Occurrence, Distribution and Behavior of Hydrophilic Ethers in the Aquatic Environment

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Occurrence, Distribution and Behavior of Hydrophilic Ethers in the Aquatic Environment Occurrence, distribution and behavior of hydrophilic ethers in the aquatic environment Dissertation for attaining the PhD degree of Natural Sciences submitted to the Faculty of the Johann Wolfgang Goethe-University in Frankfurt am Main by Daria Katarzyna Demers-Stępień from Gdynia Frankfurt (2013) (D 30) accepted as a dissertation by the Faculty of Geoscience/Geology of the Johann Wolfgang Goethe University Dean: Prof. Dr. Andreas Junge Expert assessors: Prof. Dr. Wilhelm Pütmann Prof. Dr. Ruprecht Schleyer Prof. Dr. Christoph Schüth Prof. Dr. Peter Cornel Date of the disputation: February 4th, 2014 Table of contents Table of Contents List of Tables .................................................................................................................................. 6 List of Figures ................................................................................................................................ 8 Abstract ........................................................................................................................................ 10 Zusammenfassung ....................................................................................................................... 14 Acknowledgements ...................................................................................................................... 21 Acronyms ...................................................................................................................................... 23 Chapter 1 Introduction .................................................................................................................. 25 1.1 Target analytes ................................................................................................................. 25 1.2 Toxicity ............................................................................................................................ 29 1.3 Formation of 1,4-dioxane as a by-product ....................................................................... 30 1.4 Focus of the research ....................................................................................................... 32 Chapter 2 Simultaneous determination of six hydrophilic ethers at trace levels using coconut charcoal adsorbent and gas chromatography/mass spectrometry .................................................. 34 2.1 Abstract ................................................................................................................................ 34 2.2 Introduction .......................................................................................................................... 35 2.3 Experimental ........................................................................................................................ 37 2.3.1 Chemical standards and reagents .................................................................................. 37 2.3.2 Sample collection .......................................................................................................... 38 2.3.3 Extraction procedure ..................................................................................................... 40 2.3.4 GC/MS analytical conditions ........................................................................................ 40 2.3.5 Quantification and quality control ................................................................................ 41 2.4 Results and discussion ......................................................................................................... 43 2.4.1 Optimization of the extraction method ......................................................................... 43 2.4.2 Precision and accuracy study ........................................................................................ 43 2.4.3 Detection and quantification limits ............................................................................... 45 2.4.4 Stability study ................................................................................................................ 46 2.4.5 Application to environmental water samples ................................................................ 49 2.5 Conclusions .......................................................................................................................... 51 Chapter 3 Behavior of organophosphates and hydrophilic ethers during bank filtration and their potential application as organic tracers. A field study from the Oderbruch, Germany. ................ 52 3.1 Abstract ................................................................................................................................ 52 3.2 Introduction .......................................................................................................................... 53 3.3 Area description and methods .............................................................................................. 56 3.3.1 Site description .............................................................................................................. 56 3 | P a g e Table of contents 3.3.2 Analytical methods ........................................................................................................ 59 3.3.3 Quality assurance .......................................................................................................... 61 3.4 Results and discussion ......................................................................................................... 62 3.4.1 Hydrochemistry ............................................................................................................. 62 3.4.2 Infiltration of OPs and ethers into the main drainage ditch .......................................... 64 3.4.3 Occurrence of OPs and ethers in the aquifer ................................................................. 66 3.4.4 Factors influencing OP and ether concentrations .......................................................... 67 3.4.5 Attenuation of OPs and ethers during bank filtration ................................................... 70 3.4.6 Organic pollutants as hydrological tracers .................................................................... 72 3.5 Conclusions .......................................................................................................................... 74 Chapter 4 Fate of 1,4-dioxane in the aquatic environment: from sewage to drinking water ........ 75 4.1 Abstract ................................................................................................................................ 75 4.2. Introduction ......................................................................................................................... 76 4.3. Materials and methods ........................................................................................................ 78 4.3.1. Chemicals and reagents ................................................................................................ 78 4.3.2 Analytical methods ........................................................................................................ 79 4.3.3. Quality assurance ......................................................................................................... 80 4.5. Site description and sampling methods .............................................................................. 81 4.5.1. Sewage treatment plants ............................................................................................... 81 4.5.2. Surface waters .............................................................................................................. 82 4.5.3. Bank filtration and drinking water treatment ............................................................... 83 4.6. Results and discussion ........................................................................................................ 86 4.6.1. 1,4-dioxane in municipal sewage treatment plants ...................................................... 86 4.6.2. Temporal and spatial distribution of 1,4-dioxane in surface waters ............................ 89 4.6.3. Occurrence of 1,4-dioxane in bank filtration and drinking water ................................ 97 4.7 Conclusions ........................................................................................................................ 101 Chapter 5 Source identification of high glyme concentrations in the Oder River ...................... 103 5.1. Abstract ............................................................................................................................. 103 5.2. Introduction ....................................................................................................................... 103 5.3. Materials and methods ...................................................................................................... 106 5.3.1. Chemicals and reagents .............................................................................................. 107 5.3.2. Analytical methods ..................................................................................................... 108 5.3.3. Quality assurance ....................................................................................................... 109 5.4. Site description and sampling methods ............................................................................ 109 5.4.1. Description of the study area .....................................................................................
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