Ethylene-vinyl Alcohol Copolymer–Montmorillonite Multilayer Barrier Film Coated with Mulberry Anthocyanin for Freshness Monitoring

Colorimetric films incorporated with anthocyanins as an indicator for freshness monitoring have aroused growing interest recently. However, the application of the films is limited by the easily oxidizable nature of anthocyanins. In this work, we developed a novel colorimetric film with a barrier by coating mulberry anthocyanin (MBA) on the internal side of an ethylene-vinyl alcohol copolymer-montmorillonite (EVOH-MMT) multilayer film. A facile layer-by-layer (LBL) assembly was employed under a parallel electric field to build the EVOH-MMT multilayer structure, in which the exfoliated MMT nanosheets were well-oriented and assembled on the EVOH matrix to form a tightly stacked layer between two EVOH layers. The interlayer of MMT significantly enhanced the barrier and mechanical properties of the films (below 40 layers). The interactions between EVOH and MMT and between EVOH and MBA were confirmed to be intermolecular hydrogen bonds. The colorimetric response of (EVOH-MMT)40-MBA3 to volatile ammonia and pH was sensitive, and the color change could be easily distinguished by the naked eye. The successful application of (EVOH-MMT)40-MBA3 to shrimp-freshness monitoring confirms its high potential for the freshness monitoring of packaged food.