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UCLA Electronic Theses and Dissertations UCLA UCLA Electronic Theses and Dissertations Title NDMA Formation During Drinking Water Treatment: Veterinary Antibiotics as Precursors, the Effect of Natural Organic Matter and the Significance of Treatment Practices Permalink https://escholarship.org/uc/item/94z8j3p0 Author Roback, Shannon Publication Date 2015 Peer reviewed|Thesis/dissertation eScholarship.org Powered by the California Digital Library University of California UNIVERSITY OF CALIFORNIA Los Angeles NDMA Formation During Drinking Water Treatment: Veterinary Antibiotics as Precursors, the Effect of Natural Organic Matter and the Significance of Treatment Practices A dissertation submitted in partial satisfaction of the requirements for the degree of Doctor of Environmental Science and Engineering by Shannon Louise Roback 2015 © Copyright by Shannon Louise Roback 2015 ABSTRACT OF THE DISSERTATION NDMA Formation During Drinking Water Treatment: Veterinary Antibiotics as Precursors, the Effect of Natural Organic Matter and the Significance of Treatment Practices by Shannon Louise Roback Doctor of Environment in Environmental Science and Engineering University of California, Los Angeles, 2015 Professor Irwin H. Suffet, Chair Nitrosodimethylamine (NDMA) is a nitrosated amine that has been associated with a 10-5 increase in lifetime cancer risk at the ng/L level. NDMA may be formed from a variety of anthropogenic amine precursors during drinking water treatment utilizing chloramines as a disinfectant. In this dissertation, ten veterinary antibiotics were tested for their ability to form NDMA. The antibiotics were tested at different pH, temperature, chlorine to ammonia weight ratio (Cl2/NH3) and time to determine the impact of these factors on formation. Molar conversions ranged from 0.04 to 4.9 percent, with antibiotics containing more than one dimethylamine (DMA) functional group forming significantly more NDMA. The highest formation for most of the compounds was seen near pH 8.4. The effect of Cl2/NH3 ratio, temperature, and hold time was somewhat varied for each chemical, suggesting that the effects of these parameters were compound-specific. This suggests that large-scale farming run-off may be ii a new source NDMA precursors. NDMA formation is slowed by the presence of natural organic matter (NOM). It is not currently known which components of NOM are responsible for the reduction in NDMA formation. In this dissertation, water containing NOM was fractionated into different MW size groups or separated based on polarity. The high molecular weight NOM fractions (> 10 kDa), polar and charged components were shown to be the most effective in reducing the amount of NDMA formed. Some precursors have high sorption coefficients to NOM, which is the likely mechanism for reduction of NDMA formation from these compounds. Lastly, NDMA formation can be highly impacted by numerous factors relevant to drinking water treatment. In this dissertation, water samples and treatment plant data were collected from approximately 20 drinking water treatment plants in the U.S. and Canada over 2 years. Linear mixed effects models with random intercepts, which account for variability between treatment plants, were used to assess variable significance and create predictive equations. UV254 concentration in the plant influent, sucralose concentration, polyDADMAC concentration, pre- chlorination time, Cl2/NH3 ratio, use of GAC, water pH, and biofiltration were associated with NDMA concentration in the distribution system. iii The dissertation of Shannon Louise Roback is approved. Keith Stolzenbach Michael K. Stenstrom Curtis Eckhert Irwin H. Suffet, Committee Chair University of California, Los Angeles 2015 iv TABLE OF CONTENTS Chapter I: NDMA as a Disinfection Byproduct..........................................………………………1 A. NDMA as a Water Pollutant......……..........………………………………....…..……2 B. Toxicity..........................................................................................................................3 C. Formation.......................................................................................................................4 C.1. Mechanism 1.........……………………………………...………………….…....4 C.2. Mechanism 2.........................................................................................................7 C.3. Effect of pH, Temperature and Catalysts on NDMA Formation..........................9 C.4. Formation from Ozone........................................................................................10 D. NDMA Precursors………………………………………………………….......…...11 D.1. Chemical Characteristics.....................................................................................11 D.2. Sources……………………………………………………………..………......12 D.2.a. Wastewater Treatment Plant Effluent........................................................13 D.2.b. Natural Organic Matter..............................................................................13 D.2.c. Chemicals Used During Drinking Water Treatment..................................14 E. Human and Veterinary Antibiotics...............................................................................15 E.1. Use.................................................................................................................15 E.2. Environmental Occurrence............................................................................18 E.3. Removal During Water Treatment................................................................19 F. NDMA Formation Potential Tests................................................................................21 G. Natural Organic Matter................................................................................................25 G.1. Sorption of Antibiotics to Natural Organic Matter.......................................25 H. Removal of NDMA During Drinking Water Treatment..............................................28 v H.1. Destruction of Precursors..............................................................................29 I. Modeling Disinfection Byproduct Formation...............................................................31 J. Conclusion.....................................................................................................................33 K. References....................................................................................................................35 Chapter II: Veterinary Antibiotics as a Source of NDMA Precursors………………………..….50 A. Abstract……………………………………………………………………..…….….51 B. Introduction…………………………………………………………………………..51 B.1. Veterinary Antibiotics………………….…...................................................…..53 B.1.a. Environmental Fate of Veterinary Antibiotics…………...…...….……....54 B.1.b. Fate of Veterinary Antibiotics in Water Treatment Plants.……............…55 C. Experimental………………………………..……………………..............………….57 C.1. Materials…………………………...……………………...............…………....57 C.2. NDMA Formation Potential Tests......................................................................57 C.3. NDMA Analysis..................................................................................................59 C.4. Ultraviolet Absorbance.......................................................................................59 D. Results .........................................…………………...…………………………..……60 D.1. pH Tests........................................................................................................65 D.2. Cl2/N Ratio Tests..........................................................................................67 D.3. Temperature Tests.........................................................................................70 D.4. Hold Time Tests............................................................................................70 D.5. Compounds Containing DMA Moieties and pH...........................................72 D.6. Formation of NDMA from Veterinary Antibiotics in Real World Scenarios................................................................................................................73 vi E. References....................................................................................................................75 Chapter III: Understanding the Mechanism by Which Natural Organic Matter Decreases the Rate of NDMA Formation in Drinking Water...............................................................................82 A. Abstract………………………………………...…………………………………….83 B. Introduction…………………………………………………………………………..84 B.1. NDMA…………………….............................………...…………………….…84 B.2. Natural Organic Matter.......................................................................................85 C. Experimental…………………………………............……………………...……….88 C.1. Materials……………..............................………………..…………….....……..88 C.2. Methods………………………………………………………………................89 C.2.a. Ultrafiltration…………...............................…………..………….………90 C.2.b. Polarity Fractionation.................................................................................90 C.2.c. NDMA Formation Potential Tests...............................................................91 D. Results and Discussion……………………………………...………..…………..….92 D.1. Initial Kinetic Curve………………………………………..…..…………...…..92 D.2. Molecular Weight Fractions…………………...…………….…..………….…..92 D.3. Round 2 Testing: Molecular Weight Fractions....................................................94 D.4. Polarity Fractions………….....................………………………………..……..96
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