Rational design of metal–organic cages to increase the number of components via dihedral angle control

Tsukasa Abe, Keisuke Takeuchi, Masahiro Higashi, Hirofumi Sato and Shuichi Hiraoka ()
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Tsukasa Abe: The University of Tokyo
Keisuke Takeuchi: The University of Tokyo
Masahiro Higashi: Nagoya University
Hirofumi Sato: Kyoto University
Shuichi Hiraoka: The University of Tokyo

Nature Communications, 2024, vol. 15, issue 1, 1-17

Abstract: Abstract The general principles of discrete, large self-assemblies composed of numerous components are not unveiled and the artificial formation of such entities is a challenging topic. In metal–organic cages, design strategies for tuning the coordination directions in multitopic ligands by the bend and twist angles were previously developed to solve this problem. In this study, the importance of remote geometric communications between components is emphasized, realizing several types of metal–organic assemblies based on dihedral angle control in multitopic ligands although they have the same coordination directions. Self-assembly of a tritopic ligand with dihedral angles θ = 36.5° and a cis-protected Pd(II) ion affords M9L6 and M12L8 cages as kinetic and thermodynamic products, respectively, whereas an M12L8 sheet is formed when θ = 90°. Geometric analyses of strains in the subcomponent rings reveals that remote geometric communications among neighboring multitopic ligands through coordination bonds are key for large assemblies.

Date: 2024
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DOI: 10.1038/s41467-024-50972-z

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