Leaching-resistant carrageenan-based colorimetric oxygen indicator films for intelligent food packaging

Visual oxygen indicators can give information on the quality and safety of packaged food in an economic and simple manner by changing color based on the amount of oxygen in the packaging, which is related to food spoilage. In particular, ultraviolet (UV)-activated oxygen indicators have the advantages of in-pack activation and irreversibility; however, these dye-based oxygen indicator films suffer from dye leaching upon contact with water. In this work, we introduce carrageenans, which are natural sulfated polysaccharides, to develop UV-activated colorimetric oxygen indicator films that are resistant to dye leakage. Carrageenan-based indicator films were fabricated using redox dyes [methylene blue (MB), azure A, and thionine], a sacrificial electron donor (glycerol), an UV-absorbing photocatalyst (TiO2), and an encapsulation polymer (carrageenan). They showed even lower dye leakage in water than conventional oxygen indicator films, owing to the electrostatic interaction of anionic carrageenan with cationic dyes. The MB/TiO2/glycerol/carrageenan oxygen indicator film was successfully bleached upon UV irradiation, and it regained color very rapidly in the presence of oxygen compared to the other waterproof oxygen indicator films.