Abstract
We report a microscopic model of the phonon-adsorption correlations in flexible metal-organic framework materials. We analyze the mechanism of the gate opening deformation using the notion of coupled phonon- and adsorption-induced structural transformation. Using the ZIF-8 structure as an example, we perform an analysis of transformation-related, low-frequency phonon modes of the framework. On the basis of structure-related quantities such as pore limiting diameter, void fraction, and adsorption uptake, we determine the conditions which lead to the gate opening transformation in ZIF-8. Energetic landscape of the deformation process is analyzed using grand thermodynamic potential of adsorption. We generalize our conclusions to other flexible ZIF structures with the same topology.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 7999-8005 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry C |
| Volume | 125 |
| Issue number | 14 |
| DOIs | |
| State | Published - Apr 15 2021 |
Funding
F.F. was supported by the Polish National Science Centre (NCN, Grant ETIUDA No. 2018/28/T/ST4/00234). This research was supported in part by PL-Grid Infrastructure (DFT calculations). Calculations have been carried out using resources provided by Wroclaw Centre for Networking and Supercomputing, Grant 033 (GCMC calculations). M.F. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation), Project Number 389577027 (FI 1800/5-1). Internship of FF at University of Bremen was funded by the MAPEX Center for Materials and Processes, University of Bremen, through a Ph.D. Research Grant.
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- General Energy
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films