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@ARTICLE{Metzelaars:902604,
author = {Metzelaars, Marvin and Sanz, Sergio and Rawson, Jeff and
Hartmann, Rudolf and Schneider, Claus M. and Kögerler,
Paul},
title = {{F}using pyrene and ferrocene into a chiral, redox-active
triangle},
journal = {Chemical communications},
volume = {57},
number = {54},
issn = {0009-241X},
address = {Cambridge},
publisher = {Soc.},
reportid = {FZJ-2021-04399},
pages = {6660 - 6663},
year = {2021},
abstract = {Fundamental understanding and control of electron transfer
processes in molecular building blocks are key to construct
nanoscale (spin)electronic devices. Ferrocene (Fc) has been
studied extensively in this context due to high conductance
and stability, and its well-defined and reversible
redox-switching behaviour.1 The integration of multiple Fc
groups into a single, nonlinear molecule (e.g. stars2 or
macrocycles3) generates materials with extraordinary
electronic properties that might not be observed in linear
analogues. So far only a handful of shape-persistent and
cyclic Fc-based compounds have been synthesised by linking
Fc groups either directly3g,h or via simple bridging units,
like diethynylbenzene derivatives.3c–eUsing the larger
aromatic building block pyrene (Py), we can tune the
properties for a range of applications. The Py group is
fundamental in host–guest chemistry, used in metallacycles
and -cages to entrap fullerenes and other guests.4 Preuß et
al. used linear ferrocenyl–pyrenes to disentangle and
functionalise carbon nanotubes via π–π stacking.5 We
showed that a Fc-bridged pyrenophane can be sublimed onto
ferromagnetic surfaces to craft 3D spin interfaces.6 The
photophysical properties of pyrene have been exploited in
phototransistors, “turn-on” sensors and fluorescence
switches based on Fc–Py dyads.7To construct a macrocycle
with two different functional units often entails
protracted, stepwise synthesis. We recently demonstrated a
one-step Suzuki–Miyaura cross-coupling (SMC) route to an
insoluble, pyrene-based cyclophane in $<1\%$ yield (Chart 1,
cyclophane). By this method, we synthesised a soluble
macrocycle of three Fc–Py dyads bonded into a triangle
(Chart 1, 3). Employing 2,7-bis(Bpin)pyrene as linear and
1,1′-diiodoferrocene as angular building blocks, our
optimised conditions gave a yield of $6\%$ (PdCl2(dtbpf) in
DMF). The Fc group adopts a range of angles to serve as a
vertex in linear and larger cyclic oligomers with low
solubility, which we could detect by mass spectrometry of
crude reaction mixtures, albeit not isolate. Soluble side
products, likely generated via dehalogenation or
deborylation of acyclic intermediates, were also identified
(see Fig. S12 and S13†). We synthesised noncyclic
molecules 1 and 2 that complete the series in Chart 1. The
identity of dyad 1, stack 2 and triangle 3 were confirmed by
1H/13C-NMR (Fig. S1–S7†), MALDI-HRMS (Fig. S8–S11†),
and elemental analysis.},
cin = {PGI-6},
ddc = {540},
cid = {I:(DE-Juel1)PGI-6-20110106},
pnm = {5223 - Quantum-Computer Control Systems and Cryoelectronics
(POF4-522)},
pid = {G:(DE-HGF)POF4-5223},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:34128505},
UT = {WOS:000661559200001},
doi = {10.1039/D1CC02191E},
url = {https://juser.fz-juelich.de/record/902604},
}