Designing mechanically robust one-component nanocomposites via hyperbranched cellulose nanofibril grafted vegetable oil polymers

Achieving effective interfacial compatibility between hydrophilic cellulose nanofibrils (CNFs) and hydrophobic vegetable oil polymers (VOPs) remained a significant challenge. To address this issue, we developed a one-component nanocomposite (OCN) based on hyperbranched CNF-grafted VOPs. Rigid precursor initiator poly (vinylbenzyl chloride) (PVBC) was first grafted onto the CNF surface via phase-transfer catalysis, forming a branched macroinitiator (CNF-g-PVBC) with chlorine contents ranging from 4.4 to 9.1 wt%. Subsequently, vegetable oil based monomers (lauryl methacrylate, LMA) were directly grafted onto CNF-g-PVBC through sacrificing initiator-free surface-initiated atom transfer radical polymerization (SI-ATRP). Finally, a hyperbranched CNF-based one-component nanocomposite (OCN-CVOP) was successfully prepared. Nanoscale infrared spectroscopy and microscopy confirmed the highly uniform morphology of the OCN-CVOP films, highlighting the superior dispersion of CNFs within the VOP matrix. Notably, compared to pure VOPs, OCN-CVOP exhibited remarkably low glass transition temperature (∼−15 °C) and reduced viscosity, which was attributed to the hyperbranched architecture. Even at LMA contents as high as ∼70 wt%, OCN-CVOP demonstrated excellent mechanical performance, achieving a tensile strength of 3.6 ± 0.2 MPa and a toughness of 21.5 ± 2.9 MJ/m³. This innovative design successfully addressed the mechanical limitations of conventional VOPs, offering a sustainable approach for developing environmentally friendly, high-performance VOP materials with diverse application potential.