Degradation kinetics and mechanism of oxytetracycline by hydroxyl radical-based advanced oxidation processes

被引:309
作者
Liu, Yiqing [1 ,2 ]
He, Xuexiang [2 ]
Fu, Yongsheng [1 ]
Dionysiou, Dionysios D. [2 ]
机构
[1] Southwest Jiaotong Univ, Fac Geosci & Environm Engn, Chengdu 611756, Peoples R China
[2] Univ Cincinnati, Environm Engn & Sci Program, Cincinnati, OH 45221 USA
关键词
Oxytetracycline; Advanced oxidation processes (AOPs); Hydroxyl radical; UV-254; nm/H2O2; Mechanism; WASTE-WATER TREATMENT; AQUEOUS-SOLUTION; AQUATIC ENVIRONMENT; HYDROGEN-PEROXIDE; PULSE-RADIOLYSIS; RATE CONSTANTS; PHOTOCHEMICAL DECOMPOSITION; PHOTOCATALYTIC DEGRADATION; ELECTROSPRAY-IONIZATION; VETERINARY ANTIBIOTICS;
D O I
10.1016/j.cej.2015.09.034
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study, the degradation kinetics and transformation mechanism of oxytetracycline (OTC) by UV-254 nm and UV-254 nm/H2O2 were investigated. The removal of OTC increased with increasing initial H2O2 dosage while excess H2O2 acted as an inhibitor of HO. The observed UV fluence based pseudo first-order rate constant of OTC (k(obs), cm(2) mJ(-1)) decreased while the degradation rate at the initial 13 min (mu M min(-1)) increased with increasing initial OTC concentrations. Presence of different water constituents in the reaction system had a different degree of influence on the degradation efficiency of OTC. Though after 10 h irradiation, there was only a limited elimination of total organic carbon (TOC), successful transformation of OTC was demonstrated by the detection of thirty-one degradation byproducts in the UV/H2O2 system. Potential degradation mechanisms for OTC were proposed exhibiting five main pathways, including hydroxylation (+16 Da), secondary alcohol oxidation (-2 Da), demethylation (-14 Da), decarbonylation (-28 Da) and dehydration (-18 Da). This study indicates that UV-254 nm/H2O2 is an effective technology for the removal of OTC from an aquatic environment. (c) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:1317 / 1327
页数:11
相关论文
共 70 条
[11]   HOMOGENEOUS PYROLYSIS OF ACETYLACETONE AT HIGH-TEMPERATURES IN SHOCK-WAVES [J].
CHOUDHURY, TK ;
LIN, MC .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1990, 22 (05) :491-504
[12]   PHOTOLYSIS OF FE(III)-HYDROXY COMPLEXES AS SOURCES OF OH RADICALS IN CLOUDS, FOG AND RAIN [J].
FAUST, BC ;
HOIGNE, J .
ATMOSPHERIC ENVIRONMENT PART A-GENERAL TOPICS, 1990, 24 (01) :79-89
[13]   Ametryn degradation in the ultraviolet (UV) irradiation/hydrogen peroxide (H2O2) treatment [J].
Gao, Nai-Yun ;
Deng, Yang ;
Zhao, Dandan .
JOURNAL OF HAZARDOUS MATERIALS, 2009, 164 (2-3) :640-645
[14]   Decolorization of antraquinonic dye, CI Acid Blue 25, in aqueous solution by direct UV irradiation, UV/H2O2 and UV/Fe(II) processes [J].
Ghodbane, Houria ;
Hamdaoui, Oualid .
CHEMICAL ENGINEERING JOURNAL, 2010, 160 (01) :226-231
[15]   PHOTOENOLIZATION OF 2-METHYLACETOPHENONE AND RELATED COMPOUNDS [J].
HAAG, R ;
WIRZ, J ;
WAGNER, PJ .
HELVETICA CHIMICA ACTA, 1977, 60 (08) :2595-2607
[16]   ANHYDROTETRACYCLINE IS A MAJOR PRODUCT OF TETRACYCLINE PHOTOLYSIS [J].
HASAN, T ;
ALLEN, M ;
COOPERMAN, BS .
JOURNAL OF ORGANIC CHEMISTRY, 1985, 50 (10) :1755-1757
[17]   Destruction of microcystins (cyanotoxins) by UV-254 nm-based direct photolysis and advanced oxidation processes (AOPs): Influence of variable amino acids on the degradation kinetics and reaction mechanisms [J].
He, Xuexiang ;
de la Cruz, Armah A. ;
Hiskia, Anastasia ;
Kaloudis, Triantafyllos ;
O'Shea, Kevin ;
Dionysiou, Dionysios D. .
WATER RESEARCH, 2015, 74 :227-238
[18]   Degradation kinetics and mechanism of β-lactam antibiotics by the activation of H2O2 and Na2S2O8 under UV-254 nm irradiation [J].
He, Xuexiang ;
Mezyk, Stephen P. ;
Michael, Irene ;
Fatta-Kassinos, Despo ;
Dionysiou, Dionysios D. .
JOURNAL OF HAZARDOUS MATERIALS, 2014, 279 :375-383
[19]   Degradation Mechanism of Cyanobacterial Toxin Cylindrospermopsin by Hydroxyl Radicals in Homogeneous UV/H2O2 Process [J].
He, Xuexiang ;
Zhang, Geshan ;
de la Cruz, Armah A. ;
O'Shea, Kevin E. ;
Dionysiou, Dionysios D. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (08) :4495-4504
[20]   Efficient removal of microcystin-LR by UV-C/H2O2 in synthetic and natural water samples [J].
He, Xuexiang ;
Pelaez, Miguel ;
Westrick, Judy A. ;
O'Shea, Kevin E. ;
Hiskia, Anastasia ;
Triantis, Theodoros ;
Kaloudis, Triantafyllos ;
Stefan, Mihaela I. ;
de la Cruz, Armah A. ;
Dionysiou, Dionysios D. .
WATER RESEARCH, 2012, 46 (05) :1501-1510