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Dinuclear helicate and tetranuclear cage assembly using appropriately designed ditopic triazole-azine ligands
Ist Teil von
Dalton transactions : an international journal of inorganic chemistry, 2019-10, Vol.48 (41), p.15435-15444
Ort / Verlag
England
Erscheinungsjahr
2019
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
Four new, symmetrical, bis-bidentate ditopic
Rdpt
-type,
Rat
(
R a
zine-
t
riazole), ligands have been prepared,
L
n
pym-
meta
/
para
(
n
= 2 or 4), which contain
bidentate n
-pyrimidine/triazole binding pockets connected through an appropriate aromatic spacer,
meta
/
para
-phenyl, to enable assembly into dinuclear helicates or tetranuclear tetrahedral cages, respectively. The 3 : 2 self assembly reactions of each
L
n
pym-
meta
/
para
ligand with iron(
ii
) tetrafluoroborate gave the desired complexes, as shown by X-ray crystal structure determinations of the pair of helicates [Fe
II
2
(
L
n
pym-
meta
)
3
(BF
4
)
4
]·6CH
3
CN, with
n
= 2 (
1
·6CH
3
CN) or 4 (
2
·6CH
3
CN), and the pair of Td cages [Fe
II
4
(
L
n
pym-
para
)
6
(BF
4
)
8
]·
x
solvent, with
n
= 2 (
3
·
x
solvent) or 4 (
4
·
x
solvent). Reversible Fe
II/III
processes at
E
m
= 0.95 ± 0.05 V
vs
. 0.01 M AgNO
3
/Ag in MeCN are a feature of
1-4
, with little variation in the redox potential as a function of nuclearity, architecture or choice of
n
-pyrimidine isomer. In all four complexes the iron(
ii
) centres are low spin, despite having employed the weakest field diazines, the 2- and 4-pyrimidines, in these ditopic
Rat
ligands. Nevertheless this is an exciting proof of principle that
Rdpt
-type ligands (previously used to generate about 50 spin crossover-active complexes) can be extended into ditopic forms that are suitable for supramolecular assembly of helicates and cages.
Architecture, helicate or cage, is controlled by choice of
meta vs
.
para
phenylene linker in new, robust, ditopic triazole-pyrimidine ligands.
Sprache
Englisch
Identifikatoren
ISSN: 1477-9226
eISSN: 1477-9234
DOI: 10.1039/c9dt01890e
Titel-ID: cdi_rsc_primary_c9dt01890e
Format
–
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