High‐throughput computational evaluation of low symmetry Pd
<sub>2</sub>
L
<sub>4</sub>
Cages to Aid in System Design**
<sub>2</sub>
L
<sub>4</sub>
Cages to Aid in System Design**
OA Location
Author(s)
Tarzia, Andrew
Lewis, James EM
Jelfs, Kim E
Type
Journal Article
Abstract
Unsymmetrical ditopic ligands can self-assemble into reduced-symmetry Pd2L4 metallo-cages with anisotropic cavities, with implications for high specificity and affinity guest-binding. Mixtures of cage isomers can form, however, resulting in undesirable system heterogeneity. It is paramount to be able to design components that preferentially form a single isomer. Previous data suggested that computational methods could predict with reasonable accuracy whether unsymmetrical ligands would preferentially self-assemble into single cage isomers under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial-and-error synthetic approaches. Our rapid computational workflow constructs unsymmetrical ligands and their Pd2L4 cage isomers, ranking the likelihood for exclusively forming cis-Pd2L4 assemblies. From this narrowed search space, we successfully synthesised four new, low-symmetry, cis-Pd2L4 cages.
Date Issued
2021-09-13
Date Acceptance
2021-07-01
Citation
Angewandte Chemie, 2021, 133 (38), pp.21047-21055
ISSN
0044-8249
Publisher
Wiley
Start Page
21047
End Page
21055
Journal / Book Title
Angewandte Chemie
Volume
133
Issue
38
Copyright Statement
© 2021 The Authors. Angewandte Chemie published by Wiley-VCH GmbH
This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
License URL
Identifier
https://onlinelibrary.wiley.com/doi/10.1002/ange.202106721
Subjects
03 Chemical Sciences
Organic Chemistry
Publication Status
Published
Date Publish Online
2021-08-11