Döhler, D., et al. ACS Appl. Polym. Mater., 2020, DOI:https://dx.doi.org/10.1021/acsapm.0c00755
We present a comprehensive investigation of mechanical properties of supramolecular polymer networks with rationally developed multistrength hydrogen-bonding interactions to embed self-healing properties into poly(dimethylsiloxane) (PDMS)-based elastomers. By changing the ratio between isophorone diisocyanate (IU), 4,4′-methylenebis(cyclohexyl isocyanate) (MCU), and 4,4′-methylenebis(phenyl isocyanate) (MPU) and by varying the molecular weight of the PDMS precursor, we obtained a library of poly(urea)s to study the interplay of mechanical performance and self-healability. We achieved an optimum balance between mechanical properties and self-healing performance, and by the additional reduction of the molecular weight of the precursor polymer, a minimum recovery of 80% in stress within 12 h at room temperature was observed. Selected poly(urea)s could be processed via 3D printing by the conventional extrusion method, obtaining dimensionally stable and freestanding objects.