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@ARTICLE{Breeze:167766,
author = {Breeze, Matthew I. and Clet, Guillaume and Campo, Betiana
C. and Vimont, Alexandre and Daturi, Marco and Grenèche,
Jean-Marc and Dent, Andrew J. and Millange, Franck and
Walton, Richard},
title = {{I}somorphous {S}ubstitution in a {F}lexible
{M}etal–{O}rganic {F}ramework: {M}ixed-{M}etal,
{M}ixed-{V}alent {MIL}-53 {T}ype {M}aterials},
journal = {Inorganic chemistry},
volume = {52},
number = {14},
issn = {1520-510X},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {DESY-2014-02097},
pages = {8171 - 8182},
year = {2013},
note = {© American Chemical Society},
abstract = {Mixed-metal iron–vanadium analogues of the
1,4-benzenedicarboxylate (BDC) metal–organic framework
MIL-53 have been synthesized solvothermally in
N,N′-dimethylformamide (DMF) from metal chlorides using
initial Fe:V ratios of 2:1 and 1:1. At 200 °C and short
reaction time (1 h), materials (Fe,V)II/IIIBDC(DMF1–xFx)
crystallize directly, whereas the use of longer reaction
times (3 days) at 170 °C yields phases of composition
[(Fe,V)III0.5(Fe,V)0.5II(BDC)(OH,F)]0.5–·0.5DMA+ (DMA =
dimethylammonium). The identity of the materials is
confirmed using high-resolution powder X-ray diffraction,
with refined unit cell parameters compared to known pure
iron analogues of the same phases. The oxidation states of
iron and vanadium in all samples are verified using X-ray
absorption near edge structure (XANES) spectroscopy at the
metal K-edges. This shows that in the two sets of materials
each of the vanadium and the iron centers are present in
both +2 and +3 oxidation states. The local environment and
oxidation state of iron is confirmed by 57Fe Mössbauer
spectrometry. Infrared and Raman spectroscopies as a
function of temperature allowed the conditions for removal
of extra-framework species to be identified, and the
evolution of μ2-hydroxyls to be monitored. Thus calcination
of the mixed-valent, mixed-metal phases
[(Fe,V)III0.5(Fe,V)0.5II(BDC)(OH,F)]0.5–·0.5DMA+ yields
single-phase MIL-53-type materials, (Fe,V)III(BDC)(OH,F).
The iron-rich, mixed-metal MIL-53 shows structural
flexibility that is distinct from either the pure Fe
material or the pure V material, with a thermally induced
pore opening upon heating that is reversible upon cooling.
In contrast, the material with a Fe:V content of 1:1 shows
an irreversible expansion upon heating, akin to the pure
vanadium analogue, suggesting the presence of some domains
of vanadium-rich regions that can be permanently oxidized to
V(IV).},
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:000322087100041},
pubmed = {pmid:23815225},
doi = {10.1021/ic400923d},
url = {https://bib-pubdb1.desy.de/record/167766},
}