Abstract
Novel pH and ammonia-sensitive intelligent film was fabricated with carboxymethyl cellulose (CMC) as film-forming substrate, gum Arabic (GA) as enhancer, and anthocyanins from Cinnamomum camphora fruit peel waste (ANC.P) as indicator, antioxidant, and antimicrobial. The incorporation of ANC.P on CMC-GA (CG-ANC.P) film significantly increased the mechanical property, physical properties (swelling degree, moisture content, solubility, vapor barrier properties, and oil permeability resistance), color, opacity, morphological characteristics, melting, and bioactivities (antioxidant, antibacterial, biodegradable, and pH/ammonia-sensitive manners) without significant changes in the film thickness. Computational molecular imitation analysis suggested an enhancement between ANC.P, CMC, and GA through hydrogen bonds and forces of van der Waals. Notably, the smart packaging film was tested to monitor soybean oil freshness during storage at 50 °C for 28 days. Moreover, the shelf-life characteristics proved the ability of films to retard oil oxidation. Additionally, the sensory characteristics emphasize higher scores of colors, odor, and overall acceptability with the increased concentration of anthocyanin. When applied in monitoring beef freshness at 4 °C, the CG-ANC.P film indicated sensitively with vision recognizable color changes from original pink to pink-yellow and finally to grayish-yellow, which highly correlated with the deterioration indexes of the total color difference, pH value, and total viable count of beef.
Graphical Abstract
Similar content being viewed by others
Data Availability
The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.
References
Abdillah, A. A., Lin, H.-H., & Charles, A. L. (2022). Development of halochromic indicator film based on arrowroot starch/iota-carrageenan using Kyoho skin extract to monitor shrimp freshness. International Journal of Biological Macromolecules, 211, 316–327. https://doi.org/10.1016/j.ijbiomac.2022.05.076
Abdin, M., El-Beltagy, A., El-sayed, M., & Naeem, M. A. (2021a). Production and characterization of sodium alginate/gum Arabic based films enriched with Syzygium cumini seeds extracts for food application. Journal of Polymers and the Environment, 30, 1615–1626. https://doi.org/10.1007/s10924-021-02306-z
Abdin, M., Salama, M. A., Gawad, R., Fathi, M. A., & Alnadari, F. (2021b). Two-steps of gelation system enhanced the stability of Syzygium cumini anthocyanins by encapsulation with sodium alginate, maltodextrin, chitosan and gum arabic. Journal of Polymers and the Environment, 29(11), 3679–3692. https://doi.org/10.1007/s10924-021-02140-3
Akhtar, H. M. S., Riaz, A., Hamed, Y. S., Abdin, M., Chen, G., Wan, P., & Zeng, X. (2018). Production and characterization of CMC-based antioxidant and antimicrobial films enriched with chickpea hull polysaccharides. International Journal of Biological Macromolecules, 118, 469–477. https://doi.org/10.1016/j.ijbiomac.2018.06.090
Alizadeh-Sani, M., Tavassoli, M., Mohammadian, E., Ehsani, A., Khaniki, G. J., Priyadarshi, R., & Rhim, J.-W. (2021). pH-responsive color indicator films based on methylcellulose/chitosan nanofiber and barberry anthocyanins for real-time monitoring of meat freshness. International Journal of Biological Macromolecules, 166, 741–750. https://doi.org/10.1016/j.ijbiomac.2020.10.231
Alnadari, F., Abdin, M., Ennab, W., Mohedein, A., & Nasiru, M. (2020). Metabolism of anthocyanins and modulation of gut microbiome in inflammatory bowel disease. Journal of Food Chemistry & Nanotechnology, 6(4), 207–217. https://doi.org/10.17756/jfcn.2020-103
