双酚A在河口水中的光解动力学

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摘要

为研究双酚A（BPA）在河口水中的光解动力学及水中重要溶解性组分对其光解的影响，在广西钦州大榄江连接茅尾海的河口水域采取水样，通过模拟日光实验研究了河口水中BPA的光解动力学，及河口水中的重要溶解性组分Cl^-，Br^-，溶解性有机质（DOM），NO₃^-和HCO₃^-对BPA光解的影响.结果表明，河口水中BPA的光解速率常数k值比纯水中大，且上游水样中BPA的k值是下游水样的2.5倍.稳态光解实验表明DOM及其与卤素离子作用显著影响BPA的光解，虽然NO₃^-也影响BPA光解，但与DOM共存时，NO₃^-的影响不明显.自由基淬灭和竞争反应动力学实验发现激发三重态DOM（³DOM^*）和卤素自由基（HRS）是决定河口水样中BPA光降解的主要活性物种，且³DOM^*与BPA的反应活性（二级反应速率常数k_3DOM*，BPA=4.42×10⁸L/（mol·s）要高于HRS与BPA的反应活性（k_BPA，Cl·=2.11×10⁸L/（mol·s），k_BPA，Cl2·-=8.5×10⁶L/（mol·s）.下游水样中高含量的卤素离子（292mmol/L）易淬灭³DOM^*产生反应活性较低的HRS，致使下游水体中BPA的光解速率低于上游水体.

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关键词 ：双酚A, 河口水, 光解动力学, 激发三重态溶解性有机质, 卤素自由基, 二级反应速率常数

Abstract：

To study the photodegradation kinetics of bisphenol A (BPA) and the photolysis effect of the main water components in estuarine water, the real water sample was collected in the estuarine waters connecting the Maowei Sea and the Dalan River in Qinzhou city, China. The photodegradation kinetics of BPA in estuarine water sample and the effects of Cl^-, Br^-, dissolved organic matter (DOM), NO₃^-, HCO₃^-, and ionic strength on the photolysis of BPA were studied by simulated sunlight experiment. The results showed that the photolysis rate constant (k) value of BPA in estuarine water was higher than that in pure water, and the k value of BPA in the upstream water sample was 2.5 times as compared to the downstream water sample. Steady-state photolysis experiments showed that DOM and its interaction with halogen ions significantly affect the photolysis of BPA. Although NO₃^- also affected the photodegradation kinetics of BPA, the effect of NO₃^- was not obvious when it was concomitant with DOM. Radical quenching and competitive reaction kinetics experiments found that the triplet-excited state DOM (³DOM*) and halogen radicals (HRS) are the main reactive species that dominate the photodegradation of BPA in estuarine water samples. Moreover, the reactivity of ³DOM* with BPA (second-order reaction rate constant, k_3DOM*,BPA=4.42×10⁸L/(mol·s) was higher than that of HRS with BPA (k_BPA,Cl·=2.11×10⁸L/(mol·s),k_BPA,Cl2·-=8.5×10⁶L/(mol·s). The relatively high concentrations of halide ions (292mmol/L) in downstream water samples can easily quench ³DOM* to generate HRS with relatively low reactivity towards BPA,which can explain the phenomenon that the photolysis rate constant of BPA in the downstream water sample was lower than that of the upstream water sample.

Key words： bisphenol A estuarine water photodegradation kinetics triplet-excited state dissolved organic matter halogen radicals second-order reaction rate constant

收稿日期: 2019-09-19

PACS:

X522

基金资助:

国家自然科学基金资助项目（21707058）；云南省优秀青年基金资助项目（2019FI004）；昆明理工大学引进高层次人才学科建设经费资助项目（1411909411）

通讯作者: 李英杰,副教授,liyingjie08@163.com E-mail: liyingjie08@163.com

作者简介: 房岐(1994-),男,陕西咸阳人,硕士研究生,主要研究方向为水环境中新兴有机微污染物的光化学迁移与转化.发表论文3篇.

