Development and Characterization of pH-Sensitive Starch/Pectin/DES Films with Purple Cabbage Anthocyanins for Food Spoilage Detection

Luqman Hafezee Nordin; Nursyfiqah Haifa Mohd Salleh; Rizana Yusof

doi:10.56532/mjsat.v6iS1.793

Authors

Luqman Hafezee Nordin Faculty of Applied Sciences, Universiti Teknologi MARA Perlis Branch, Arau Campus, 02600 Arau, Perlis, Malaysia https://orcid.org/0009-0005-0707-4891
Nursyfiqah Haifa Mohd Salleh Faculty of Applied Sciences, Universiti Teknologi MARA Perlis Branch, Arau Campus, 02600 Arau, Perlis, Malaysia
Rizana Yusof Faculty of Applied Sciences, Universiti Teknologi MARA Perlis Branch, Arau Campus, 02600 Arau, Perlis, Malaysia https://orcid.org/0000-0001-7080-9655

DOI:

https://doi.org/10.56532/mjsat.v6iS1.793

Keywords:

Bioplastic, Anthocyanin, Deep Eutectic Solvent, pH indicator, Food Spoilage

Abstract

Innovations in food packaging are increasingly employing smart indicators to boost safety, monitor quality, and minimize waste. However, most of synthetic dyes in indicator systems can leach harmful substances into food. This study developed a natural, biodegradable pH-indicator film using starch-pectin matrix plasticized with a deep eutectic solvent (DES) and functionalized with anthocyanin extract from purple cabbage. The films were formulated with varying anthocyanin concentrations (3%, 6%, and 9%) and evaluated for mechanical properties, water vapor transmission rate (WVTR) and sensitivity to pH and ammonia vapor. FTIR analysis confirmed molecular interactions between the biopolymer matrix, DES and anthocyanins. Increasing anthocyanin concentration to 9% enhanced film flexibility (20.66 ± 3.19%) and increased WVTR (86.22 g/m²·day), but produced darker hues that reduced the visibility of color changes. In contrast, the film with 3% anthocyanin (S/P/DES/3A) exhibited clearly color transitions from bright pink to bright green at high pH level (pH 10). It also had the lowest WVTR (78.11 g/m²·day) and was flexible enough. Furthermore, this film effectively detected ammonia vapor, a crucial spoilage marker; via a visible shift to dark green. These results suggest that S/P/DES/3A is the most effective formulation and offers a promising natural alternative for real-time food spoilage detection.

References

Chandra, D. K., Kumar, A., & Mahapatra, C. (2024). Ecofriendly bioplastics from biowaste: Antimicrobial and functional enhancements for sustainable packaging. European Polymer Journal, 113557. doi: https://doi.org/10.1016/j.eurpolymj.2024.113557

Poudel, R., Dutta, N., & Karak, N. (2023). A mechanically robust biodegradable bioplastic of citric acid modified plasticized yam starch with anthocyanin as a fish spoilage auto-detecting smart film. International journal of biological macromolecules, 242, 125020.. doi: https://doi.org/10.1016/j.ijbiomac.2023.125020

Xiao, Z., Han, L., Gu, M., Zhu, Y., Zhang, Y., Li, Z., Xie, T., & Lu, F. (2023). Performance comparison of anthocyanin-based smart indicator films. Food Packaging and Shelf Life, 40, 101187. doi: https://doi.org/10.1016/j.fpsl.2023.101187

Noiwan, D., Suppakul, P., & Rachtanapun, P. (2022). Preparation of methylcellulose film-based CO2 indicator for monitoring the ripeness quality of mango fruit cv. Nam Dok Mai Si Thong. Polymers, 14(17), 3616. doi: https://doi.org/10.3390/polym14173616

Sharma, K., Pandit, S., Mathuriya, A. S., Gupta, P. K., Pant, K., & Jadhav, D. A. (2022). Microbial electrochemical treatment of methyl red dye degradation using co-culture method. Water, 15(1), 56. doi: https://doi.org/10.3390/w15010056

Xiong, G., Zhou, X., Zhang, C., & Xu, X. (2024). A comprehensive review of intelligent packaging materials based on biopolymers: Role of anthocyanins, type and properties of materials, and their application in monitoring meat freshness. International Journal of Biological Macromolecules, 137462. doi: https://doi.org/10.1016/j.ijbiomac.2024.137462

