Elucidating Instabilities Contributing to Capacity Fade in Bipyridine‐Based Materials for Non‐aqueous Flow Batteries

Journal Article · 18 January 2022 · ChemElectroChem

DOI: https://doi.org/10.1002/celc.202101490 · OSTI ID:1854642

Kolesnichenko, Claudina X. ^[1]; Pratt, III, Harry D. ^[1]; Small, Leo J. ^[1]; Anderson, Travis M.  ^[1]

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1. Sandia National Laboratories Albuquerque New Mexico 87185-00613 USA

Abstract Metal‐based non‐aqueous redox flow batteries have the potential for long‐term energy storage if stability requirements can be achieved. One such stability issue in metal coordination complexes arises from ligand shedding in the anolyte upon reduction. Recognizing that the free ligands are relatively more stable than the metal coordination complex under highly reducing conditions, we evaluated a family of metal‐free bipyridinium materials as flow battery anolytes with the corresponding iron coordination complex as the catholyte. Bipyridinium compounds were functionalized for increased electrochemical stability, cycled in flow cells to understand efficiencies, and analyzed for degradation products. Methylation of the bipyridine nitrogens increased electrochemical stability yet left the reduced molecule susceptible to radical‐induced bond cleavage. Subsequent functionalization of bipyridine with carbomethoxy groups resulted in good battery performance with 96 % Coulombic and 90 % voltage efficiency, and improved cycling stability over a methoxy‐substituted anolyte with 14 % vs 36 % capacity fade in the first charge‐discharge cycle.

• Sponsoring Organization: USDOE
• OSTI ID: 1854642
• Journal Information: ChemElectroChem, Journal Name: ChemElectroChem Journal Issue: 6 Vol. 9; ISSN 2196-0216
• Publisher: Wiley Blackwell (John Wiley & Sons)Copyright Statement
• Country of Publication: Germany
• Language: English