模拟泳池水中氯化消毒副产物的生成规律
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摘要
以模拟泳池水为研究对象,研究不同的氯化时间、氯投加量、pH值、反应温度条件对泳池水在氯化消毒过程中生成消毒副产物(DBPs)的影响.研究结果表明:延长氯化反应时间,二氯乙酸(DCAA)、三氯乙酸(TCAA)和三氯甲烷(TCM)的浓度不断升高,二氯乙腈(DCAN)、三氯硝基甲烷(TCNM)和1,1,1-三氯丙酮(1,1,1-TCP)的浓度则先升高再降低.DBPs浓度在氯化反应的前24h增幅较大,48h后趋于平缓;随着氯投加量的增加,DCAA、TCAA、TCM、TCNM和1,1,1-TCP浓度一直呈上升趋势,而DCAN浓度则先升高再降低.在氯投加量为2mg/L时,DBPs的浓度较低;在pH值从6升高到8的过程中,DCAA、TCAA、DCAN和1,1,1-TCP浓度先升高再降低,TCM和TCNM浓度则一直升高.pH值在6～7范围内可有效控制DBPs的形成;随着反应温度的升高,DCAA、TCAA、TCM和TCNM浓度持续升高,DCAN和1,1,1-TCP则逐渐降低.综上所述,应合理调节泳池水的氯化消毒条件,在保证舒适度的同时有效控制DBPs的生成.
The objective of present study was to investigate the formation of disinfection by-products by simulated swimming pool water chlorination process under different conditions. Evaluated factors included chlorination time, chlorine dosages, p H and reaction temperature. The concentration of DCAA, TCAA and TCM increased constantly, the concentration of DCAN, TCNM and 1,1,1-TCP increased firstly and then decreased with the prolonged chlorination time. The concentration of DBPs increased significantly within 24 h of chlorination reaction, and became flat after 48 h. In response to increased dosage of chlorine, the concentration of DCAA, TCAA,TCM, TCNM and 1,1,1-TCP showed a tendency of increase, but the concentration of DCAN increased firstly and then decreased. The concentration of DBPs was lower when the chlorine dosage was controlled at 2 mg/L; With the p H increased from 6 to 8, the concentration of DCAA, TCAA, DCAN and 1,1,1-TCP initially increased and then decreased, and the concentration of TCM and TCNM increased gradually. When the p H was between 6 and 7, the formation of DBPs can be effectively controlled; With the increased of reaction temperature, the concentration of DCAA, TCAA, TCM and TCNM increased continuously, while the concentration of DCAN and 1,1,1-TCP decreased gradually. Overall, the chlorination conditions of the swimming pool water should be reasonably adjusted to effectively control the generation of DBPs and ensure the comfort level of the pool.
The objective of present study was to investigate the formation of disinfection by-products by simulated swimming pool water chlorination process under different conditions. Evaluated factors included chlorination time, chlorine dosages, p H and reaction temperature. The concentration of DCAA, TCAA and TCM increased constantly, the concentration of DCAN, TCNM and 1,1,1-TCP increased firstly and then decreased with the prolonged chlorination time. The concentration of DBPs increased significantly within 24 h of chlorination reaction, and became flat after 48 h. In response to increased dosage of chlorine, the concentration of DCAA, TCAA,TCM, TCNM and 1,1,1-TCP showed a tendency of increase, but the concentration of DCAN increased firstly and then decreased. The concentration of DBPs was lower when the chlorine dosage was controlled at 2 mg/L; With the p H increased from 6 to 8, the concentration of DCAA, TCAA, DCAN and 1,1,1-TCP initially increased and then decreased, and the concentration of TCM and TCNM increased gradually. When the p H was between 6 and 7, the formation of DBPs can be effectively controlled; With the increased of reaction temperature, the concentration of DCAA, TCAA, TCM and TCNM increased continuously, while the concentration of DCAN and 1,1,1-TCP decreased gradually. Overall, the chlorination conditions of the swimming pool water should be reasonably adjusted to effectively control the generation of DBPs and ensure the comfort level of the pool.
引文
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[2]Anipsitakis G P,Tufano T P,Dionysiou D D.Chemical and microbial decontamination of pool water using activated potassium peroxymonosulfate[J].Water Research,2008,42(12):2899-2910.
[3]Barbot E,Moulin P.Swimming pool water treatment by ultrafiltrationadsorption process[J].Journal of Membrane Science,2008,314(1/2):50-57.
[4]Judd S J,Bullock G.The fate of chlorine and organic materials in swimming pools[J].Chemosphere,2003,51(9):869-879.
[5]Weil L,Jandik J,Eichelsd E.Organic halogenated compounds in swimming pool water,Indetermination of volatile halogenated hydrocarbons[J].Z Wass Abwass Forsch,1980,13:165-169.
