Designing Redox-Active Oligomers for Crossover-Free, Nonaqueous Redox-Flow Batteries with High Volumetric Energy Density

Miranda J. Baran, Miles N. Braten, Elena C. Montoto, Zachary T. Gossage, Lin Ma, Etienne Chénard, Jeffrey S. Moore, Joaquín Rodríguez-López, Brett A. Helms

Research output: Contribution to journalArticle

Abstract

Here we show how to design organic redox-active solutions for use in redox-flow batteries, with an emphasis on attaining high volumetric capacity electrodes that minimize active-material crossover through the flow cell's membrane. Specifically, we advance oligoethylene oxides as versatile core motifs that grant access to liquid redox-active oligomers having infinite miscibility with organic electrolytes. The resulting solutions exhibit order-of-magnitude increases in volumetric capacity and obviate deleterious effects on redox stability. The design is broadly applicable, allowing both low potential and high potential redox centers to be appended to these core motifs, as demonstrated by benzofurazan, nitrobenzene, 2,2,6,6-tetramethylpiperidin-1-yl)oxyl, and 2,5-di-tert-butyl-1-methoxy-4-(2′-methoxy)benzene pendants, whose reduction potentials range from -1.87 to 0.76 V vs Ag/Ag+ in acetonitrile. Notably, the oligoethylene oxide scaffold minimizes membrane crossover relative to redox-active small molecules, while also providing mass- and electron-transfer kinetic advantages over other macromolecular architectures. These characteristics collectively point toward new opportunities in grid-scale energy storage using all-organic redox-flow batteries.

Original languageEnglish (US)
Pages (from-to)3861-3866
Number of pages6
JournalChemistry of Materials
Volume30
Issue number11
DOIs
StatePublished - Jun 12 2018

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ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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