Recyclable and Mendable Cellulose-Reinforced Composites Crosslinked with Diels–Alder Adducts

Owing to their natural abundance and exceptional mechanical properties, cellulose fibers (CFs) have been used for reinforcing polymers. Despite these merits, dispersing hydrophilic CFs in a hydrophobic polymer matrix is challenging. To address this, an amphiphilic ammonium salt was employed as the dispersant for CFs in this study. The hydrophobic CFs were mixed with a healable polymer to produce CF-reinforced composites. As the thermosetting polymer was crosslinked with Diels–Alder (DA) adducts, it was mended and recycled via a retro DA reaction at 120 °C. Interestingly, the CF-reinforced polymer composites were mended and recycled as well. When 5 wt % of the hydrophobic CFs was added to the polymer, maximum tensile strength, elongation at break, Young’s modulus, and toughness increased by 70%, 183%, 75%, and 420%, respectively. After recycling, the CF-reinforced composites still featured better mechanical properties than recycled polymer.