Brittleness has hindered commercialization of cellulose nanofibril (CNF) films. The use of synthetic polymers and plasticizers is a known detour that impairs biodegradability and carbon footprint of the product. Herein, we utilize a variety of softwood Kraft lignin morphologies to obtain strong and ductile CNF nanocomposite films. An optimum 10 wt % content of colloidal lignin particles (CLPs) produced films with nearly double the toughness compared to a CNF film without lignin. CLPs rendered the films waterproof, provided antioxidant activity and UV-shielding with better visible light transmittance than obtained with irregular lignin aggregates. We conclude based on electron microscopy, dynamic water sorption analysis, and tp-DSC that homogeneously distributed CLPs act as ball bearing lubricating and stress transferring agents in the CNF matrix. Overall, our results open new avenues for the utilization of lignin nanoparticles in biopolymer composites equipped with versatile functionalities for applications in food packaging, water purification, and biomedicine.

The mechanism of lignin nanoprecipitation and subsequent self-assembly was elucidated by studying generation of lignin nanoparticles (LNPs) from aqueous ethanol. LNP formation was found to follow a kinetically controlled nucleation–growth mechanism in which large lignin molecules formed the initial critical nuclei. Using this information, we demonstrate entrapment of budesonide in LNPs and subsequent pH-triggered and surfactant-responsive release of this synthetic anti-inflammatory corticosteroid. Overall, our results not only provide a promising intestinal delivery system for budesonide but also deliver fundamental mechanistic understanding for the entrapment of actives in LNPs with controlled size and release properties.

A critical review on spherical lignin nanoparticles highlighting aspects associated to their shape, performance in applications, sustainability, stability and degradation.