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.
Original language | English |
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Pages (from-to) | 20879-20887 |
Number of pages | 9 |
Journal | Angewandte Chemie (International Edition) |
Volume | 60 |
Issue number | 38 |
Early online date | 13 Jul 2021 |
DOIs | |
Publication status | Published - 13 Sept 2021 |
Keywords
- cage compounds
- computational screening
- high-throughput
- low-symmetry
- self-assembly