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Thermally self-healing graphene-nanoplate/polyurethane (GNP/PU) nanocomposites were prepared via a bulk in-situ Diels⁻Alder (DA) reaction. Graphene-nanoplate (GNP) was used as a reinforcement and crosslinking platform by a DA reaction with a furfuryl-based chain extender of polyurethane (PU). Results showed that a DA reaction occurred in GNP during the PU forming cure process. This procedure is simple and solvent free because of the absence of any independent surface modification process. Through the calculation of the interfacial tensions, the conditions of the bulk in-situ DA reaction were determined to ensure that GNP and the furfuryl group can react with each other at the interface during the curing process without a solvent. The prepared composites were characterized in terms of thermal, mechanical, and thermally self-healing properties via the DA reaction. In the PU capable of a DA reaction (DPU), characteristic peaks of DA and retro DA reactions were observed in the Fourier transform infrared (FT-IR) spectroscopy and endothermic peaks of retro DA reactions appeared in differential scanning calorimetry (DSC) thermograms. The DPU showed significantly enhanced physical properties and chemical resistance. The thermally self-healing capability was confirmed at 110 °C via the retro DA reactions. It is inferred that thermally self-healable crosslinked GNP/PU nanocomposites via DA reactions could be prepared in a simple bulk process through the molecular design of a chain extender for the in-situ reaction at the interface.

Thermally Self-Healing Graphene-Nanoplate/Polyurethane Nanocomposites via Diels–Alder Reaction through a One-Shot Process