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Structure sensitivity in gas sorption and conversion on metal-organic frameworks

Author

Listed:
  • Guusje Delen

    (Utrecht University)

  • Matteo Monai

    (Utrecht University)

  • Katarina Stančiaková

    (Utrecht University)

  • Bettina Baumgartner

    (Utrecht University)

  • Florian Meirer

    (Utrecht University)

  • Bert M. Weckhuysen

    (Utrecht University)

Abstract

Many catalytic processes depend on the sorption and conversion of gaseous molecules on the surface of (porous) functional materials. These events often preferentially occur on specific, undercoordinated, external surface sites. Here we show the combination of in situ Photo-induced Force Microscopy (PiFM) with Density Functional Theory (DFT) calculations to study the site-specific sorption and conversion of formaldehyde on the external surfaces of well-defined faceted ZIF-8 microcrystals with nanoscale resolution. We observed preferential adsorption of formaldehyde on high index planes. Moreover, in situ PiFM allowed us to visualize unsaturated nanodomains within extended external crystal planes, showing enhanced sorption behavior on the nanoscale. Additionally, on defective ZIF-8 crystals, structure sensitive conversion of formaldehyde through a methoxy- and a formate mechanism mediated by Lewis acidity was found. Strikingly, sorption and conversion were influenced more by the external surface termination than by the concentration of defects. DFT calculations showed that this is due to the presence of specific atomic arrangements on high-index crystal surfaces. With this research, we showcase the high potential of in situ PiFM for structure sensitivity studies on porous functional materials.

Suggested Citation

  • Guusje Delen & Matteo Monai & Katarina Stančiaková & Bettina Baumgartner & Florian Meirer & Bert M. Weckhuysen, 2023. "Structure sensitivity in gas sorption and conversion on metal-organic frameworks," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-022-35762-9
    DOI: 10.1038/s41467-022-35762-9
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    References listed on IDEAS

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