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@ARTICLE{Benchimol:611899,
author = {Benchimol, Elie and Regeni, Irene and Zhang, Bo and Kabiri,
Michele and Holstein, Julian J. and Clever, Guido},
title = {{H}eteromeric {C}ompletive {S}elf-{S}orting in
{C}oordination {C}age {S}ystems},
journal = {Journal of the American Chemical Society},
volume = {146},
number = {10},
issn = {0002-7863},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {PUBDB-2024-05113},
pages = {6905-6911},
year = {2024},
note = {Copyright @ACS},
abstract = {Heteroleptic coordination cages, nonstatistically assembled
from a set of matching ligands, can be obtained by mixing
individual components or via cage-to-cage transformations
from homoleptic precursors. Based on the latter approach, we
here describe a new level of self-sorting in coordination
cage systems, namely, ‘heteromeric completive
self-sorting’. Here, two heteroleptic assemblies of type
Pd$_2$A$_2$B$_2$ and Pd$_2$A$_2$C$_2$, sharing one common
ligand component A but differing in the other, are shown to
coexist in solution. This level of self-sorting can be
reached either from a statistical mixture of assemblies
based on some ligands B and C or, alternatively, following a
first step of integrative self-sorting giving a distinct
Pd$_2$B$_2$C$_2$ intermediate. While subtle enthalpic
factors dictate the outcome of the self-sorting, we found
that it is controllable. From a unique set of three ligands,
we demonstrate the transition from strict integrative
self-sorting forming a Pd$_2$AB$_2$C cage to heteromeric
completive self-sorting to give Pd$_2$A$_2$B$_2$ and
Pd$_2$A$_2$C$_2$ by variation of the ligand ratio.
Cage-to-cage transformations were followed by NMR and MS
experiments. Single crystal X-ray structures for three new
heteroleptic cages were obtained, impressively highlighting
the versatility of ligand A to either form a π-stacked
trans-figure-of-eight arrangement in Pd$_2$A$_2$B$_2$ or
occupy two cis-edges in Pd$_2$A$_2$C$_2$ or only a single
edge in Pd$_2$AB$_2$C. This study paves the way toward the
control of heteroleptic cage populations in a systems
chemistry context with emerging features such as chemical
information processing, adaptive guest selectivity, or
stimuli-responsive catalytic action.},
cin = {DOOR ; HAS-User},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20211437
(I-20211437) / FS-Proposal: I-20210921 (I-20210921) / GRK
2376 - GRK 2376: Umgrenzungsgesteuerte Chemie (331085229) /
DFG project 390677874 - EXC 2033: RESOLV (Ruhr Explores
Solvation) (390677874)},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20211437 /
G:(DE-H253)I-20210921 / G:(GEPRIS)331085229 /
G:(GEPRIS)390677874},
experiment = {EXP:(DE-H253)P-P11-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:38423558},
UT = {WOS:001179247700001},
doi = {10.1021/jacs.3c14168},
url = {https://bib-pubdb1.desy.de/record/611899},
}