Oxidation of acetamide herbicides in natural waters by ozone and by the combination of ozone/hydrogen peroxide: Kinetic study and process modeling

被引:23
作者
Acero, JL [1 ]
Benitez, FJ [1 ]
Real, FJ [1 ]
Maya, C [1 ]
机构
[1] Univ Extremadura, Dept Ingn Quim & Energet, E-06071 Badajoz, Spain
关键词
D O I
10.1021/ie030229y
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
The oxidation by ozone and by the combination O-3/H2O2 of four herbicides included in the acetamide group (acetochlor, metolachlor, propachlor, and butachlor) was studied. In, a first step, the rate constants were determined for the reactions of the selected herbicides with ozone (k(o3)) and OH radicals (k(OH)). The sequence of reactivities for solutions in ultrapure water were as follows: for ozonation, metolachlor < propachlor < acetochlor < butachlor; for oxidation by hydroxyl radicals, propachlor < acetochlor < metolachlor < butachlor. The rate constants for the reaction with ozone ranged from 1.1 to 5.3 L/(mol(.)s), indicating that direct reactions with ozone will play a minor role during ozonation processes. Values for kOH ranged from 4.6 x 10(9) to 7.4 x 10(9) L/(mol(.)s). Therefore, reactions with OH radicals will be the major pathway for the oxidative transformation of these four herbicides, even when conventional ozonation is applied. In a second step, the oxidation of the investigated herbicides during ozonation processes in some natural and mineral waters was studied, including the influence of the operating variables, and the herbicide oxidation levels were determined. Next, the oxidation process was characterized in terms of oxidant concentrations (ozone and OH radicals), and finally the evolution of the herbicide concentration in an ozonation process was modeled and predicted by applying a kinetics approach based on the rate constants for the reactions with ozone and OH radicals and the calculated concentrations of the active oxidants.
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收藏
页码:5762 / 5769
页数:8
相关论文
共 30 条
[1]  
Acero JL, 2001, J AM WATER WORKS ASS, V93, P90
[2]   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
[3]   PHOTOMETRIC-METHOD FOR THE DETERMINATION OF LOW CONCENTRATIONS OF HYDROGEN-PEROXIDE BY THE PEROXIDASE CATALYZED OXIDATION OF N,N-DIETHYL-P-PHENYLENEDIAMINE (DPD) [J].
BADER, H ;
STURZENEGGER, V ;
HOIGNE, J .
WATER RESEARCH, 1988, 22 (09) :1109-1115
[4]   DETERMINATION OF OZONE IN WATER BY THE INDIGO METHOD [J].
BADER, H ;
HOIGNE, J .
WATER RESEARCH, 1981, 15 (04) :449-456
[5]   Major herbicides in ground water: Results from the National Water-Quality Assessment [J].
Barbash, JE ;
Thelin, GP ;
Kolpin, DW ;
Gilliom, RJ .
JOURNAL OF ENVIRONMENTAL QUALITY, 2001, 30 (03) :831-845
[6]  
Beltrán FJ, 2000, B ENVIRON CONTAM TOX, V65, P668, DOI 10.1007/s001280000175
[7]   Degradation of carbofuran by using ozone, UV radiation and advanced oxidation processes [J].
Benitez, FJ ;
Acero, JL ;
Real, FJ .
JOURNAL OF HAZARDOUS MATERIALS, 2002, 89 (01) :51-65
[8]   ACUCHEM - A COMPUTER-PROGRAM FOR MODELING COMPLEX CHEMICAL-REACTION SYSTEMS [J].
BRAUN, W ;
HERRON, JT ;
KAHANER, DK .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1988, 20 (01) :51-62
[9]   Indirect photolysis of acetochlor: Rate constant of a nitrate-mediated hydroxyl radical reaction [J].
Brekken, JF ;
Brezonik, PL .
CHEMOSPHERE, 1998, 36 (12) :2699-2704
[10]   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