Degradation of atrazine in aqueous medium by electrocatalytically generated hydroxyl radicals. A kinetic and mechanistic study

被引:180
作者
Balci, Beytul [1 ]
Oturan, Nihal [1 ]
Cherrier, Richard [2 ]
Oturan, Mehmet A. [1 ]
机构
[1] Univ Paris Est, Lab Geomat & Geol Ingenieur G2I, F-77454 Marne La Vallee 2, France
[2] INRA, INPL, Lab Sols & Environm ENSAIA, UMR 1120, F-54505 Vandoeuvre Les Nancy, France
关键词
Atrazine; Electro-Fenton; BDD anode; Hydroxyl radicals; Cyanuric acid; Mineralization; ADVANCED OXIDATION PROCESSES; ELECTRO-FENTON DEGRADATION; PHOTOCATALYTIC DEGRADATION; ELECTROCHEMICAL TREATMENT; ORGANIC POLLUTANTS; ANODIC-OXIDATION; OH RADICALS; WATER; MINERALIZATION; ACID;
D O I
10.1016/j.watres.2009.01.021
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
oxidative degradation of atrazine by hydroxyl radicals ((OH)-O-center dot) was studied in aqueous medium. (OH)-O-center dot were formed in situ from electrochemically generating Fenton's reagent by an indirect electrochemical advanced oxidation process. identification and evolution of seven main aromatic metabolites and four short-chain carboxylic acids were performed by using liquid chromatography analyses. Total organic carbon (TOC) and ionic chromatography were used in order to evaluate the mineralization efficiency of treated aqueous solutions. A high mineralization rate of 82% (never reported until now) was obtained. The oxidative degradation of cyanuric acid, the ultimate product of atrazine degradation, was highlighted for the first time. The absolute rate constant of the reaction between atrazine and hydroxyl radicals was evaluated by competition kinetics method as (2.54 +/- 0.22) x 10(9) M-1 s(-1). Considering all oxidation reaction intermediates and end products a general reaction sequence for atrazine degradation by hydroxyl radicals was proposed. (C) 2009 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1924 / 1934
页数:11
相关论文
共 56 条
[1]   Degradation kinetics of atrazine and its degradation products with ozone and OH radicals: A predictive tool for drinking water treatment [J].
Acero, JL ;
Stemmler, K ;
Von Gunten, U .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (04) :591-597
[2]  
Ammar S., 2007, Journal of Environmental Engineering and Management, V17, P89
[3]   DEGRADATION OF ATRAZINE BY FENTONS REAGENT - CONDITION OPTIMIZATION AND PRODUCT QUANTIFICATION [J].
ARNOLD, SM ;
HICKEY, WJ ;
HARRIS, RF .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1995, 29 (08) :2083-2089
[4]   2,4-Dichlorophenoxyacetic acid (2,4-D) sorption and degradation dynamics in three agricultural soils [J].
Boivin, A ;
Amellal, S ;
Schiavon, M ;
van Genuchten, MT .
ENVIRONMENTAL POLLUTION, 2005, 138 (01) :92-99
[5]   Aniline mineralization by AOP's: anodic oxidation, photocatalysis, electro-Fenton and photoelectro-Fenton processes [J].
Brillas, E ;
Mur, E ;
Sauleda, R ;
Sanchez, L ;
Peral, J ;
Domenech, X ;
Casado, J .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 16 (01) :31-42
[6]   Mineralization of paracetamol in aqueous medium by anodic oxidation with a boron-doped diamond electrode [J].
Brillas, E ;
Sirés, I ;
Arias, C ;
Cabot, PL ;
Centellas, F ;
Rodríguez, RM ;
Garrido, JA .
CHEMOSPHERE, 2005, 58 (04) :399-406
[7]   Catalytic effect of Fe2+, Cu2+ and UVA light on the electrochemical degradation of nitrobenzene using an oxygen-diffusion cathode [J].
Brillas, E ;
Baños, MA ;
Camps, S ;
Arias, C ;
Cabot, PL ;
Garrido, JA ;
Rodríguez, RM .
NEW JOURNAL OF CHEMISTRY, 2004, 28 (02) :314-322
[8]   ATRAZINE AND OTHER S-TRIAZINE HERBICIDES IN LAKES AND IN RAIN IN SWITZERLAND [J].
BUSER, HR .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1990, 24 (07) :1049-1058
[9]   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
[10]   Electrochemical oxidation of phenolic wastes with boron-doped diamond anodes [J].
Cañizares, P ;
Lobato, J ;
Paz, R ;
Rodrigo, MA ;
Sáez, C .
WATER RESEARCH, 2005, 39 (12) :2687-2703