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Selective Anion Anchoring in MOF-Based Supercapacitors Revealed with Operando Small-Angle X-Ray Scattering

Author

Listed:
  • Malina Seyffertitz

    (Montanuniversität Leoben)

  • Chloe J. Balhatchet

    (University of Cambridge)

  • Max V. Rauscher

    (Montanuniversität Leoben)

  • Sebastian Stock

    (Montanuniversität Leoben)

  • Gerhard Fritz-Popovski

    (Montanuniversität Leoben)

  • Thomas Leiner

    (Montanuniversität Leoben)

  • David Holec

    (Montanuniversität Leoben)

  • Heinz Amenitsch

    (Graz University of Technology)

  • Alexander C. Forse

    (University of Cambridge)

  • Oskar Paris

    (Montanuniversität Leoben)

Abstract

Understanding how ions interact with electrodes in electric double-layer capacitors (EDLCs) is key to advancing energy storage, yet many fundamental aspects remain unclear. Here, we employ operando small-angle X-ray scattering (SAXS) to investigate charge storage in metal-organic framework (MOF)-based supercapacitor electrodes as a model system. Using Ni3(2,3,6,7,10,11-hexaiminotriphenylene)2 (Ni3(HITP)2) MOF electrodes and 1 M aqueous sodium bis(trifluoromethanesulfonyl)imide (NaTFSI) as the electrolyte, we show that TFSI- anions are immobilised near MOF pore walls via fluorine-hydrogen interactions with N-H functional groups of the MOF. We quantify the concentration of pinned anions and demonstrate that their immobilization persists across different applied cell voltages, resulting in a cation-dominated charge storage mechanism governed solely by Na+ adsorption and desorption. Charge balancing is unaffected by whether voltage is applied stepwise or gradually, with no dynamic differences between in-pore and out-of-pore environments and no ion intercalation taking place.

Suggested Citation

  • Malina Seyffertitz & Chloe J. Balhatchet & Max V. Rauscher & Sebastian Stock & Gerhard Fritz-Popovski & Thomas Leiner & David Holec & Heinz Amenitsch & Alexander C. Forse & Oskar Paris, 2025. "Selective Anion Anchoring in MOF-Based Supercapacitors Revealed with Operando Small-Angle X-Ray Scattering," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-63772-w
    DOI: 10.1038/s41467-025-63772-w
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