Electrospraying assisted by pressurized gas as an innovative high-throughput process for the microencapsulation and stabilization of docosahexaenoic acid-enriched fish oil in zein prolamine

[EN] Zein, a prolamine obtained from maize, was employed to encapsulate a fish oil highly enriched with docosahexaenoic acid (DHA) by an innovative process termed electrospraying assisted by pressurized gas (EAPG). This technology combines high electric voltage with pneumatic spray to yield a high-throughput encapsulation process. Semi-spherical zein flowable capsules with mean sizes of 1.4 mu m containing the DHA-enriched fish oil were produced by EAPG from inert ethanol solutions at room conditions, presenting a high encapsulation efficiency. The oxidative stability tests carried out in the zein microcapsules obtained by EAPG showed that the DHA-enriched fish oil was efficiently protected over storage time. Sensory tests were also performed on fortified reconstituted milk with the freshly prepared zein/DHA-enriched fish oil microcapsules, suggesting negligible oxidation effects after 45 days. The results described herein indicate that EAPG is a promising innovative high-throughput electrospraying-based methodology for the encapsulation of bioactives and, therefore, the resultant DHA-enriched fish oil containing microcapsules can be industrially applied for the formulation of fortified foods. Industrial relevance: An innovative process, termed electrospraying assisted by pressurized gas (EAPG), is herein originally presented as a novel encapsulation methodology. This technology is based on the combination of high voltage and pneumatic spray, allowing the formation of microcapsules at room temperature conditions. Thus, EAPG shows a great deal of potential to encapsulate nutraceuticals and other bioactives that are sensitive to thermal degradation and/or oxidation. The resultant bioactive-containing capsules can be, thereafter, applied to develop novel fortified food products.The authors would like to thank the Spanish Ministry of Economy and Competitiveness (MINECO) project AGL2015-63855-C2-1-R and to the H2020 EU project YPACK (reference number 773872) for funding.Busolo, M.; Torres-Giner, S.; Prieto, C.; Lagaron, JM. (2019). Electrospraying assisted by pressurized gas as an innovative high-throughput process for the microencapsulation and stabilization of docosahexaenoic acid-enriched fish oil in zein prolamine. Innovative Food Science & Emerging Technologies. 51:12-19. https://doi.org/10.1016/j.ifset.2018.04.007S121951Aghbashlo, M., Mobli, H., Madadlou, A., & Rafiee, S. (2012). The correlation of wall material composition with flow characteristics and encapsulation behavior of fish oil emulsion. Food Research International, 49(1), 379-388. doi:10.1016/j.foodres.2012.07.031Anwar, S. H., & Kunz, B. (2011). The influence of drying methods on the stabilization of fish oil microcapsules: Comparison of spray granulation, spray drying, and freeze drying. Journal of Food Engineering, 105(2), 367-378. doi:10.1016/j.jfoodeng.2011.02.047Anwar, S. H., Weissbrodt, J., & Kunz, B. (2010). Microencapsulation of Fish Oil by Spray Granulation and Fluid Bed Film Coating. Journal of Food Science, 75(6), E359-E371. doi:10.1111/j.1750-3841.2010.01665.xBakry, A. M., Abbas, S., Ali, B., Majeed, H., Abouelwafa, M. Y., Mousa, A., & Liang, L. (2015). Microencapsulation of Oils: A Comprehensive Review of Benefits, Techniques, and Applications. Comprehensive Reviews in Food Science and Food Safety, 15(1), 143-182. doi:10.1111/1541-4337.12179Busolo, M. A., & Lagaron, J. M. (2012). Oxygen scavenging polyolefin nanocomposite films containing an iron modified kaolinite of interest in active food packaging applications. Innovative Food Science & Emerging Technologies, 16, 211-217. doi:10.1016/j.ifset.2012.06.008Chen, W., Wang, H., Zhang, K., Gao, F., Chen, S., & Li, D. (2016). Physicochemical Properties and Storage Stability of Microencapsulated DHA-Rich Oil with Different Wall Materials. Applied Biochemistry and Biotechnology, 179(7), 