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Self-Healable Poly(ionic liquid) Copolymers Driven by Polar and Dipolar Forces
Samruddhi Gaikwad1, Jiahui Liu1, Nyx Mashkow1
1Department of Materials Science and Engineering, Clemson University, Clemson, SC, 29634, USA.
Angewandte Chemie (International Ed. in English)
|June 30, 2025
Summary
Covalently incorporating ionic liquids into copolymers enhances self-healing properties. Longer aliphatic tails and controlled interactions improve material recovery for sustainable energy applications.
Area of Science:
- Polymer Science
- Materials Chemistry
- Supramolecular Chemistry
Background:
- Acrylic-based copolymers exhibit self-healing via van der Waals (vdW) interactions.
- The impact of covalently incorporated ionic liquids (ILs) on these interactions and self-healing is largely unknown.
Purpose of the Study:
- To investigate how poly(ionic liquid) copolymers (PILCs) affect vdW interactions and mechanical/electrical properties.
- To determine the role of IL cation-anion pairs and aliphatic tail length in self-healing.
Main Methods:
- Synthesis of PILCs from pentafluorostyrene and imidazolium-based IL monomers with varying aliphatic tails.
- Characterization using 2D NMR (¹H-¹H, ¹⁹F-¹⁹F NOESY), FTIR, and molecular dynamics (MD) simulations.
Main Results:
- Alternating/random PILC topologies were found to facilitate self-healing.
- Cation-anion moieties alter fluorophilic-σ-lock interactions.
- Longer aliphatic tails increased cation-anion mobility, leading to faster mechanical damage recovery.
Conclusions:
- Precise control over dipolar and ionic interactions via copolymer composition enables self-healing in PILCs.
- Findings offer pathways for designing sustainable, mechanically resilient materials for energy storage and harvesting.
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