Thermoplastic Molding of Silk-Curcumin Sustainable Composite Materials with Antibacterial Properties

Silk fibroin (SF) is a natural protein generated from the Bombyx mori silkworm cocoons. It is useful for many different material applications. Versatile aqueous process engineering options can be used to support the morphological and structural modifications of silk materials related to tailored physical, chemical, and biological properties. Conventional solution-based processing methods, while effective, present process control limitations, thus, thermoplastic molding of regenerated SF-based composites was pursued to fabricate dense, functionalized plastics consisting of silk and curcumin. Curcumin, the active compound in turmeric (Curcuma longa) was incorporated into SF during the high-temperature processing, with the objective to investigate composite thermoplastics with enhanced biological properties from the curcumin due to the protective role of silk during processing. The results showed that a significantly higher amount of curcumin (∼25-fold) could be added into thermoplastic molded silk materials compared with the solution route, attributed to the hydrophobicity and low solubility of curcumin in solution-based routes. The curcumin-incorporated silk thermoplastics provided stability in acidic environments like the human gut, and slow curcumin (∼2% over 8 days) release from the materials. The protective silk-curcumin materials supported improved cytocompatibility with immortalized human colorectal adenocarcinoma (Caco-2) cells at high doses. The intestinal epithelial barrier integrity based on zonula occluden 1 (ZO-1) testing showed that the higher amount of curcumin in the thermoplastic molded silk had no negative effects on the intestinal barrier. The functionalized silk-based plastics also displayed microwave stability and antibacterial efficacy against both Gram-positive S. aureus and Gram-negative E. coli. These silk-based sustainable plastics, functionalized with curcumin, offer potential utility for a range of consumer and medical devices.