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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...
Autores principales: | , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2021
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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. |
format | Online Article Text |
id | pubmed-8518684 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
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
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title_full | High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
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title_fullStr | High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
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title_full_unstemmed | High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
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title_short | High‐Throughput Computational Evaluation of Low Symmetry Pd(2)L(4) Cages to Aid in System Design
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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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