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Publié par | goethe_universitat_frankfurt_am_main |
Publié le | 01 janvier 2006 |
Nombre de lectures | 49 |
Langue | Deutsch |
Poids de l'ouvrage | 1 Mo |
Extrait
Methyl tert-Butyl Ether (MTBE) in the Aquatic Environment
in Germany
Dissertation
zur Erlangung des Doktorgrades
der Naturwissenschaften
vorgelegt beim Fachbereich Geowissenschaften
der Johann Wolfgang Goethe-Universität Frankfurt am Main
von
Dipl.-Geol. Christine Achten
geb. Eichler
aus Buchholz in der Nordheide
Frankfurt am Main 2001 Contents
Danksagung............................................................................................................................... V
Kurzfassung (Short Summary).................................................................................................VI
Zusammenfassung (Summary) ...............................................................................................1
Introduction ............................................................................................................................11
1 Use, History, Political and Legal Aspects of Methyl tert-Butyl Ether (MTBE)........14
1.1 Use, History and Political Aspects ...................................................................................14
1.1.1 United States of America (U.S.) ............................................................................14
1.1.2 European Union (EU) ............................................................................................18
1.1.3 Germany.................................................................................................................21
1.2 Legal Aspects ...................................................................................................................24
1.2.1 27
1.2.2 European Union (EU)27
1.2.3 Germany28
2 Synthesis, Properties of MTBE and its Behavior in the Environment......................29
2.1 Synthesis...........................................................................................................................29
2.2 Physico-Chemical Properties............................................................................................30
2.3 Degradation.......................................................................................................................34
2.3.1 Water and Soil........................................................................................................34
2.3.2 Air ..........................................................................................................................36
2.4 Toxicity.............................................................................................................................37
2.5 Emission Pathways into the Aquatic Environment ..........................................................39
2.6 Behavior in the Environment............................................................................................41
2.7 Comparison to Other Oxygenates ....................................................................................42
3 Analytical Methods.........................................................................................................47
3.1 Method for Determination of MTBE in Gasoline by Gas Chromatography (GC)...........47
3.1.1 Abstract ..................................................................................................................47
3.1.2 Introduction............................................................................................................47
3.1.3 Experimental Section .............................................................................................48
3.1.3.1 Materials and Methods ....................................................................................48
3.1.3.2 Instrumental.....................................................................................................48
3.1.4 Results and Discussion...........................................................................................50
3.1.5 Conclusion .............................................................................................................53
3.2 Determination of MTBE in Surface Water by Use of Direct Solid-Phase
Microextraction/ Gas Chromatography-Mass Spectrometry (SPME/ GC-MS)...............55
3.2.1 Abstract............................................................................................................55
3.2.2 Introduction55
3.2.3 Experimental Section.......................................................................................56
3.2.3.1 Materials and Methods..............................................................................56
3.2.3.2 GC/ MS56
3.2.4 Results and Discussion ....................................................................................58
3.3 Improvement of the Method: SPME in Headspace (HS-SPME) .....................................63
II3.3.1 Abstract ..................................................................................................................63
3.3.2 Introduction............................................................................................................63
3.3.3 Experimental Section .............................................................................................65
3.3.3.1 Materials and Methods ....................................................................................65
3.3.3.2 HS-SPME/ GC-MS .........................................................................................66
3.3.3.3 Starting Conditions..........................................................................................67
3.3.4 Results and Discussion...........................................................................................67
3.3.4.1 Method Development ......................................................................................67
3.3.4.1.1 Location of the Fiber and Sample Volume ...............................................67
3.3.4.1.2 Extraction Time and Time of the Total Analytical Cycle.........................68
3.3.4.1.3 Sample Temperature .................................................................................68
3.3.4.1.4 Sodium Chloride Concentration................................................................71
3.3.4.2 Method Validation71
3.3.4.2.1 Blanks........................................................................................................71
3.3.4.2.2 Calibration and Linearity ..........................................................................71
3.3.4.2.3 Accuracy and Precision.............................................................................73
3.3.4.2.4 Field Study ................................................................................................75
3.3.5 Conclusions............................................................................................................76
4 MTBE Concentrations in Environmental Water Samples in Germany ...................77
4.1 MTBE in Urban and Rural Precipitation77
4.1.1 Abstract ..................................................................................................................77
4.1.2 Introduction77
4.1.3 Sampling79
4.1.4 Results and Discussion...........................................................................................80
4.1.4.1 Precipitation.....................................................................................................80
4.1.4.2 Comparison of the MTBE Concentrations in Precipitation to Other Data......86
4.1.4.3 Urban Runoff...................................................................................................88
4.1.5 Conclusions............................................................................................................89
4.2 MTBE in River and Waste Water ....................................................................................89
4.2.1 Abstract ..................................................................................................................89
4.2.2 Introduction90
4.2.3 Waste Water Processing at Sewage Plants Frankfurt/ M-Niederrad and
Sindlingen ..............................................................................................................93
4.2.4 Sampling ................................................................................................................94
4.2.5 Results....................................................................................................................94
4.2.5.1 MTBE in German River Water .......................................................................94
4.2.5.2 MTBE in Domestic and Industrial Waste Water...........................................102
4.2.6 Discussion ............................................................................................................103
4.2.7 Conclusions..........................................................................................................110
4.3 MTBE in Bank-Filtered Water and Drinking Water Produced by Riverbank
Filtration .........................................................................................................................111
4.3.1 Abstract111
4.3.2 Introduction112
4.3.2.1 Site Locations .........................................................................................