Development of lignin-based polyurethane thermoplastics

Here we report utilizing a tailored feedstock to synthesize mechanically robust thermoplastic polyurethanes at very high lignin contents (65–75 wt%). The molecular weight and glass transition temperature (Tg) of lignin were altered through cross-linking with formaldehyde. The cross-linked lignin was coupled with diisocyanate-based telechelic polybutadiene as a network-forming soft segment. The appearance of two Tg's, around −35 and 154 °C, for the polyurethanes indicates the existence of two-phase morphology, a characteristic of thermoplastic copolymers. A calculated Flory–Huggins interaction parameter of 7.71 also suggests phase immiscibility in the synthesized lignin polyurethanes. An increase in lignin loading increased the modulus, and an increase in crosslink-density increased the modulus in the rubbery plateau region of the thermoplastic. This path for synthesis of novel lignin-based polyurethane thermoplastics provides a design tool for high performance lignin-based biopolymers.