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Origami Inspired Self-assembly of Patterned and Reconfigurable Particles

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Circular Heterochiral Titanium-Based Self-Assembled Architectures.

Pierre Mobian¹, David-Jérôme Pham¹, Alain Chaumont²

¹Université de Strasbourg, CNRS, CMC UMR 7140 (team SFAM), F-67000 Strasbourg, France.

Journal of the American Chemical Society

|May 10, 2024

Summary

This summary is machine-generated.

Researchers synthesized circular trinuclear titanium helicates, discovering that solvent choice influences their symmetry. Ligand A in titanium helicates exhibits a unique solvent-dependent equilibrium between heterochiral and homochiral forms.

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Area of Science:

Coordination Chemistry
Supramolecular Chemistry
Materials Science

Background:

Self-assembly of metal-organic architectures offers pathways to complex structures.
Titanium-based helicates are of interest for their unique structural and electronic properties.
Controlling symmetry in supramolecular assemblies is crucial for functional applications.

Purpose of the Study:

To synthesize and characterize circular trinuclear titanium helicates using various diimine ligands.
To investigate the influence of diimine ligands and solvent on the symmetry and aggregation of these helicates.
To elucidate the mechanism and thermodynamics of solvent-induced stereochemical transformations in titanium helicates.

Main Methods:

Synthesis of circular trinuclear helicates from bis-biphenol strands, titanium isopropoxide, and diimine ligands.
Structural characterization using X-ray crystallography and solution-state analysis (NMR spectroscopy).
Computational studies including DFT calculations and classical molecular dynamics simulations.

Main Results:

Formation of heterochiral (C1 symmetry) trinuclear titanium helicates with ligands A, B, C, and D.
Ligand F yielded homochiral (C3 symmetry) aggregates, while ligand E formed hexameric aggregates.
Ligand A in [Ti3L3(A)3] exhibited a solvent-dependent equilibrium between heterochiral and homochiral forms in dichloromethane, with a K value of 0.34.

Conclusions:

The symmetry of titanium helicates is controllable by the choice of diimine ligand and solvent.
A unique solvent-induced, intramolecular stereochemical transformation occurs in [Ti3L3(A)3] helicates.
Computational studies rationalize the observed solvent-induced symmetry switch, highlighting its dependence on the trinuclear assembly structure.