Cross-linked poly(ester urethane)/starch composite films with high starch content as sustainable food-packaging materials: Influence of cross-link density

This study focused on the development of cross-linked poly(ester urethane)/starch (PEUST) composites containing 50 wt% starch content for food-packaging materials. The NCO-terminated poly(caprolactone-urethane) prepolymer (PCUP) was first synthesized through bulk condensation. Then, low-moisture starch (0.21 wt%) and PCUP-based PEUST films were fabricated through an intensive extrusion process, followed by thermo-compression molding. The chemical structure of PCUP and PEUST was confirmed using Fourier transform infrared spectroscopy. Moreover, a comprehensive evaluation was conducted to assess the influence of cross-link density on the physicochemical properties of the composite films. The results showed that an increase in the cross-link density within the composites improved component compatibility and tensile strength but reduced crystallinity, water sensitivity, hydrolytic degradability, and water vapor permeability (WVP) of the films. In addition, the cytotoxicity tests were conducted to evaluate the safety of the composite films, and the high cell viability demonstrated non-toxicity for food application. The PEUST-II films with moderate cross-link density exhibited a suitable degradation rate (27.7 % weight loss at degradation for 140 d), optimal tensile properties (tensile strength at break: 12.4 MPa; elongation at break: 352 %), and low WVP (68.4 g/(m²⋅24h) at 30 % relative humidity). These characteristics make them highly promising as fresh-keeping food packaging.