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.
High-Throughput Computational Evaluation of Low Symmetry Pd2L4 Cages to Aid in System Design** / Tarzia, A.; Lewis, J. E. M.; Jelfs, K. E.. - In: ANGEWANDTE CHEMIE. INTERNATIONAL EDITION. - ISSN 1433-7851. - 60:38(2021), pp. 20879-20887. [10.1002/anie.202106721]
High-Throughput Computational Evaluation of Low Symmetry Pd2L4 Cages to Aid in System Design**
Tarzia A.;
2021
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.File | Dimensione | Formato | |
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https://hdl.handle.net/11583/2981640