Gamarra-Castillo, O., Hernández-Carrión, M., & del Pilar Sánchez-Camargo, A. (2025). Revalorization of purple passion fruit peel: Compositional analysis, anthocyanin microwave-assisted extraction, and beverage application Future Foods, 11, 100536. doi: https://doi.org/10.1016/j.fufo.2024.100536

Faisal, M., Bevilacqua, M., Bro, R., Bordallo, H. N., Kirkensgaard, J. J. K., Hebelstrup, K. H., and Blennow, A. (2023). Colorimetric pH indicators based on well-defined amylose and amylopectin matrices enriched with anthocyanins from red cabbage. International Journal of Biological Macromolecules, 250. doi: https://doi.org/10.1016/j.ijbiomac.2023.126250

Smith, E. L., Abbott, A. P., and Ryder, K. S. (2014). Deep Eutectic Solvents (DESs) and Their Applications. In Chemical Reviews (Vol. 114, Issue 21, pp. 11060–11082). American Chemical Society. doi: https://doi.org/10.1021/cr300162p

Rolińska, K., Jakubowska, E., Żmieńko, M., & Łęczycka-Wilk, K. (2024). Choline chloride-based deep eutectic solvents as plasticizer and active agent in chitosan films. Food Chemistry, 444, 138375. doi: https://doi.org/10.1016/j.foodchem.2024.138375

Hikmawanti, N. P. E., Ramadon, D., Jantan, I., and Mun'im, A. (2021). Natural Deep Eutectic Solvents (NADES): Phytochemical Extraction Performance Enhancer for Pharmaceutical and Nutraceutical Product Development. Plants, 10(10), 2091. doi: https://doi.org/10.3390/plants10102091

Kurek, M. A., Custodio-Mendoza, J. A., Aktaş, H., and Pokorski, P. (2024). Exploring deep eutectic solvent extraction's impact on anthocyanin degradation kinetics in various conditions. LWT, 198. doi: https://doi.org/10.1016/j.lwt.2024.115994

Thakur, R., Gupta, V., Ghosh, T., and Das, A. B. (2022). Effect of anthocyanin-natural deep eutectic solvent (lactic acid/fructose) on mechanical, thermal, barrier, and pH-sensitive properties of polyvinyl alcohol based edible films. Food Packaging and Shelf Life, 33. doi: https://doi.org/10.1016/j.fpsl.2022.100914

Thakur, D., Kumar, Y., Sharanagat, V. S., Srivastava, T., & Saxena, D. (2023). Development of pH-sensitive films based on buckwheat starch, critic acid and rose petal extract for active food packaging. Sustainable Chemistry and Pharmacy, 36, 101236 doi: https://doi.org/10.1016/j.scp.2023.101236

Bouftou, A., Aghmih, K., Belfadil, D., Lakhdar, F., Gmouh, S., & Majid, S. (2025). Intelligent and active films with thymol and red cabbage anthocyanin for advanced fish packaging. Food Science and Biotechnology, 34(2), 337-348. doi: https://doi.org/10.1007/s10068-024-01662-5

Zhou, H., Guan, Y., Yan, X., Pan, Z., Xu, J., Dai, L., Zhang, M., & Si, C. (2023). All-lignocellulose-based hard bioplastic. Industrial Crops and Products, 193, 116164. doi: https://doi.org/10.1016/j.indcrop.2022.116164

do Nascimento, R. A., Uchida, D. T., Balbinot, R. B., Nakamura, C. V., Uesu, N. Y., Reis, A. V., & Bruschi, M. L. (2025). Effect of glycerol diglycidyl ether crosslinker on pectin-starch blended pharmaceutical films. International journal of biological macromolecules, 307, 142257. doi: https://doi.org/10.1016/j.ijbiomac.2025.142257

Zhou, H., Guan, Y., Yan, X., Pan, Z., Xu, J., Dai, L., Zhang, M., & Si, C. (2023). All-lignocellulose-based hard bioplastic. Industrial Crops and Products, 193, 116164 doi: https://doi.org/10.1016/j.indcrop.2022.116164

