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). 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Development of Electrospun Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Monolayers Containing Eugenol and Their Application in Multilayer Antimicrobial Food Packaging

[EN] In this research, different contents of eugenol in the 2.5-25 wt.% range were first incorporated into ultrathin fibers of poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) by electrospinning and then subjected to annealing to obtain antimicrobial monolayers. The most optimal concentration of eugenol in the PHBV monolayer was 15 wt.% since it showed high electrospinnability and thermal stability and also yielded the highest bacterial reduction against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). This eugenol-containing monolayer was then selected to be applied as an interlayer between a structural layer made of a cast-extruded poly(3-hydroxybutyrate) (PHB) sheet and a commercial PHBV film as the food contact layer. The whole system was, thereafter, annealed at 160°C for 10 s to develop a novel multilayer active packaging material. The resultant multilayer showed high hydrophobicity, strong adhesion and mechanical resistance, and improved barrier properties against water vapor and limonene vapors. The antimicrobial activity of the multilayer structure was also evaluated in both open and closed systems for up to 15 days, showing significant reductions (R ¿ 1 and < 3) for the two strains of food-borne bacteria. Higher inhibition values were particularly attained against S. aureus due to the higher activity of eugenol against the cell membrane of Gram positive (G+) bacteria. The multilayer also provided the highest antimicrobial activity for the closed system, which better resembles the actual packaging and it was related to the headspace accumulation of the volatile compounds. Hence, the here-developed multilayer fully based on polyhydroxyalkanoates (PHAs) shows a great deal of potential for antimicrobial packaging applications using biodegradable materials to increase both quality and safety of food products.This research was funded by the Spanish Ministry of Science and Innovation (MICI) through the RTI2018-097249-B-C21 program number and the H2020 EU project YPACK (reference number 773872). KF-L is a recipient of a Santiago Grisolía (Ref. 0001426013N810001A201) research contract of the Valencian Government (GVA) whereas ST-G holds a Juan de la Cierva¿ Incorporación contract (IJCI-2016-29675) from MICI. The authors would also like to thank the Unidad Asociada IATA-UJI Plastics Technology.Figueroa-López, KJ.; Cabedo, L.; Lagaron, JM.; Torres Giner, S. (2020). Development of Electrospun Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Monolayers Containing Eugenol and Their Application in Multilayer Antimicrobial Food Packaging. 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Overall and specific migration from multilayer high barrier food contact materials – kinetic study of cyclic polyester oligomers migration. Food Additives & Contaminants: Part A, 34(10), 1784-1794. doi:10.1080/19440049.2017.1346390Anukiruthika, T., Sethupathy, P., Wilson, A., Kashampur, K., Moses, J. A., & Anandharamakrishnan, C. (2020). Multilayer packaging: Advances in preparation techniques and emerging food applications. Comprehensive Reviews in Food Science and Food Safety, 19(3), 1156-1186. doi:10.1111/1541-4337.12556Mount, E. (2010). Coextrusion equipment for multilayer flat films and sheets. Multilayer Flexible Packaging, 75-95. doi:10.1016/b978-0-8155-2021-4.10006-1Torres-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.24274Torres-Giner, S., Martinez-Abad, A., & Lagaron, J. M. (2014). Zein-based ultrathin fibers containing ceramic nanofillers obtained by electrospinning. II. Mechanical properties, gas barrier, and sustained release capacity of biocide thymol in multilayer polylactide films. Journal of Applied