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@ARTICLE{Krause:878318,
author = {Krause, Simon and Bon, Volodymyr and Du, Hongchu and
Dunin-Borkowski, Rafal E and Stoeck, Ulrich and Senkovska,
Irena and Kaskel, Stefan},
title = {{T}he impact of crystal size and temperature on the
adsorption-induced flexibility of the {Z}r-based
metal–organic framework {DUT}-98},
journal = {Beilstein journal of nanotechnology},
volume = {10},
issn = {2190-4286},
address = {Frankfurt, M.},
publisher = {Beilstein-Institut zur Förderung der Chemischen
Wissenschaften},
reportid = {FZJ-2020-02774},
pages = {1737 - 1744},
year = {2019},
abstract = {In this contribution we analyze the influence of adsorption
cycling, crystal size, and temperature on the switching
behavior of the flexible Zr-based metal–organic framework
DUT-98. We observe a shift in the gate-opening pressure upon
cycling of adsorption experiments for micrometer-sized
crystals and assign this to a fragmentation of the crystals.
In a series of samples, the average crystal size of DUT-98
crystals was varied from 120 µm to 50 nm and the obtained
solids were characterized by X-ray diffraction, infrared
spectroscopy, as well as scanning and transmission electron
microscopy. We analyzed the adsorption behavior by nitrogen
and water adsorption at 77 K and 298 K, respectively, and
show that adsorption-induced flexibility is only observed
for micrometer-sized crystals. Nanometer-sized crystals were
found to exhibit reversible type I adsorption behavior upon
adsorption of nitrogen and exhibit a crystal-size-dependent
steep water uptake of up to 20 mmol g−1 at 0.5 p/p0 with
potential for water harvesting and heat pump applications.
We furthermore investigate the temperature-induced
structural transition by in situ powder X-ray diffraction.
At temperatures beyond 110 °C, the open-pore state of the
nanometer-sized DUT-98 crystals is found to irreversibly
transform to a closed-pore state. The connection of crystal
fragmentation upon adsorption cycling and the crystal size
dependence of the adsorption-induced flexibility is an
important finding for evaluation of these materials in
future adsorption-based applications. This work thus extends
the limited amount of studies on crystal size effects in
flexible MOFs and hopefully motivates further investigations
in this field.},
cin = {ER-C-1 / ER-C-2},
ddc = {620},
cid = {I:(DE-Juel1)ER-C-1-20170209 / I:(DE-Juel1)ER-C-2-20170209},
pnm = {143 - Controlling Configuration-Based Phenomena (POF3-143)
/ DFG project 167917811 - SFB 917: Resistiv schaltende
Chalkogenide für zukünftige Elektronikanwendungen:
Struktur, Kinetik und Bauelementskalierung "Nanoswitches"
(167917811)},
pid = {G:(DE-HGF)POF3-143 / G:(GEPRIS)167917811},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:31501745},
UT = {WOS:000482478100001},
doi = {10.3762/bjnano.10.169},
url = {https://juser.fz-juelich.de/record/878318},
}