Atmospheric distribution and seasonality of airborne polyfluorinated compounds [Elektronische Ressource] : spatial and temporal concentration variations from ship-and land-based measurements in Northern Germany, the Atlantic Ocean, and Polar regions / vorgelegt von Annekatrin Dreyer

Maik Röder

Informations

• Publié par: universitat_bayreuth
• Publié le: 01 janvier 2009
• Nombre de lectures: 27
• Langue: Deutsch
• Poids de l'ouvrage: 37 Mo

Extrait

Atmospheric Distribution and Seasonality
of Airborne Polyfluorinated Compounds

Spatial and Temporal Concentration Variations from Ship-
and Land-Based Measurements in Northern Germany,
the Atlantic Ocean, and Polar Regions






Dissertation zur Erlangung des Grades
Doktor der Naturwissenschaften
(Dr. rer. nat.)
an der Fakultät Biologie/Chemie/Geowissenschaften
der Universität Bayreuth


vorgelegt von

Annekatrin Dreyer
geb. am 05.02.1980 in Wismar


Bayreuth, Mai 2009




Die Arbeiten zur vorliegenden Dissertation wurden in der Zeit von April 2006 bis Mai 2009
in der Abteilung Umweltchemie des Instituts für Küstenforschung am GKSS
Forschungszentrum durchgeführt.



Vollständiger Abdruck der von der Fakultät für Chemie/Biologie/Geowissenschaften der
Universität Bayreuth genehmigten Dissertation zur Erlangung des Grades eines Doktors der
Naturwissenschaften (Dr. rer. nat.).








Tag der Einreichung: 19.05.2009

Tag des wissenschaftlichen Kolloquiums: 10.12.2009



Prüfungsausschuss:

Prof. Dr. Thomas Foken (Vorsitzender) Hartmut Frank (1. Gutachter)
Prof. Dr. Ralf Ebinghaus (2.
Prof. Dr. Cornelius Zetzsch
PD Dr. Bruno Glaser





























We had the experience but missed the meaning,
And approach to the meaning restores the experience in a different form
T. S. Eliot


TABLE OF CONTENTS

Table of Contents
............................................................................................................................... i
List of Figures ................................................................................................................................... iv
List of Tables ................................................................................................................................... vii
Abbreviations .................................................................................................................................... x
Summary ......................................................................................................................................... xiii
Zusammenfassung .......................................................................................................................... xvi

Extended Summary .............................................................................................................. 1
1. Introduction .............................................................................................................................. 3
1.1. Rationale ........................................................................................................................................ 3
1.2. Background .................................................................................................................................... 4
1.3. Environmental Concerns ................................................................................................................ 8
1.3.1. Persistence .................................................................................................................................. 8
1.3.2. Bioaccumulation ......................................................................................................................... 9
1.3.3. Toxicity .................................................................................................................................... 10
1.3.4. Long-Range Transport .............................................................................................................. 12
1.4. Atmospheric Chemistry of Polyfluorinated Compounds ............................................................. 17
1.5. Research Objectives ..................................................................................................................... 18
2. Experimental ........................................................................................................................... 20
2.1. Sampling ...................................................................................................................................... 20
2.2. Extraction ..................................................................................................................................... 22
2.3. Instrumental Analysis & Quantification ...................................................................................... 24
2.4. Quality Assurance & Quality Control .......................................................................................... 25
2.5. Air Mass Back Trajectories .......................................................................................................... 25
3. Results & Discussion .............................................................................................................. 26
3.1. Synopsis of PFC Concentrations in Ambient Air ........................................................................ 26
3.2. Temporal Concentration Variations of Polyfluorinated Compounds in Ambient Air .................. 27
3.3. Spatial Concentration Distribution of Polyfluorinated Compounds in Ambient Air ................... 29
3.4. Influence of Air Mass Origin on Concentrations of Polyfluorinated Compounds ....................... 31
3.5. Atmospheric Residence Times ..................................................................................................... 33
3.6. Where Did They Come From? – A Discussion About Sources of Atmospheric Polyfluorinated
Compounds .................................................................................................................................. 34
4. Conclusion ............................................................................................................................... 37
References ........................................................................................................................................ 39
Contributions to the Included Studies .......................................................................................... 53

Cumulative Study ................................................................................................................ 55
Study 1
An Optimized Method Avoiding Solvent-Induced Response Enhancement in the Analysis
of Volatile and Semi-Volatile Polyfluorinated Alkylated Compounds Using Gas
Chromatography-Mass Spectrometry ..................................................................................... 57
i
TABLE OF CONTENTS

Abstract ............................................................................................................................................ 59
Keywords ......................................................................................................................................... 59
1. Introduction ............................................................................................................................ 59
2. Experimental ........................................................................................................................... 61
2.1. Chemicals ..................................................................................................................................... 61
2.2. Sample Preparation ...................................................................................................................... 62
2.3. Instrumental Analysis & Quantification ...................................................................................... 63
2.4. Quality Assurance & Quality Control .......................................................................................... 64
3. Results & Discussion .............................................................................................................. 65
3.1. Recovery Experiments on Solvents ............................................................................................. 65
3.2. Extraction Experiments ................................................................................................................ 69
Acknowledgements ......................................................................................................................... 72
References ........................................................................................................................................ 72
Supporting Information ................................................................................................................. 75
Study 2
Annual Time Series of Air Concentrations of Polyfluorinated Compounds ........................ 91
Abstract ............................................................................................................................................ 93
1. Introduction ............................................................................................................................ 93