Unlike living organisms, synthetic materials are not able to recover from damages and possess therefore a limited lifetime. To counteract this fragility, supramolecular assemblies have shown a great interest since a couple of decades for their strong ability to allow reprocessing of polymers. Recently, the emergence of intrinsic self-healing polymers making use of reversible physical associations such as hydrogen bonds established itself as a promising way to extend shelf-life. In this study, we selected silicone-based systems for their hydrophobicity, flexibility and thermal stability.<br/><br/>Starting from published results, we first set up a fundamental study by reacting liquid α,ω-amino-PDMS with urea, to generate a variety of functional groups likely to interact through H-bonding. The influence of the nature of the associating groups, along with chain length and hydrophilic to hydrophobic ratio, was investigated and related to the nanostructuration and bulk properties of thus-prepared materials. Different analytical studies allowed correlating the chemistry (NMR, IR and SEC) and the physical chemical properties (rheology, DMA, TGA, DSC) as well as structural characteristics (SAXS) and self-healing abilities.<br/><br/>With a complete understanding of those supramolecular interactions, we have also been able to generate new polydimethylsiloxanes with autonomous self-healing abilities that will likely be presented here.

Supramolecular silicone self-healing materials

256th National Meeting (2018)

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