Alnadari, F., Al-Dalali, S., Nasiru, M. M., Frimpong, E. B., Hu, Y., Abdalmegeed, D., Dai, Z., Abdulrahman, A.-A., Chen, G., & Zeng, X. (2023). A new natural drying method for food packaging and preservation using biopolymer-based dehydration film. Food Chemistry, 404, 134689. https://doi.org/10.1016/j.foodchem.2022.134689
Alnadari, F., Bassey, A. P., Abdin, M., Salama, M. A., Nasiru, M. M., Dai, Z., Hu, Y., Zeng, X. J. J., & o. P., & Environment, t. (2022). Development of hybrid film based on carboxymethyl chitosan-gum Arabic incorporated citric acid and polyphenols from Cinnamomum camphora seeds for active food packaging. Journal of Polymers and the Environment, 30, 3582–3597. https://doi.org/10.1007/s10924-022-02453-x
Atakoohi, S. E., Naeiji, P., Peyvandi, K., & Sanatgar, S. M. (2021). The experimental study and molecular dynamic simulation of THF hydrate growth kinetics in the presence of Arabic and Guar gum: new approaches in promotion of THF hydrate formation. Journal of Molecular Liquids, 325, 115249. https://doi.org/10.1016/j.molliq.2020.115249
Bao, Y., Cui, H., Tian, J., Ding, Y., Tian, Q., Zhang, W., Wang, M., Zang, Z., Sun, X., & Li, B. (2022). Novel pH sensitivity and colorimetry-enhanced anthocyanin indicator films by chondroitin sulfate co-pigmentation for shrimp freshness monitoring. Food Control, 131, 108441. https://doi.org/10.1016/j.foodcont.2021.108441
Chen, J., Luo, L., Cen, C., Liu, Y., Li, H., & Wang, Y. (2022). The nano antibacterial composite film carboxymethyl chitosan/gelatin/nano ZnO improves the mechanical strength of food packaging. International Journal of Biological Macromolecules, 220, 462–471. https://doi.org/10.1016/j.ijbiomac.2022.08.005
Chen, S., Wu, M., Lu, P., Gao, L., Yan, S., & Wang, S. (2020). Development of pH indicator and antimicrobial cellulose nanofibre packaging film based on purple sweet potato anthocyanin and oregano essential oil. International Journal of Biological Macromolecules, 149, 271–280. https://doi.org/10.1016/j.ijbiomac.2020.01.231
Cheng, M., Yan, X., Cui, Y., Han, M., Wang, X., Wang, J., & Zhang, R. (2022). An eco-friendly film of pH-responsive indicators for smart packaging. Journal of Food Engineering, 321, 110943. https://doi.org/10.1016/j.jfoodeng.2022.110943
Cox, K. D., Covernton, G. A., Davies, H. L., Dower, J. F., Juanes, F., & Dudas, S. E. (2019). Human consumption of microplastics. Environmental Science & Technology, 53(12), 7068–7074. https://doi.org/10.1021/acs.est.9b01517
de Souza, K. C., Correa, L. G., da Silva, T. B. V., Moreira, T. F. M., de Oliveira, A., Sakanaka, L. S., ... & Shirai, M. A. (2020). Soy protein isolate films incorporated with Pinhão (Araucaria angustifolia (Bertol.) Kuntze) extract for potential use as edible oil active packaging. Food and Bioprocess Technology, 13, 998–1008. https://doi.org/10.1007/s11947-020-02454-5
Deshmukh, R. K., Akhila, K., Ramakanth, D., & Gaikwad, K. K. (2022). Guar gum/carboxymethyl cellulose based antioxidant film incorporated with halloysite nanotubes and litchi shell waste extract for active packaging. International Journal of Biological Macromolecules, 201, 1–13. https://doi.org/10.1016/j.ijbiomac.2021.12.198
Dong, W., Su, J., Chen, Y., Xu, D., Cheng, L., Mao, L., Gao, Y., & Yuan, F. (2022). Characterization and antioxidant properties of chitosan film incorporated with modified silica nanoparticles as an active food packaging. Food Chemistry, 373, 131414. https://doi.org/10.1016/j.foodchem.2021.131414
Emir, A. A., Yildiz, E., Aydogdu, Y., & Sumnu, G. (2022). Active films based on Faba bean (Vicia faba L.) flour incorporated with Sumac (Rhus coriaria): Assessment of antioxidant and antimicrobial performances of packaging for shelf life of chicken breast. Food and Bioprocess Technology, 16, 327–341. https://doi.org/10.1007/s11947-022-02940-y
