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Advancing petroleomics methodologies and their application to crude and heavy fuel oils, asphaltenes, and the environment
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Thomas, Mary Joanna (2020) Advancing petroleomics methodologies and their application to crude and heavy fuel oils, asphaltenes, and the environment. PhD thesis, University of Warwick.
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Official URL: http://webcat.warwick.ac.uk/record=b3736674
Abstract
The work presented herein describes advancing analytical procedures utilising, and associated with, ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS), applied to characterising ultracomplex petroleum-related samples. A proof-of-concept FTICR MS characterisation of marine heavy fuel oils (HFOs) is initially performed. Building upon this, the asphaltene fractions of eight HFOs, including one that may have undergone desulfurization via an oxidation process, were studied. Infra-red multi photon dissociation (IRMPD) fragmentation was utilised for structural insight. Statistical analyses and novel visualisation modes provide a comprehensive, simplified, means of comparison.
The impact of oxidation on lubricant base oils was explored through the application of both direct infusion (DI) and gas chromatography (GC) FTICR MS. The effectiveness of antioxidant additive packages is demonstrated, with the semi-quantitative analysis indicating the extent to which benchtop oxidation procedures may provide a robust alternative to full engine tests.
The operating parameters of FTICR MS vary widely, with the impact on the relative spectral intensity of analyte species poorly understood. The influence of solvent system and flow rate on the observed profile and the ion-type ratio in positive-ion atmospheric pressure ionization (APPI) analyses is demonstrated. Furthermore, the O2/O4 class relative intensity ratio, proposed as a means by which to monitor the presence of anthropogenic compounds in the environment is found to invert at low pH in negative-ion electrospray (ESI) analyses.
The emerging role of petroleomics in environmental research is demonstrated further, with soil extracts characterised using DI and GC-FTICR MS. Differing relative contributions from a range of anthropogenic contaminants, and the isomeric complexity underlying individual assignments, are observed between sampling depths.
Finally, key findings are summarized and future research directions, with respect to advancing petroleomics methodologies and enhancing understanding of complex samples.
Item Type: | Thesis (PhD) | ||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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Library of Congress Subject Headings (LCSH): | Ion cyclotron resonance spectrometry, Fourier transform spectroscopy, Petroleum -- Analysis, Heavy oil as fuel, Asphaltene | ||||
Official Date: | June 2020 | ||||
Dates: |
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Institution: | University of Warwick | ||||
Theses Department: | Molecular Analytical Science Centre for Doctoral Training | ||||
Thesis Type: | PhD | ||||
Publication Status: | Unpublished | ||||
Supervisor(s)/Advisor: | Barrow, Mark P. | ||||
Format of File: | |||||
Extent: | xxviii, 229 leaves : illustrations, map | ||||
Language: | eng |
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