Characterizing the Impact of Oligomerization on Redox Flow Cell Performance

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...

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Main Authors: Weiss, Trent A, Fan, Gang, Neyhouse, Bertrand J, Moore, Evan B, Furst, Ariel, Brushett, Fikile R
Other Authors: Massachusetts Institute of Technology. Department of Chemical Engineering
Format: Article
Language:English
Published: Wiley 2024
Online Access:https://hdl.handle.net/1721.1/157757
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author Weiss, Trent A
Fan, Gang
Neyhouse, Bertrand J
Moore, Evan B
Furst, Ariel
Brushett, Fikile R
author2 Massachusetts Institute of Technology. Department of Chemical Engineering
author_facet Massachusetts Institute of Technology. Department of Chemical Engineering
Weiss, Trent A
Fan, Gang
Neyhouse, Bertrand J
Moore, Evan B
Furst, Ariel
Brushett, Fikile R
author_sort Weiss, Trent A
collection MIT
description 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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spelling mit-1721.1/1577572024-12-23T05:30:24Z 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 Massachusetts Institute of Technology. Department of Chemical Engineering 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. 2024-12-05T18:11:58Z 2024-12-05T18:11:58Z 2023-08 2024-12-05T17:39:32Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/157757 T. A. Weiss, G. Fan, B. J. Neyhouse, E. B. Moore, A. Furst, F. R. Brushett, Batteries & Supercaps 2023, 6, e202300034. en 10.1002/batt.202300034 Batteries & Supercaps Creative Commons Attribution https://creativecommons.org/licenses/by/4.0/ application/pdf Wiley Wiley
spellingShingle Weiss, Trent A
Fan, Gang
Neyhouse, Bertrand J
Moore, Evan B
Furst, Ariel
Brushett, Fikile R
Characterizing the Impact of Oligomerization on Redox Flow Cell Performance
title Characterizing the Impact of Oligomerization on Redox Flow Cell Performance
title_full Characterizing the Impact of Oligomerization on Redox Flow Cell Performance
title_fullStr Characterizing the Impact of Oligomerization on Redox Flow Cell Performance
title_full_unstemmed Characterizing the Impact of Oligomerization on Redox Flow Cell Performance
title_short Characterizing the Impact of Oligomerization on Redox Flow Cell Performance
title_sort characterizing the impact of oligomerization on redox flow cell performance
url https://hdl.handle.net/1721.1/157757
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