Author ORCID Identifier

https://orcid.org/0000-0002-0246-0735

Semester

Summer

Date of Graduation

2025

Document Type

Dissertation

Degree Type

PhD

College

Eberly College of Arts and Sciences

Department

Chemistry

Committee Chair

Lisa Holland

Committee Member

Stephen Valentine

Committee Member

Peng Li

Committee Member

Harry Finklea

Committee Member

Parviz Famouri

Abstract

Capillary electrophoresis (CE) coupled to mass spectrometry (MS) offers a powerful analytical platform that unites high-efficiency separation with molecular-level identification. Despite its potential, limitations in interfacing and usability have constrained the widespread application of CE-MS. This thesis presents methodological advancements to enhance CE-based analysis through innovative interfacing, automation, and application to both small molecules and nanoparticle vaccine formulations. First, a nanoflow sheath CE-VSSI-MS interface is developed to overcome the limitations associated with flow-dependent ionization, enabling the use of narrow-bore capillaries, high separation voltages, and flexible pH conditions. This configuration effectively separated and detected diverse analytes, including β-blockers, amino acids, and nonsteroidal anti-inflammatory drugs across nanomolar to micromolar concentrations using both normal and reversed polarity modes. Building on this, a dual-function CE-VSSI-MS platform is fabricated to integrate ionization and make-up flow into a compact, user-friendly interface that supports the automation of commercial Beckman Coulter P/ACE™ MDQ. The analytical performance of this novel configuration is validated using small molecules under near-neutral and acidic pH. Moreover, this interface is employed to detect biologically relevant peptides, including transferrin digestion products and Huntington’s disease-associated peptides, enabling detection of peptide oligomers that are not observable with conventional CE-UV detection. Recognizing the growing importance of nanoparticle-based biopharmaceuticals, the scope of this work is extended to vaccine analysis using CE with UV detection. A robust capillary zone electrophoresis (CZE) method is developed and validated according to ICH Q2 guidelines for the simultaneous quantification of Human Papillomavirus (HPV) Virus-Like Particles (VLPs) and squalene nano-emulsion (SNE) adjuvants. These are two heterogeneous nanoparticles with similar sizes but distinct physicochemical properties. Utilizing the charge-to-size separation mechanism, the method achieved excellent linearity, accuracy, and precision with minimal sample preparation and demonstrated applicability for broader nanoparticle–adjuvant systems. Together, these studies demonstrate the versatility and analytical power of CE-based platforms, whether coupled with mass spectrometry or UV detection, for analysis of pharmaceutical small molecules and complex vaccine nanoparticle mixtures.

Available for download on Monday, June 22, 2026

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