Two sets of waterborne polyurethane dispersions were synthesised from polycarbonate polyol with molecular mass of 500 Da and hexamethylene diisocyanate or isophorone diisocyanate. Formulations were prepared without a chain extender, with aliphatic diol with two to five carbon atoms or with diethylene glycol. Coatings were prepared on cellulose triacetate sheets, damaged by a steel-wool scratch instrument and left to heal at room temperature and at 60 °C. Self-healing efficiency was examined by comparison of haze before damage and at intervals after damage. Samples were analysed using Differential Scanning Calorimetry, Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy and Scanning Electron Microscopy. The tests were repeated after 12 weeks to investigate ageing of the polymers. Samples were also tested for their stability to weathering.

Optimally designed coatings obtained up to 100% recovery within 10 min at 60 °C and partial recovery at room temperature. The self-healing properties of coatings were found to be linked to macro-organisation of polymer chains caused by interactions between hard segments and soft segments of the polyurethane moiety, leading to phase-mixing, promoted by bulky, non-symmetrical isophorone diisocyanate, or phase-separation, promoted by linear, symmetrical hexamethylene diisocyanate. The length of chain extender was found to have large influence on formulations prepared with hexamethylene diisocyanate, increasing phase-separation and haze with the increase of chain length. Diethylene glycol was found to improve phase-mixing and self-healing properties of hexamethylene diisocyanate based materials. The influence of chain extenders was found to be minimal for isophorone diisocyanate based materials.

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Volume 122, September 2018, Pages 1–9