Ezati, P., Khan, A., Rhim, J. W., Roy, S., & Hassan, Z. U. (2022). Saffron: Perspectives and sustainability for active and intelligent food packaging applications. Food and Bioprocess Technology. https://doi.org/10.1007/s11947-022-02949-3
Hanwell, M. D., Curtis, D. E., Lonie, D. C., Vandermeersch, T., Zurek, E., & Hutchison, G. R. (2012). Avogadro: An advanced semantic chemical editor, visualization, and analysis platform. Journal of Cheminformatics, 4, 17. https://doi.org/10.1186/1758-2946-4-17
Hauser, C., Peñaloza, A., Guarda, A., Galotto, M. J., Bruna, J. E., & Rodríguez, F. J. (2016). Development of an active packaging film based on a methylcellulose coating containing murta (Ugni molinae Turcz) leaf extract. Food and Bioprocess Technology, 9, 298–307. https://doi.org/10.1007/s11947-015-1623-8
Huang, G.-Q., Liu, L.-N., Han, X.-N., & Xiao, J.-X. (2017). Intestine-targeted delivery potency of the O-carboxymethyl chitosan-gum Arabic coacervate: Effects of coacervation acidity and possible mechanism. Materials Science and Engineering: C, 79, 423–429. https://doi.org/10.1016/j.msec.2017.05.074
Humphrey, W., Dalke, A., & Schulten, K. (1996). VMD: Visual molecular dynamics. Journal of Molecular Graphics, 14(1), 33–38. https://doi.org/10.1016/0263-7855(96)00018-5
Kang, S., Xiao, Y., Guo, X., Huang, A., & Xu, H. (2021). Development of gum arabic-based nanocomposite films reinforced with cellulose nanocrystals for strawberry preservation. Food Chemistry, 350, 129199. https://doi.org/10.1016/j.foodchem.2021.129199
Khanjanzadeh, H., Park, B.-D., & Pirayesh, H. (2022). Intelligent pH-and ammonia-sensitive indicator films using neutral red immobilized onto cellulose nanofibrils. Carbohydrate Polymers, 296, 119910. https://doi.org/10.1016/j.carbpol.2022.119910
Kumar, H., Ahuja, A., Kadam, A. A., Rastogi, V. K., & Negi, Y. S. (2022). Antioxidant film based on chitosan and tulsi essential oil for food packaging. Food and Bioprocess Technology, 16, 342–355. https://doi.org/10.1007/s11947-022-02938-6
Lefebvre, C., Rubez, G., Khartabil, H., Boisson, J.-C., Contreras-García, J., & Hénon, E. (2017). Accurately extracting the signature of intermolecular interactions present in the NCI plot of the reduced density gradient versus electron density. Physical Chemistry Chemical Physics, 19(27), 17928–17936. https://doi.org/10.1039/C7CP02110K
Li, C., Zhu, W., Xue, H., Chen, Z., Chen, Y., & Wang, X. (2015). Physical and structural properties of peanut protein isolate-gum Arabic films prepared by various glycation time. Food Hydrocolloids, 43, 322–328. https://doi.org/10.1016/j.foodhyd.2014.06.003
Liu, C.-M., Perng, M.-H., & Chen, C.-Y. (2018). Antioxidant activities of crude extracts from peel and seed of Cinnamomum camphora. Biomedical Research 29, 2854–2858. https://doi.org/10.4066/biomedicalresearch.29-18-789
Lu, T., & Chen, F. (2012). Multiwfn: A multifunctional wavefunction analyzer. Journal of Computational Chemistry, 33(5), 580–592. https://doi.org/10.1002/jcc.22885
Lu, T. M. (2019). Accessed 20 March. program, Version 1.8. http://www.keinsci.com/research/molclus.html
Ma, Q., & Wang, L. (2016). Preparation of a visual pH-sensing film based on tara gum incorporating cellulose and extracts from grape skins. Sensors and Actuators b: Chemical, 235, 401–407. https://doi.org/10.1016/j.snb.2016.05.107
Maroufi, L. Y., Ghorbani, M., & Tabibiazar, M. (2020). A gelatin-based film reinforced by covalent interaction with oxidized guar gum containing green tea extract as an active food packaging system. Food and Bioprocess Technology, 13, 1633–1644. https://doi.org/10.1007/s11947-020-02509-7
