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@ARTICLE{Gasevic:602305,
author = {Gasevic, Thomas and Bamberg, Marcel and Wicke, Julius and
Bolte, Michael and Virovets, Alexandr and Lerner,
Hans-Wolfram and Grimme, Stefan and Hansen, Andreas and
Wagner, Matthias and Bursch, Markus},
title = {{C}onfined {L}ewis {P}airs: {I}nvestigation of the ${X}^−
→$ {S}i$_{20}$ {I}nteraction in
{H}alogen‐{E}ncapsulating {S}ilafulleranes},
journal = {Angewandte Chemie / International edition},
volume = {63},
number = {6},
issn = {1433-7851},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {PUBDB-2024-00580},
pages = {e202314238},
year = {2024},
abstract = {A joint theoretical and experimental study on 32 endohedral
silafullerane derivatives [X@Sii$_{20}$Yi$_{20}$] (X = F-I;
Y = F-I, H, Me, Et) and Th-[Cl@Sii$_{20}$Hi$_{12}$Y$_8$] (Y
= F-I) is presented. First, we evaluated the structure
determining template effect of Cl in a systematic series of
concave silapolyquinane model systems. Second, we
investigated the X$^- \to$ Si$_{20}$ interaction energy
(Eint) as a function of X and Y and found the largest Eint
values for electron-withdrawing exohedral substituents Y.
Given that X ions can be considered as Lewis bases and empty
Sii$_{20}$Yi$_{20}$ clusters as Lewis acids, we classify our
inseparable host–guest complexes [X@Sii$_{20}$Yi$_{20}$]
as “confined Lewis pairs”. Third, $^{35}$Cl NMR
spectroscopy proved to be highly diagnostic for an
experimental assessment of the Cl$^- \to$ Sii$_{20}$
interaction as the paramagnetic shielding and, in turn,
delta($^{35}$Cl) of the endohedral Cl ion correlate
inversely with Eint. Finally, we disclose the synthesis of
[PPN][Cl@Sii$_{20}$Yi$_{20}$](Y = Me, Et, Br) and provide a
thorough characterization of these new silafulleranes.},
cin = {DOOR ; HAS-User},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / DFG project 506550642 -
Siladodecahedrane: Untersuchungen zu Reaktivität,
Bindungssituation und optoelektronischen Eigenschaften
(506550642)},
pid = {G:(DE-HGF)POF4-6G3 / G:(GEPRIS)506550642},
experiment = {EXP:(DE-H253)P-P24-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:38059423},
UT = {WOS:001138626400001},
doi = {10.1002/anie.202314238},
url = {https://bib-pubdb1.desy.de/record/602305},
}