Enhancing performance of in-situ synthesized biocompatible shape memory polyurethane acrylate by cellulose...

This study presents the development of biocompatible and biodegradable nanocomposites utilizing renewable cellulose nanocrystals (CNCs) in polycaprolactone (PCL)-based polyurethane acrylates (PUA) through in situ polymerization. First, CNCs were derived from cotton linter via acid hydrolysis; then functionalized with 3-methacryloxypropyltrimethoxysilane to produce silane-modified CNCs (S-CNCs). CNCs offered uniform dispersion in PUA up to 2 wt% loading, resulting in significant property enhancements, including ∼60 % increase in tensile strength and ∼25 % increase in Young's modulus. Despite the chemical interaction of S-CNCs with PUA, they tended to agglomerate beyond 0.5 wt% loading due to the promotion of chemical interactions between S-CNC particles at higher concentrations. Despite this, comparable improvements (e.g. ∼50 % in tensile strength and ∼25 % in Young's modulus) were observed at just 0.5 wt% S-CNC loading. Both neat PUA and PUA nanocomposites demonstrated exceptional shape memory properties, with shape fixity exceeding 95 % and shape recovery approaching 100 %. However, S-CNCs also halved the shape recovery time compared to neat PUA, a critical advancement for time-sensitive applications. Meanwhile, the biocompatibility of PUA was largely preserved in the presence of the nanoparticles, particularly for S-CNC.