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Guillermo Colon Quintana dissertation (FINAL).pdf (18.41 MB)

ELECTROCHEMICALLY DRIVEN PHASE FORMATION IN MULTIPHASE SYSTEMS

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posted on 2024-06-20, 01:15 authored by Guillermo Sebastian Colon QuintanaGuillermo Sebastian Colon Quintana

Nature has been shown to build environments to drive specific reactivity across boundaries; multiphase systems, for example, have been shown to drive reactions that would otherwise not occur in bulk, continuous phases. Within this work, we show how multiphase environments are essential in driving specific reactivity at phase boundaries and offer unique physicochemical and electrochemical opportunities that are usually inaccessible in continuous phases alone. Here, we present several diverse approaches toward harnessing observed interfacial phenomena to study and take advantage of three-phase systems. Firstly, we demonstrate precise manipulation of nucleation at the water|1,2-dichloroethane (DCE)|electrode interface through electrode geometry adjustment, resulting in selective precipitation of ferrocenemethanol (FcMeOH). Cyclic voltammetry and numerical simulations elucidate this phenomenon's physico-chemical foundations, enabling localized precipitation and reactivity control. Secondly, we introduce a novel mechanism for emulsion formation driven by interfacial solute flux induced via phase transfer agents. Systematically exploring phase combinations and ion interactions, we elucidate the microscopic mechanisms governing droplet formation and propose design principles for tailored emulsion synthesis. Furthermore, leveraging current-driven ion flux, we achieve emulsification across oil|water interfaces, offering control over droplet size and charge. This low-energy, robust method presents an efficient alternative to traditional emulsification techniques. Additionally, we demonstrate facile electrodeposition of gold nanorings at water|oil interfaces, enabled by spontaneous emulsification facilitated by quaternary ammonium salts. We further demonstrate deposition parameters for control over nanoring array characteristics, offering a streamlined approach to nanoring fabrication. Finally, we introduce biphasic electrodeposition as a versatile method for fabricating ultra-high aspect ratio gold nanowires. By manipulating antagonistic metal salt interactions at liquid|liquid interfaces, we achieve precise control over nanowire geometry and positioning, opening new avenues for nanowire synthesis with enhanced simplicity and versatility.

Funding

R35-GM138133-01

CAREER: Electro-Shock Synthesis of High Entropy Alloy Nanoparticles from Sub-Femtoliter Reactors

Directorate for Mathematical & Physical Sciences

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History

Degree Type

  • Doctor of Philosophy

Department

  • Chemistry

Campus location

  • West Lafayette

Advisor/Supervisor/Committee Chair

Dr. Jeffrey E. Dick

Additional Committee Member 2

Dr. Julia Laskin

Additional Committee Member 3

Dr. Cristophe Renault

Additional Committee Member 4

Dr. Chi Zhang