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Isolation of pseudocapacitive surface processes at monolayer MXene flakes reveals delocalized charging mechanism

Author

Listed:
  • Marc Brunet Cabré

    (Trinity College Dublin)

  • Dahnan Spurling

    (Trinity College Dublin)

  • Pietro Martinuz

    (Trinity College Dublin
    Università degli Studi di Milano, Dipartimento di Chimica)

  • Mariangela Longhi

    (Università degli Studi di Milano, Dipartimento di Chimica)

  • Christian Schröder

    (Trinity College Dublin)

  • Hugo Nolan

    (Trinity College Dublin)

  • Valeria Nicolosi

    (Trinity College Dublin)

  • Paula E. Colavita

    (Trinity College Dublin)

  • Kim McKelvey

    (Trinity College Dublin
    Victoria University of Wellington)

Abstract

Pseudocapacitive charge storage in Ti3C2Tx MXenes in acid electrolytes is typically described as involving proton intercalation/deintercalation accompanied by redox switching of the Ti centres and protonation/deprotonation of oxygen functional groups. Here we conduct nanoscale electrochemical measurements in a unique experimental configuration, restricting the electrochemical contact area to a small subregion (0.3 µm2) of a monolayer Ti3C2Tx flake. In this unique configuration, proton intercalation into interlayer spaces is not possible, and surface processes are isolated from the bulk processes, characteristic of macroscale electrodes. Analysis of the pseudocapacitive response of differently sized MXene flakes indicates that entire MXene flakes are charged through electrochemical contact of only a small basal plane subregion, corresponding to as little as 3% of the flake surface area. Our observation of pseudocapacitive charging outside the electrochemical contact area is suggestive of a fast transport of protons mechanism across the MXene surface.

Suggested Citation

  • Marc Brunet Cabré & Dahnan Spurling & Pietro Martinuz & Mariangela Longhi & Christian Schröder & Hugo Nolan & Valeria Nicolosi & Paula E. Colavita & Kim McKelvey, 2023. "Isolation of pseudocapacitive surface processes at monolayer MXene flakes reveals delocalized charging mechanism," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-35950-1
    DOI: 10.1038/s41467-023-35950-1
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    References listed on IDEAS

    as
    1. Hengxing Ji & Xin Zhao & Zhenhua Qiao & Jeil Jung & Yanwu Zhu & Yalin Lu & Li Li Zhang & Allan H. MacDonald & Rodney S. Ruoff, 2014. "Capacitance of carbon-based electrical double-layer capacitors," Nature Communications, Nature, vol. 5(1), pages 1-7, May.
    2. Maria R. Lukatskaya & Sankalp Kota & Zifeng Lin & Meng-Qiang Zhao & Netanel Shpigel & Mikhael D. Levi & Joseph Halim & Pierre-Louis Taberna & Michel W. Barsoum & Patrice Simon & Yury Gogotsi, 2017. "Ultra-high-rate pseudocapacitive energy storage in two-dimensional transition metal carbides," Nature Energy, Nature, vol. 2(8), pages 1-6, August.
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