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2020-04-20-Disorder_Switchability__kaskel.pdf (3.5 MB)
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Adaptive Response of a Metal–organic Framework Through Reversible Disorder–disorder Transitions

preprint
submitted on 19.05.2020 and posted on 19.05.2020 by Sebastian Ehrling, Emily M. Reynolds, Volodymyr Bon, Irena Senkovska, Tatiana E. Gorelik, Marcus Rauche, Matthias Mendt, Manfred S. Weiss, A. Poeppl, Eike Brunner, Ute Kaiser, Andrew Goodwin, Stefan Kaskel
A highly porous metal-organic framework (DUT-8(Ni), DUT = Dresden University of Technology) is found to adopt a configurationally-degenerate family of disordered states that respond adaptively to specific guest stimuli. This disorder originates from non-linear carboxylate linkers arranging paddlewheels in closed loops of different local symmetries that in turn propagate as tilings of characteristic complex superstructures. Solvent exchange stimulates the formation of distinct disordered superstructures for specific guest molecules. Electron diffraction by desolvated DUT-8(Ni) nanoparticles demonstrates these superstructures to persist on the nanodomain level. Remarkably, guest exchange stimulates reversible and repeatable switching transitions between distinct disorder states. Deuterium NMR spectroscopy and in situ PXRD studies identify the transformation mechanism as an adaptive singular transformation event.

Funding

DFG (FOR2433)

ERC (788144)

DFG (CRC 1279)

History

Email Address of Submitting Author

stefan.kaskel@tu-dresden.de

Institution

TU Dresden

Country

Germany

ORCID For Submitting Author

0000-0003-4572-0303

Declaration of Conflict of Interest

No conflict

Version Notes

Version 2020-April-20

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