University of Illinois Urbana-Champaign

Systematic study of redox-active polymers for energy storage: Exploring structural modulation, electrolyte interactions and programmable degradation

Ibrahim, Nafisa Aden

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https://hdl.handle.net/2142/129515

Description

Title
Systematic study of redox-active polymers for energy storage: Exploring structural modulation, electrolyte interactions and programmable degradation
Author(s)
Ibrahim, Nafisa Aden
Issue Date
2025-04-16
Director of Research (if dissertation) or Advisor (if thesis)
  • Rodríguez-López, Joaquín
  • Zimmerman, Steven C
Doctoral Committee Chair(s)
  • Rodríguez-López, Joaquín
  • Zimmerman, Steven C
Committee Member(s)
  • Diao, Ying
  • Shen, Mei
Department of Study
Chemistry
Discipline
Chemistry
Degree Granting Institution
University of Illinois Urbana-Champaign
Degree Name
Ph.D.
Degree Level
Dissertation
Keyword(s)
Redox-active polymers, electrochemistry, Mesolytic cleavage
Abstract
The development of sustainable energy storage solutions necessitates innovative materials that offer high efficiency, stability, and recyclability. Redox-active polymers (RAPs) are a promising alternative to traditional small-molecule redox species due to their modularity, tunability, and potential for eco-friendly applications. However, their widespread implementation ishindered by key challenges, including electrolyte-induced redox behavior shifts, irreversible degradation, and electrode fouling. This dissertation investigates strategies to overcome these challenges through three interconnected research themes. Chapter 1 provides an overview of RAP limitations and research directions, focusing on: (1) the influence of electrolyte composition on RAP reactivity and charge transport, (2) the development of mesolytic cleavage strategies for controlled polymer degradation, and (3) the design of tunable ferrocene-based RAPs for optimized redox behavior. Chapter 2 explores the potential of mesolytic cleavage using homobenzylic ether linkers to enable programmed RAP degradation, facilitating electrode defouling and active material recovery. Chapter 3 examines the integration of Jeffamine copolymers in ferrocene-containing RAPs, demonstrating tailored redox properties, reduced electrostatic interactions, and enhanced electrochemical stability. By employing electrochemical characterization, spectroelectrochemical analysis, and strategic polymer design, this work advances the understanding and development of next-generation RAPs. The findings presented here contribute to the broader goal of creating sustainable, high-performance materials for energy storage applications, particularly in redox flow batteries.
Graduation Semester
2025-05
Type of Resource
Thesis
Handle URL
https://hdl.handle.net/2142/129515
Copyright and License Information
Copyright 2025 Nafisa Ibrahim

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