Mat & Medi Ambient, Dept Quim Fis, E-08028 Barcelona, Spain
关键词
Atrazine; Boron-doped diamond; Cyanuric acid; Electrochemical advanced oxidation processes; Mineralization; Kinetics; DEGRADATION; WATER;
D O I
10.1007/s10311-011-0337-z
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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)-O-aEuro cent) 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)-O-aEuro cent. 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)-O-aEuro cent 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)-O-aEuro cent 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.
引用
收藏
页码:165 / 170
页数:6
相关论文
共 16 条
[1]   Degradation of atrazine in aqueous medium by electrocatalytically generated hydroxyl radicals. A kinetic and mechanistic study [J].
Balci, Beytul ;
Oturan, Nihal ;
Cherrier, Richard ;
Oturan, Mehmet A. .
WATER RESEARCH, 2009, 43 (07) :1924-1934
[2]   Degradation of Atrazine by Electrochemical Advanced Oxidation Processes Using a Boron-Doped Diamond Anode [J].
Borras, Nuria ;
Oliver, Ramon ;
Arias, Conchita ;
Brillas, Enric .
JOURNAL OF PHYSICAL CHEMISTRY A, 2010, 114 (24) :6613-6621
[3]   Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton's Reaction Chemistry [J].
Brillas, Enric ;
Sires, Ignasi ;
Oturan, Mehmet A. .
CHEMICAL REVIEWS, 2009, 109 (12) :6570-6631
[4]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[5]   Modeling the reaction kinetics of Fenton's process on the removal of atrazine [J].
Chan, KH ;
Chu, W .
CHEMOSPHERE, 2003, 51 (04) :305-311
[6]   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 [J].
De Laat, J ;
Gallard, H ;
Ancelin, S ;
Legube, B .
CHEMOSPHERE, 1999, 39 (15) :2693-2706
[7]   Electrochemical abatement of the antibiotic sulfamethoxazole from water [J].
Dirany, Ahmad ;
Sires, Ignasi ;
Oturan, Nihal ;
Oturan, Mehmet A. .
CHEMOSPHERE, 2010, 81 (05) :594-602
[8]   Degradation of some biorecalcitrant pesticides by homogeneous and heterogeneous photocatalytic ozonation [J].
Farré, MJ ;
Franch, MI ;
Malato, S ;
Ayllón, JA ;
Peral, J ;
Doménech, X .
CHEMOSPHERE, 2005, 58 (08) :1127-1133
[9]   Degradation of selected pesticide active ingredients and commercial formulations in water by the photo-assisted Fenton reaction [J].
Huston, PL ;
Pignatello, JJ .
WATER RESEARCH, 1999, 33 (05) :1238-1246
[10]   Toxicity of atrazine to the juvenile hard clam, Mercenaria mercenaria [J].
Lawton, Jennifer C. ;
Pennington, Paul L. ;
Chung, Katy W. ;
Scott, Geoffrey I. .
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY, 2006, 65 (03) :388-394