Polymer Science, 131(18), n/a-n/a. doi:10.1002/app.40768Fabra, M. J., Lopez-Rubio, A., & Lagaron, J. M. (2013). High barrier polyhydroxyalcanoate food packaging film by means of nanostructured electrospun interlayers of zein. Food Hydrocolloids, 32(1), 106-114. doi:10.1016/j.foodhyd.2012.12.007Fabra, M. J., Lopez-Rubio, A., & Lagaron, J. M. (2014). Nanostructured interlayers of zein to improve the barrier properties of high barrier polyhydroxyalkanoates and other polyesters. Journal of Food Engineering, 127, 1-9. doi:10.1016/j.jfoodeng.2013.11.022Cherpinski, A., Torres‐Giner, S., Cabedo, L., Méndez, J. A., & Lagaron, J. M. (2017). Multilayer structures based on annealed electrospun biopolymer coatings of interest in water and aroma barrier fiber‐based food packaging applications. Journal of Applied Polymer Science, 135(24), 45501. doi:10.1002/app.45501Cherpinski, A., Torres-Giner, S., Vartiainen, J., Peresin, M. S., Lahtinen, P., & Lagaron, J. M. (2018). Improving the water resistance of nanocellulose-based films with polyhydroxyalkanoates processed by the electrospinning coating technique. Cellulose, 25(2), 1291-1307. doi:10.1007/s10570-018-1648-zQuiles-Carrillo, L., Montanes, N., Lagaron, J., Balart, R., & Torres-Giner, S. (2019). Bioactive Multilayer Polylactide Films with Controlled Release Capacity of Gallic Acid Accomplished by Incorporating Electrospun Nanostructured Coatings and Interlayers. Applied Sciences, 9(3), 533. doi:10.3390/app9030533Akinalan Balik, B., Argin, S., Lagaron, J. M., & Torres-Giner, S. (2019). 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Electrospun Oxygen Scavenging Films of Poly(3-hydroxybutyrate) Containing Palladium Nanoparticles for Active Packaging Applications

[EN] This paper reports on the development and characterization of oxygen scavenging films made of poly(3-hydroxybutyrate) (PHB) containing palladium nanoparticles (PdNPs) prepared by electrospinning followed by annealing treatment at 160 degrees C. The PdNPs were modified with the intention to optimize their dispersion and distribution in PHB by means of two different surfactants permitted for food contact applications, i.e., hexadecyltrimethylammonium bromide (CTAB) and tetraethyl orthosilicate (TEOS). Analysis of the morphology and characterization of the chemical, thermal, mechanical, and water and limonene vapor barrier properties and the oxygen scavenging capacity of the various PHB materials were carried out. From the results, it was seen that a better dispersion and distribution was obtained using CTAB as the dispersing aid. As a result, the PHB/PdNP nanocomposites containing CTAB provided also the best oxygen scavenging performance. These films offer a significant potential as new active coating or interlayer systems for application in the design of novel active food packaging structures.This research has received funding from the Spanish Ministry of Economy and Competitiveness (MINECO, project AGL2015-63855-C2-1-R) and the EU H2020 project YPACK (reference number 773872). A.C. and S.T.-G. would like to thank the Brazilian Council for Scientific and Technological Development (CNPq) and MINECO for her predoctoral grant (205955/2014-2) and his Juan de la Cierva contract (IJCI-2016-29675), respectively.Cherpinski, A.; Gozutok, M.; Turkoglu Sasmazel, H.; Torres-Giner, S.; Lagaron, JM. (2018). Electrospun Oxygen Scavenging Films of Poly(3-hydroxybutyrate) Containing Palladium Nanoparticles for Active Packaging Applications. Nanomaterials. 8(7):1-19. https://doi.org/10.3390/nano8070469S11987Puglia, D., Fortunati, E., D’Amico, D. A., Manfredi, L. B., Cyras, V. P., & Kenny, J. M. (2014). 