Maroufi, L. Y., Shahabi, N., Ghanbarzadeh, M. D., & Ghorbani, M. (2022). Development of antimicrobial active food packaging film based on gelatin/dialdehyde quince seed gum incorporated with apple peel polyphenols. Food and Bioprocess Technology, 15(3), 693–705. https://doi.org/10.1007/s11947-022-02774-8
Neese, F. (2018). Software update: the ORCA program system, version 4.0. Wiley Interdisciplinary Reviews: Computational Molecular Science, 8(1), e1327. https://doi.org/10.1002/wcms.1606
Qin, Y., Liu, Y., Yong, H., Liu, J., Zhang, X., & Liu, J. (2019). Preparation and characterization of active and intelligent packaging films based on cassava starch and anthocyanins from Lycium ruthenicum Murr. International Journal of Biological Macromolecules, 134, 80–90. https://doi.org/10.1016/j.ijbiomac.2019.05.029
Reyes-Avalos, M. C., Minjares-Fuentes, R., Femenia, A., Contreras-Esquivel, J. C., Quintero-Ramos, A., Esparza-Rivera, J. R., & Meza-Velázquez, J. A. (2019). Application of an alginate–chitosan edible film on figs (Ficus carica): Effect on bioactive compounds and antioxidant capacity. Food and Bioprocess Technology, 12, 499–511. https://doi.org/10.1007/s11947-018-2226-y
Riahi, Z., Rhim, J.-W., Bagheri, R., Pircheraghi, G., & Lotfali, E. (2022). Carboxymethyl cellulose-based functional film integrated with chitosan-based carbon quantum dots for active food packaging applications. Progress in Organic Coatings, 166, 106794. https://doi.org/10.1016/j.porgcoat.2022.106794
Riaz, A., Lagnika, C., Luo, H., Dai, Z., Nie, M., Hashim, M. M., Liu, C., Song, J., & Li, D. (2020). Chitosan-based biodegradable active food packaging film containing Chinese chive (Allium tuberosum) root extract for food application. International Journal of Biological Macromolecules, 150, 595–604. https://doi.org/10.1016/j.ijbiomac.2020.02.078
Ribeiro, A. M., Estevinho, B. N., & Rocha, F. (2020). Edible films prepared with different biopolymers, containing polyphenols extracted from elderberry (Sambucus Nigra L.), to protect food products and to improve food functionality. Food and Bioprocess Technology, 13, 1742–1754. https://doi.org/10.1007/s11947-020-02516-8
Roy, S., & Rhim, J.-W. (2020). Carboxymethyl cellulose-based antioxidant and antimicrobial active packaging film incorporated with curcumin and zinc oxide. International Journal of Biological Macromolecules, 148, 666–676. https://doi.org/10.1016/j.ijbiomac.2020.01.204
Sadeghizadeh-Yazdi, J., Habibi, M., Kamali, A. A., & Banaei, M. (2019). Application of edible and biodegradable starch-based films in food packaging: a systematic review and meta-analysis. Current Research in Nutrition and Food Science, 7(3), 624–637. https://doi.org/10.12944/CRNFSJ.7.3.03
Salama, M. A., El Harkaoui, S., Nounah, I., Sakr, H., Abdin, M., Owon, M., Ibrahim, A., Charrouf, Z., & Matthäus, B. (2020). Oxidative stability of Opuntia ficus-indica seeds oil blending with Moringa oleifera seeds oil. Oilseeds & Fats Crops and Lipids, 27, 53. https://doi.org/10.1051/ocl/2020061
Singh, M. R., Gupta, P., & Gupta, K. (2019). The litchi (Litchi Chinensis) peels extract as a potential green inhibitor in prevention of corrosion of mild steel in 0.5 M H2SO4 solution. Arabian Journal of Chemistry, 12(7), 1035–1041. https://doi.org/10.1016/j.arabjc.2015.01.002
Spackman, M. A., & Jayatilaka, D. (2009). Hirshfeld surface analysis. CrystEngComm, 11(1), 19–32. https://doi.org/10.1039/B818330A
Stewart. (2016). MOPAC2016. Stewart Computational Chemistry. Colorado Springs, CO.
