Date of Award

May 2020

Document Type

Thesis

Degree Name

Master of Science (MS)

Department

Chemistry

Committee Member

Richard K Marcus

Committee Member

Carlos D Garcia

Committee Member

George Chumanov

Abstract

Mass spectrometry is a powerful analytical tool that can be used to identify and quantify diverse classes of analytes, including atomic, small molecular, and large biological species. The limitation in this powerful technique, however, lies in the fact that these various analytes require vastly different instrumental configurations. Elemental analysis, for example, requires instrumentation capable of hard ionization, such as inductively coupled plasma mass spectrometry (ICP-MS) and thermal ionization mass spectrometry (TIMS). These instruments also require very high-resolution mass analyzers so isobaric elemental isotopes can be clearly resolved and quantified, typically employing sector field and Fourier transform ion cyclotron resonance (FT-ICR) analyzers. Conversely, large biomolecules require soft ionization methods that preserve the analytes’ native state, such as electrospray (ESI) and matrix-assisted laser desorption ionization (MALDI). The most common mass analyzers used for biological mass spectrometry are ion-traps, quadrupoles, and time-of-flight (TOF) analyzers. In this work, a novel liquid-sampling atmospheric pressure glow discharge (LS-APGD) ionization source is coupled to a high-resolution Orbitrap mass analyzer for the analysis of diverse analytical species. The potential powering modes and geometries of the LS-APGD were evaluated for the analysis of a multi-element solution as well as for the analysis of uranium isotope ratios for nuclear nonproliferation applications. The LS-APGD was then evaluated for the analysis of a seleno-mercury complex.

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