High-performance elastomers are expected to possess excellent healing and recycling ability, damage resistance in conjunction with high strength and toughness. Herein, a dual dynamic crosslinking strategy is implemented by multiple hydrogen and disulfide bonds to obtain a novel amorphous and transparent polyurethane/nanocellulose elastomer with excellent self-healing, self-reinforcing and toughening performance. First, hydrogen bonds are introduced in TEMPO-oxidized cellulose nanofibers (TCNF) by modification with 2-ureido-4[1H]-pyrimidone (UTCNF), while disulfide bonds (SS) are introduced in the polyurethane (PU) main chain, leading to the formation of dual dynamic cross-linking networks. The PU-SS-UTCNF elastomer can fully self-heal within 4.0 h at 50 °C. Surprisingly, for the first time, the PU-SS-UTCNF elastomer also self-strengthens and self-toughens after multiple hot-pressing, with tensile strength and toughness that increase by up to 401% and 257% compared to original elastomer samples, up to 50.0 MPa and 132.5 MJ m -3 . The selfstrength and self-toughening effects are attributed to 1) reconstruction of dual dynamic networks that increase the cross-linking degree during the multiple hot-pressing processes; 2) multiple hydrogen bonds in the system are beneficial to the orientation of highly crystallized UTCNF, as a replacement of stressinduced process in deformation under external tensile force.
This article reports the preparation, by means of a masterbatch procedure, of poly (lactic acid) (PLA)/ cellulose nanocrystal (CNC) films via premixing 1% wt of CNC into PLA or glycidyl methacrylate (GMA) grafted PLA (g-PLA). These films were obtained by reactive extrusion and subsequent film processing. In this study, 10% wt of GMA with respect to neat PLA was used in the extrusion phase, after that a final grafting degree of 5.69% was obtained. The film obtained by using the masterbatch steps were compared with the system obtained by a direct extrusion of 1% wt of CNC in PLA/g-PLA. Thermogravimetric, crystallization and mechanical properties, as well as morphology of CNC reinforced PLA nanocomposites were characterized. Differential scanning calorimetry and thermogravimetric analysis showed enhanced crystallization ability and an improved heat resistance for the resulting nanocomposites obtained after the use of masterbatches, for example field emission scanning electron microscopy confirmed that the masterbatch preparation procedure was beneficial to the dispersion of CNC in the final nanocomposites. Furthermore, different mechanical performance was obtained when using different masterbatches, which were considered to contribute to extend the applications of PLA based composites as food packaging materials in different sectors.
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