Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS

Internal combustion powered vehicles will be used in road, rail, marine and aviation applications for the foreseeable future, particularly in developing nations. Formation of insoluble deposits on key engine components, such as fuel injectors and filters, affect all these vehicle types to cause incr...

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Main Author: Edney, Max
Format: Thesis (University of Nottingham only)
Language:English
Published: 2022
Subjects:
Online Access:https://eprints.nottingham.ac.uk/71790/
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author Edney, Max
author_facet Edney, Max
author_sort Edney, Max
building Nottingham Research Data Repository
collection Online Access
description Internal combustion powered vehicles will be used in road, rail, marine and aviation applications for the foreseeable future, particularly in developing nations. Formation of insoluble deposits on key engine components, such as fuel injectors and filters, affect all these vehicle types to cause increased emissions and fuel consumption. Despite years of research, little is known of the molecular composition, origin of contributing species and formation pathways of deposits, especially of their carbonaceous matrix. This is due to their insolubility and layered nature, meaning traditional solvent-based analysis techniques are unsuited to probe their composition and structure. This thesis first details previous attempts of characterizing deposits and shows the need for high resolution mass spectrometry (MS) techniques to analyse deposits in-situ (i.e., on the component itself). To address this knowledge gap, 3D Orbitrap secondary ion mass spectrometry (3D OrbiSIMS) Ar3000+ gas cluster ion beam (GCIB) depth profiling and chemical imaging is applied to deposits from gasoline and diesel vehicles. Molecular species are accurately identified and confirmed using MS/MS for the first time, with supporting X-ray photoelectron spectroscopy (XPS) data. Key species identified include trace levels of lubricating oil derived alkyl benzyl sulfonates, inorganic salts (up to 16 %) in diesel samples and nitrogen containing species (up to 5 %) in the gasoline deposit. Finally, high amounts (> 80 %) of carbon in all samples, which are attributed to polycyclic aromatic hydrocarbon (PAH) type species, previously only speculated to exist in deposits.
first_indexed 2025-11-14T20:55:34Z
format Thesis (University of Nottingham only)
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institution University of Nottingham Malaysia Campus
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language English
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publishDate 2022
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spelling nottingham-717902024-12-13T04:30:11Z https://eprints.nottingham.ac.uk/71790/ Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS Edney, Max Internal combustion powered vehicles will be used in road, rail, marine and aviation applications for the foreseeable future, particularly in developing nations. Formation of insoluble deposits on key engine components, such as fuel injectors and filters, affect all these vehicle types to cause increased emissions and fuel consumption. Despite years of research, little is known of the molecular composition, origin of contributing species and formation pathways of deposits, especially of their carbonaceous matrix. This is due to their insolubility and layered nature, meaning traditional solvent-based analysis techniques are unsuited to probe their composition and structure. This thesis first details previous attempts of characterizing deposits and shows the need for high resolution mass spectrometry (MS) techniques to analyse deposits in-situ (i.e., on the component itself). To address this knowledge gap, 3D Orbitrap secondary ion mass spectrometry (3D OrbiSIMS) Ar3000+ gas cluster ion beam (GCIB) depth profiling and chemical imaging is applied to deposits from gasoline and diesel vehicles. Molecular species are accurately identified and confirmed using MS/MS for the first time, with supporting X-ray photoelectron spectroscopy (XPS) data. Key species identified include trace levels of lubricating oil derived alkyl benzyl sulfonates, inorganic salts (up to 16 %) in diesel samples and nitrogen containing species (up to 5 %) in the gasoline deposit. Finally, high amounts (> 80 %) of carbon in all samples, which are attributed to polycyclic aromatic hydrocarbon (PAH) type species, previously only speculated to exist in deposits. 2022-12-13 Thesis (University of Nottingham only) NonPeerReviewed application/pdf en cc_by https://eprints.nottingham.ac.uk/71790/1/Thesis_MKE.pdf Edney, Max (2022) Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS. EngD thesis, University of Nottingham. Molecular compositions Engine deposits OrbiSIMS Gas cluster ion beam GCIB
spellingShingle Molecular compositions
Engine deposits
OrbiSIMS
Gas cluster ion beam
GCIB
Edney, Max
Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS
title Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS
title_full Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS
title_fullStr Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS
title_full_unstemmed Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS
title_short Uncovering the molecular compositions, origins and formation pathways of engine deposits using OrbiSIMS
title_sort uncovering the molecular compositions, origins and formation pathways of engine deposits using orbisims
topic Molecular compositions
Engine deposits
OrbiSIMS
Gas cluster ion beam
GCIB
url https://eprints.nottingham.ac.uk/71790/