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High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design

Unsymmetrical ditopic ligands can self‐assemble into reduced‐symmetry Pd(2)L(4) 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...

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Detalles Bibliográficos
Autores principales: Tarzia, Andrew, Lewis, James E. M., Jelfs, Kim E.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8518684/
https://www.ncbi.nlm.nih.gov/pubmed/34254713
http://dx.doi.org/10.1002/anie.202106721
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author Tarzia, Andrew
Lewis, James E. M.
Jelfs, Kim E.
author_facet Tarzia, Andrew
Lewis, James E. M.
Jelfs, Kim E.
author_sort Tarzia, Andrew
collection PubMed
description Unsymmetrical ditopic ligands can self‐assemble into reduced‐symmetry Pd(2)L(4) 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 Pd(2)L(4) cage isomers, ranking the likelihood for exclusively 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.
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spelling pubmed-85186842021-10-21 High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design Tarzia, Andrew Lewis, James E. M. Jelfs, Kim E. Angew Chem Int Ed Engl Research Articles Unsymmetrical ditopic ligands can self‐assemble into reduced‐symmetry Pd(2)L(4) 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 Pd(2)L(4) cage isomers, ranking the likelihood for exclusively 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. John Wiley and Sons Inc. 2021-08-11 2021-09-13 /pmc/articles/PMC8518684/ /pubmed/34254713 http://dx.doi.org/10.1002/anie.202106721 Text en © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Tarzia, Andrew
Lewis, James E. M.
Jelfs, Kim E.
High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
title High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
title_full High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
title_fullStr High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
title_full_unstemmed High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
title_short High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
title_sort high‐throughput computational evaluation of low symmetry pd(2)l(4) cages to aid in system design
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8518684/
https://www.ncbi.nlm.nih.gov/pubmed/34254713
http://dx.doi.org/10.1002/anie.202106721
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