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Selective ligand removal to improve accessibility of active sites in hierarchical MOFs for heterogeneous photocatalysis

Author

Listed:
  • Shaghayegh Naghdi

    (Technische Universität Wien)

  • Alexey Cherevan

    (Technische Universität Wien)

  • Ariane Giesriegl

    (Technische Universität Wien)

  • Rémy Guillet-Nicolas

    (Faculty of Chemistry, Universität Wien
    Laboratoire Catalyse et Spectrochimie)

  • Santu Biswas

    (Technion - Israel Institute of Technology)

  • Tushar Gupta

    (Technische Universität Wien)

  • Jia Wang

    (Technische Universität Wien)

  • Thomas Haunold

    (Technische Universität Wien)

  • Bernhard Christian Bayer

    (Technische Universität Wien)

  • Günther Rupprechter

    (Technische Universität Wien)

  • Maytal Caspary Toroker

    (Technion - Israel Institute of Technology
    Technion - Israel Institute of Technology)

  • Freddy Kleitz

    (Faculty of Chemistry, Universität Wien)

  • Dominik Eder

    (Technische Universität Wien)

Abstract

Metal-organic frameworks (MOFs) are commended as photocatalysts for H2 evolution and CO2 reduction as they combine light-harvesting and catalytic functions with excellent reactant adsorption capabilities. For dynamic processes in liquid phase, the accessibility of active sites becomes a critical parameter as reactant diffusion is limited by the inherently small micropores. Our strategy is to introduce additional mesopores by selectively removing one ligand in mixed-ligand MOFs via thermolysis. Here we report photoactive MOFs of the MIL-125-Ti family with two distinct mesopore architectures resembling either large cavities or branching fractures. The ligand removal is highly selective and follows a 2-step process tunable by temperature and time. The introduction of mesopores and the associated formation of new active sites have improved the HER rates of the MOFs by up to 500%. We envision that this strategy will allow the purposeful engineering of hierarchical MOFs and advance their applicability in environmental and energy technologies.

Suggested Citation

  • Shaghayegh Naghdi & Alexey Cherevan & Ariane Giesriegl & Rémy Guillet-Nicolas & Santu Biswas & Tushar Gupta & Jia Wang & Thomas Haunold & Bernhard Christian Bayer & Günther Rupprechter & Maytal Caspar, 2022. "Selective ligand removal to improve accessibility of active sites in hierarchical MOFs for heterogeneous photocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-021-27775-7
    DOI: 10.1038/s41467-021-27775-7
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    Cited by:

    1. Zheao Huang & Zhouzhou Wang & Hannah Rabl & Shaghayegh Naghdi & Qiancheng Zhou & Sabine Schwarz & Dogukan Hazar Apaydin & Ying Yu & Dominik Eder, 2024. "Ligand engineering enhances (photo) electrocatalytic activity and stability of zeolitic imidazolate frameworks via in-situ surface reconstruction," Nature Communications, Nature, vol. 15(1), pages 1-14, December.

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