Date of Award

12-2026

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Chemistry and Chemical Engineering

First Advisor

Yi Liao

Second Advisor

M. Toufiq Reza

Third Advisor

Nasri Nesnas

Fourth Advisor

Roberto Peverati

Abstract

Control over proton transfer enables the regulation of many pH-dependent chemical and material processes. Stimuli-responsive functional materials provide a means of achieving this control. Functional materials such as Metastable-state photoacids (mPAHs) reversibly release large amounts of protons when stimulated by light from a weakly acidic site within their structure. However, the dark acidities of previously reported mPAHs limit their use under basic conditions. To address this limitation, a benzimidazole-type mPAH was developed with an improved ground-state pKa of 11.9 and a metastable-state pKa of 9.8, enabling reversible proton transfer under mildly basic conditions. Additional mPAHs were examined to determine how structural modifications influence their physicochemical properties. Temperature-dependent proton transfer, or thermal acidity, was investigated using m-cresol to promote CO₂ release from a morpholine-based sorbent and using phenol to mitigate the thermal thinning of poly(4-vinylpyridine) viscosity. Together, these studies demonstrate light- and temperature-controlled proton transfer in photoacid, CO₂-capture, and polymer systems.

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