Removal, transformation and risk assessment of UV-filter BP9 during chlorination disinfection
LI Jia-qi1, DU Er-deng1,2, FAN Xin-xin1, YANG Yun-yi1, WANG Li-ping1
1. School of Environmental & Safety Engineering, Changzhou University, Changzhou 213164, China; 2. Nanjing Institute of Environmental Sciences, Ministry of Environmental Protection of the People's Republic of China, Nanjing 210042, China
Abstract:The issue of new disinfection by-products in drinking water is attracting increasing concern.Chlorination of a typical UV-filter benzophenone-9(BP9) was studied.The effect of initial BP9 concentration,initial residual chlorine,pH value,and ammonia nitrogen concentration on the reaction were also investigated.The degradation mechanism and the ecological risk were further discussed.The results indicated that,BP9 removal could reach 91.3% in 90s under the conditions of initial BP9 concentration 5mg/L,initial residual chlorine 5mg/L.BP9 chlorination process obeyed the pseudo-first-order kinetics.The degradation rate decreased with the increase of initial BP9 concentration and ammonia nitrogen concentration,while increased with the increase of initial residual chlorine.Neutral conditions are favorable for BP9 chlorination.Seven intermediates were identified by HPLC-MS/MS and GC-MS,and possible degradation pathways were also proposed.Luminescent bacteria experiment and ECOSAR prediction both showed that intermediates produced in BP9 chlorination have higher toxicity than the parent compound,which pose a potential risk to drinking water safety.
李佳琦, 杜尔登, 樊鑫鑫, 杨韵一, 王利平. 氯消毒中有机防晒剂BP9的去除转化与风险评价[J]. 中国环境科学, 2018, 38(3): 968-976.
LI Jia-qi, DU Er-deng, FAN Xin-xin, YANG Yun-yi, WANG Li-ping. Removal, transformation and risk assessment of UV-filter BP9 during chlorination disinfection. CHINA ENVIRONMENTAL SCIENCECE, 2018, 38(3): 968-976.
Liu Y S, Ying G G, Shareef A, et al. Occurrence and removal of benzotriazoles and ultraviolet filters in a municipal wastewater treatment plant[J]. Environmental Pollution, 2012,165:225-232.
[2]
Zhang Z, Ren N, Li Y F, et al. Determination of benzotriazole and benzophenone UV filters in sediment and sewage sludge[J]. Environmental Science and Technology, 2011,45(9):3909-3916.
[3]
Tsui M M, Leung H W, Lam P K, et al. Seasonal occurrence, removal efficiencies and preliminary risk assessment of multiple classes of organic UV filters in wastewater treatment plants[J]. Water Research, 2014,53:58-67.
[4]
Rodil R, Quintana J B, Concha-Graña E, et al. Emerging pollutants in sewage, surface and drinking water in Galicia (NW Spain)[J]. Chemosphere, 2012,86(10):1040-1049.
[5]
Fent K, Zenker A, Rapp M. Widespread occurrence of estrogenic UV-filters in aquatic ecosystems in Switzerland[J]. Environmental Pollution, 2010,158(5):1817-1824.
[6]
Wu M H, Xie D G, Xu G, et al. Benzophenone-type UV filters in surface waters:An assessment of profiles and ecological risks in Shanghai, China[J]. Ecotoxicology and Environmental Safety, 2017,141:235-241.
Buth J M, Arnold W A, Mcneill K. Unexpected products and reaction mechanisms of the aqueous chlorination of cimetidine[J]. Environmental Science and Technology, 2007,41(17):6228-6233.
Bedner M, Maccrehan W A. Transformation of acetaminophen by chlorination produces the toxicants 1,4-benzoquinone and N-acetyl-p-benzoquinone imine[J]. Environmental Science and Technology, 2006,40(2):516-522.
[13]
Xiao M, Wei D, Yin J, et al. Transformation mechanism of benzophenone-4in free chlorine promoted chlorination disinfection[J]. Water Research, 2013,47(16):6223-6233.
[14]
Sapozhnikova Y, Hedespeth M, Wirth E, et al. Analysis of selected natural and synthetic hormones by LC-MS-MS using the US EPA method 1694[J]. Analytical Methods, 2011,3(5):1079-1086.
[15]
纪夏玲.次氯酸钠氧化降解水体中萘普生的研究[D]. 广州:广东工业大学, 2015.
[16]
Du E D, Feng X X, Guo Y Q, et al. Dimethyl phthalate degradation by UV/H2O2:combination of experimental methods and quantum chemical calculation[J]. CLEAN-Soil, Air, Water, 2015,43(6):811-821.
Gallard H, Von G U. Chlorination of phenols:kinetics and formation of chloroform[J]. Environmental Science and Technology, 2002,36(5):884-890.
[20]
Rebenne L M, Gonzalez A C, Olson T M. Aqueous chlorination kinetics and mechanism of substituted dihydroxybenzenes[J]. Environmental Science and Technology, 1996,30(7):2235-2242.
[21]
Ge F, Zhu L, Chen H. Effects of pH on the chlorination process of phenols in drinking water[J]. Journal of Hazardous Materials, 2006,133(1):99-105.
Negreira N, Canosa P, Rodriguez I, et al. Study of some UV filters stability in chlorinated water and identification of halogenated by-products by gas chromatography-mass spectrometry[J]. Journal of Chromatography A, 2008,1178(1):206-214.
[25]
Xiao M, Wei D, Li L, et al. Formation pathways of brominated products from benzophenone-4chlorination in the presence of bromide ions[J]. Journal of Environmental Sciences, 2014,26(12):2387-2396.
[26]
Jones O, Voulvoulis N, Lester J. Aquatic environmental assessment of the top 25 English prescription pharmaceuticals[J]. Water Research, 2002,36(20):5013-5022.
[27]
Giddings J, Salvito D, Putt A. Acute toxicity of 4-amino musk xylene to Daphnia magna in laboratory water and natural water[J]. Water Research, 2000,34(14):3686-3689.
[28]
Yan C, Yang Y, Zhou J, et al. Antibiotics in the surface water of the Yangtze Estuary:occurrence, distribution and risk assessment[J]. Environmental Pollution, 2013,175:22-29.