Multiscale development of electrochemical separations: from molecular design of redox-moieties to interfacial characterization and process simulation
Candeago, Riccardo
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https://hdl.handle.net/2142/132731
Description
Title
Multiscale development of electrochemical separations: from molecular design of redox-moieties to interfacial characterization and process simulation
Author(s)
Candeago, Riccardo
Issue Date
2025-08-21
Director of Research (if dissertation) or Advisor (if thesis)
Su, Xiao
Doctoral Committee Chair(s)
Su, Xiao
Committee Member(s)
Diao, Ying
Mironenko, Alexander
Murphy, Catherine J
Browning, James F
Department of Study
Chemical & Biomolecular Engr
Discipline
Chemical Engineering
Degree Granting Institution
University of Illinois Urbana-Champaign
Degree Name
Ph.D.
Degree Level
Dissertation
Keyword(s)
separations
electrochemistry
redox-active polymers
neutron reflectometry
solvation effects
volatile fatty acids
finite-elements
physics-based modeling
water purification
remediation
selectivity
Language
eng
Abstract
Pressing separations challenges, such as the recovery of critical materials from low-grade sources, the environmental remediation of trace pollutants from water, and the improvement of downstream separations in chemical manufacturing, highlight the need for novel approaches with lower energy consumption, higher selectivity, and reduced chemical inputs. Electrochemistry can meet these stringent requirements with the added benefit of being suitable for both small- and large-scale applications, thanks to the modular nature of electrochemical devices. Still, lots of the design and optimization space of electrochemical separations systems remains uncharted.
In this thesis, we investigate multiple electrochemical separations (i.e., electrosorption, electrodialysis, electrodeposition, bulk electrolysis of redox-sorbents) with a multiscale approach, spanning from the molecular design and in situ characterization of redox-sorbents up to large-scale process simulation and design of multistage redox-mediated electrodialysis. Our case studies involve the separation of species featuring very similar physical and chemical behavior, or species present in very dilute concentrations, i.e. cases where state-of-the-art separation techniques are highly chemical and energy intensive. For example, we considered critical metals (separation of rhenium from molybdenum), commodity chemicals (alkenes from alkanes), fermentation products (volatile fatty acids fractionation), and environmental pollutants (removal of mercury from water).
Our in situ studies offer guidelines on how to choose and rationally design more selective redox-sorbents, while our process modeling and simulation approach provides a framework to translate bench-scale redox-mediated electrodialysis to pilot-plant operation.
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