1129-1142. doi:10.1007/s12010-016-2054-3Eltayeb, M., Stride, E., Edirisinghe, M., & Harker, A. (2016). Electrosprayed nanoparticle delivery system for controlled release. Materials Science and Engineering: C, 66, 138-146. doi:10.1016/j.msec.2016.04.001Encina, C., Vergara, C., Giménez, B., Oyarzún-Ampuero, F., & Robert, P. (2016). Conventional spray-drying and future trends for the microencapsulation of fish oil. Trends in Food Science & Technology, 56, 46-60. doi:10.1016/j.tifs.2016.07.014Fernandez, A., Torres-Giner, S., & Lagaron, J. M. (2009). Novel route to stabilization of bioactive antioxidants by encapsulation in electrospun fibers of zein prolamine. Food Hydrocolloids, 23(5), 1427-1432. doi:10.1016/j.foodhyd.2008.10.011Filippidi, E., Patel, A. R., Bouwens, E. C. M., Voudouris, P., & Velikov, K. P. (2014). All-Natural Oil-Filled Microcapsules from Water-Insoluble Proteins. Advanced Functional Materials, 24(38), 5962-5968. doi:10.1002/adfm.201400359Ganesan, B., Brothersen, C., & McMahon, D. J. (2013). Fortification of Foods with Omega-3 Polyunsaturated Fatty Acids. Critical Reviews in Food Science and Nutrition, 54(1), 98-114. doi:10.1080/10408398.2011.578221García-Moreno, P. J., Özdemir, N., Stephansen, K., Mateiu, R. V., Echegoyen, Y., Lagaron, J. M., … Jacobsen, C. (2017). Development of carbohydrate-based nano-microstructures loaded with fish oil by using electrohydrodynamic processing. Food Hydrocolloids, 69, 273-285. doi:10.1016/j.foodhyd.2017.02.013García-Moreno, P. J., Stephansen, K., van der Kruijs, J., Guadix, A., Guadix, E. M., Chronakis, I. S., & Jacobsen, C. (2016). Encapsulation of fish oil in nanofibers by emulsion electrospinning: Physical characterization and oxidative stability. Journal of Food Engineering, 183, 39-49. doi:10.1016/j.jfoodeng.2016.03.015Gomez-Estaca, J., Balaguer, M. P., Gavara, R., & Hernandez-Munoz, P. (2012). Formation of zein nanoparticles by electrohydrodynamic atomization: Effect of the main processing variables and suitability for encapsulating the food coloring and active ingredient curcumin. Food Hydrocolloids, 28(1), 82-91. doi:10.1016/j.foodhyd.2011.11.013Heinzelmann, K., Franke, K., Jensen, B., & Haahr, A.-M. (2000). Protection of fish oil from oxidation by microencapsulation using freeze-drying techniques. European Journal of Lipid Science and Technology, 102(2), 114-121. doi:10.1002/(sici)1438-9312(200002)102:23.0.co;2-0Hogan, S. A., O’Riordan, E. D., & O’Sullivan, M. (2003). Microencapsulation and oxidative stability of spray-dried fish oil emulsions. Journal of Microencapsulation, 20(5), 675-688. doi:10.3109/02652040309178355Hong, X., Mahalingam, S., & Edirisinghe, M. (2017). Simultaneous Application of Pressure-Infusion-Gyration to Generate Polymeric Nanofibers. Macromolecular Materials and Engineering, 302(6), 1600564. doi:10.1002/mame.201600564Lopez-Huertas, E. (2010). Health effects of oleic acid and long chain omega-3 fatty acids (EPA and DHA) enriched milks. A review of intervention studies. Pharmacological Research, 61(3), 200-207. doi:10.1016/j.phrs.2009.10.007Moomand, K., & Lim, L.-T. (2014). Oxidative stability of encapsulated fish oil in electrospun zein fibres. Food Research International, 62, 523-532. doi:10.1016/j.foodres.2014.03.054Park, J.-M., Kwon, S.-H., Han, Y.-M., Hahm, K.-B., & Kim, E.-H. (2013). Omega-3 Polyunsaturated Fatty Acids as Potential Chemopreventive Agent for Gastrointestinal Cancer. Journal of Cancer Prevention, 18(3), 201-208. doi:10.15430/jcp.2013.18.3.201Partanen, R., Raula, J., Seppänen, R., Buchert, J., Kauppinen, E., & Forssell, P. (2008). Effect of Relative Humidity on Oxidation of Flaxseed Oil in Spray Dried Whey Protein Emulsions. Journal of Agricultural and Food Chemistry, 56(14), 5717-5722. doi:10.1021/jf8005849Pereira, D., Valentão, P., & Andrade, P. (2014). Nano- and Microdelivery Systems for Marine Bioactive Lipids. Marine Drugs, 12(12), 6014-6027. doi:10.3390/md12126014Prieto, C., & Calvo, L. (2017). The encapsulation of low viscosity omega-3 rich fish oil in polycaprolactone by supercritical fluid extraction of