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The Use of 185 Nm Radiation for Drinking Water Treatment Influence of Major Solutes and Temperature on the Degradation of Trace Organic Contaminants

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The Use of 185 Nm Radiation for Drinking Water Treatment Influence of Major Solutes and Temperature on the Degradation of Trace Organic Contaminants The Use of 185 nm Radiation for Drinking Water Treatment Influence of Major Solutes and Temperature on the Degradation of Trace Organic Contaminants by Laith Furatian B.Sc., The University of Alberta, 1999 M.Sc., The University of New Hampshire, 2011 A THESIS SUBMITTED IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY in The Faculty of Graduate and Postdoctoral Studies (Chemical and Biological Engineering) THE UNIVERSITY OF BRITISH COLUMBIA (Vancouver) June 2017 © Laith Furatian 2017 Abstract The treatment of water via 185 nm radiation allows for the oxidative degra- dation of trace organic contaminants without the need for chemical addition. Critical information required for the practical application of such a process has been lacking. Carbamazepine was determined to be an ideal probe com- pound for study of the 185 nm regime due to negligible direct photolysis at 254 nm. An increase in probe degradation rate due to 185 nm is observed with increasing temperature when water is the only significant absorber of photons. A comparison with the temperature dependence of the 254 nm - H2O2 process is made and a fundamental explanation proposed. Experi- mental evidence reveals that probe degradation rate is strongly influenced by anionic composition at environmentally relevant concentrations, partic- ularly chloride. Evidence for the role of the chlorine radical is obtained by kinetic studies involving select probes, radical scavengers, and ionic strength. Interactions between the major organic and inorganic solutes indicate that resulting degradation kinetics are highly sensitive to the composition of the water matrix, a fact that has been neglected from the literature. A method to quantify molar absorption coefficients is developed that is not prone to errors due to stray radiant energy or wavelength inaccuracies. A method to quantify the 185:254 nm output of a low pressure mercury lamp is presented with results in agreement with values reported in the literature. In addition to the hydroxyl radical ( OH), other radical species such as chlorine (Cl ) { and sulphate (SO4 ) are proposed to be involved in oxidative degradation of trace organics in the 185 nm regime. This suggests that the degradation rate of a given target contaminant depends on the composition of the water matrix, the second-order rate constants with the relevant radicals, and the relative reaction rate constants of the target and the matrix. ii Lay Summary Certain types of chemical impurities are difficult to remove from water. One method that may be useful in destroying certain chemicals is to split water molecules using ultraviolet radiation to produce an aggressive oxidant that will then attack impurities. However, this process is highly dependent on the types and amounts of naturally occurring substances also dissolved in water. A complex mixture of oxidants may be produced with potentially significant differences in their abilities to attack a given impurity. Thus, since the composition of water differs between places and over the seasons, the efficiency of this approach may differ substantially between locations and over time. An attempt to understand how the natural composition of water and its temperature influence the efficiency of this process were the goals of this research. This information could then be used to optimize the pro- cess and even determine under what conditions its use would be impractical. iii Preface This dissertation is original, unpublished, independent work by the author, Laith Furatian. iv Table of Contents Abstract ................................. ii Lay Summary .............................. iii Preface .................................. iv Table of Contents ............................v List of Tables .............................. viii List of Figures ..............................x Nomenclature .............................. xiii Acknowledgements ........................... xv Dedication ................................ xvii 1 Introduction .............................1 1.1 Public Drinking Water Supplies . .1 1.2 A Recent History of Water Treatment . .4 1.3 UV Disinfection . 10 1.4 Advanced Oxidation Processes . 13 1.5 185 nm Advanced Oxidation . 18 1.6 Knowledge Gaps . 21 1.7 Research Objectives . 27 2 Experimental Approach ...................... 29 2.1 General Approach . 29 v Table of Contents 2.2 The Probe Compound and the Observable k0 ......... 29 2.3 Expressing the Extent of Reaction . 32 2.4 A 185 nm Kinetic Model . 36 2.5 Experimental Apparatus . 40 2.6 Materials . 43 2.7 Probe Compound Selection and Characterization . 43 2.7.1 Molar Absorption Coefficients at 254 nm . 