Multiscale development of electrochemical separations: from molecular design of redox-moieties to interfacial characterization and process simulation

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.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemical Engineering

Grantor

University of Illinois Urbana-Champaign

Year dc:date

2025

Author dc:creator

• Candeago, Riccardo

Contributors dc:contributor

• Su, Xiao
• Diao, Ying
• Mironenko, Alexander
• Murphy, Catherine J
• Browning, James F

• separations
• electrochemistry
• redox-active polymers
• neutron reflectometry
• solvation effects
• volatile fatty acids
• finite-elements
• physics-based modeling
• water purification
• remediation
• selectivity

Statement dc:rights

• Copyright 2025 Riccardo Candeago

Language dc:language

en

Handle dc:identifier

https://hdl.handle.net/2142/132731

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/132731