United States Environmental Protection Agency Municipal Environmental Research ^ Laboratory " Cincinnati OH 45268 Research and Development EPA-600/S2-82-017 Sept. 1982 Project Summary Nonvolatile Organics in Disinfected Wastewater Effluents: Chemical Characterization and Mutagenicity R. L Jolley, R. B. Cumming, N. E. Lee, L R. Lewis, J. E. Thompson, W. W. Pitt, M. S. Denton, and S. J. Hartman The overall objectives of this research program were to examine the effects of three disinfectants on the chemical composition and mutagenic activity of wastewater effluents. The disinfec- tants studied were chlorine, ozone, and ultraviolet light. Nine different treatment plant efflu- ents were examined before and after disinfection (Table 1); fractions of con- centrates were isolated to determine the identity of mutagenic components. The investigation used the following methodology: grab sample collection, concentration by lyophilization, high- pressure liquid chromatography (both analytical and preparative scales), and mass spectrometry. Mutagenic activity was determined largely by the Ames Bacterial Test Method using two strains of organisms (TA 1535 and TA 1538). On one occasion, another test (in vivo un- scheduled DNA synthesis in mice), was used to determine whether the sample constituents or metabolites reached the germ cells and damaged DNA in these cells. No consistent pattern was noted in this study. Interplant comparison revealed considerable variability. Moreover, samples collected at the same plant at different periods varied significantly in chemical composition and in mutagenic activity. This Project Summary was devel- oped by EPA's Municipal Environ- mental Research Laboratory, Cincin- nati, OH. to announce key findings of the research project that is fully documented in a separate report of the same title (see Project Report ordering information at back). Introduction The severity of waterborne disease epidemics has been greatly reduced because of disinfection treatment of wastewater and potable waters, mainly with chlorine. Recently, however, harmful chloro-organics have been established as byproducts of this disinfection process. Ozonation and ultraviolet light irradiation are two disinfectants that are being considered as viable alternatives. But first an evaluation is needed of possible harmful byproducts, like those produced with chlorination. Within the last decade, rapid progress has been made in the analysis of volatile organic constituents of water and wastewater. The determination and characterization of nonvolatile organics, however, have not advanced as rapidly, even though the greatest portion of ------- Table 1. Sources of Effluent Samples Name of Treatment Plant Oak Ridge West Wastewater Treatment Plant Oak Ridge East Wastewater Treatment Plant Lyons Bend Fourth Creek Wastewater Treatment Plant Moccasin Bend Wastewater Treatment Plant Marlborough Easterly Advanced Waste Treatment Plant Upper Thompson Sanitation District Taft Center, USEPA Pilot Wastewater Treatment Plant Meander Creek Wastewater Treatment Plant Northwest Bergen County Wastewater Treatment Plant Location Oak Ridge, TN Oak Ridge, TN Knoxville. TN Chattanooga, TN Marlborough, MA Estes Park, CO Cincinnati, OH Mineral Ridge, OH Waldwick. NJ Type of Treatment Primary Secondary13 Secondary* Secondary* Secondary0 Secondary0 Secondary* Secondary* Secondary* Disinfection Method Chlorine Ozone" Ultraviolet Chlorine Ozone* Ultraviolet* Chlorine Chlorine Ozone Chlorine Ozone Ozone Ozone Chlorine Ultraviolet" Type of Wastewater Primarily residential Primarily residential Primarily residential Residential Industrial Primarily residential Residential, relatively clean Residential and industrial Primarily residential Primarily residential "Conducted in laboratory tests. "Activated sludge. soluble organics in wastewater and natural water fall into that category- An understanding of the possible environ- mental and health-related effects of these pollutants based on definitive data is essential. Scope This research program was developed into four major tasks: (1) laboratory- scale disinfection of wastewater effluent to assess the chemical and mutagenic effects of each disinfectant on the effluent; (2) analysis of concentrated samples from eight operational waste- water treatment plants and one pilot plant, representing all three disinfec- tants and varying levels of domestic and industrial wastewater sources; (3) characterization and identification of constituents separated from the effluent concentrates of operating plants, and (4) screening of concentrated effluents for mutagenic activity. In the later phases of the research program, mutagenic activity was used as the criterion for character- ization of the separated chromatographic components. Results and Conclusion Disinfection of secondary effluent by chlorination and ozonation was found to destroy some nonvolatile organics and to produce others, as illustrated in Figure 1 showing high-pressure liquid chromatograms of effluent before and after treatment with three disinfectants. This pattern was found to prevail in all samples. A few