引用本文:

房岐, 徐子豪, 刘宁彧, 赵群, 田森林, 李英杰. 双酚A在河口水中的光解动力学[J]. 中国环境科学, 2020, 40(4): 1659-1666. FANG Qi, XU Zi-hao, LIU Ning-yu, ZHAO Qun, TIAN Sen-lin, LI Ying-jie. Photodegradation kinetics of bisphenol A in estuarine water. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(4): 1659-1666.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2020/V40/I4/1659

[1]	Klecka G M, Staples C A, Clark K E, et al. Exposure analysis of bisphenol A in surface water systems in America and Europe[J]. Environmental Science and Technology, 2009,43(16):6145-6150.
[2]	Mihaich E, Staples C, Ortego L, et al. Life-cycle studies with 2marine species and bisphenol A:The mysid shrimp (Americamysis bahia) and sheepshead minnow (Cyprinodon variegatus)[J]. Environmental Toxicology and Chemistry, 2018,37(2):398-410.
[3]	Staples C, Hoeven N V D, Clark K, et al. Distributions of concentrations of bisphenol A in North American and European surface waters and sediments determined from 19years of monitoring data[J]. Chemosphere, 2018,201:448-458.
[4]	Andra S S, Austin C, Yang J, et al. Recent advances in simultaneous analysis of bisphenol A and its conjugates in human matrices:Exposure biomarker perspectives[J]. Science of the Total Environment, 2016,572:770-781.
[5]	Barbier E B, Hacker S D, Kennedy C, et al. The value of estuarine and coastal ecosystem services[J]. Ecological Monographs, 2011,81(2):169-193.
[6]	陈玫宏,郭敏,刘丹,等.典型内分泌干扰物在太湖及其支流水体和沉积物中的污染特征[J]. 中国环境科学, 2017,37(11):4323-4332. Chen M H, Guo M, Liu D, et al. Occurrence and distribution of typical endocrine disruptors in surface water and sediments from Taihu Lake and its tributaries[J]. China Environmental Science, 2017,37(11):4323~4332
[7]	Huang Y Q, Wong C K C, Zheng J S, et al. Bisphenol A (BPA) in China:A review of sources, environmental levels, and potential human health impacts[J]. Environment International, 2012,42(1):91-99.
[8]	展漫军,杨曦,杨洪生,等.天然水体腐殖质对双酚A光降解影响的研究[J]. 环境科学学报, 2005,25(6):816-820. Zhan M J, Yang X, Yang H H, et al. Study on the effect of natural aquatic humic substances on the photodegradation of bisphenol A[J]. Acta Scientiae Circumstantiae, 2005,25(6):816-820.
[9]	Wenk J, Gunten U V, Canonica S. Effect of dissolved organic matter on the transformation of contaminants induced by excited triplet states and the hydroxyl radical[J]. Environmental Science and Technology, 2011,45(4):1334-1340.
[10]	Varanasi L, Coscarelli E, Khaksari M, et al. Transformations of dissolved organic matter induced by UV photolysis, hydroxyl radicals, chlorine radicals, and sulfate radicals in aqueous-phase UV-Based advanced oxidation processes[J]. Water Research, 2018,135:22-30.
[11]	Parker K M, Mitch W A. Halogen radicals contribute to photooxidation in coastal and estuarine waters[J]. Proceedings of the National Academy of Sciences, 2016,113(21):5868-5873.
[12]	Parker K M, Reichwaldt E S, Ghadouani A, et al. Halogen radicals promote the photodegradation of microcystins in estuarine systems[J]. Environmental Science and Technology, 2016,50(16):8505-8513.
[13]	Vione D, Minella M, Maurino V, et al. Indirect Photochemistry in sunlit surface waters:photoinduced production of reactive transient species[J]. Chemistry-A European Journal, 2014,20(34):10590-10606.
[14]	Zhao Q, Fang Q, Liu H Y, et al. Halide-specific enhancement of photodegradation for sulfadiazine in estuarine waters:Roles of halogen radicals and main water constituents[J]. Water Research, 2019,160:209-216.
[15]	GB/T8538-2008饮用天然矿泉水检测方法[S]. GB/T8538-2008 Methods for examination of drinking natural mineral water[S].
[16]	Fang J, Fu Y, Shang C. The roles of reactive species in micropollutant degradation in the UV/free chlorine system[J]. Environmental Science and Technology, 2014,48(3):1859-1868.
