Engineering the interfacial interactions of lignocellulosic building blocks is the key to designing biobased and biodegradable materials. The inherent surface hydroxyl groups in cellulosic materials limit their combination with hydrophobic polymeric systems. To introduce attractive interactions between cellulose and hydrophobic materials, an adjacent interfacial mediator between them is essential. Recently, converting of crude lignin into colloidal lignin nanoparticles (CLPs) has generated vast attraction in the materials community due to overcoming the hurdles commonly posed by lignin’s complex structural heterogeneity. Apart from the CLPs' potential applications in coating, adhesive and cosmetic fields, their excellent performance as an emulsion stabilizer can be innovatively used as an interfacial compatibilizer for developing sustainable materials. The amphiphilic characteristic of CLPs and their active surface sites promote the interfacial bonding between hydrophilic nanocellulose and hydrophobic polyesters such as polycaprolactone (PCL), addressing the major bottlenecks in using nanocellulose, including poor compatibility with hydrophobic polymeric matrix and moisture sensitivity. In this work, combining CLPs with cellulose nanofibrils (CNF) enabled the production of stable Pickering emulsion of PCL with small droplet sizes. After drying the emulsion, nanocomposites with an even distribution of components were achieved. The free-standing nanocomposite films exhibited unprecedented mechanical properties in both dry and wet states due to the favorable intercomponent interactions. These interactions were studied using quartz crystal microbalance with dissipation monitoring (QCM-D) to understand the interactions between CLPs and PCL and between CLPs and CNF. Furthermore, the inclusion of CLPs induced excellent protection against UV and oxidation properties in the developed nanocomposite films, proposing packaging applications for the developed nanocomposite films. Our strategy offers a facile route to design multifunctional cellulose-based nanocomposites using only biodegradable polymers and lignocellulosic nanoparticles without any chemical modifications.

Lignin nanoparticles as an interfacial compatibilizer between nanocellulose and biodegradable polyesters

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