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Cage-To-Cage Transformations in Self-Assembled Coordination Cages Using "Acid/Base" or "Guest Binding-Induced Strain"
Vellaiyadevan Sivalingam1, Minaz Parbin1, Shobhana Krishnaswamy1
1IoE Center of Molecular Architecture, Department of Chemistry, Indian Institute of Technology Madras, Chennai, 600036, India.
Angewandte Chemie (International Ed. in English)
|April 3, 2024
Summary
Researchers developed acid/base responsive palladium cages that interconvert between two forms. These cages show tunable guest binding, enabling control over supramolecular systems and providing a three-state switching mechanism.
Area of Science:
- Supramolecular Chemistry
- Coordination Chemistry
- Materials Science
Background:
- Controlling supramolecular systems with stimuli like acids/bases is challenging, particularly with labile coordination bonds.
- Developing responsive systems requires precise control over structure and function.
Purpose of the Study:
- To design and synthesize acid/base responsive, interconvertible palladium cages.
- To investigate their differential guest binding abilities towards disulfonates.
- To achieve a controllable three-state switching mechanism for supramolecular systems.
Main Methods:
- Synthesis of 1,5-enedione/pyrylium based Pd2L4-type cages.
- Utilizing acids and bases as stimuli for cage transformation and disassembly.
- Employing competitive guest binding studies to assess binding capabilities.
Main Results:
- A pair of interconvertible cages responsive to weak and strong bases, and strong acids were successfully prepared.
- Differential guest binding towards disulfonates of varying sizes was observed.
- A three-state switching mechanism (cage-to-cage transformation, disassembly, regeneration) was demonstrated.
- Guest binding was found to facilitate cage transformations by inducing strain and opening pyrylium rings.
Conclusions:
- The study presents a novel approach to reversibly modulate guest binding properties of self-assembled coordination cages using acid/base stimuli.
- The findings offer a reliable method for controlling supramolecular systems with labile coordination bonds.
- The superior binding capability of the octacationic pyrylium cage was confirmed over a tetracationic analogue.
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