emulsions. The Journal of Supercritical Fluids, 128, 227-234. doi:10.1016/j.supflu.2017.06.003Ruxton, C. H. S., Reed, S. C., Simpson, M. J. A., & Millington, K. J. (2004). The health benefits of omega-3 polyunsaturated fatty acids: a review of the evidence. Journal of Human Nutrition and Dietetics, 17(5), 449-459. doi:10.1111/j.1365-277x.2004.00552.xShams, T., Parhizkar, M., Illangakoon, U. E., Orlu, M., & Edirisinghe, M. (2017). Core/shell microencapsulation of indomethacin/paracetamol by co-axial electrohydrodynamic atomization. Materials & Design, 136, 204-213. doi:10.1016/j.matdes.2017.09.052Shantha, N. C., & Decker, E. A. (1994). Rapid, Sensitive, Iron-Based Spectrophotometric Methods for Determination of Peroxide Values of Food Lipids. Journal of AOAC INTERNATIONAL, 77(2), 421-424. doi:10.1093/jaoac/77.2.421Siriwardhana, N., Kalupahana, N. S., & Moustaid-Moussa, N. (2012). Health Benefits of n-3 Polyunsaturated Fatty Acids. Advances in Food and Nutrition Research, 211-222. doi:10.1016/b978-0-12-416003-3.00013-5Tapia-Hernández, J. A., Torres-Chávez, P. I., Ramírez-Wong, B., Rascón-Chu, A., Plascencia-Jatomea, M., Barreras-Urbina, C. G., … Rodríguez-Félix, F. (2015). Micro- and Nanoparticles by Electrospray: Advances and Applications in Foods. Journal of Agricultural and Food Chemistry, 63(19), 4699-4707. doi:10.1021/acs.jafc.5b01403Tihminlioglu, F., Atik, İ. D., & Özen, B. (2010). Water vapor and oxygen-barrier performance of corn–zein coated polypropylene films. Journal of Food Engineering, 96(3), 342-347. doi:10.1016/j.jfoodeng.2009.08.018Torres-Giner, S., Gimenez, E., & Lagaron, J. M. (2008). Characterization of the morphology and thermal properties of Zein Prolamine nanostructures obtained by electrospinning. Food Hydrocolloids, 22(4), 601-614. doi:10.1016/j.foodhyd.2007.02.005Torres-Giner, S., Martinez-Abad, A., Ocio, M. J., & Lagaron, J. M. (2010). Stabilization of a Nutraceutical Omega-3 Fatty Acid by Encapsulation in Ultrathin Electrosprayed Zein Prolamine. Journal of Food Science, 75(6), N69-N79. doi:10.1111/j.1750-3841.2010.01678.xTorres-Giner, S., Pérez-Masiá, R., & Lagaron, J. M. (2016). A review on electrospun polymer nanostructures as advanced bioactive platforms. Polymer Engineering & Science, 56(5), 500-527. doi:10.1002/pen.24274Vaughan, V. C., Hassing, M.-R., & Lewandowski, P. A. (2013). Marine polyunsaturated fatty acids and cancer therapy. British Journal of Cancer, 108(3), 486-492. doi:10.1038/bjc.2012.586Wang, Y., Liu, W., Chen, X. D., & Selomulya, C. (2016). Micro-encapsulation and stabilization of DHA containing fish oil in protein-based emulsion through mono-disperse droplet spray dryer. Journal of Food Engineering, 175, 74-84. doi:10.1016/j.jfoodeng.2015.12.007Woods, J., & Mellon, M. (1941). Thiocyanate Method for Iron: A Spectrophotometric Study. Industrial & Engineering Chemistry Analytical Edition, 13(8), 551-554. doi:10.1021/i560096a013Xiao, D., Davidson, P. M., & Zhong, Q. (2011). Release and antilisterial properties of nisin from zein capsules spray-dried at different temperatures. LWT - Food Science and Technology, 44(10), 1977-1985. doi:10.1016/j.lwt.2011.07.017Yang, H., Feng, K., Wen, P., Zong, M.-H., Lou, W.-Y., & Wu, H. (2017). Enhancing oxidative stability of encapsulated fish oil by incorporation of ferulic acid into electrospun zein mat. LWT, 84, 82-90. doi:10.1016/j.lwt.2017.05.045Zainal, Z., Longman, A. J., Hurst, S., Duggan, K., Caterson, B., Hughes, C. E., & Harwood, J. L. (2009). Relative efficacies of omega-3 polyunsaturated fatty acids in reducing expression of key proteins in a model system for studying osteoarthritis. Osteoarthritis and Cartilage, 17(7), 896-905. doi:10.1016/j.joca.2008.12.009Zeisel, S. H. (1999). Regulation of «Nutraceuticals». Science, 285(5435), 1853-1855. doi:10.1126/science.285.5435.1853Zhang, Y., Cui, L., Li, F., Shi, N., Li, C., Yu, X., … Kong, W. (2016). Design, fabrication and biomedical applications of zein-based nano/micro-carrier systems. International Journal of Pharmaceutics, 513(1-2), 191-210. doi:10.1016/j.ijpharm.2016.09.02