High‐throughput computational evaluation of low symmetry Pd2L4 cages to aid in system design
File(s)
Published version
Author(s)
Tarzia, Andrew
Lewis, James
Jelfs, Kim E
Type
Journal Article
Abstract
The use of unsymmetrical components in metallo-supramolecular chemistry allows for low- symmetry architectures with anisotropic cavities toward guest-binding with high specificity and affinity. Unsymmetrical ditopic ligands mixed with Pd(II) have the potential to self-assemble into reduced symmetry Pd 2 L 4 metallo-architectures. Mixtures of isomers can form, however, resulting in potentially undesirable heterogeneity within a system. Therefore 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 a single isomer under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial-and-error synthetic approaches. Our low-cost computational workflow rapidly constructs new unsymmetrical ligands (and Pd 2 L 4 cage isomers) and ranks their likelihood for forming cis -Pd 2 L 4 assemblies. From this narrowed search space, we successfully synthesised four new low-symmetry, cis -Pd 2 L 4 cages, with cavities of different shapes and sizes.
Date Issued
2021-09-13
Date Acceptance
2021-07-01
Citation
Angewandte Chemie International Edition, 2021, 60 (38), pp.20879-20887
ISSN
1433-7851
Publisher
Wiley
Start Page
20879
End Page
20887
Journal / Book Title
Angewandte Chemie International Edition
Volume
60
Issue
38
Copyright Statement
© 2021 The Authors. Angewandte Chemie International Edition 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
Sponsor
The Royal Society
Commission of the European Communities
The Royal Society
The Royal Society
Identifier
https://onlinelibrary.wiley.com/doi/10.1002/anie.202106721
Grant Number
UF120469
758370
URF\R\180012
RGF\EA\181066
Subjects
Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
cage compounds
computational screening
high-throughput
low-symmetry
self-assembly
M2L4 COORDINATION CAPSULES
UNIVERSAL FORCE-FIELD
MOLECULAR CAPSULE
BASIS-SETS
COMPLEXES
ENCAPSULATION
PARAMETERS
STRATEGIES
EXTENSION
EFFICIENT
cage compounds
computational screening
high-throughput
low-symmetry
self-assembly
Organic Chemistry
03 Chemical Sciences
Publication Status
Published
Article Number
anie.202106721
Date Publish Online
2021-07-13