Suriyatem, R., Auras, R. A., Rachtanapun, C., & Rachtanapun, P. (2018). Biodegradable rice starch/carboxymethyl chitosan films with added propolis extract for potential use as active food packaging. Polymers, 10(9), 954. https://doi.org/10.3390/polym10090954
Tan, S. L., Jotani, M. M., & Tiekink, E. R. (2019). Utilizing Hirshfeld surface calculations, non-covalent interaction (NCI) plots and the calculation of interaction energies in the analysis of molecular packing. Acta Crystallographica Section e: Crystallographic Communications, 75(3), 308–318. https://doi.org/10.1107/S2056989019001129
Wang, C., Li, M., Zhang, L., Fu, S., & Wang, C. (2017). Extraction of natural dyes from Cinnamomum camphora (L.) presl fruit and their application on wool fabric. Textile Research Journal, 87(20), 2550–2560. https://doi.org/10.1177/0040517516665266
Wang, H., Gong, X., Miao, Y., Guo, X., Liu, C., Fan, Y. Y., Zhang, J., Niu, B., & Li, W. (2019a). Preparation and characterization of multilayer films composed of chitosan, sodium alginate and carboxymethyl chitosan-ZnO nanoparticles. Food Chemistry, 283, 397–403. https://doi.org/10.1016/j.foodchem.2019.01.022
Wang, S., Xia, P., Wang, S., Liang, J., Sun, Y., Yue, P., & Gao, X. (2019b). Packaging films formulated with gelatin and anthocyanins nanocomplexes: Physical properties, antioxidant activity and its application for olive oil protection. Food Hydrocolloids, 96, 617–624. https://doi.org/10.1016/j.foodhyd.2019.06.004
Yang, X., & Boyle, R. A. (2016). Sensory evaluation of oils/fats and oil/fat–based foods. In Oxidative stability and shelf life of foods containing oils and fats, 157–185. https://doi.org/10.1016/B978-1-63067-056-6.00003-3
Yong, H., Wang, X., Bai, R., Miao, Z., Zhang, X., & Liu, J. (2019). Development of antioxidant and intelligent pH-sensing packaging films by incorporating purple-fleshed sweet potato extract into chitosan matrix. Food Hydrocolloids, 90, 216–224. https://doi.org/10.1016/j.foodhyd.2018.12.015
Zhang, P., Zhao, Y., & Shi, Q. (2016). Characterization of a novel edible film based on gum ghatti: Effect of plasticizer type and concentration. Carbohydrate Polymers, 153, 345–355. https://doi.org/10.1016/j.carbpol.2016.07.082
Zhao, L., Pan, F., Mehmood, A., Zhang, H., Rehman, A. U., Li, J., Hao, S., & Wang, C. (2021). Improved color stability of anthocyanins in the presence of ascorbic acid with the combination of rosmarinic acid and xanthan gum. Food Chemistry, 351, 129317. https://doi.org/10.1016/j.foodchem.2021.129317
Funding
This work was supported by a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions and Taif University Researchers Supporting Project Number (TURSP-2020/140).
Author information
Authors and Affiliations
Contributions
Fawze Alnadari: conceptualization, methodology, software, writing an original draft. Sam Al-Dalali: methodology, software, writing an original draft. Fei Pan: methodology, software, validation, data curation. Mohamed Abdin: conceptualization, methodology. Evans Boateng Frimpong: methodology, data curation. Zhuqing Dai: visualization, investigation. Aisha AL-Dherasi: investigation. Xiaoxiong Zeng: supervision, resources, project administration, writing and editing draft.
Corresponding author
Ethics declarations
Conflict of Interest
The authors declare no competing interests.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Alnadari, F., Al-Dalali, S., Pan, F. et al. Physicochemical Characterization, Molecular Modeling, and Applications of Carboxymethyl Chitosan-Based Multifunctional Films Combined with Gum Arabic and Anthocyanins. Food Bioprocess Technol 16, 2984–3002 (2023). https://doi.org/10.1007/s11947-023-03122-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11947-023-03122-0