Method development and determination of anthropogenic poly- and perfluorinated compounds in air, water, soil, house dust, and several consumer products [Elektronische Ressource] / Stefan Andreas Fiedler

Stefan Löfving

Sujets

• Biologie

Informations

• Publié par: technische_universitat_munchen
• Publié le: 01 janvier 2010
• Nombre de lectures: 25
• Langue: Deutsch
• Poids de l'ouvrage: 2 Mo

Extrait

TECHNISCHE UNIVERSITÄT MÜNCHEN
Department für Biowissenschaftliche Grundlagen



Method development and determination of anthropogenic poly- and perfluorinated compounds in air,
water, soil, house dust, and several consumer products



Stefan Andreas Fiedler



Vollständiger Abdruck der von der Fakultät Wissenschaftszentrum Weihenstephan für Ernährung,
Landnutzung und Umwelt der Technischen Universität München zur Erlangung des akademischen
Grades eines
Doktors der Naturwissenschaften
genehmigten Dissertation.


Vorsitzender: Univ.-Prof. Dr. J. Durner
Prüfer der Dissertation:
1. apl. Univ.-Prof. Dr. K.-W. Schramm
2. Univ.-Prof. Dr. Dr. h. c. H. Parlar



Die Dissertation wurde am 21.05.2010 bei der Technischen Universität München eingereicht und
durch die Fakultät Wissenschaftszentrum Weihenstephan für Ernährung, Landnutzung und Umwelt
am 13.10.2010 angenommen.


Table of Contents
Table of Contents
Table of Contents .......................................................................................................................... i
List of Publications...................................................................................................................... iv
List of Abbreviations.................................................................................................................... v
List of Figures ...........................................................................................................................viii
List of Tables...............................................................................................................................ix
Summary .....................................................................................................................................xi
Zusammenfassung.....................................................................................................................xiii
1 Introduction ........................................................................................................................... 1
1.1 Poly- and perfluorinated compounds ........................................................................... 1
1.1.1 Investigated poly- and perfluorinated compounds ............................................... 1
1.1.2 Properties of PFC ................................................................................................. 2
1.1.3 Sources and fate of PFC in the environment........................................................ 3
1.1.4 Concentrations and effects of PFC in humans and the environment ................... 7
1.1.5 Instrumental analysis of PFC ............................................................................. 14
1.2 Objectives................................................................................................................... 16
2 Material and Methods.......................................................................................................... 19
2.1 Chemicals and reagents.............................................................................................. 19
2.2 Quality assurance / Quality control............................................................................ 20
2.3 Optimisation of PFC determination by nanoflow UPLC – TOF MS......................... 20
2.4 Method development for the determination of FTOH in SPMD ............................... 21
2.4.1 Theory of passive sampling................................................................................ 21
2.4.2 Semipermeable membrane devices .................................................................... 22
2.4.3 Purification of SPMD extracts by GPC.............................................................. 24
2.4.4 Optimisation of solid phase extraction of SPMD extracts ................................. 24
2.4.5 Optimisation of SPMD extraction...................................................................... 24
2.4.6 Final method for FTOH determination in SPMD .............................................. 25
i Table of Contents
2.5 Accumulation and elimination of FTOH in SPMD ................................................... 25
2.5.1 FTOH migration out of SPMD........................................................................... 25
2.5.1.1 FTOH migration out of SPMD into air .......................................................... 25
2.5.1.2 FTOH migration out of SPMD into solvent................................................... 26
2.5.2 FTOH migration from air into SPMD and pure triolein .................................... 26
2.5.2.1 High FTOH level experiments ....................................................................... 27
2.5.2.2 Low FTOH level experiments........................................................................ 27
2.6 Comparison of SPMD with XAD impregnated PUF disks and high volume active
sampling for determination of FTOH in air ........................................................................... 28
2.7 Determination of fluorotelomer alcohols on spruce needles...................................... 30
2.8 Determination of PFOA and PFOS in deposition samples collected at three sites in
the Alps .................................................................................................................................. 30
2.9 FTOH in housedust .................................................................................................... 32
2.10 PFC in household consumer products........................................................................ 33
2.10.1 Analysis of PFC in household consumer products............................................. 33
2.10.2 Calculation of consumer exposure ..................................................................... 33
2.11 Analysis of PFC in water and soil samples collected in the national park Serra dos
Órgãos, Brazil......................................................................................................................... 34
2.12 Chromatographic separation and detection of PFC.................................................... 35
2.12.1 PFC determination by nanoflow Aquity UPLC-TOF-MS ................................. 35
2.12.2 PFC determination by GC-MS........................................................................... 36
2.13 Quantification of PFC ................................................................................................ 37
3 Results and Discussion........................................................................................................ 39
3.1 Optimisation of PFC determination by nanoflow UPLC – TOF MS......................... 39
3.2 Method development for the determination of FTOH in SPMD ............................... 39
3.2.1 Purification of SPMD extracts by GPC.............................................................. 39
3.2.2 Purification of SPMD extracts by solid phase extraction .................................. 40
3.2.3 Optimisation of SPMD extraction...................................................................... 41
3.2.4 Final analytical method for the determination of FTOH in SPMD.................... 42
3.3 Accumulation and elimination of FTOH in SPMD ................................................... 43
3.3.1 Analytical parameters and quality assurance ..................................................... 43
3.3.2 FTOH migration out of SPMD........................................................................... 43
3.3.2.1 FTOH migration out of SPMD into air .......................................................... 43
ii Table of Contents
3.3.2.2 FTOH migration out of SPMD into solvent................................................... 45
3.3.3 FTOH migration from air into SPMD and pure triolein .................................... 45
3.3.3.1 High FTOH level experiments ....................................................................... 45
3.3.3.2 Low FTOH level experiments........................................................................ 46
3.3.4 Evaluation of SPMD as passive air samplers for FTOH.................................... 47
3.4 Comparison of SPMD with XAD impregnated PUF disks and high volume active
sampling for determination of FTOH in air ........................................................................... 49
3.4.1 Estimation of SPMD sampling rates and calibration of SPMD by High volume
active sampling................................................................................................................... 49
3.4.2 Calculation of SPMD derived FTOH air concentrations and comparison with
SIP and high volume active sampling................................................................................ 51
3.4.3 Determination of SIP derived FTOH air concentrations and comparison to the
other research groups ......................................................................................................... 54
3.4.4 Comparison of the determination of FTOH standard solutions analysed by the
laboratories of HMGU, GKSS, Lancaster University, and Environment Canada ............. 56
3.5 Method development for determination of F