In situ polymerization of mechanically reinforced, thermally healable graphene oxide/polyurethane composites based on Diels-Alder chemistry

Covalently bonded graphene oxide/polyurethane (GO/PU) composites with significant reinforcement and thermally healable properties were developed via in situ polymerization based on Diels-Alder (DA) chemistry. The PU prepolymer was prepared with GO, 4,4-diphenylmethane diisocyanate, and poly(tetramethylene glycol) and blocked by using furfuryl alcohol firstly. Then the prepolymer was crosslinked by using bifunctional maleimide via DA chemistry. SEM shows that the GO was dispersed uniformly in the PU matrix. The DA and retro-DA reactions were characterized by Fourier transform infrared spectroscopy and differential scanning calorimetry separately. Tensile tests showed that with the incorporation of 0.1 wt% of GO, the tensile modulus of GO/PU composites increased from 9.80 MPa to 21.95 MPa, and the tensile strength and elongation at break of the GO/PU composites increased by more than 367% and 210%, respectively. Furthermore, the composites had thermally healable ability which was inspected by using an atomic force microscope and the strain-stress test. The healing efficiency of 78% on average was achieved which was determined by the recovery of breaking stress and a healing mechanism was tentatively proposed. Therefore, the covalently bonded self-healing GO/PU composites could be used as smart materials and structural materials.