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浙江大学学报(工学版)
浙江大学学报(工学版)
土木工程     
紫外光降解水中氟比洛芬的动力学与机理
周慧慧, 叶苗苗, 张土乔, 邵煜
浙江大学 市政工程研究所,浙江 杭州310058
Photodegradation efficiency and mechanism of flurbiprofen in water by UV irradiation
ZHOU Hui-hui, YE Miao-miao, ZHANG Tu-qiao, SHAO Yu
Institute of Municipal Engineering, Zhejiang University, Hangzhou 310058, China
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摘要：

为了研究水中氟比洛芬紫外光降解的动力学与机理,通过单因素试验考查反应温度、氟比洛芬初始浓度、溶液初始pH值、溶液腐殖酸浓度、常见阴阳离子对氟比洛芬紫外光降解的影响；并通过液相色谱质谱联用定性检测光降解的中间产物,推测可能的光降解途径.结果表明,氟比洛芬紫外光降解过程符合准一级动力学方程；提高反应体系温度,或降低氟比洛芬初始浓度都有助于降解速率常数的提高；氟比洛芬在偏酸性（pH在6～7之间）环境中光降解效果最好；低浓度腐殖酸对光降解几乎没有作用,但当腐殖酸质量浓度超过10 mg/L时,会产生很大抑制作用；天然水中常见阴阳离子对光降解影响很小.此外,在光解过程中,氟原子很容易从苯环上脱落下来,形成F-,继而发生去羧基化和羟基化.
Abstract:

Parameters affecting the photodegradation processes were carried out through the single factor experiments, including reaction temperature, initial flurbiprofen concentration, initial solution pH, humic acid concentration and inorganic ions. The intermediate products were identified by LCMS analysis, and a photodegradation pathway of FBP was proposed. Results show that the photodegradation of FBP follow spseudo-first-order kinetics. The apparent degradation rate constant (k) increases with the increasing reaction temperature or the decreasing initial FBP concentration. And the weak acidity environment (pH=6~7) boasts the best performance on FBP degradation. The low concentration of humic acid has little effect on the photodegradation, while the high concentration (≥10 mg/L) has obviously negative effect. In addition, the inorganic ions have no significant effects on the photodegradation. Finally, the F atom in the FBP molecule could be completely replaced by OH group to form the F , followed by decarboxylation and hydroxylation.
出版日期: 2014-08-01
:  X 131.2  
基金资助:

国家自然科学基金青年资助项目(51108406,51108407)；中央高校基本科研业务费专项资金资助项目(2013QNA4026).
通讯作者: 邵煜,男,讲师     E-mail: shaoyu1979@zju.edu.cn
作者简介: 周慧慧(1988—),女,硕士生,主要从事水处理研究.E-mail: vivichou9@gmail.com
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周慧慧, 叶苗苗, 张土乔, 邵煜. 紫外光降解水中氟比洛芬的动力学与机理[J]. 浙江大学学报(工学版), 10.3785/j.issn.1008-973X.2014.08.005.

ZHOU Hui-hui, YE Miao-miao, ZHANG Tu-qiao, SHAO Yu. Photodegradation efficiency and mechanism of flurbiprofen in water by UV irradiation. JOURNAL OF ZHEJIANG UNIVERSITY (ENGINEERING SCIENCE), 10.3785/j.issn.1008-973X.2014.08.005.

链接本文:

http://www.zjujournals.com/eng/CN/10.3785/j.issn.1008-973X.2014.08.005    或    http://www.zjujournals.com/eng/CN/Y2014/V1/I8/1376