[17]	Wu Z H, Guo K H, Fang J Y, et al. Factors affecting the roles of reactive species in the degradation of micropollutants by the UV/chlorine process[J]. Water Research, 2017,126:351-360.
[18]	Zhou C, Chen J, Xie H, et al. Modeling photodegradation kinetics of organic micropollutants in water bodies:A case of the Yellow River estuary[J]. Journal of hazardous materials, 2018,349:60-67.
[19]	Li Y J, Wei X X, Chen J W, et al. Photodegradation mechanism of sulfonamides with excited triplet state dissolved organic matter:A case sulfadidazine with 4-carboxybenzophenone as a proxy[J]. Journal of Hazardous Materials, 2015,290:9-15.
[20]	Buxton G V, Greenstock C L, Helman W P, et al. Critical Review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (·OH/·O- in Aqueous Solution[J]. Journal of Physical and Chemical Reference Data, 1988,17(2):513-886.
[21]	Canonica S, Hellrung B, MüllerPavel, et al. aqueous oxidation of phenylurea herbicides by triplet aromatic ketones[J]. Environmental Science and Technology, 2006,40(21):6636-6641.
[22]	Canonica S. Oxidation of aquatic organic contaminants induced by excited triplet ttates[J]. CHIMIA International Journal for Chemistry, 2007,61(10):641-644.
[23]	Vione D, Scozzaro A. The photochemistry of surface freshwaters in the framework of climate change[J]. Environmental Science and Technology, 2019,53(14):7945-7963.
[24]	Pedersen E J, Urbansky E T, Mariñas B J, et al. Formation of cyanogen chloride from the reaction of monochloramine with formaldehyde[J]. Environmental Science and Technology, 1999, 33(23):4239-4249.
[25]	Kim E, Ahn H, Jo H Y, et al. Chlorite alteration in aqueous solutions and uranium removal by altered chlorite[J]. Journal of Hazardous Materials, 2017,327:161-170.
[26]	Zhang K, Parker, Kimberly M. Halogen radical oxidants in natural and engineered aquatic systems.[J]. Environmental Science and Technology, 2018,17(52):9579-9594.
[27]	Zhang W Q, Zhou S Q, Sun J L, et al. Impact of chloride ions on UV/H2O2 and UV/persulfate advanced oxidation processes[J]. Environmental Science and Technology, 2018,52(13):7380-7389.
[28]	Sun P, Lee W N, Zhang R, et al. Degradation of DEET and caffeine under UV/chlorine and simulated sunlight/chlorine conditions[J]. Environmental Science and Technology, 2016,24(50):13265-13273.
[29]	Wang C, Zhu L, Wei M, et al. Photolytic reaction mechanism and impacts of coexisting substances on photodegradation of bisphenol A by Bi2WO6 in water[J]. Water Research, 2012,46(3):845-853.
[30]	Espinoza L A T, Neamtu M, Frimmel F H. The effect of nitrate, Fe (III) and bicarbonate on the degradation of bisphenol A by simulated solar UV-irradiation[J]. Water Research, 2007,41(19):4479-4487.
[31]	刘相良,张彪军,房岐,等.海水溶解组分复合作用对磺胺吡啶光解的影响[J]. 中国环境科学, 2018,38(8):3029-3034. Liu X L, Zhang B J, Fang Q, et al. Multivariate effects of dissolved seawater components on photodegradation of sulfapyridine.[J]. China Environmental Science, 2018,38(8):3029-3034.
[32]	Vione D, Khanra S, Man S C, et al. Inhibition vs. enhancement of the nitrate-induced phototransformation of organic substrates by the ·OH scavengers bicarbonate and carbonate[J]. Water Research, 2009, 43:4718-4728.
[33]	Zhou Y, Gao Y, Pang S Y, et al. Oxidation of fluoroquinolone antibiotics by peroxymonosulfate without activation:Kinetics, products, and antibacterial deactivation[J]. Water Research, 2018,145:210-219.
[34]	Sun P Z, Meng T, Wang Z J, et al. Degradation of organic micro-pollutants in UV/NH2Cl advanced oxidation process[J]. Environmental Science and Technology, 2019,53(15):9024-9033.
[35]	Grebel J E, Pignatello J J, Mitch W A. Sorbic acid as a quantitative probe for the formation, scavenging and steady-state concentrations of the triplet-excited state of organic compounds[J]. Water Research, 2011,45:6535-6544.