more mutagenic fractions were found in chlorinated and ozonated samples than in the corresponding nondisinfected control effluent of most plants sampled. But inconsistent data prevent the conclusion that disinfection caused this effect. Many mutagenic fractions were isolated from a nonmu- tagenic concentrate and vice versa. Chlorination of primary effluent produces far more mutagenic compo- nents that does chlorination of secondary effluent. This pattern was not observed with ozonation. Ultraviolet irradiation had only a slight effect on the chemical composition of secondary effluent, but it destroyed the mutagenic activity of several fractions. Samples collected from the same plant on different dates showed varying chemical compositions and mutagenic components. Table 2 lists the 103 components identified in concentrates of the controls and disinfected effluents. Seventy- seven were in the mutagenic fractions, and 48 were in the nonmutagenic fractions, with 22 of these compounds being common to both sets. None of the identified compounds are known to be mutagenic. The full report was submitted in fulfillment of Interagency Agreement EPA-IAG-D7-01027, DOE 40-593-76, by Oak Ridge National Laboratory under the sponsorship of the U.S. Environ- mental Protection Agency. ------- Control UV irradiated Chlorinated Ozonated Concentrated Untreated - 2350X 21,200 uW sec/cm2 ---- 2350X 0.5-mg/L residual ------ 2220X 8-mg Os/ L --------- -2220X 0 1 23 4 5 678 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 Time, hr Figure 1. Chromatograms of ultraviolet- absorbing constituents in secondary effluents disinfected with chlorine, ozone, and ultraviolet light. Table 2. Summary of Identified Compounds in High-Pressure Liquid Chromatography Fractions of Effluent Concentrates Alcohols 4-Butoxy-1 -butanola Cyclobutanol* 2,4-Dimethyl-3-pentanola 4-Methyl-2-propyl-1 -pentanol* Aliphatic Acids Diglycolic acid*1" 2,2-Dimethyl-3-hydroxybutyric acid* 3,2-Dimethyl-3 -hydroxybutyric acida Glutamic acid" 3-Hydroxybutyric acid* 2-Hydroxyisobutyric acid*1* 3-Hydroxyisovaleric acid* tsovaleric acid" Ketoglutaric acida Lactic acid3"* Malonic acid* 2-Methyl-2-hydroxybutyric acid" Muconic acid* Oxalic acida'* Propanoic acida Amines Canavanine* N,N'-diethyl-N,N'-dimethyl-p-phenylenediaminea Amino Acids Alanine"'* Aminoisobutyric acid* Aspartic acid* Cystine* Glycine* Histidine* Homocystine* Phenylalanine" Serine" Tyrosine* Aromatic Acids Benzole acid*'* 4-Chlorobenzoic acid"* Dichlorobenzoic * 0-hydroxyphenylacetic acid* Phthalic acid" Phenylpuruvic acid" 2-Pyridinecarboxylic acid* Carbohydrates Erythrose*'* Erythrono- 1.4-lactone* Galactose* Glucose* Gluconic acid* 1 -Methylmannofuranoside* 2-Methylxylopyranoside* Rhamnose* Rib/no- 1,4-lactone* Threono-1,4-lactone*"* Xylono- 1,4-lactone* Xylose*'* Epoxide 2-Methyl-3-propyl oxiranea Fatty Acids Linoleic acida Myristic acid* Oleic acid* Palmitic acid*'* Stearic ac«/a'b Tetradecanoic acid* Hydrocarbons Decane* 2,4-Dimethylhexanea Dodecane* Ethylindan* 4-Ethyltetradecane* Methyleicosane* 5-Methyl-5-ethyldecane* 2-Methylhexadecane* 2-Methyloctanea 2-Methyl-1,3,6-trioxocane* Nordodecane* Pentacosane* Pentadecane* 2,2,3,3- Tetramethylhexane*'* Phenols Phenol*'* Phthalates Di-n-Butylphthalate* Diethylphthalate* Diisobutylphthalate*'* Polyols Cyclohexane- 1.4-diof* Dihydroxyacetone* 2,5-Dimethyl-3,4-hexanediol* Erythritol*1* « U.S.QOVERNMENTPBINTINQOFFICE: 19B2-559-017/0827 ------- Table 2. (continued) Ethylene glycol^" G/uc/fo/"* Glycerol** Inositol* T,3-Propanediota* Propylene gtyco/* Xytitol* Threitol^ Purines and Pyrimidines Adenosine* Caffeine* 6-Dimethyladenosine" 5-Hydroxyuridine" Thymine* Miscellaneous 2-Aminoethanola Decylhydroxyl amine" 2,4-Dimethyl-2,4-disiffipentanea 3,7-Dioxa-2,8--disilanortane-2-one-2,2,8,8-tetramethy/a L -ct-G/ycerophosphate" Phenytacetamide" Phenylpyruvic ox/me* 1,2,3- Trimethoxypentane" 3.6,9- Trioxa-2-silaundecane-2-3-dimethyla Urea" Identified in mutagenic high-pressure liquid chromatography fraction. ^Identified in a nonmutagenic high-pressure liquid chromatography fraction. R. L Jolley, R. B. Gumming, N. E. Lee. L. R. Lewis, J. E. Thompson, W. W. Pitt, M. S. Denion, and S. J. Hartman are with Oak Ridge National Laboratory, Oak Ridge, TN3783O. Charles I. Mashni is the EPA Project Officer (see below). The complete report, entitled "Nonvolatile Organics in Disinfected Wastewater Effluents: Chemical Characterization and Mutagenicity." (Order No. PB 82- 254 053; Cost: $18.00, subject to change) will be available only from: National Technical Information Service 5285 Port Royal Road Springfield, VA 22161 Telephone: 703-487-4650 The EPA Project Officer can be contacted at Municipal Environmental Research Laboratory U.S. Environmental Protection Agency Cincinnati, OH 46268 United States Environmental Protection Agency Center for Environmental Research Information Cincinnati OH 45268 Postage and Fees Paid Environmental Protection Agency EPA 335 Official Business Penalty for Private Use $300 RETURN POSTAGE GUARANTEED Third-Class Bulk Rate IfcRL0167053 US tPA HFblON V LIBRAKY 230 S DtARBURN ST ChlCAbO IL 60604 ------- |