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Hydrocarbon Sorption in Flexible MOFs-Part II: Understanding Adsorption Kinetics.

Hannes Preißler-Kurzhöfer1,2, Andrei Kolesnikov2, Marcus Lange2

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The sorption rate of n-butane in a flexible metal-organic framework ([Cu2(H-Me-trz-ia)2]) depends on structural transitions. Fine-tuning pressure steps allows control over gas uptake velocity, even showing anti-Arrhenius behavior.

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flexible materialskinetic analysismetal–organic frameworks

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Area of Science:

  • Materials Science
  • Chemical Engineering
  • Physical Chemistry

Background:

  • Structurally flexible metal-organic frameworks (MOFs) exhibit dynamic responses to guest molecules.
  • Understanding gas sorption kinetics in MOFs is crucial for applications like gas storage and separation.

Purpose of the Study:

  • To investigate the sorption kinetics of n-butane in the flexible MOF [Cu2(H-Me-trz-ia)2].
  • To elucidate the interplay between gas adsorption, structural transitions, and diffusion within the MOF.
  • To develop a kinetic model for independent analysis of diffusion and structural transition rates.

Main Methods:

  • Sorption gravimetry to measure gas uptake.
  • Infrared (IR) spectroscopy and powder X-ray diffraction (PXRD) to monitor structural changes.
  • Kinetic modeling using the linear driving force (LDF) approach.

Main Results:

  • Sorption kinetics are influenced by external surface adsorption, structural transition, and pore diffusion.
  • Temperature and pressure steps significantly impact the rate of structural transition and overall gas uptake.
  • Reduced structural transition rates at specific pressure steps allow for fine-tuning of sorption velocity.
  • Observed anti-Arrhenius behavior in sorption kinetics under certain conditions.

Conclusions:

  • The study provides a detailed understanding of n-butane sorption dynamics in a flexible MOF.
  • The rate of structural transition is a key factor controlling overall gas uptake velocity.
  • The findings offer a pathway for controlling and optimizing gas sorption processes in flexible MOFs.