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Poly(3-hydroxybutyrate-co -3-hydroxyvalerate)/clay nanocomposites for replacement of mineral oil based materials. Polymer Composites, 34(7), 1033-1040. doi:10.1002/pc.22510Castro-Mayorga, J. L., Fabra, M. J., & Lagaron, J. M. (2016). Stabilized nanosilver based antimicrobial poly(3-hydroxybutyrate-co-3-hydroxyvalerate) nanocomposites of interest in active food packaging. Innovative Food Science & Emerging Technologies, 33, 524-533. doi:10.1016/j.ifset.2015.10.019Bartczak, Z., Galeski, A., Kowalczuk, M., Sobota, M., & Malinowski, R. (2013). Tough blends of poly(lactide) and amorphous poly([R,S]-3-hydroxy butyrate) – morphology and properties. European Polymer Journal, 49(11), 3630-3641. doi:10.1016/j.eurpolymj.2013.07.033Furukawa, T., Sato, H., Murakami, R., Zhang, J., Duan, Y.-X., Noda, I., … Ozaki, Y. (2005). Structure, Dispersibility, and Crystallinity of Poly(hydroxybutyrate)/Poly(l-lactic acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry. Macromolecules, 38(15), 6445-6454. doi:10.1021/ma0504668Zhang, M., & Thomas, N. L. (2011). Blending polylactic acid with polyhydroxybutyrate: The effect on thermal, mechanical, and biodegradation properties. Advances in Polymer Technology, 30(2), 67-79. doi:10.1002/adv.20235Yildirim, S., Röcker, B., Rüegg, N., & Lohwasser, W. (2015). Development of Palladium-based Oxygen Scavenger: Optimization of Substrate and Palladium Layer Thickness. Packaging Technology and Science, 28(8), 710-718. doi:10.1002/pts.2134Cernohorsky, O., Zdansky, K., Zavadil, J., Kacerovsky, P., & Piksova, K. (2011). Palladium nanoparticles on InP for hydrogen detection. Nanoscale Research Letters, 6(1). doi:10.1186/1556-276x-6-410Damaj, Z., Joly, C., & Guillon, E. (2014). Toward New Polymeric Oxygen Scavenging Systems: Formation of Poly(vinyl alcohol) Oxygen Scavenger Film. Packaging Technology and Science, 28(4), 293-302. doi:10.1002/pts.2112Torres-Giner, S., Pérez-Masiá, R., & Lagaron, J. M. (2016). 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The impact of electrospun films of poly(epsilon-caprolactone) filled with nanostructured zeolite and silica microparticles on in vitro histamine formation by Staphylococcus aureus and Salmonella Paratyphi A

[EN] This research study originally reports the preparation and characterization of electrospun films based on poly(epsilon-caprolactone) (PCL) with high histamine-binding capacity. To this end, submicron PCL fibers filled with nanostructured zeolite or silica (SiO2) microparticles in the 5-20 wt% range were first prepared by solution electrospinning. The resultant electrospun composite fiber mats were thereafter thermally post-treated at 55 degrees C to successfully develop contact-transparent films with reduced porosity and improved mechanical strength. The capacity of the developed composite films to entrap histamine was evaluated in vitro by the culture media method using Staphylococcus aureus (S. aureus) and Salmonella Paratyphi A (S. Paratyphi A) foodborne bacteria. Both electrospun zeolite- and SiO2-containing PCL films exhibited high histamine-binding capacity, being more effective for S. aureus. The histamine entrapment performance was significantly higher for the PCL films filled with zeolite due to the enhanced porous structure and more optimal adsorption selectivity of this inorganic filler. The here-developed electrospun composite films can be applied as novel active-scavenging packaging materials to entrap heat-stable histamine and other biogenic amines released from fish and fishery products.This research was funded by the Spanish Ministry of Science, Innovation, and Universities (MICIU) program number AGL2015-63855-C2-1-R and by the EU H2020 YPACK project (reference number 773872). The authors also thank the Republic of Turkey Ministry of Agriculture and Forestry General Directorate of Agricultural Research and Policies (TAGEM) and Central Fisheries Research Institute SUMAE) for funding support through the projects TAGEM/HSGYAD/14/A05/P05/70 and TAGEM/HSGYAD/17/A03/P05/133. Figueroa Lopez is a recipient of a Santiago Grisolia (GRISOLIAP/2017/101) grant of the Generalitat Valenciana (GVA) and Torres-Giner is on a Juan de la Cierva-Incorporacion contract (IJCI-2016-29675) from