[6]Beech J A,Diaz R,Ordaz C,et al.Nitrates,chlorates and trihalomethanes in swimming pool water[J].American Journal of Public Health,1980,70(1):79-82.
[7]Chen M J,Lin C H,Duh J M,et al.Development of a multi-pathway probabilistic health risk assessment model for swimmers exposed to chloroform in indoor swimming pools[J].Journal of Hazardous Materials,2011,185(2/3):1037-1044.
[8]Richardson S D,Demarini D M,Kogevinas M,et al.What’s in the Pool?A Comprehensive identification of disinfection By-products and assessment of mutagenicity of chlorinated and brominated swimming pool water[J].Environmental Health Perspectives,2010,118(11):1523-1530.
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[11]Thickett K M,Mccoach J S,Gerber J M,et al.Occupational asthma caused by chloramines in indoor swimming-pool air[J].European Respiratory Journal,2002,19(5):827-832.
[12]Richardson S D,Plewa M J,Wagner E D,et al.Occurrence,genotoxicity,and carcinogenicity of regulated and emerging disinfection by-products in drinking water:a review and roadmap for research[J].Mutation Research-Reviews in Mutation Research,2007,636(1-3):178-242.
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[15]Kanan A,Karanfil T.Formation of disinfection by-products in indoor swimming pool water:the contribution from filling water natural organic matter and swimmer body fluids[J].Water Research,2011,45(2):926-932.
[16]Caro J,Gallego M.Assessment of exposure of workers and swimmers to trihalomethanes in an indoor swimming pool[J].Environmental Science&Technology,2007,41(13):4793-4798.
[17]Villanueva C M,Cantor K P,Grimalt J O,et al.Bladder cancer and exposure to water disinfection by-products through ingestion,bathing,showering,and swimming in pools[J].American Journal of Epidemiology,2007,165(2):148-156.
[18]Liviac D,Wagner E D,Mitch W A,et al.Genotoxicity of water concentrates from recreational pools after various disinfection methods[J].Environmental Science&Technology,2010,44(9):3527-3532.
[19]Munch D J,Hautman D J.Method 551.1:Determination of chlorination disinfection byproducts,chlorinated solvents,and halogenated pesticides/herbicides in drinking water by liquid-liquid extraction and gas chromatography with electron-capture detection[M].National Exposure Research Laboratory Office of Research and Development U.S.Environmental Protection Agency.1995.
[20]Gallard H,Von G U.Chlorination of natural organic matter:kinetics of chlorination and of THM formation[J].Water Research,2002,36(1):65-74.
[21]Nikolaou A D,Lekkas T D,Golfinopoulos S K.Kinetics of the formation and decomposition of chlorination by-products in surface waters[J].Chemical Engineering Journal,2004,100(1-3):139-148.
[22]Westerhoff P,Chao P,Mash H.Reactivity of natural organic matter with aqueous chlorine and bromine[J].Water Research,2004,38(6):1502-1513.
[23]Glezer V,Harris B,Tal N,et al.Hydrolysis of haloacetonitriles:linear free energy relationship,kinetics and products[J].Water Research,1999,33(8):1938-1948.
[24]Chu W H,Gao N Y,Deng Y,et al.Precursors of dichloroacetamide,an emerging nitrogenous DBP formed during chlorination or chloramination[J].Environmental Science&Technology,2010,44(10):3908-3912.
[25]Reckhow D A,Singer P C,Malcolm R L.Chlorination of humic materials:byproduct formation and chemical interpretations[J].Environmental Science&Technology,1990,24(11):1655-1664.
[26]CJ 244-2007游泳池水质标准[S].CJ 244-2007 Water quality standards for swimming pools[S].
[27]Hua G,Reckhow D A.Characterization of disinfection byproduct precursors based on hydrophobicity and molecular size[J].Environmental Science&Technology,2007,41(9):3309-3315.
[28]Hong H C,Wong M H,Liang Y.Amino acids as precursors of trihalomethane and haloacetic acid formation during chlorination[J].Archives of Environmental Contamination&Toxicology,2009,56(4):638-645.
[29]方晶云.蓝藻细胞及藻类有机物在氯化消毒中副产物的形成机理与控制[D].哈尔滨:哈尔滨工业大学,2010.Fang J Y.Formation and control of disinfection by-products in chlorination of blue-green algae and algal organic matter(AOM)[D].Harbin:Harbin Institute of Technology,2010.
[30]Hua G,Reckhow D A.DBP formation during chlorination and chloramination:Effect of reaction time,pH,dosage,and temperature[J].Journal American Water Works Association,2008,100(8):82-95.
[31]李林林,刘佳蒙,宋弼尧,等.饮用水中典型微生物消毒过程中消毒副产物的生成规律[J].中国环境科学,2016,36(12):3631-3638.Li L L,Liu J M,Song B Y,et al.Formation of major disinfection by-products from representative microorganisms during drinking water chlorination[J].China Environmental Science,2016,36(12):3631-3638.
