Characterizing the Impact of Oligomerization on Redox Flow Cell Performance

Weiss, Trent A.; Fan, Gang; Neyhouse, Bertrand J.; Moore, Evan B.; Furst, Ariel; Brushett, Fikile R.

doi:10.1002/batt.202300034

Title: Characterizing the Impact of Oligomerization on Redox Flow Cell Performance

Journal Article · 19 July 2023 · Batteries & Supercaps

DOI: https://doi.org/10.1002/batt.202300034 · OSTI ID:1991634

^[1]; Fan, Gang ^[1];

^[2]; Moore, Evan B. ^[1];

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Department of Chemical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
Department of Chemical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA, Joint Center for Energy Storage Research Massachusetts Institute of Technology Cambridge MA 02139 USA

Abstract Redox flow batteries (RFBs) are hindered by complex failure modes, particularly crossover through the membrane, resulting in capacity fade and reduced cycling efficiencies. Redox‐active oligomers (RAOs) have recently been proposed for mitigating this phenomenon while maintaining sufficient transport properties; however, to date, few studies have quantified how the chemical and electrochemical properties of RAOs influence their performance in redox flow cells. Here, we demonstrate that oligomeric derivatives of 2,2,6,6‐tetramethylpiperidine 1‐oxyl (TEMPO) exhibit lower diffusivities than the monomeric species but retain facile charge transfer characteristics. The size‐dependent variations in mass transport rates directly translate to differences in flow cell polarization and symmetric cycling performance. Post‐mortem analyses reveal that oligomerization does not meaningfully alter decay processes as evinced by similar capacity fade across all species. Broadly, these findings corroborate and extend upon previously developed relationships between molecular size, electrochemical properties, and flow cell performance.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1991634

Journal Information:: Batteries & Supercaps, Journal Name: Batteries & Supercaps Journal Issue: 8 Vol. 6; ISSN 2566-6223

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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36 MATERIALS SCIENCE
Cyclic voltammetry
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Oligomerization
Redox flow battery
TEMPO

Title: Characterizing the Impact of Oligomerization on Redox Flow Cell Performance

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