MICIU.Alp-Erbay, E.; Figueroa-López, KJ.; Lagaron, JM.; Çaglak, E.; Torres-Giner, S. (2019). The impact of electrospun films of poly(epsilon-caprolactone) filled with nanostructured zeolite and silica microparticles on in vitro histamine formation by Staphylococcus aureus and Salmonella Paratyphi A. Food Packaging and Shelf Life. 22:1-13. https://doi.org/10.1016/j.fpsl.2019.100414S11322Alp Erbay, E., Dağtekin, B. B. (Gözü), Türe, M., Yeşilsu, A. F., & Torres-Giner, S. (2017). Quality improvement of rainbow trout fillets by whey protein isolate coatings containing electrospun poly(ε-caprolactone) nanofibers with Urtica dioica L. extract during storage. LWT, 78, 340-351. doi:10.1016/j.lwt.2017.01.002Alp-Erbay, E., Yeşi̇lsu, A. F., & Türe, M. (2019). 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Development and Characterization of Electrospun Biopapers of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Derived from Cheese Whey with Varying 3-Hydroxyvalerate Contents

[EN] In the present study, three different newly developed copolymers of poly(3-hydroxybutyrate-co-3-hydroxyval-erate) (PHBV) with 20, 40, and 60 mol % contents in 3-hydroxyvalerate (3HV) were produced by the biotechnological process of mixed microbial cultures (MMCs) using cheese whey (CW), a by-product from the dairy industry, as feedstock. The CW-derived PHBV copolyesters were first purified and then processed by solution electrospinning, yielding fibers of approximately 2 mu m in cross-section in all cases. The resultant electrospun PHBV mats were, thereafter, post-processed by annealing at different temperatures, below their maximum of melting, selected according to their 3HV content in order to obtain continuous films based on coalesced fibers, so-called biopapers. The resultant PHBV films were characterized in terms of their morphology, crystallinity, and mechanical and barrier properties to assess their potential application in food packaging. The CW-derived PHBV biopapers showed high contact transparency but a slightly yellow color. The fibers of the 20 mol % 3HV copolymer were seen to contain mostly poly(3-hydroxybutyrate) (PHB) crystals, the fibers of the 40 mol % 3HV copolymer a mixture of PHB and poly(3-hydroxyvalerate) (PHV) crystals and lowest crystallinity, and the fibers of the 60 mol % 3HV sample were mostly made of PHV crystals. To understand the interfiber coalesce process undergone by the materials during annealing, the crystalline morphology was also assessed by variable-temperature both combined small-angle and wide-angle X-ray scattering synchrotron and Fourier transform infrared experiments. From these experiments and, different from previously reported biopapers with lower 3HV contents, all samples were inferred to have a surface energy reduction mechanism for interfiber coalescence during annealing, which is thought to be activated by a temperature-induced decrease in molecular order. Due to their reduced crystallinity and molecular order, the CW-derived PHBV biopapers, especially the 40 mol % 3HV sample, were found to be more ductile and tougher. In terms of barrier properties, the three copolymers performed similarly to water and limonene, but to oxygen, the 40 mol % sample showed the highest relative permeability. Overall, the materials developed, which are compatible with the Circular Bioeconomy organic recycling strategy, can have an excellent potential as barrier interlayers or coatings of application interest in food packaging.This research work was funded by the H2020 EU project YPACK (reference number 773872) and by the Spanish Ministry of Science and Innovation (MICI) project RTI2018-097249-B-C21. B.M.-R. would like to acknowledge the MICI for her FPI fellowship (BES-2016-077972) and S.T.