| Summary: | Calcium alginate based controlled release films with moderate mechanical properties were fabricated in this paper. The diffusion mechanism of these films contacting food simulating solvent (FSS) was explored in some detail. With the increase of glycerol content, the diffusion coefficient (<i>D</i>) values of cinnamon essential oils (CEOs) diffusing to ethanol first increased slowly (0.3–0.6 mL), then vigorously (0.6–0.9 mL), and then mildly (0.9–1.2 mL). The <i>D</i> values of the CEOs diffused to water are all in the order of magnitude of 10<sup>−10</sup> cm<sup>2</sup>/s. The <i>D</i> values of CEOs diffused from films EG3 and EGC1 to aqueous ethanol altered enormously at a small moisture percentage (<i>w</i> = 0.3), then continuously varied vigorously, and at last altered mildly in the range of <i>w</i> = 0.3–1. All the results above indicate that, considering the FSS, the diffusion ability of molecules is jointly determined by the size and distribution of free volume in the system (polymer + diffusive substance + solvents), the intermolecular interaction, and the partition coefficient of the solvents. In addition, several pairs of <i>D</i> values, such as <i>D</i><sub>EG</sub> and <i>D</i><sub>GA</sub>, are very close to each other, indicating that different kinds of interactions between different groups may have the same effect on the diffusion ability of molecules. The correlation between <i>D</i><sub>1</sub> and <i>D</i><sub>2</sub> indicates that polymeric emulsifier chains also exist in the polymer-rich layer. All the findings and analysis could provide the theoretical basis and data support for further molecular dynamic simulation and could guide the design of controlled release food packaging for food protection.
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