Development of a Novel Mass Spectrometric ... - Jacobs University
Development of a Novel Mass Spectrometric ... - Jacobs University Development of a Novel Mass Spectrometric ... - Jacobs University
Acknowledgements First and farmost, thanks are to ‘God’ for my life through all tests in the past years. You have made my life more bountiful. May your name be exalted, honoured, and glorified. My sincere gratitude goes to Prof. Dr. Nikolai Kuhnert for his continuous supervision, advice, support and inspiration as well as for his confidence he gifted to work in generous freedom. Thanks for being able to work with modern analytical techniques and to attend interesting international conferences. I’m so glad to have come to know him. I’d like to deeply thank the Fond für Angewandte Umweltforschung des Landes Bremen and the Bremer Entsorgungsbetriebe (BEB Company) for the support given to this project. I would like to thank my dear wife Adal for support and love through out the study years, my parents Mahmoud and Salwa Hourani, my brothers Wassim, Ibrahim and Hamzi, and my sisters Fatemah and Kawkab, all my dear friends and in particular Hany Nour. My sincere love and gratitude goes for Dr. Ursula Zimoch whose splendid care and support were more than intriguing for me during my study. Needless to say how much gratitude I owe to Prof. Dr. Angela Danil De Namor for continued support and advice. Without her contribution this Ph.D study wouldn’t have been achieved. I am tempted to individually thank all my colleagues in our laboratory in as much as thanks to Mrs Anja Müller, for the technical support.
This work has been carried out under the supervision of Prof. Dr. Nikolai Kuhnert in the analytical and organic laboratory of Chemistry Department at Jacobs University Bremen in Germany. Abstract The lack of a routine characterization method for non-volatile hydrocarbons has been an ongoing problem preventing mass spectrometry from the analysis of these hydrocarbons within many sources. Non-polar hydrocarbons are still difficult to be detected by mass spectrometry. Although several studies targeted this problem, lack of self-ionization has been limiting the ability of mass spectrometry to examine these hydrocarbons. A novel identification method for saturated straight-chain hydrocarbons in light shredder waste fraction under atmospheric pressure chemical ionization mass spectrometry (APCI-MS) has been developed. Ionization of alkanes under nitrogen gas source favoured hydrogen abstraction producing majorly (M-H) + ions which are strictly corresponding to their respective series of n-alkanes between n-decane (C10) and n-tetracontane (C40). The method is shown to produce intact gas phase ions of n- alkane in both reference and real life waste samples. APCI-MS 2 fragmentation data assisted in the structural verification of the n-alkanes investigated in both standard and waste mixtures. Additionally the total chemical composition of the light shredder waste fraction was translated by the same method. The mass spectrum displayed a bimodal distribution of odd and even mass ions with a molecular weight distribution range of m/z 200-900 Da. Molecular formulas for a 1000 unsaturated hydrocarbon compounds suggested a dehydrogenation process. The molecular masses were plotted on a Kendrick plot which was successfully employed for monitoring sample degradation. Another selection of high mass linear, branched and cyclic hydrocarbons, reported to be notoriously difficult to ionize, were examined during this study. Using optimized APCI conditions all of these analytes could be ionized without the use of an additional
- Page 1 and 2: Development of a Novel Mass Spectro
- Page 3: Declaration of Authorship I ,Nadim
- Page 7 and 8: Contents Contents Declaration of Au
- Page 9 and 10: List of Figures List of Figures Fig
- Page 11 and 12: List of Figures Figure 3-39 MS 2 fr
- Page 13 and 14: List of Tables List of Tables Table
- Page 15 and 16: Abbreviations Abbreviations APCI AP
- Page 17 and 18: Abbreviations UV VGOs VOCs VRs ultr
- Page 19 and 20: Introduction Analytical chemistry h
- Page 21 and 22: Introduction 1.2 Presence and Fate
- Page 23 and 24: Introduction aliphatic hydrocarbons
- Page 25 and 26: Introduction Figure 1-1 Examples of
- Page 27 and 28: Introduction Figure 1-2 Range of io
- Page 29 and 30: Introduction fractions. 42 Another
- Page 31 and 32: Introduction 1.3.5 APLI Other crude
- Page 33 and 34: Introduction products). Other molec
- Page 35 and 36: Introduction Other studies performe
- Page 37 and 38: Introduction APLI-FT ICR-MS Crude o
- Page 39 and 40: Introduction spectrometry in as muc
- Page 41 and 42: Introduction catalytic processing t
- Page 43 and 44: Introduction Figure 1-6 Kendrick ma
- Page 45 and 46: Introduction including determinatio
- Page 47 and 48: Introduction 1.5 Scope and Signific
- Page 49 and 50: Experimental e) Other model mixture
- Page 51 and 52: Experimental 2.2.2 Preparation of O
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This work has been carried out under the supervision <strong>of</strong> Pr<strong>of</strong>. Dr. Nikolai Kuhnert in<br />
the analytical and organic laboratory <strong>of</strong> Chemistry Department at <strong>Jacobs</strong> <strong>University</strong><br />
Bremen in Germany.<br />
Abstract<br />
The lack <strong>of</strong> a routine characterization method for non-volatile hydrocarbons has been<br />
an ongoing problem preventing mass spectrometry from the analysis <strong>of</strong> these<br />
hydrocarbons within many sources. Non-polar hydrocarbons are still difficult to be<br />
detected by mass spectrometry. Although several studies targeted this problem, lack <strong>of</strong><br />
self-ionization has been limiting the ability <strong>of</strong> mass spectrometry to examine these<br />
hydrocarbons.<br />
A novel identification method for saturated straight-chain hydrocarbons in light<br />
shredder waste fraction under atmospheric pressure chemical ionization mass<br />
spectrometry (APCI-MS) has been developed. Ionization <strong>of</strong> alkanes under nitrogen gas<br />
source favoured hydrogen abstraction producing majorly (M-H) + ions which are<br />
strictly corresponding to their respective series <strong>of</strong> n-alkanes between n-decane (C10)<br />
and n-tetracontane (C40). The method is shown to produce intact gas phase ions <strong>of</strong> n-<br />
alkane in both reference and real life waste samples. APCI-MS 2 fragmentation data<br />
assisted in the structural verification <strong>of</strong> the n-alkanes investigated in both standard and<br />
waste mixtures. Additionally the total chemical composition <strong>of</strong> the light shredder<br />
waste fraction was translated by the same method. The mass spectrum displayed a<br />
bimodal distribution <strong>of</strong> odd and even mass ions with a molecular weight distribution<br />
range <strong>of</strong> m/z 200-900 Da. Molecular formulas for a 1000 unsaturated hydrocarbon<br />
compounds suggested a dehydrogenation process. The molecular masses were plotted<br />
on a Kendrick plot which was successfully employed for monitoring sample<br />
degradation.<br />
Another selection <strong>of</strong> high mass linear, branched and cyclic hydrocarbons, reported to<br />
be notoriously difficult to ionize, were examined during this study. Using optimized<br />
APCI conditions all <strong>of</strong> these analytes could be ionized without the use <strong>of</strong> an additional
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