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Applications of Novel Fragmentation Methods in Mass Spectrometry: Expanding the Mass Spectrometry Toolbox for Glycomics
Abstract
Carbohydrates and glycoconjugates are critical components of biological systems, playing large roles in molecular function and misfunction. Understanding these roles can be difficult as small changes to structure and concentration can cause large changes in the surrounding system. Mass spectrometry (MS) is one tool well suited for elucidating the structures of free carbohydrates and glycoconjugates. Most of the work presented herein is focused on fragmentation studies to improve the methods available to derive structure, with an emphasis on glycoproteins and oligosaccharides.Chapter 1 provides an introduction to MS and MSMS techniques, providing an extended explanation for two-dimensional (2D) Fourier transform ion cyclotron resonance (FTICR) MS.Chapter 2 demonstrates that 2D FTICR with infrared multiphoton dissociation and electron capture dissociation can be applied to glycoproteomics samples to derive the site of glycosylation and information regarding the structure of the glycan. Chapter 3 utilizes matrix spray deposition techniques from MS imaging (MSI) to utilize matrix-assisted laser desorption ionization (MALDI) as the ionization mode for 2D FTICR experiments. Chapter 4 describes work seeking to reduce or eliminate oligosaccharide rearrangement using surface-induced dissociation. Chapter 5 describes a collaboration with the Du Group to confirm that a small molecule, lysochelin, produced by Lysobacter enzymogenes is secreted by colonies using MSI.Lastly, chapter 6 summarizes the work discussed in this dissertation and provides suggestions for further work to improve 2D FTICR, including work to better understand the effects of secondary fragmentation and energetics in 2D spectra as well as apply MALDI and 2D FTICR to surface analysis.
Subject Area
Chemistry
Recommended Citation
Bell, Richard J, "Applications of Novel Fragmentation Methods in Mass Spectrometry: Expanding the Mass Spectrometry Toolbox for Glycomics" (2022). ETD collection for University of Nebraska-Lincoln. AAI29068434.
https://digitalcommons.unl.edu/dissertations/AAI29068434