Date of Award

2025-07-01

Degree Name

Doctor of Philosophy

Department

Chemistry

Advisor(s)

Dino Villagran

Abstract

Understanding the fundamental electrochemistry of perfluoroalkyl substances (PFAS) is key to developing effective water remediation and sensing strategies. This work explores the thermodynamics and kinetics of perfluorooctanoic acid (PFOA) electroreduction, focusing on C-F bond cleavage. These insights were applied to design a highly sensitive electrochemical sensor for detecting trace levels of PFOA in water. This dissertation focuses on the electrochemical investigation of the reduction reaction of PFOA in aqueous and organic media employing different electrode materials. This exploration allows to understand the defluorination reaction of PFAS to further propose potential strategies for water treatment and PFOA electrosensing. Through electrochemical, spectroscopical and computational techniques, insights into the mechanism are obtained, covering the kinetics, thermodynamics, adsorption, and reorganization effects. In addition, the use of nanomaterials enabled us to design a highly sensitive electrochemical sensor with the potential usability in real water samples. Besides, a new decoration based on molecular electrografted layers (MELS) by attaching tetrafluoro-1,4-benzene moieties on GCE. This system also achieved ppt-level sensitivity and selectivity for PFOA and PFOS across various water matrices, with high stability and tunable molecular recognition. Overall, this dissertation provides a dual contribution: elucidating PFAS electrochemical degradation pathways and delivering practical sensing platforms for environmental monitoring. Future work will focus on full analytical validation and broader application in complex water systems, as well as the exploration of rational designed materials for water treatment.

Language

en

Provenance

Received from ProQuest

File Size

141 p.

File Format

application/pdf

Rights Holder

Jonathan Josue Calvillo Solis

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