Bao, Y., Cui, H., Tian, J., Ding, Y., Tian, Q., Zhang, W., Wang, M., Zang, Z., Sun, X., & Li, D. (2022). Novel pH sensitivity and colorimetry-enhanced anthocyanin indicator films by chondroitin sulfate co-pigmentation for shrimp freshness monitoring. Food Control, 131, 108441. doi: https://doi.org/10.1016/j.foodcont.2021.108441

Sun, L., Han, J., Tang, C., Wu, J., Fang, S., Li, Y., Mao, Y., Wang, L., & Wang, Y. (2022). Choline chloride-based deep eutectic solvent system as a pretreatment for microcrystalline cellulose. Cellulose, 29(15), 8133-8150. doi: https://doi.org/10.1007/s10570-022-04771-8

Matchim Kamdem, M. C., Tamafo Fouegue, A. D., & Lai, N. (2023). A comprehensive study on DES pretreatment application to microalgae for enhanced lipid recovery suitable for biodiesel production: Combined experimental and theoretical investigations. Energies, 16(9), 3806. doi: https://doi.org/10.3390/en16093806

Maylinda, E. V., Rinadi, A., Putri, E. A., Fadillah, G., & Wayuningsih, S. (2019). Color Stability of Anthocyanins Copigmentation from Red Rice (Oryza sativa L.) Bran by Spectrophotometry UV-Vis. IOP Conference Series: Materials Science and Engineering, 578(1). doi: https://doi.org/10.1088/1757-899x/578/1/012001

Zacheski, J. B. A., Rojas, C. E. B., Gerhardt, R., Cappellari, N. P., De Farias, B. S., Ribeiro, A. C., Cadaval, T. R. S., Junior, & De Almeida Pinto, L. A. (2025). Chitosan-based films enriched with anthocyanin compounds for potential use as food packaging. International Journal of Biological Macromolecules, 317, 144867. doi: https://doi.org/10.1016/j.ijbiomac.2025.144867

Erna, K. H., Felicia, W. X. L., Vonnie, J. M., Rovina, K., Yin, K. W., & Nur'Aqilah, M. N. (2022). Synthesis and physicochemical characterization of polymer film-based anthocyanin and starch. Biosensors, 12(4), 211. doi: https://doi.org/10.3390/bios12040211

Hasan, M., Tasya, G., Khaldun, I., Rusman, R., & Hasanah, U. (2025). Eco-friendly bio-nanocomposite films for sustainable packaging. Journal of Ecological Engineering, 26(4), 301-312. doi: https://doi.org/10.12911/22998993/200335

Li, Y., Xie, L., Jiang, X., Cai, G., Zhu, G., Zheng, Z., & Liu, F. (2023). Effect of anthocyanins on mechanical and physicochemical properties of wheat dough. Journal of Cereal Science, 110, 103652. doi: https://doi.org/10.1016/j.jcs.2023.103652

Halász, K., Kóczán, Z. & Joóbné Preklet, E. pH-dependent color response of cellulose-based time-temperature indicators impregnated with red cabbage extract. Food Measure 17, 2555–2565 (2023). doi: https://doi.org/10.1007/s11694-023-01805-y

Qin, Y., Wang, Y., Tang, Z., Chen, K., Wang, Z., Cheng, G., Chi, H., & Soteyome, T. (2024). A pH-sensitive film based on chitosan/gelatin and anthocyanin from Zingiber striolatum Diels for monitoring fish freshness. Food Chemistry: X, 23, 101639. doi: https://doi.org/10.1016/j.fochx.2024.101639

Wu, K., Zhu, D., Zeng, Y., Cheng, J., Wang, R., Peng, B., Chen, K., Deng, P., Jiang, F., & Zhao, X. (2024). Impact of anthocyanin extract sources on the physical properties and pH sensitivity of konjac glucomannan/zein composite film. Food and Bioprocess Technology, 17(11), 3926-3943. doi: https://doi.org/10.1007/s11947-024-03358-4

Ren, M., Wang, N., Lu, Y., & Wang, C. (2025). Preparation and Characterization of Antioxidative and pH-Sensitive Films Based on κ-Carrageenan/Carboxymethyl Cellulose Blended with Purple Cabbage Anthocyanin for Monitoring Hairtail Freshness. Foods, 14(4), 694. doi: https://doi.org/10.3390/foods14040694