[32]Hu J.Exploring formation and distribution of halonitromethanes in drinking waters[D].Clemson,SC:Clemson University,2009.
[33]Li J,Blatchley III E R.Volatile disinfection byproduct formation resulting from chlorination of organic-nitrogen precursors in swimming pools[J].Environmental Science&Technology,2007,41(19):6732-6739.
[34]Plewa M J.Comparative mammalian cell toxicity of N-DBPs and C-DBPs[J].Acs Symposium,2008,995:36-50.
[35]Kramer M,Hübner I,R?rden O,et al.Haloacetonitriles-another important group of disinfection byproducts in swimming pool water[C].London,UK:Swimming Pool&Spa International Conference,2009.
[36]Lifongo L L,Bowden D J,Brimblecombe P.Thermal degradation of haloacetic acids in water[J].International Journal of Physical Sciences,2010,5(6):738-747.
[37]孙兴滨,胡阳,袁婷,等.高锰酸钾预氧化对剑水蚤DBPsFP的去除特征研究[J].中国环境科学,2015,35(11):3296-3302.Sun X B,Hu Y,Yuan T,et al.The removal characteristic of DBPsFPby potassium permanganate preoxidation during chlorination of Cyclops metabolite[J].China Environmental Science,2015,35(11):3296-3302.
[38]Nikolaou A D,Golfinopoulos S K,Kostopoulou M N,et al.Decomposition of dihaloacetonitriles in water solutions and fortified drinking water samples[J].Chemosphere,2000,41(8):1149-1154.
[2]Anipsitakis G P,Tufano T P,Dionysiou D D.Chemical and microbial decontamination of pool water using activated potassium peroxymonosulfate[J].Water Research,2008,42(12):2899-2910.
[3]Barbot E,Moulin P.Swimming pool water treatment by ultrafiltrationadsorption process[J].Journal of Membrane Science,2008,314(1/2):50-57.
[4]Judd S J,Bullock G.The fate of chlorine and organic materials in swimming pools[J].Chemosphere,2003,51(9):869-879.
[5]Weil L,Jandik J,Eichelsd E.Organic halogenated compounds in swimming pool water,Indetermination of volatile halogenated hydrocarbons[J].Z Wass Abwass Forsch,1980,13:165-169.
[6]Beech J A,Diaz R,Ordaz C,et al.Nitrates,chlorates and trihalomethanes in swimming pool water[J].American Journal of Public Health,1980,70(1):79-82.
[7]Chen M J,Lin C H,Duh J M,et al.Development of a multi-pathway probabilistic health risk assessment model for swimmers exposed to chloroform in indoor swimming pools[J].Journal of Hazardous Materials,2011,185(2/3):1037-1044.
[8]Richardson S D,Demarini D M,Kogevinas M,et al.What’s in the Pool?A Comprehensive identification of disinfection By-products and assessment of mutagenicity of chlorinated and brominated swimming pool water[J].Environmental Health Perspectives,2010,118(11):1523-1530.
[9]Chiswell B,Wildsoet C F.The causes of eye irritation in swimming pools[J].Water Science&Technology,1989,21(2):241-244.
[10]Erdinger L,Kirsch F,Sonntag H G.Irritating effects of disinfection by-products in swimming pools[J].Zentralblatt für Hygiene und Umweltmedizin,1998,200(5/6):491-503.
[11]Thickett K M,Mccoach J S,Gerber J M,et al.Occupational asthma caused by chloramines in indoor swimming-pool air[J].European Respiratory Journal,2002,19(5):827-832.
[12]Richardson S D,Plewa M J,Wagner E D,et al.Occurrence,genotoxicity,and carcinogenicity of regulated and emerging disinfection by-products in drinking water:a review and roadmap for research[J].Mutation Research-Reviews in Mutation Research,2007,636(1-3):178-242.
[13]Goodman M,Hays S.Asthma and swimming:a meta-analysis[J].Journal of Asthma Research,2008,45(8):639-647.
[14]Karanfil T.Recent advances in disinfection by-product formation,occurrence,control,health effects,and regulations[J].ACSSymposium Series,2008,995:2-19.
[15]Kanan A,Karanfil T.Formation of disinfection by-products in indoor swimming pool water:the contribution from filling water natural organic matter and swimmer body fluids[J].Water Research,2011,45(2):926-932.
[16]Caro J,Gallego M.Assessment of exposure of workers and swimmers to trihalomethanes in an indoor swimming pool[J].Environmental Science&Technology,2007,41(13):4793-4798.
