Simultaneous Reinforcing and Toughening of Polyurethane via Grafting on the Surface of Microfibrillated Cellulose

In the present work, a series of thermoplastic polyurethane (TPU)/microfibrillated cellulose (MFC) nanocomposites were successfully synthesized via in situ polymerization. TPU was covalently grafted onto the MFC by particular association with the hard segments, as evidenced by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis. The adequate dispersion and network structure of MFC in the TPU matrix and the strong interfacial interaction through covalent grafting and hydrogen bonding between MFC and TPU resulted in significantly improved mechanical properties and thermostability of the prepared nanocomposites. The tensile strength and elongation-at-break of the nanocomposite containing only 1 wt % MFC were increased by 4.5-fold and 1.8-fold compared with that of neat TPU, respectively. It was also very interesting to find that the glass transition temperature (Tg) of TPU was decreased significantly with the introduction of MFC, indicating potential for low-temperature resistance applications. Most importantly, compared with TPU nanocomposites reinforced with other nanofillers, the TPU/MFC nanocomposites prepared in this work exhibited excellent transparency and higher reinforcing efficiency.