Electrochemical systems are increasingly being developed and deployed as sustainable technologies that support reductions in greenhouse gas emissions across the electric power, transportation, and industrial sectors. However, the need to overcome challenges related to cost, performance, and scalability continues to motivate exploration into alternative material sets and reactor designs that offer new pathways to widespread adoption. Redox-mediated processes, which decouple electrode reactions that activate a soluble mediator from “off-electrode” reactions where the activated mediator exchanges electrons with a solid material, are of growing interest.1,2 Recent literature has illustrated the potential of this approach for increasing the charge-storage capacity of redox flow batteries,2 performing impractical electrochemical processes,3 enhancing selectivity and efficiency of electrochemical separations and recycling,1,4,5 and unlocking spatial and temporal flexibility in electrochemical operations.6 Previously, we have developed and qualitatively validated a model capable of capturing key dynamics observed in redox-mediated flow batteries.7 Grounded in first principles and contextualized by experiments, this model has the potential to rapidly assess tradeoffs and opportunities for redox-mediated systems for applications in energy storage and conversion as well as materials recovery and recycling.Here, we describe how our model can be used to gain generalizable insights into the design-space for redox-mediated electrochemical processes. By incorporating models for pressure drop in porous media with simulated electrochemical performance, we assess the trade-offs associated with capacity utilization, power output, and parasitic pumping losses. Furthermore, we demonstrate how the model can support constrained optimization to guide the design of a system of known physical parameters. Ultimately, we seek to translate these findings into universal design principles for how electrochemical protocol and solid incorporation can be tuned to develop high-performing redox-mediated systems. Acknowledgements N.J.M gratefully acknowledges the NSF Graduate Research Fellowship Program under Grant Number 2141064. Any opinion, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the NSF. References Xue et al., Green Chem. 2020, 22 (19): 6288-6309.Yan and Wang, Mat. 2018, 30 (47).Vardner et al., ChemElectroChem 2022, 9 (24).Cotty et al., ACS Sustain Chem Eng. 2023, 11(9):3975-3986.Park et al., ACS Sustain Chem Eng. 2021, 9 (24): 8214-8221.Wang et al, Joule 2021, 5 (1): 149-165.Matteucci et al., ECS Meeting s 2023, MA2023-01 (3), 765.
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