Interrogation of Ion-Neutral Complexes by Trapped Ion Mobility-Mass Spectrometry and Theoretical Calculations

Authors

Alan A. McKenzie Coe, Florida International UniversityFollow

Document Type

Dissertation

Degree

Doctor of Philosophy (PhD)

Major/Program

Chemistry

First Advisor's Name

Francisco Alberto Fernandez-Lima

First Advisor's Committee Title

Committee Chair

Second Advisor's Name

José R. Almirall

Second Advisor's Committee Title

Committee Member

Third Advisor's Name

Hebin Li

Third Advisor's Committee Title

Committee Member

Fourth Advisor's Name

Alexander M. Mebel

Fourth Advisor's Committee Title

Committee Member

Fifth Advisor's Name

James Martin E. Quirke

Fifth Advisor's Committee Title

Committee Member

Keywords

Analytical Chemistry, Trapped Ion Mobility Spectrometry, Mass Spectrometry, Ion-Neutral Complexes, Adduct Complexes, Ion Stability

Date of Defense

3-22-2019

Abstract

In the present study, the fundamentals of molecular ion trapping and the application of trapped ion mobility spectrometry coupled to mass spectrometry (TIMS-MS) to the separation and identification of molecular components in complex mixtures are shown. In particular, ion-neutral complexes lifetimes, relative stability, binding energies and candidate structures are described for common explosives during TIMS-MS, as well as the effect of the micro-environment, during complex sample analysis. A novel TIMS-MS workflow was developed for the detection of both inorganic residues (IGSR; inorganic gunshot residues) and organic residues (OGSR) of firearm discharge residue from skin swabs, capable of high specificity and short analysis time (few min) from a small sample size (µL). The TIMS-MS workflow provided fast, post-ionization, high resolution mobility (R_IMS ~ 150–250) and mass separations (R_MS ~ 20–40k) with isotopic pattern recognition. In addition, for the first time, liquid chromatography, trapped ion mobility spectrometry and mass spectrometry are combined for fast separation, identification and quantitation of labile juvenile hormones (JHs) with increased sensitivity and confidence levels. In particular, the use of the parent ion and in-source diagnostic fragment ions in a LC-TIMS-MS workflow was developed, complemented with novel extraction and labeled standards for the detection and quantitation of JHs in biological samples.

Identifier

FIDC007648

Recommended Citation

McKenzie Coe, Alan A., "Interrogation of Ion-Neutral Complexes by Trapped Ion Mobility-Mass Spectrometry and Theoretical Calculations" (2019). FIU Electronic Theses and Dissertations. 4035.
https://digitalcommons.fiu.edu/etd/4035