The synthesis of eco-friendly and biocompatible waterborne
polyurethanes
(WPUs) through judicious molecular engineering with supreme mechanical
strength, good shape recoverability, and high self-healing efficiency
is still a formidable challenge because of some mutually exclusive
conflicts among these properties. Herein, we report a facile method
to develop a transparent (80.57–91.48%), self-healable (efficiency
67–76%) WPU elastomer (strain 3297–6356%) with the highest
reported mechanical toughness (436.1 MJ m–3), ultrahigh
fracture energy (126.54 kJ m–2), and good shape
recovery (95% within 40 s at 70 °C in water). These results were
accomplished by introducing high-density hindered urea-based hydrogen
bonds, an asymmetric alicyclic architecture (isophorone diisocyanate–isophorone
diamine), and the glycerol ester of citric acid (a bio-based internal
emulsifier) into the hard domains of the WPU. Most importantly, platelet
adhesion activity, lactate dehydrogenase activity, and erythrocyte
or red blood corpuscle lysis demonstrated the hemocompatibility of
the developed elastomer. Simultaneously, the cellular viability (live/dead)
assay and the cell proliferation (Alamar blue) assay of human dermal
fibroblasts corroborated the biocompatibility under in vitro conditions.
Furthermore, the synthesized WPUs showed melt re-processability with
retention of mechanical strength (86.94%) and microbe-assisted biodegradation.
The overall results, therefore, indicate that the developed WPU elastomer
might be used as a potential smart biomaterial and coating for biomedical
devices.