［1］ DAUGHTON C G, TERNES T A. Pharmaceuticals and personal care products in the environment: Agents of subtle change？ ［J］. Environmental Health Perspectives, 1999, 107(Suppl 6): 907.
［2］ JONES O A H, VOULVOULIS N, LESTER J N. Aquatic environmental assessment of the top 25 English prescription pharmaceuticals ［J］. Water research, 2002, 36(20): 5013-5022.
［3］ KOLPIN D, FURLONG E, MEUER M, et al. Pharmaceuticals, hormones, and other organic wastewater contaminants in US streams, 1999-2000: A national reconnaissance ［J］. Environmental science & technology, 2002, 36(6): 1202-1211.
［4］ KIM I, TANAKA H. Photodegradation characteristics of PPCPs in water with UV treatment ［J］. Environment international, 2009, 35(5): 793-802.
［5］ ANDERSEN K, LAUNER L J, OTT A, et al. Do nonsteroidal anti-inflammatory drugs decrease the risk for Alzheimer’s disease？ The Rotterdam Study ［J］. Neurology, 1995, 45(8): 1441-1445.
［6］ GASPARINI L, ONGINI E, WILCOCK D, et al. Activity of flurbiprofen and chemically related anti-inflammatory drugs in models of Alzheimer’s disease ［J］. Brain research reviews, 2005, 48(2): 400-408.
［7］ CASTELL J V, GOMEZ-LECHON M J, MIRANDA M A, et al. Phototoxicity of non-steroidal anti-inflammatory drugs:<i> in vitro</i> testing of the photoproducts of ButibufenandFlurbiprofen ［J］. Journal of Photochemistry and Photobiology B: Biology, 1992, 13(1): 71-81.
［8］ DOLL T E, FRIMMEL F H. Fate of pharmaceuticals-photodegradation by simulated solar UV-light ［J］. Chemosphere, 2003, 52(10): 1757-1769.
［9］ 张楠, 刘国光, 刘海津, 等. 双氯芬酸在水环境中光降解的初步研究［J］. 环境化学, 2013, 32(001): 42-47.
ZHANG Nan, LIU Guo-guang, LIU Hai-jin, etal. A preliminary study on photodegradation of diclofenac in water ［J］.Environmental Chemistry, 2013, 32(001): 42-47.
［10］ LI W, LU S, CHEN N, et al. Photo-degradation of clofibric acid by ultraviolet light irradiation at 185 nm ［J］. Water Science and Technology, 2009, 60(11): 2983-2989.
［11］ 刘小为. UV/O3降解水中新兴微污染物的特性与机理研究［D］. 哈尔滨: 哈尔滨工业大学, 2012.
LIU Xiao-wei. Characteristics and mechanism for degrandation of emerging micropollutants in water by UV/ozone process ［D］. Harbin: Harbin Institute of Technology, 2012.
［12］ WEI X, CHEN J, XIE Q, et al. Distinct photolytic mechanisms and products for different dissociation species of ciprofloxacin ［J］. Environmental science & technology, 2013, 47(9): 4284-4290.
［13］ GE L, CHEN J, WEI X, et al. Aquatic photochemistry of fluoroquinolone antibiotics: kinetics, pathways, and multivariate effects of main water constituents ［J］. Environmental science & technology, 2010, 44(7): 2400-2405.
［14］ 刘国光, 张楠, 张敏利. 4, 4-二溴联苯在水溶液中光降解的动力学研究［J］. 环境科学与技术, 2012, 35(012): 92-95.
LIU Guo-guang, ZHANG Nan, ZHANG Min-li. Photo-degradation kinetics of 4,4-dibromobiphenyl in aqueous solution ［J］. Environmental Science & Technology, 2012, 35(12): 92-95.
［15］ ZHANG S, CHEN J, QIAO X, et al. Quantum chemical investigation and experimental verification on the aquatic photochemistry of the sunscreen 2-phenylbenzimidazole-5-sulfonic acid ［J］. Environmental science & technology, 2010, 44(19): 7484-7490.
［16］ HUBICKA U, KRZEK J, UROMSKA B, et al. Determination of photostability and photod-egradation products of moxifloxacin in the presence of metal ions in solutions and solid phase. Kinetics and identification of photoproducts ［J］. Photochemical &Photo-biological Sciences, 2012, 11(2): 351-357.
［17］ CHEN S N, HOFFMAN M Z, PARSONS JR G H. Reactivity of the carbonate radical toward aromatic compounds in aqueous solution ［J］. The Journal of Physical Chemistry, 1975, 79(18): 1911-1912.
［18］ LARSON R A, ZEPP R G. Reactivity of the carbonate radical with aniline derivatives ［J］. Environmental toxicology and chemistry, 1988, 7(4): 265-274.
［19］ DELL’ARCIPRETE M L, SOLER J M, LUCAS SJ, et al. Reactivity of neonicotinoid insecticides with carbonate radicals ［J］. Water research, 2012: 3479-3489.
［20］ ZEPP R G, HOIGNE J, BADER H. Nitrate-induced photooxidation of trace organic chemicals in water ［J］. Environmental science & technology, 1987, 21(5): 443-450.
［21］ NEAMTU M, POPA D M, FRIMMEL F H. Simulated solar UV-irradiation of endocrine disrupting chemical octylphenol ［J］. Journal of hazardous materials, 2009, 164(2): 1561-1567.
［22］ MUSA K A K, ERIKSSON L A. Photochemical and photophysical properties, and photodegradation mechanism, of the non-steroid anti-inflammatory drug Flurbiprofen ［J］. Journal of Photochemistry and Photobiology A: Chemistry, 2009, 202(1): 48-56.
［23］ CHAO S H, HO H T, CHEN F A, et al. Identification of flurbiprofen and its photoproducts in methanol by gas chromatography-mass spectrometry ［J］. Biomedical Chromatography, 2007, 21(5): 527-533.
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