Analysis of possible sources and pathways of methyl tertiary-butyl ether (MTBE) in the aquatic environment [Elektronische Ressource] / von Axel Kolb

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Informations

• Publié par: goethe_universitat_frankfurt_am_main
• Publié le: 01 janvier 2006
• Nombre de lectures: 51
• Langue: Deutsch

Extrait

Analysis of Possible Sources and Pathways of Methyl tertiary-Butyl Ether
(MTBE) in the Aquatic Environment




Dissertation
zur Erlangung des Doktorgades
der Naturwissenschaften




vorgelegt beim Fachbereich Chemische und Pharmazeutische Wissenschaften
der Johann Wolfgang Goethe-Universität
in Frankfurt am Main


von
Axel Kolb
aus Freiburg im Breisgau


Frankfurt (2004)
(DF 1)










vom Fachbereich Chemische und Pharmazeutische Wissenschaften der Johann Wolfgang
Goethe-Universität als Dissertation angenommen.


Dekan: Prof. Dr. Harald Schwalbe

Gutachter: Prof. Dr. Bernd O. Kolbesen
Prof. Dr. Wilhelm Püttmann


Datum der Disputation: 07. April 2005






















Für meine Mutter



Contents

Danksagung................................................................................................................................ 6

Zusammenfassung (Summary) ............................................................................................... 8

Introduction .................................................................................................................. 20

1. Production, Usage and Legal Emission Control of MTBE ........................................... 24
1.1. Production and Usage .............................................................................................. 24
1.1.1. USA ............................................................................................................ 24
1.1.2. European Union .......................................................................................... 28
1.1.3. Germany ..................................................................................................... 31
1.2. Legal Emission Control of MTBE........................................................................... 33
1.2.1. USA 33
1.2.2. European Union 34
1.2.3. Germany 35
2. Properties of MTBE and Its Behavior in the Environment........................................... 37
2.1. Synthesis .................................................................................................................. 37
2.2. Physico-Chemical Properties................................................................................... 38
2.3. MTBE Releases into the Aquatic Environment....................................................... 41
2.4. Distribution of MTBE in the Environment.............................................................. 43
2.5. Degradation.............................................................................................................. 45
2.5.1. Water and Soil ............................................................................................ 45
2.5.2. Air............................................................................................................... 47
2.6. Toxicity.................................................................................................................... 48
2.7. Economical and Environmental Aspects of MTBE Substitutes .............................. 49
3. Analytical Methods............................................................................................................ 53
3.1. Analysis of MTBE in Environmental Water Samples............................................. 53
3.1.1. Extraction/Enrichment................................................................................ 53
3.1.2. Separation ................................................................................................... 55
3.1.3. Detection..................................................................................................... 55
3.2. Determination of MTBE in Water Samples by HS-SPME Combined
with GC/MS............................................................................................................. 56
3.2.1. Sampling 56
3.2.2. Standard Solutions ...................................................................................... 57
3.2.3. Headspace-Solid Phase Microextraction (HS-SPME)................................ 57
3.2.4. Gas Chromatography (GC)......................................................................... 58
3.2.5. Mass Spectrometry (MS)............................................................................ 59
3.2.6. Calibration .................................................................................................. 61
3.2.7. Accuracy and Precision .............................................................................. 62
4. MTBE in Finished Drinking Water in Germany............................................................ 64
4.1. Abstract.................................................................................................................... 64
4.2. Introduction.............................................................................................................. 64
4.3. Experimental Section............................................................................................... 67
4.3.1. Community Water Systems (CWS) 67
4.3.2. Sampling and Analysis ............................................................................... 69
4.4. Results...................................................................................................................... 70
4.5. Discussion................................................................................................................ 73
5. Influence of Possible MTBE Sources on the Spatial MTBE Distribution in
Three German Rivers........................................................................................................ 79
5.1. Abstract.................................................................................................................... 79
5.2. Introduction.............................................................................................................. 79
5.3. Experimental Section............................................................................................... 82
5.3.1. Study Sites .................................................................................................. 82
5.3.2. Sampling and Analysis ............................................................................... 85
5.4. Results...................................................................................................................... 85
5.4.1. Lippe/Wesel-Datteln-Canal ........................................................................ 85
5.4.2. Saale............................................................................................................ 87
5.4.3. Rhine........................................................................................................... 87
5.5. Discussion................................................................................................................ 88
5.5.1. Lippe/Wesel-Datteln-Canal 88
5.5.2. Saale 90
5.5.3. Rhine 91
5.5.4. General Aspects .......................................................................................... 91
6. MTBE in Snow Samples in Germany .............................................................................. 94
6.1. Abstract.................................................................................................................... 94
6.2. Introduction.............................................................................................................. 94
6.3. Experimental............................................................................................................ 96
6.4. Results and Discussion ............................................................................................ 97
6.5. Conclusions 106
7. Comparison of MTBE Concentrations in Groundwater of Urban and
Non-Urban Areas in Germany ......................................................................................... 108
7.1. Abstract 108
7.2. Introduction.............................................................................................................. 108
7.3. Experimental............................................................................................................ 110
7.3.1. Contaminated Sites ..................................................................................... 110
7.3.2. Non-Urban Samples.................................................................................... 111
7.3.3. Urban Samples............................................................................................ 111
7.3.4. Sampling and Analysis ............................................................................... 112
7.4. Results and Discussion 112
7.4.1. Contaminated Sites 112
7.4.2. Non-Urban Samples 114
7.4.3. Urban Samples 117
7.4.4. Comparison of MTBE Data in Germany and the USA .............................. 119
7.5. Conclusions...............................................................