University of Illinois Urbana-Champaign

Structure and solvation control of redox-metallopolymers for electrochemically-mediated ion separations

Chen, Raylin

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https://hdl.handle.net/2142/121211

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Title
Structure and solvation control of redox-metallopolymers for electrochemically-mediated ion separations
Author(s)
Chen, Raylin
Issue Date
2023-07-05
Director of Research (if dissertation) or Advisor (if thesis)
Su, Xiao
Doctoral Committee Chair(s)
Su, Xiao
Committee Member(s)
  • Higdon, Jonathan J. L.
  • Kenis, Paul J. A.
  • Gewirth, Andrew A.
Department of Study
Chemical & Biomolecular Engr
Discipline
Chemical Engineering
Degree Granting Institution
University of Illinois at Urbana-Champaign
Degree Name
Ph.D.
Degree Level
Dissertation
Keyword(s)
electrochemical separations
Abstract
Electroresponsive polymer materials have garnered interest as selective and electrically switchable adsorbent materials. The improved selectivity of these materials would allow for the increased efficiency of existing adsorption separation processes and electrically switchable nature of these materials could greenify adsorption separations processes by reducing the need for chemical elution. This thesis presents some work on elucidating the underlying physicochemical mechanisms that govern the selectivity of ferrocene polymers toward target anion species. After a critical review of the current state of the art literature, the results are summarized in two parts. First, we demonstrated that a change in the ferrocene polymer structure, from a pendant ferrocene to a main-chain ferrocene, resulted in different ion selectivity towards a range of transition metal oxyanions. Through electronic structure calculations, we showed that the addition of a electron donation silane substituent on ferrocene can change ion binding energies with the ferrocenium binding cite based on the the ionization energy of the ion. Second, through copolymerization of a ferrocene moiety with another hydrophilic moiety, we could change the hydrophilicity of the polymer, independent of the ferrocene cite charge transfer. This change in hydrophilicity resulted in different ion selectivity as well. Overall, these results may provide for future metallopolymer design for targeted ion capture in aqueous systems.
Graduation Semester
2023-08
Type of Resource
Thesis
Copyright and License Information
Copyright 2023 Raylin Chen

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