[17]Villanueva C M,Cantor K P,Grimalt J O,et al.Bladder cancer and exposure to water disinfection by-products through ingestion,bathing,showering,and swimming in pools[J].American Journal of Epidemiology,2007,165(2):148-156.
[18]Liviac D,Wagner E D,Mitch W A,et al.Genotoxicity of water concentrates from recreational pools after various disinfection methods[J].Environmental Science&Technology,2010,44(9):3527-3532.
[19]Munch D J,Hautman D J.Method 551.1:Determination of chlorination disinfection byproducts,chlorinated solvents,and halogenated pesticides/herbicides in drinking water by liquid-liquid extraction and gas chromatography with electron-capture detection[M].National Exposure Research Laboratory Office of Research and Development U.S.Environmental Protection Agency.1995.
[20]Gallard H,Von G U.Chlorination of natural organic matter:kinetics of chlorination and of THM formation[J].Water Research,2002,36(1):65-74.
[21]Nikolaou A D,Lekkas T D,Golfinopoulos S K.Kinetics of the formation and decomposition of chlorination by-products in surface waters[J].Chemical Engineering Journal,2004,100(1-3):139-148.
[22]Westerhoff P,Chao P,Mash H.Reactivity of natural organic matter with aqueous chlorine and bromine[J].Water Research,2004,38(6):1502-1513.
[23]Glezer V,Harris B,Tal N,et al.Hydrolysis of haloacetonitriles:linear free energy relationship,kinetics and products[J].Water Research,1999,33(8):1938-1948.
[24]Chu W H,Gao N Y,Deng Y,et al.Precursors of dichloroacetamide,an emerging nitrogenous DBP formed during chlorination or chloramination[J].Environmental Science&Technology,2010,44(10):3908-3912.
[25]Reckhow D A,Singer P C,Malcolm R L.Chlorination of humic materials:byproduct formation and chemical interpretations[J].Environmental Science&Technology,1990,24(11):1655-1664.
[26]CJ 244-2007游泳池水质标准[S].CJ 244-2007 Water quality standards for swimming pools[S].
[27]Hua G,Reckhow D A.Characterization of disinfection byproduct precursors based on hydrophobicity and molecular size[J].Environmental Science&Technology,2007,41(9):3309-3315.
[28]Hong H C,Wong M H,Liang Y.Amino acids as precursors of trihalomethane and haloacetic acid formation during chlorination[J].Archives of Environmental Contamination&Toxicology,2009,56(4):638-645.
[29]方晶云.蓝藻细胞及藻类有机物在氯化消毒中副产物的形成机理与控制[D].哈尔滨:哈尔滨工业大学,2010.Fang J Y.Formation and control of disinfection by-products in chlorination of blue-green algae and algal organic matter(AOM)[D].Harbin:Harbin Institute of Technology,2010.
[30]Hua G,Reckhow D A.DBP formation during chlorination and chloramination:Effect of reaction time,pH,dosage,and temperature[J].Journal American Water Works Association,2008,100(8):82-95.
[31]李林林,刘佳蒙,宋弼尧,等.饮用水中典型微生物消毒过程中消毒副产物的生成规律[J].中国环境科学,2016,36(12):3631-3638.Li L L,Liu J M,Song B Y,et al.Formation of major disinfection by-products from representative microorganisms during drinking water chlorination[J].China Environmental Science,2016,36(12):3631-3638.
[32]Hu J.Exploring formation and distribution of halonitromethanes in drinking waters[D].Clemson,SC:Clemson University,2009.
[33]Li J,Blatchley III E R.Volatile disinfection byproduct formation resulting from chlorination of organic-nitrogen precursors in swimming pools[J].Environmental Science&Technology,2007,41(19):6732-6739.
[34]Plewa M J.Comparative mammalian cell toxicity of N-DBPs and C-DBPs[J].Acs Symposium,2008,995:36-50.
[35]Kramer M,Hübner I,R?rden O,et al.Haloacetonitriles-another important group of disinfection byproducts in swimming pool water[C].London,UK:Swimming Pool&Spa International Conference,2009.
[36]Lifongo L L,Bowden D J,Brimblecombe P.Thermal degradation of haloacetic acids in water[J].International Journal of Physical Sciences,2010,5(6):738-747.
[37]孙兴滨,胡阳,袁婷,等.高锰酸钾预氧化对剑水蚤DBPsFP的去除特征研究[J].中国环境科学,2015,35(11):3296-3302.Sun X B,Hu Y,Yuan T,et al.The removal characteristic of DBPsFPby potassium permanganate preoxidation during chlorination of Cyclops metabolite[J].China Environmental Science,2015,35(11):3296-3302.
[38]Nikolaou A D,Golfinopoulos S K,Kostopoulou M N,et al.Decomposition of dihaloacetonitriles in water solutions and fortified drinking water samples[J].Chemosphere,2000,41(8):1149-1154.