title: Progressive Increase in Disinfection Byproducts and Mutagenicity from Source to Tap to Swimming Pool and Spa Water: Impact of Human Inputs.
abstract: Pools and spas are enjoyed throughout the world for exercise and relaxation. However, there are no previous studies on mutagenicity of disinfected spa (hot tub) waters or comprehensive identification of disinfection byproducts (DBPs) formed in spas. Using 28 water samples from seven sites, we report the first integrated mutagenicity and comprehensive analytical chemistry of spas treated with chlorine, bromine, or ozone, along with pools treated with these same disinfectants. Gas chromatography (GC) with high-resolution mass spectrometry, membrane-introduction mass spectrometry, and GC-electron capture detection were used to comprehensively identify and quantify DBPs and other contaminants. Mutagenicity was assessed by the Salmonella mutagenicity assay. More than 100 DBPs were identified, including a new class of DBPs, bromoimidazoles. Organic extracts of brominated pool/spa waters were 1.8× more mutagenic than chlorinated ones; spa waters were 1.7× more mutagenic than pools. Pool and spa samples were 2.4 and 4.1× more mutagenic, respectively, than corresponding tap waters. The concentration of the sum of 21 DBPs measured quantitatively increased from finished to tap to pool to spa; and mutagenic potency increased from finished/tap to pools to spas. Mutagenic potencies of samples from a chlorinated site correlated best with brominated haloacetic acid concentrations (Br-HAAs) (r = 0.98) and nitrogen-containing DBPs (N-DBPs) (r = 0.97) and the least with Br-trihalomethanes (r = 0.29) and Br-N-DBPs (r = 0.04). The mutagenic potencies of samples from a brominated site correlated best (r = 0.82) with the concentrations of the nine HAAs, Br-HAAs, and Br-DBPs. Human use increased significantly the DBP concentrations and mutagenic potencies for most pools and spas. These data provide evidence that human precursors can increase mutagenic potencies of pools and spas and that this increase is associated with increased DBP concentrations.
authors.affiliation: Student Services Authority, U.S. Environmental Protection Agency, National Exposure Research Laboratory, Athens, Georgia 30605, United States.
authors.forename: Eric J
authors.initials: EJ
authors.lastname: Daiber
authors.affiliation: National Health and Environmental Effects Research Laboratory, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina 27711, United States.
authors.forename: David M
authors.initials: DM
authors.lastname: DeMarini
authors.affiliation: Student Services Authority, U.S. Environmental Protection Agency, National Exposure Research Laboratory, Athens, Georgia 30605, United States.
authors.forename: Sridevi A
authors.initials: SA
authors.lastname: Ravuri
authors.affiliation: Department of Chemistry and Biochemistry, University of South Carolina , 631 Sumter St., Columbia, South Carolina 29208, United States.
authors.forename: Hannah K
authors.initials: HK
authors.lastname: Liberatore
authors.affiliation: Department of Chemistry and Biochemistry, University of South Carolina , 631 Sumter St., Columbia, South Carolina 29208, United States.
authors.forename: Amy A
authors.initials: AA
authors.lastname: Cuthbertson
authors.affiliation: Department of Chemistry and Biochemistry, University of South Carolina , 631 Sumter St., Columbia, South Carolina 29208, United States.
authors.forename: Alexis
authors.initials: A
authors.lastname: Thompson-Klemish
authors.affiliation: LECO Corp., 3000 Lakeview Ave., St. Joseph, Michigan 49085, United States.
authors.forename: Jonathan D
authors.initials: JD
authors.lastname: Byer
authors.affiliation: National Health and Environmental Effects Research Laboratory, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina 27711, United States.
authors.forename: Judith E
authors.initials: JE
authors.lastname: Schmid
authors.affiliation: Lyles School of Civil Engineering, Purdue University , 550 Stadium Mall Drive, West Lafayette, Indiana 47907, United States.
authors.forename: Mehrnaz Z
authors.initials: MZ
authors.lastname: Afifi
authors.affiliation: Lyles School of Civil Engineering, Purdue University , 550 Stadium Mall Drive, West Lafayette, Indiana 47907, United States.|Division of Environmental & Ecological Engineering, Purdue University , 500 Central Drive, West Lafayette, Indiana 47907, United States.
authors.forename: Ernest R
authors.initials: ER
authors.lastname: Blatchley
authors.affiliation: Department of Chemistry and Biochemistry, University of South Carolina , 631 Sumter St., Columbia, South Carolina 29208, United States.
authors.forename: Susan D
authors.initials: SD
authors.lastname: Richardson
mesh_terms: D004202:Disinfectants / Q000737:chemistry; D004203:Disinfection; D006801:Humans; D009153:Mutagens; D013551:Swimming Pools; D014867:Water; D014874:Water Pollutants, Chemical
chemical_list: D004202:Disinfectants; D009153:Mutagens; D014874:Water Pollutants, Chemical; D014867:Water