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On the role of history-dependent adsorbate distribution and metastable states in switchable mesoporous metal-organic frameworks

Author

Listed:
  • Francesco Walenszus

    (Technische Universität Dresden)

  • Volodymyr Bon

    (Technische Universität Dresden)

  • Jack D. Evans

    (The University of Adelaide)

  • Simon Krause

    (Max Planck Institute for Solid State Research)

  • Jürgen Getzschmann

    (Technische Universität Dresden)

  • Stefan Kaskel

    (Technische Universität Dresden
    Fraunhofer Institute IWS)

  • Muslim Dvoyashkin

    (Universität Leipzig)

Abstract

A unique feature of metal-organic frameworks (MOFs) in contrast to rigid nanoporous materials is their structural switchabilty offering a wide range of functionality for sustainable energy storage, separation and sensing applications. This has initiated a series of experimental and theoretical studies predominantly aiming at understanding the thermodynamic conditions to transform and release gas, but the nature of sorption-induced switching transitions remains poorly understood. Here we report experimental evidence for fluid metastability and history-dependent states during sorption triggering the structural change of the framework and leading to the counterintuitive phenomenon of negative gas adsorption (NGA) in flexible MOFs. Preparation of two isoreticular MOFs differing by structural flexibility and performing direct in situ diffusion studies aided by in situ X-ray diffraction, scanning electron microscopy and computational modelling, allowed assessment of n-butane molecular dynamics, phase state, and the framework response to obtain a microscopic picture for each step of the sorption process.

Suggested Citation

  • Francesco Walenszus & Volodymyr Bon & Jack D. Evans & Simon Krause & Jürgen Getzschmann & Stefan Kaskel & Muslim Dvoyashkin, 2023. "On the role of history-dependent adsorbate distribution and metastable states in switchable mesoporous metal-organic frameworks," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38737-6
    DOI: 10.1038/s41467-023-38737-6
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    References listed on IDEAS

    as
    1. Jack D. Evans & Volodymyr Bon & Irena Senkovska & Hui-Chun Lee & Stefan Kaskel, 2020. "Four-dimensional metal-organic frameworks," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    2. Simon Krause & Volodymyr Bon & Irena Senkovska & Ulrich Stoeck & Dirk Wallacher & Daniel M. Többens & Stefan Zander & Renjith S. Pillai & Guillaume Maurin & François-Xavier Coudert & Stefan Kaskel, 2016. "A pressure-amplifying framework material with negative gas adsorption transitions," Nature, Nature, vol. 532(7599), pages 348-352, April.
    3. Rustem Valiullin & Sergej Naumov & Petrik Galvosas & Jörg Kärger & Hyung-June Woo & Fabien Porcheron & Peter A. Monson, 2006. "Exploration of molecular dynamics during transient sorption of fluids in mesoporous materials," Nature, Nature, vol. 443(7114), pages 965-968, October.
    4. Simon Krause & Jack D. Evans & Volodymyr Bon & Irena Senkovska & Paul Iacomi & Felicitas Kolbe & Sebastian Ehrling & Erik Troschke & Jürgen Getzschmann & Daniel M. Többens & Alexandra Franz & Dirk Wal, 2019. "Towards general network architecture design criteria for negative gas adsorption transitions in ultraporous frameworks," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
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