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Автор(ы) : Abylgazina L., Senkovska I., Ehrling S., Bon V., St. Petkov P., Evans J. D., Krylova S. N., Krylov A. S., Kaskel S.
Заглавие : Tailoring adsorption induced switchability of a pillared layer MOF by crystal size engineering
Место публикации : CrystEngComm. - 2021. - Vol. 23, Is. 3. - P.538-549. - ISSN 14668033 (ISSN), DOI 10.1039/d0ce01497d
Примечания : Cited References: 71. - The authors thank the DFG (FOR 2433 MOF Switches, Project No. 279409724) for financial support. P.P. and J. D. E. thank Center for Information Services and High Performance Computing (ZIH) at TU Dresden for providing high-performance computing facilities. Authors acknowledge Helmholtz-Zentrum Berlin für Materialien und Energie for allocated beamtime at KMC-2 and MX14.2 beamlines. J. D. E. acknowledges the support of the Alexander von Humboldt foundation and HPC platforms provided by a GENCI grant (A0070807069)
Аннотация: The pillared layer framework DUT-8(Zn) (Zn2(2,6-ndc)2(dabco), 2,6-ndc = 2,6-naphthalenedicarboxylate, dabco = 1,4-diazabicyclo-[2.2.2]-octane, DUT = Dresden University of Technology) is a prototypical switchable MOF, showing characteristic adsorption and desorption induced open phase (op) to closed phase (cp) transformation associated with huge changes in cell volume. We demonstrate switchability strongly depends on a framework-specific critical particle size (dcrit). Superposed, the solvent removal process (pore desolvation stress contracting the framework) significantly controls the cp/op ratio after desolvation and, subsequently, the adsorption induced switchability characteristics of the system. After desolvation, the dense cp phase of DUT-8(Zn) shows no adsorption-induced reopening and therefore is non-porous for N2 at 77 K and CO2 at 195 K. However, polar molecules with a higher adsorption enthalpy, such as chloromethane at 249 K and dichloromethane (DCM) at 298 K can reopen the macro-sized crystals upon adsorption. For macro-sized particles, the outer surface energy is negligible and only the type of metal (Zn, Co, Ni) controls the DCM-induced gate opening pressure. The node hinge stiffness increases from Zn to Ni as confirmed by DFT calculations, X-ray crystal structural analysis, and low frequency Raman spectroscopy. This softer Zn-based node hinges and overall increased stabilization of cp vs. op phase shift the critical particle size at which switchability starts to become suppressed to even lower values (dcrit ‹ 200 nm) as compared to the Ni-based system (dcrit ≈ 500 nm). Hence, the three factors affecting switchability (energetics of the empty host, (Eop–Ecp) (I), particle size (II), and desolvation stress (III)) appear to be of the same order of magnitude and should be considered collectively, not individually.
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