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@ARTICLE{VandeVoorde:167838,
author = {Van de Voorde, Ben and Munn, Alexis and Guillou, Nathalie
and Millange, Franck and De Vos, Dirk E. and Walton,
Richard},
title = {{A}dsorption of {N}/{S} heterocycles in the flexible
metal–organic framework {MIL}-53({F}e{III}) studied by in
situ energy dispersive {X}-ray diffraction},
journal = {Physical chemistry, chemical physics},
volume = {15},
number = {22},
issn = {1463-9084},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {DESY-2014-02164},
pages = {8606 - 8615},
year = {2013},
note = {© The Owner Societies},
abstract = {The adsorption of N/S-containing heterocyclic organic
molecules in the flexible iron(III) terephthalate MIL-53,
FeIII(OH)0.6F0.4(O2C–C6H4–CO2)·(H2O), from the liquid
phase was studied with in situ energy dispersive X-ray
diffraction (EDXRD), in order to follow the
adsorption-induced expansion of the structure. For
comparison with the diffraction data, liquid phase
adsorption isotherms were recorded for uptake of
benzothiophene, benzothiazole and indole in isopropanol and
in heptane. The solvent not only influences pore opening but
is also a competing guest. The in situ EDXRD experiments
allow the kinetics of guest uptake and the competition with
solvent to be monitored directly. Indole uptake is limited;
this adsorbate is barely capable of opening the closed,
either hydrated or dehydrated, MIL-53(Fe) structure, or of
penetrating the isopropanol-containing material in the
concentration range under study. When isopropanol is used as
a solvent, the guest molecules benzothiophene and
benzothiazole must be present at a certain threshold
concentration before substantial adsorption into the
metal–organic framework takes place, eventually resulting
in full opening of the structure. The fully expanded
structures of benzothiophene or benzothiazole loaded
MIL-53(Fe) materials have Imcm symmetry and a unit cell
volume of ca. 1600 Å3, and upon uptake of the guest
molecules by the closed form (unit cell volume [similar]1000
Å3) no intermediate crystalline phases are seen. Successful
uptake by MIL-53(Fe) requires that the adsorbate is
primarily a good hydrogen bond acceptor; additionally, based
on UV-visible spectroscopy, a charge-transfer interaction
between the S atoms of benzothiophene and the aromatic rings
in the MOF pore wall is proposed.},
cin = {DOOR},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {DORIS Beamline F3 (POF2-54G13)},
pid = {G:(DE-H253)POF2-F3-20130405},
experiment = {EXP:(DE-H253)D-F3-20150101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000319006100017},
pubmed = {pmid:23439974},
doi = {10.1039/c3cp44349c},
url = {https://bib-pubdb1.desy.de/record/167838},
}