Doctor of Philosophy (PhD)
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First Advisor's Name
First Advisor's Committee Title
Second Advisor's Name
Jeremy W. Chambers
Second Advisor's Committee Title
Third Advisor's Name
Third Advisor's Committee Title
Fourth Advisor's Name
Fourth Advisor's Committee Title
Fifth Advisor's Name
Fifth Advisor's Committee Title
Mass spectrometry, ion mobility, biological samples
Date of Defense
There is a need for fast, accurate and cost-effective protocols capable of assessing biomolecules at the molecular level (e.g., proteins, lipids and metabolites) from biological specimens. Mass spectrometry (MS) based techniques have become the analytical gold standard for identification and characterization of biomarkers in biological samples. The high throughput and short analysis time scales enables to follow biological processes while providing detailed chemical and spatial characterization. One of the current challenges in biological MS, is the high molecular complexity, chemical diversity and dynamic range. In this dissertation, the use of multi-modal mass spectrometry workflows -mass spectrometry imaging and ion mobility spectrometry - enables the untargeted and targeted analysis of biomolecules. The performance of mass spectrometry imaging techniques such as TOF-SIMS and MALDI-FTICR MS was evaluated for the spatial characterization of lipids, a chemotherapeutic drug agent, and neuropeptides. The orthogonality between ambient sampling liquid extraction surface analysis (LESA), ion mobility spectrometry and mass spectrometry (LESA-IMS-MS) was evaluated for the detection of small molecules from complex biological samples, such as common biological organs (e.g., liver, brain, and skin) and three-dimensional multicellular spheroid (MCS) models of cancer cell lines. This dissertation showcases the development of new workflows that integrate ambient sampling with complementary gas-phase post-ionization separation techniques to study complex biological samples.
Previously Published In
Haler, J.; Sisley, E.; Cintron-Diaz, Y.; Meitei, S.; Cooper, H.; Fernandez-Lima, F., Workflow for fast lipid screening using LESA-FT-ICR-MS. Anal Methods, 2019, 11, 2385. DOI: 10.1039/c8ay02739k
Cintron-Diaz, Y.; Acanda de la Rocha, A.; Castellanos, A.; Chambers, J.; and Fernandez-Lima, F., Mapping chemotherapeutic drug distribution in cancer cell spheroids using 2D-TOF-SIMS and LESA-TIMS-MS. Analyst, 2020, DOI: 10.1039/C9AN02245G
K. Jeanne Dit Fouque, M. Wellmann, D. Leyva Bombuse, M. Santos-Fernandez, Y. L. Cintron-Diaz, M. E. Gomez-Hernandez, D. Kaplan, V. G. Voinov and F. Fernandez-Lima, Effective Discrimination of Gas-Phase Peptide Conformers using TIMS-ECD-ToF MS/MS. Analytical Methods (accepted for publication on 10-18-2021)
Cintron-Diaz, Yarixa L., "Characterization of Biological Samples using Multi-modal Mass Spectrometry" (2021). FIU Electronic Theses and Dissertations. 4854.
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