Electrostatically Complexed Natural Polysaccharides as Aqueous Barrier Coatings for Sustainable and Recyclable Fiber-Based Packaging.

Driven by the ever-growing awareness of sustainability and circular economy, renewable, biodegradable, and recyclable fiber-based packaging materials are emerging as alternatives to fossil-derived, nonbiodegradable single-use plastics for the packaging industry. However, without functional barrier coatings, the water/moisture vulnerability and high permeability of fiber-based packaging significantly restrain its broader application as primary packaging for food, beverages, and drugs. Herein, we develop waterborne complex dispersion barrier coatings consisting of natural, biodegradable polysaccharides (i.e., chitosan and carboxymethyl cellulose) through a scalable, one-pot mechanochemical pathway. By tailoring the electrostatic complexation, the key element to form a highly crosslinked and interpenetrated polymer network structure, we formulate complex dispersion barrier coatings with excellent film-forming property and adaptable solid-viscosity profiles suitable for paperboard and molded pulp substrates. Our complex dispersions enable the formation of a uniform, defect-free, and integrated coating layer, leading to a remarkable oil and grease barrier and efficient water/moisture sensitivity reduction while still exhibiting excellent recyclability profile of the resulting fiber-based substrates. This natural, biorenewable, and repulpable barrier coating is a promising candidate to serve as a sustainable option for fiber-based packaging intended for the food and food service packaging industry.