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Synthesis and Characterization of Lithium-Conducting Composite Polymer–Ceramic Membranes for Use in Nonaqueous Redox Flow Batteries

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Mater. Interfaces 2021, 13, 45, 53746-53757
    Energy, Environmental, and Catalysis Applications

    Synthesis and Characterization of Lithium-Conducting Composite Polymer–Ceramic Membranes for Use in Nonaqueous Redox Flow Batteries
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 45, 53746–53757
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    https://doi.org/10.1021/acsami.1c13759
    Published November 4, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Redox flow batteries (RFBs) are a burgeoning electrochemical platform for long-duration energy storage, but present embodiments are too expensive for broad adoption. Nonaqueous redox flow batteries (NAqRFBs) seek to reduce system costs by leveraging the large electrochemical stability window of organic solvents (>3 V) to operate at high cell voltages and to facilitate the use of redox couples that are incompatible with aqueous electrolytes. However, a key challenge for emerging nonaqueous chemistries is the lack of membranes/separators with suitable combinations of selectivity, conductivity, and stability. Single-ion conducting ceramics, integrated into a flexible polymer matrix, may offer a pathway to attain performance attributes needed for enabling competitive nonaqueous systems. Here, we explore composite polymer-inorganic binder-filler membranes for lithium-based NAqRFBs, investigating two different ceramic compounds with NASICON-type (NASICON: sodium (Na) superionic conductor) crystal structure, Li1.3Al0.3Ti1.7(PO4)3 (LATP) and Li1.4Al0.4Ge0.2Ti1.4(PO4)3 (LAGTP), each blended with a polyvinylidene fluoride (PVDF) polymeric matrix. We characterize the physicochemical and electrochemical properties of the synthesized membranes as a function of processing conditions and formulation using a range of microscopic and electrochemical techniques. Importantly, the electrochemical stability window of the as-prepared membranes lies between 2.2–4.5 V vs Li/Li+. We then integrate select composite membranes into a single electrolyte flow cell configuration and perform polarization measurements with different redox electrolyte compositions. We find that mechanically robust, chemically stable LATP/PVDF composites can support >40 mA cm–2 at 400 mV cell overpotential, but further improvements are needed in selectivity. Overall, the insights gained through this work begin to establish the foundational knowledge needed to advance composite polymer-inorganic membranes/separators for NAqRFBs.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c13759.

    • Additional information on casting substrate cleaning, electronic conductivity tests, electrochemical stability window assessment, crossover experiments, post mortem SEM images, and ohmic resistance data (PDF)

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    Cited By

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    This article is cited by 2 publications.

    1. Carlos M. Costa, Vanessa F. Cardoso, Pedro Martins, Daniela M. Correia, Renato Gonçalves, Pedro Costa, Vitor Correia, Clarisse Ribeiro, Margarida M. Fernandes, Pedro M. Martins, Senentxu Lanceros-Méndez. Smart and Multifunctional Materials Based on Electroactive Poly(vinylidene fluoride): Recent Advances and Opportunities in Sensors, Actuators, Energy, Environmental, and Biomedical Applications. Chemical Reviews 2023, 123 (19) , 11392-11487. https://doi.org/10.1021/acs.chemrev.3c00196
    2. Zainab Waris, Nikita O. Akhmetov, Mariam A. Pogosova, Svetlana A. Lipovskikh, Sergey V. Ryazantsev, Keith J. Stevenson. A Complex Investigation of LATP Ceramic Stability and LATP+PVDF Composite Membrane Performance: The Effect of Solvent in Tape-Casting Fabrication. Membranes 2023, 13 (2) , 155. https://doi.org/10.3390/membranes13020155
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 45, 53746–53757
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.1c13759
    Published November 4, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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