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Monodentate ligand binding is facilitated by supramolecular chirality transformations from propeller-shaped chirality into single-twist chirality by altering the self-assembly of C  3 -symmetric chiral ligands. The C  3 -symmetric chiral ligands ( Im  R   3 Bz and Im  S   3 Bz ) contain three chiral imidazole side arms (Im  R   and Im  S  ) at the 1,3,5-positions of a central benzene ring. Upon coordination to zinc ions (Zn 2+ ), which have a tetrahedral coordination preference, the C  3 -symmetric chiral ligands assemble, in a stepwise manner, into a propeller-shaped assembly with a general formula ( Im (   R   or   S   )  3 Bz ) 4 (Zn 2+ ) 3 . In this structure each Zn 2+ ion coordinates to the three individual imidazole side arms. The resulting assembly is formally coordinatively unsaturated (coordination number, n = 3) and capable of accepting monodentate co-ligands (imidazole: ImH 2 ) to afford a coordinatively saturated assembly [(ImH 2 ) 3 ( Im  R   3 Bz ) 4 (Zn 2+ ) 3 ]. The preformed propeller-shaped chirality is preserved during this transformation. However, an excess of the monodentate co-ligand (ImH 2 /Zn 2+ molar ratio of ∼1.7) alters the propeller-shaped assembly into a stacked dimer assembly [(ImH 2 )  m  ( Im  R   3 Bz ) 2 (Zn 2+ ) 3 ] ( m = 4-6) with single-twist chirality. This switch alters the degree of enhancement and the circular dichroism (CD) pattern, suggesting a structural transition into a chiral object with a different shape. This architectural chirality transformation presents a new approach to forming dynamic coordination-assemblies, which have transformable geometric chiral structures.

chemical science

Supramolecular chirality transformation driven by monodentate ligand binding to a coordinatively unsaturated self-assembly based on <i>C</i><sub>3</sub>-symmetric ligands

Supramolecular chirality transformation driven by monodentate ligand binding to a coordinatively unsaturated self-assembly based on C3-symmetric ligands

Supramolecular chirality transformation driven by monodentate ligand binding to a coordinatively unsaturated self-assembly based on C₃-symmetric ligands