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Development and application of a novel mass spectrometry ionization source for biological chemistry / Rhodri Owen

Swansea University Author: Rhodri Owen

DOI (Published version): 10.23889/SUthesis.61500

Abstract

Since its development, electrospray ionization (ESI) for the analysis of thermally labile, polar compounds and particularly biomolecules has been extremely useful. Not all compounds can be easily protonated and electron ionization (EI) is still a widely used ionization method for compounds like hydr...

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Published: Swansea 2022
Institution: Swansea University
Degree level: Doctoral
Degree name: Ph.D
Supervisor: Kelly, Steven L.
URI: https://cronfa.swan.ac.uk/Record/cronfa61500
first_indexed 2022-10-10T12:25:45Z
last_indexed 2023-01-13T19:22:17Z
id cronfa61500
recordtype RisThesis
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spelling 2022-10-10T13:39:21.3563946 v2 61500 2022-10-10 Development and application of a novel mass spectrometry ionization source for biological chemistry d58c5d38a44d72be924cdf2e1b62ad9f 0000-0002-3109-6653 Rhodri Owen Rhodri Owen true false 2022-10-10 MEDS Since its development, electrospray ionization (ESI) for the analysis of thermally labile, polar compounds and particularly biomolecules has been extremely useful. Not all compounds can be easily protonated and electron ionization (EI) is still a widely used ionization method for compounds like hydrocarbons. However, the low-pressure environment of the EI source requires complex and expensive vacuum systems and inlets. Therefore, a source which can ionises non-polar compounds while operating at atmospheric pressure would be highly advantageous. In this thesis I have undertaken development and characterisation of four prototype atmospheric pressure glow discharge ionization sources for the analysis of compounds not normally amiable to ionization by conventional atmospheric pressure ionization sources. A helium micro-glow discharge source (“Prototype V”) operated using a direct current power supply was studied and its discharge characterised. Its current-voltage relationship increased linearly which is typical of the abnormal glow regime while thermal imaging showed it had a “cold” discharge. Prototype V was successfully interfaced with a Xevo G2-S time-of-flight and a Xevo TQ-S triple quadrupole (Waters Corp, Wilmslow, UK) and used with a range of sample introduction methods, initially a solids probe, but later APCI and ESI probes. These probes enabled prototype V to readily integrate with separation sciences; specifically liquid chromatography was demonstrated for complex mixture analysis. Prototype V exhibited high analytical sensitivity in the nanogram range in both positive and negative modes and could ionize a wide range of compound chemistries from polar to non-polar. In particular it showed sensitivity to non-polar compounds in negative-ion mode when compared to ESI. This gives the source the potential to operate in conjunction with a range of sample inlets and in combination with other ionization techniques as part of a multimodal platform to analyse the widest range of samples and a step towards a universal source. E-Thesis Swansea ORCiD identifier: https://orcid.org/0000-0002-3109-6653 2 9 2022 2022-09-02 10.23889/SUthesis.61500 COLLEGE NANME Medical School COLLEGE CODE MEDS Swansea University Kelly, Steven L. Doctoral Ph.D EPSRC: EP/R51312x/1 2022-10-10T13:39:21.3563946 2022-10-10T13:22:38.9778047 Faculty of Medicine, Health and Life Sciences Swansea University Medical School - Medicine Rhodri Owen 0000-0002-3109-6653 1 61500__25380__4420f8877f8a41c5b69b1bfe47577ab2.pdf Owen_Rhodri_N_PhD_Thesis_Final_Redacted_Cronfa.pdf 2022-10-10T13:36:44.5701550 Output 9916717 application/pdf E-Thesis – open access true Copyright: The author, Rhodri N. Owen, 2022 true eng
title Development and application of a novel mass spectrometry ionization source for biological chemistry
spellingShingle Development and application of a novel mass spectrometry ionization source for biological chemistry
Rhodri Owen
title_short Development and application of a novel mass spectrometry ionization source for biological chemistry
title_full Development and application of a novel mass spectrometry ionization source for biological chemistry
title_fullStr Development and application of a novel mass spectrometry ionization source for biological chemistry
title_full_unstemmed Development and application of a novel mass spectrometry ionization source for biological chemistry
title_sort Development and application of a novel mass spectrometry ionization source for biological chemistry
author_id_str_mv d58c5d38a44d72be924cdf2e1b62ad9f
author_id_fullname_str_mv d58c5d38a44d72be924cdf2e1b62ad9f_***_Rhodri Owen
author Rhodri Owen
author2 Rhodri Owen
format E-Thesis
publishDate 2022
institution Swansea University
doi_str_mv 10.23889/SUthesis.61500
college_str Faculty of Medicine, Health and Life Sciences
hierarchytype
hierarchy_top_id facultyofmedicinehealthandlifesciences
hierarchy_top_title Faculty of Medicine, Health and Life Sciences
hierarchy_parent_id facultyofmedicinehealthandlifesciences
hierarchy_parent_title Faculty of Medicine, Health and Life Sciences
department_str Swansea University Medical School - Medicine{{{_:::_}}}Faculty of Medicine, Health and Life Sciences{{{_:::_}}}Swansea University Medical School - Medicine
document_store_str 1
active_str 0
description Since its development, electrospray ionization (ESI) for the analysis of thermally labile, polar compounds and particularly biomolecules has been extremely useful. Not all compounds can be easily protonated and electron ionization (EI) is still a widely used ionization method for compounds like hydrocarbons. However, the low-pressure environment of the EI source requires complex and expensive vacuum systems and inlets. Therefore, a source which can ionises non-polar compounds while operating at atmospheric pressure would be highly advantageous. In this thesis I have undertaken development and characterisation of four prototype atmospheric pressure glow discharge ionization sources for the analysis of compounds not normally amiable to ionization by conventional atmospheric pressure ionization sources. A helium micro-glow discharge source (“Prototype V”) operated using a direct current power supply was studied and its discharge characterised. Its current-voltage relationship increased linearly which is typical of the abnormal glow regime while thermal imaging showed it had a “cold” discharge. Prototype V was successfully interfaced with a Xevo G2-S time-of-flight and a Xevo TQ-S triple quadrupole (Waters Corp, Wilmslow, UK) and used with a range of sample introduction methods, initially a solids probe, but later APCI and ESI probes. These probes enabled prototype V to readily integrate with separation sciences; specifically liquid chromatography was demonstrated for complex mixture analysis. Prototype V exhibited high analytical sensitivity in the nanogram range in both positive and negative modes and could ionize a wide range of compound chemistries from polar to non-polar. In particular it showed sensitivity to non-polar compounds in negative-ion mode when compared to ESI. This gives the source the potential to operate in conjunction with a range of sample inlets and in combination with other ionization techniques as part of a multimodal platform to analyse the widest range of samples and a step towards a universal source.
published_date 2022-09-02T05:39:30Z
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score 11.0583515

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