Carboxyl-modified nanocellulose (cNC) enhances the stability of cNC/pullulan bio-nanocomposite hard capsule against moisture variation.

The quality of polysaccharide-based films and hard capsules is often affected by changes in relative humidity, manifesting as unstable water content, and changes in mechanical strength that make them brittle or soft. Herein, carboxyl-modified nanocellulose (cNC) was prepared and used as a new component to successfully improve the moisture resistance of cNC/pullulan/high-acyl gellan bio-nanocomposite hard capsules (NCPGs). Homogenously dispersed cNC in the pullulan/high-acyl gellan matrix could render the formation of more hydrogen bonds that provided additional water-binding sites and limited the free movement of pullulan and high-acyl gellan molecular chains within NCPGs. This contributed to a decreased amount of pooling adsorption water and an increased amount of Langmuir adsorption water in NCPGs, as compared to pullulan/high-acyl gellan hard capsules (PGs) without cNC. Therefore, the equilibrium moisture content (EMC) values of NCPGs decreased at 83 % relative humidity and increased at 23 % relative humidity compared to those of PGs. Together with enhanced mechanical and barrier properties, NCPGs effectively protected encapsulated amoxicillin and probiotic powder from changes in the outside humidity. Additionally, NCPGs exhibited faster drug release. This study presents a new mechanism and strategy for fabricating films and hard capsules with enhanced stability against moisture variation.