Hydrocarbon Sorption in Flexible MOFs—Part II: Understanding Adsorption Kinetics

Author:

Preißler-Kurzhöfer Hannes12,Kolesnikov Andrei2,Lange Marcus2,Möllmer Jens2,Erhart Oliver3,Kobalz Merten3,Hwang Seungtaik4ORCID,Chmelik Christian4,Krautscheid Harald3ORCID,Gläser Roger1ORCID

Affiliation:

1. Institut für Technische Chemie, Fakultät für Chemie und Mineralogie, Universität Leipzig, Linnéstraße 3, D-04103 Leipzig, Germany

2. Institut für Nichtklassische Chemie e.V., Universität Leipzig, Permoserstraße 15, D-04318 Leipzig, Germany

3. Institut für Anorganische Chemie, Fakultät für Chemie und Mineralogie, Universität Leipzig, Johannisallee 21, D-04103 Leipzig, Germany

4. Fakultät für Physik und Geowissenschaften, Universität Leipzig, Linnéstraße 5, D-04103 Leipzig, Germany

Abstract

The rate of sorption of n-butane on the structurally flexible metal-organic framework [Cu2(H-Me-trz-ia)2], including its complete structural transition between a narrow-pore phase and a large-pore phase, was studied by sorption gravimetry, IR spectroscopy, and powder X-ray diffraction at close to ambient temperature (283, 298, and 313 K). The uptake curves reveal complex interactions of adsorption on the outer surface of MOF particles, structural transition, of which the overall rate depends on several factors, including pressure step, temperature, as well as particle size, and the subsequent diffusion into newly opened pores. With the aid of a kinetic model based on the linear driving force (LDF) approach, both rates of diffusion and structural transition were studied independently of each other. It is shown that temperature and applied pressure steps have a strong effect on the rate of structural transition and thus, the overall velocity of gas uptake. For pressure steps close to the upper boundary of the gate-opening, the rate of structural transition is drastically reduced. This feature enables a fine-tuning of the overall velocity of sorption, which can even turn into anti-Arrhenius behavior.

Funder

Deutsche Forschungsgemeinschaft

Publisher

MDPI AG

Subject

General Materials Science,General Chemical Engineering

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