Transformation kinetics of biochemically active compounds in low-pressure UV Photolysis and UV/H2O2 advanced oxidation processes

被引:172
作者
Baeza, Carolina [2 ]
Knappe, Detlef R. U. [1 ]
机构
[1] N Carolina State Univ, Dept Civil Construct & Environm Engn, Raleigh, NC 27695 USA
[2] Univ Concepcion, Environm Sci Ctr EULA Chile, Concepcion, Chile
基金
美国国家科学基金会;
关键词
Antibiotics; Endocrine disrupting chemicals; Pharmaceuticals; Photooxidation; Quantum yield; WATER-TREATMENT PROCESSES; SIMULATED DRINKING-WATER; RATE CONSTANTS; HETEROCYCLIC GROUPS; PHOTOCHEMICAL FATE; MIGRATION BEHAVIOR; HYDROXYL RADICALS; NATURAL-WATERS; SULFA DRUGS; WASTE-WATER;
D O I
10.1016/j.watres.2011.05.039
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Factors controlling photolysis and UV/H2O2 photooxidation rates of the biochemically active compounds (BACs) sulfamethoxazole, sulfamethazine, sulfadiazine, trimethoprim, bisphenol A, and diclofenac were determined. Experiments were conducted with a quasi-collimated beam apparatus equipped with low-pressure UV lamps. The effects of pH, H2O2 concentration, and background water matrix (ultrapure water, lake water, wastewater treatment plant effluent) on BAC transformation rates were evaluated. For the sulfa drugs, solution pH affected direct photolysis rates but had little effect on the hydroxyl radical oxidation rate. For sulfamethoxazole, the neutral form photolyzed more easily than the anionic form while the reverse was the case for sulfamethazine and sulfadiazine. For trimethoprim, the hydroxyl radical oxidation rate was higher for the cationic form (pH 3.6) than for the neutral form (pH 7.85). Quantum yields and second order rate constants describing the reaction between the hydroxyl radical and BACs were determined and used together with background water quality data to predict fluence-based BAC transformation rate constants (k'). For both the lake water and wastewater treatment plant effluent matrices, predicted k' values were generally in good agreement with experimentally determined k' values. At typical UV/H2O2 treatment conditions (fluence = 540 mJ cm(-2), H2O2 dose = 6 mg L-1), BAC transformation percentages in North Carolina lake water ranged from 43% for trimethoprim to 98% for diclofenac. In wastewater treatment plant effluent, BAC transformation percentages were lower (31-97%) at the same treatment conditions because the hydroxyl radical scavenging rate was higher. (C) 2011 Elsevier Ltd. All rights reserved.
引用
收藏
页码:4531 / 4543
页数:13
相关论文
共 33 条
[21]   Photochemical fate of pharmaceuticals in the environment: Naproxen, diclofenac, clofibric acid, and ibuprofen [J].
Packer, JL ;
Werner, JJ ;
Latch, DE ;
McNeill, K ;
Arnold, WA .
AQUATIC SCIENCES, 2003, 65 (04) :342-351
[22]   UV degradation kinetics and modeling of pharmaceutical compounds in laboratory grade and surface water via direct and indirect photolysis at 254 nm [J].
Pereira, Vanessa J. ;
Weinberg, Howard S. ;
Linden, Karl G. ;
Singer, Philip C. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (05) :1682-1688
[23]   Endocrine disrupting compounds and other emerging contaminants in the environment:: A survey on new monitoring strategies and occurrence data [J].
Petrovic, M ;
Eljarrat, E ;
de Alda, MJL ;
Barceló, D .
ANALYTICAL AND BIOANALYTICAL CHEMISTRY, 2004, 378 (03) :549-562
[24]   Potentiometric determination of acid dissociation constants (pKa) for human and veterinary antibiotics [J].
Qiang, ZM ;
Adams, C .
WATER RESEARCH, 2004, 38 (12) :2874-2890
[25]   The iodide/iodate actinometer in UV disinfection: Determination of the fluence rate distribution in UV reactors [J].
Rahn, RO ;
Bolton, J ;
Stefan, MI .
PHOTOCHEMISTRY AND PHOTOBIOLOGY, 2006, 82 (02) :611-615
[26]   Evaluation of UV/H2O2 treatment for the oxidation of pharmaceuticals in wastewater [J].
Rosario-Ortiz, Fernando L. ;
Wert, Eric C. ;
Snyder, Shane A. .
WATER RESEARCH, 2010, 44 (05) :1440-1448
[27]   Degradation of endocrine disrupting chemicals bisphenol A, ethinyl estradiol, and estradiol during UV photolysis and advanced oxidation processes [J].
Rosenfeldt, EJ ;
Linden, KG .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (20) :5476-5483
[28]  
Schwarzenbach R.P., 2003, ENV ORGANIC CHEM, P611
[29]   Experimental and model comparisons of low- and medium-pressure Hg lamps for the direct and H2O2 assisted UV photodegradation of N-nitrosodimethylamine in simulated drinking water [J].
Sharpless, CM ;
Linden, KG .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (09) :1933-1940
[30]  
Snyder EM, 2005, J AM WATER WORKS ASS, V97, P32