title: Comparison of chlorination and chloramination in carbonaceous and nitrogenous disinfection byproduct formation potentials with prolonged contact time.
abstract: Due to decreasing water demands in Japan, hydraulic retention times of water in piped supply systems has been extended, resulting in a longer contact time with disinfectants. However, the effects of extended contact time on the formation of various disinfection byproducts (DBPs), including carbonaceous DBPs such as trihalomethane (THM) and haloacetic acid (HAA), and nitrogenous DBPs such as nitrosodimethylamine (NDMA) and nitrosomorpholine (NMor), have not yet been investigated in detail. Herein, we compared the formation of these DBPs by chlorination and chloramination for five water samples collected from rivers and a dam in Japan, all of which represent municipal water supply sources. Water samples were treated by either filtration or a combination of coagulation and filtration. Treated samples were subjected to a DBP formation potential test by either chlorine or chloramine for contact times of 1 day or 4 days. Four THM species, nine HAA species, NDMA, and NMor were measured by GC-ECD or UPLC-MS/MS. Lifetime cancer risk was calculated based on the Integrated Risk Information System unit risk information. The experiment and analysis focused on (i) prolonged contact time from 1 day to 4 days, (ii) reduction efficiency by conventional treatment, (iii) correlations between DBP formation potentials and water quality parameters, and (iv) the contribution of each species to total risk. With an increased contact time from 1 day to 4 days, THM formation increased to 420% by chloramination. Coagulation-filtration treatment showed that brominated species in THMs are less likely to be reduced. With the highest unit risk among THM species, dibromochloromethane (DBCM) showed a high correlation with bromine, but not with organic matter parameters. NDMA contributed to lifetime cancer risk. The THM formation pathway should be revisited in terms of chloramination and bromine incorporation. It is also recommended to investigate nitrosamine formation potential by chloramination.
authors.affiliation: Department of Urban Engineering, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan. Electronic address: h_sakai@env.t.u-tokyo.ac.jp.
authors.forename: Hiroshi
authors.initials: H
authors.lastname: Sakai
authors.affiliation: Hitachi, Ltd., 6-6, Marunouchi 1, Chiyoda-ku, Tokyo, 100-8280, Japan.
authors.forename: Shunsuke
authors.initials: S
authors.lastname: Tokuhara
authors.affiliation: Fukushima Medical University, 1, Hikariga-oka, Fukushima City, 960-1295, Japan; Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo, 153-8505, Japan.
authors.forename: Michio
authors.initials: M
authors.lastname: Murakami
authors.affiliation: National Institute of Public Health, 2-3-6 Minami, Wako-shi, Saitama 351-0197, Japan.
authors.forename: Koji
authors.initials: K
authors.lastname: Kosaka
authors.affiliation: Department of Urban Engineering, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.
authors.forename: Kumiko
authors.initials: K
authors.lastname: Oguma
authors.affiliation: Department of Urban Engineering, School of Engineering, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.
authors.forename: Satoshi
authors.initials: S
authors.lastname: Takizawa
mesh_terms: D000586:Amination; D002700:Chloramines / Q000737:chemistry*; D002713:Chlorine / Q000737:chemistry*; D004202:Disinfectants / Q000737:chemistry*; D060766:Drinking Water / Q000032:analysis*; D004784:Environmental Monitoring; D006016:Glycolates / Q000032:analysis; D054879:Halogenation; D006812:Humic Substances / Q000032:analysis; D007564:Japan; D060106:Lakes / Q000032:analysis; D009602:Nitrosamines / Q000032:analysis; D045483:Rivers; D013997:Time Factors; D022882:Trihalomethanes / Q000032:analysis; D014874:Water Pollutants, Chemical / Q000032:analysis*; D018508:Water Purification
chemical_list: D002700:Chloramines; D004202:Disinfectants; D060766:Drinking Water; D006016:Glycolates; D006812:Humic Substances; D009602:Nitrosamines; D022882:Trihalomethanes; D014874:Water Pollutants, Chemical; D002713:Chlorine; C030816:chloramine
keywords: Cancer risk; Contact time; Disinfection byproduct; Haloacetic acid (HAA); Nitrosodimethylamine (NDMA); Nitrosomorpholine (NMor); Speciation; Species; Trihalomethane (THM)