High temperature dependence of 2,4-dichlorophenoxyacetic acid degradation by Fe3+/H2O2 system

被引:61
作者
Lee, Y [1 ]
Lee, C [1 ]
Yoon, J [1 ]
机构
[1] Seoul Natl Univ, Sch Chem Engn, Coll Engn, Gwanak Gu, Seoul 151744, South Korea
关键词
Fenton reaction; reaction temperature; 2,4-D; H2O2; -OH; advanced oxidation process;
D O I
10.1016/S0045-6535(03)00043-2
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study demonstrates-the importance of reaction temperature on the degradation of 2,4-dichlorophenoxyacetic acid 2,4-D. In addition, we provide a mechanistic explanation for the temperature dependence of 2,4-D degradation. Thermal enhancement of 2,4-D degradation and H2O2 decomposition was measured in the absence and in the presence of the .OH scavenger (t-butanol). The half-life for 2,4-D degradation was reduced by more than 70-fold in the absence of t-butanol, and by more than 700-fold, in the presence of t-butanol, when the reaction temperature was increased from 10 to 50 degreesC. In addition, similar temperature relationships were found for H2O2 decomposition. The major reason for the high temperature dependence of the Fe3+/H2O2 system in the case of 2,4-D degradation is due to the dependence of the initiation reaction of the Fe3+/H2O2 system (i.e., Fe3+ + H2O2 --> Fe2+ + HO2. + H+ upon temperature), which is entirely consistent with the kinetics of the activation energy. In the presence, of (OH)-O-. scavenger, the initiation reaction of the Fe3+/H2O2 system became a determining factor of this temperature dependence, whereas in the absence of (OH)-O-. scavenger, several other radical reactions played a role and this result in an apparent decrease in the activation energy for 2,4-D degradation. Moreover, the enhanced 2,4-D removal at higher temperatures did not alter H2O2 utilization. The practical implications of the thermal enhancement of the Fe3+/H2O2 system are discussed. (C) 2003 Elsevier Science Ltd. All rights reserved.
引用
收藏
页码:963 / 971
页数:9
相关论文
共 30 条
[1]   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
[2]  
BAHNEMANN DW, 1993, TR MET ENV, V3, P301
[3]  
Balzani V., 1970, PHOTOCHEMISTRY COORD
[4]   REACTIONS OF FERROUS AND FERRIC IONS WITH HYDROGEN PEROXIDE .1. THE FERROUS ION REACTION [J].
BARB, WG ;
BAXENDALE, JH ;
GEORGE, P ;
HARGRAVE, KR .
TRANSACTIONS OF THE FARADAY SOCIETY, 1951, 47 (05) :462-500
[5]  
Bigda RJ, 1995, CHEM ENG PROG, V91, P62
[6]   Role of quinone intermediates as electron shuttles in Fenton and photoassisted Fenton oxidations of aromatic compounds [J].
Chen, RZ ;
Pignatello, JJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1997, 31 (08) :2399-2406
[7]   REACTIONS OF HYDROXYL RADICALS WITH HYDROGEN-PEROXIDE AT AMBIENT AND ELEVATED-TEMPERATURES [J].
CHRISTENSEN, H ;
SEHESTED, K ;
CORFITZEN, H .
JOURNAL OF PHYSICAL CHEMISTRY, 1982, 86 (09) :1588-1590
[8]   Catalytic decomposition of hydrogen peroxide by Fe(III) in homogeneous aqueous solution: Mechanism and kinetic modeling [J].
De Laat, J ;
Gallard, H .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1999, 33 (16) :2726-2732
[9]   Chemical oxidation of methylene blue using a Fenton-like reaction [J].
Dutta, K ;
Mukhopadhyay, S ;
Bhattacharjee, S ;
Chaudhuri, B .
JOURNAL OF HAZARDOUS MATERIALS, 2001, 84 (01) :57-71
[10]   Colorimetric determination of hydrogen peroxide [J].
Eisenberg, GM .
INDUSTRIAL AND ENGINEERING CHEMISTRY-ANALYTICAL EDITION, 1943, 15 :327-328