Non-isocyanate Polyurethane Coating with High Hardness, Superior Flexibility, and Strong Substrate Adhesion.

Flexible hard coatings with strong adhesion are critical requirements for several foldable devices and marine applications; however, only a few such coatings have been reported. Herein, we report a non-isocyanate polyurethane (NIPU) coating prepared by the epoxy-oligosiloxane nanocluster-amine curing reaction and cyclic carbonate-amine polyaddition, where the former provides the coating with ceramic-like hardness and polymer-like flexibility while the latter polymerization results in NIPU with strong substrate adhesion. The coating is transparent (>92% transmittance), hard (5-7 H), and flexible (2 mm bending diameter). It has strong adhesion to various substrates including aluminum alloy, titanium, steel, glass, ceramic, epoxy, and polyethylene terephthalate (2-8 MPa), which can be attributed to the high density of polar groups in NIPU. Moreover, we can facilely endow the coating with anti-icing, self-cleaning, and anti-smudge capabilities by incorporating amine-terminated low-surface-tension polydimethylsiloxane (PDMS) to replace a part of the amine curing agent. Particularly, the mechanical properties of NIPU coatings are only slightly affected by the introduction of low-content PDMS since it intends to enrich on the surface. The novel coating has promising future for use in fields of foldable devices and marine applications.