E-Thesis 423 views 225 downloads
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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Swansea
2022
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Institution: | Swansea University |
Degree level: | Doctoral |
Degree name: | Ph.D |
Supervisor: | Kelly, Steven L. |
URI: | https://cronfa.swan.ac.uk/Record/cronfa61500 |
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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 BMS 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 Biomedical Sciences COLLEGE CODE BMS 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 |
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E-Thesis |
publishDate |
2022 |
institution |
Swansea University |
doi_str_mv |
10.23889/SUthesis.61500 |
college_str |
Faculty of Medicine, Health and Life Sciences |
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|
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 |
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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 |
2022-09-02T04:20:21Z |
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1763754347656642560 |
score |
11.021648 |