45 2.7.2 Photolysis Quantum Yields at 254 nm . 45 2.7.3 Second-order OH Rate Constants . 46 2.8 Analytical Methods . 47 2.9 Initial Testing of 185 nm Experimental Methods . 48 3 Temperature ............................. 54 3.1 Temperature and Water Treatment . 54 3.2 Temperature Dependence of UV AOPs . 54 3.3 Experimental Approach . 58 3.4 Results . 59 3.4.1 Temperature Effects in the 254 nm - H2O2 Regime . 59 3.4.2 Temperature Effects in the 185 nm Regime . 61 3.5 Discussion . 64 3.6 Summary . 66 4 Dissolved Organic Matter .................... 67 4.1 Dissolved Organic Matter in Natural Waters . 67 4.2 The 185 nm AOP and Influence of Dissolved Organic Matter 70 4.3 Use of Reference Materials . 71 4.4 Pure Substances as Model Organic Matter . 75 4.5 Estimation of 185 nm Incident Fluence Rate . 82 4.6 Summary . 84 5 Chloride ................................ 86 5.1 Chloride in Natural Waters . 86 5.2 Impact of Chloride on AOPs . 87 5.3 Chloride in the 254 nm - H2O2 Regime . 90 vi Table of Contents 5.4 Chloride in the 185 nm Regime . 92 5.5 Relative Reactivity of OH and Cl ............... 100 5.6 Evidence for Cl from Probe-Scavenger Systems . 101 5.7 Evidence from Ionic Strength Effects . 107 5.8 Product Studies of Phenol Degradation . 112 5.9 Bleaching of Dissolved Organic Matter in 185 nm Regime . 113 5.10 Molar Absorption Coefficient of Chloride at 185 nm . 114 5.11 Potential Cl to OH Interconversion . 118 5.12 Summary . 119 6 Sulphate, Bicarbonate and Interactions of Major Solutes 122 6.1 The 185 nm AOP and Other Solutes . 122 6.2 Sulphate . 123 6.2.1 Sulphate in the 254 nm - H2O2 Regime . 124 6.2.2 Sulphate in the 185 nm Regime . 127 6.3 Bicarbonate . 131 6.4 Interactions Among Major Solutes . 137 6.4.1 Sulphate and Bicarbonate . 140 6.4.2 Chloride and Bicarbonate . 143 6.4.3 Chloride, Sulphate, and Bicarbonate . 146 6.5 Summary . 151 7 Conclusions and Recommendations .............. 153 7.1 Conclusions . 153 7.2 Recommendations . 156 Bibliography ............................... 158 Appendices A Experimental Data and Calculations .............. 179 vii List of Tables 1.1 Molar absorption coefficient () and quantum yield (Φ) for { 2{ Cl and SO4 at 185 nm . 22 { 1.2 Comparison of rate constants for OH, Cl , and SO4 with { 2{ HCO3 and CO3 ......................... 24 { { 1.3 Important reactions involving Cl , Cl2 , and SO4 ...... 25 2.1 Photochemical reaction parameters for probe compounds at 254 nm . 44 3.1 Effect of temperature on removal rate of carbamazepine probe in 254 nm-H2O2 regime . 59 3.2 Effect of temperature on removal rate of carbamazepine probe in 185 nm regime . 63 3.3 Experimental activation energies for carbamazepine degra- dation in the presence of tert-butanol in 254 nm-H2O2 and 185 nm regimes . 63 3.4 Summary of fundamental activation energies estimated from this work . 64 4.1 The removal rate of probe for varying concentration and source of DOM in 185 nm regime . 72 4.2 Selected pure compounds used as model organic matter in studies of 185 nm regime . 75 4.3 The removal rate of probe for pure scavengers tert-butanol, methanol, and acetone in 185 nm regime . 79 viii List of Tables 5.1 Comparison of OH and Cl reactivities for pure compounds used as model organic matter in the 185 nm regime . 102 5.2 Model evaluation using the degradation of nitrobenzene with increasing Cl{ in the 185 nm regime . 118 6.1 Numerical values used in calculation of the second-order rate { constant for the reaction of SO with carbamazepine (k { ) 4 SO4 ;CBZ with equation 6.2 . 130 6.2 Experimental determination of the second-order rate constant { for the reaction of SO with carbamazepine (k { ) with 4 SO4 ;CBZ equation 6.2 . 130 6.3 Comparison of the calculated and experimental rates due to { HCO3 in the 185 nm regime . 136 2{ 6.4 Comparison of calculated and experimental rates due to SO4 { and HCO3 in the 185 nm regime . 141 6.5 Experimental degradation rates of carbamazepine due to Cl{ { and HCO3 in the 185 nm regime . 144 { 2{ { 6.6 Interactions of Cl , SO4 and HCO3 , in the presence of Suwan- nee River NOM . 150 ix List of Figures 2.1 The 185 nm Collimated Beam Apparatus . 42 3.1 Temperature dependence in 254 nm - H2O2 regime. 60 3.2 Arrhenius plots for 254 nm-H2O2 regime . 61 3.3 Temperature dependence in 185 nm regime. 62 3.4 Arrhenius plots for 185 nm regime . 63 4.1 Suwannee River DOM in 185 nm regime. 73 4.2 Nordic DOM in 185 nm regime. 74 4.3 Removal rate of probe with type and concentration of DOM . 74 4.4 Tert-Butanol in 185 nm regime. 76 4.5 Methanol in 185 nm regime. 77 4.6 Acetone in 185 nm regime. 77 4.7 Removal rate of probe with pure compounds as model DOM 78 5.1 Tert-Butanol in the 254 nm - H2O2 regime and influence of chloride. 91 5.2 Suwannee River NOM in the 254 nm - H2O2 regime and in- fluence of chloride. 92 5.3 Tert-Butanol in the 185 nm regime and influence of chloride, using carbamazepine as a probe. 93 5.4 Suwannee River NOM in the 185 nm regime and influence of chloride, using carbamazepine as a probe.
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