Reactive melt crosslinking of cellulose nanocrystals/poly(ε-caprolactone) for heat-shrinkable network

Focusing on the challenge of non-biodegradable plastics replacement, we propose a design for peroxide-initiated crosslinking biodegradable poly(ε-caprolactone) (PCL) and renewable cellulose nanocrystals (CNCs) bionanocomposites. An industrially scalable water-assisted reactive melt-processing (REx) is studied to explore hypothesis synergy between simultaneous effects water improving CNC dispersion boosting PCL branching/crosslinking. We demonstrate that melt processing control enables preparation targeted thermoplastic/thermoset bionanocomposites with gel content up ≈ 40 %, identified as limit their melt-processability. Structural characterization reveals 70 wt% initial irreversibly incorporated in percolating network, enhancing crosslinked properties. The bionanocomposites' complex viscosity elastic character increase content, thus performance. Furthermore, irreversible entrapment CNCs 3D network provides heat-shrinkability, indicating potential reacted heat-triggered shape-memory.