-G. for his MICI Juan de la Cierva-Incorporacion contract (IJCI-2016-29675). The ALBA Synchrotron is also acknowledged for the funding received through the project "Time-resolved Combined Wide-and Small-angle X-ray Scattering Characterization as a Function of Temperature of Electrospun Polyhydroxyalkanoates Derived from Biowaste" (2018022619). The authors would also like to thank the Unidad Asociada IATA(CSIC)-UJI in "Plastics Technology".Meléndez-Rodríguez, B.; Reis, MAM.; Carvalheira, M.; Sammon, C.; Cabedo, L.; Torres-Giner, S.; Lagaron, JM. (2021). Development and Characterization of Electrospun Biopapers of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Derived from Cheese Whey with Varying 3-Hydroxyvalerate Contents. Biomacromolecules. 22(7):2935-2953. https://doi.org/10.1021/acs.biomac.1c00353S2935295322

Organocatalyzed closed-loop chemical recycling of thermo-compressed films of poly(ethylene furanoate)

[EN] Monomers obtained from renewable feedstocks have emerged as a sustainable alternative to petroleum derived polymers. One of the biomass derived polyesters that has recently been gaining attention as an alternative to petrochemical polyethylene terephtalate (PET) for food and beverage packaging applications is poly(ethylene furanoate) (PEF). However, similar to PET, PEF is not biodegradable or compostable and its end-of-life options must be thus considered to avoid contributing to the accumulation of plastic waste. In this manuscript, PEF films were first produced using thermo-compression, an industrially relevant processing method, and their thermal, mechanical, and barrier properties were determined and compared to those of PET and other biopolyesters to ascertain their suitability for food packaging. Thereafter, the chemical glycolysis of PEF film waste was investigated using a sustainable and thermally stable acid-base organocatalyst. After succesfully deconstructing PEF into bis(2-hydroxyethyl)-furan-2,5-dicarboxylate (BHEF), the obtained BHEF diester was used to resynthesize PEF using the same catalyst to generate a new biopolyester with similar thermal properties to the virgin one in a closed-loop cycle.The authors thank for technical and human support provided by IZO-SGI SGIker of UPV/EHU and European funding (ERDF and ESF). Authors gratefully acknowledge financial support from Spanish Ministry of Science and Innovation (MICI) through projects MAT2017-83373-R and RTI 2018-097249-B-C21. S. T.-G. acknowledges MICI for the funding received during his previous Juan de la Cierva-Incorporacion contract (IJCI-2016-29675) and his current Ramon y Cajal contract (RYC2019-027784-I). A. M. I. acknowledges Prof. Cor Koning for the SSP reactor donated to POL group of Barcelona. Authors also thank India Glycols Ltd for kindly supplying bio-EG.Gabirondo, E.; Meléndez-Rodríguez, B.; Arnal, C.; Lagaron, JM.; Martínez De Ilarduya, A.; Sardon, H.; Torres-Giner, S. (2021). Organocatalyzed closed-loop chemical recycling of thermo-compressed films of poly(ethylene furanoate). Polymer Chemistry. 12(10):1571-1580. https://doi.org/10.1039/d0py01623cS15711580121

Development of Active Barrier Multilayer Films Based on Electrospun Antimicrobial Hot-Tack Food Waste Derived Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and Cellulose Nanocrystal Interlayers

[EN] Active multilayer films based on polyhydroxyalkanoates (PHAs) with and without high barrier coatings of cellulose nanocrystals (CNCs) were herein successfully developed. To this end, an electrospun antimicrobial hot-tack layer made of poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) derived from cheese whey, a by-product from the dairy industry, was deposited on a previously manufactured blown film of commercial food contact PHA-based resin. A hybrid combination of oregano essential oil (OEO) and zinc oxide nanoparticles (ZnONPs) were incorporated during the electrospinning process into the PHBV nanofibers at 2.5 and 2.25 wt%, respectively, in order to provide antimicrobial properties. A barrier CNC coating was also applied by casting from an aqueous solution of nanocellulose at 2 wt% using a rod at 1m/min. The whole multilayer structure was thereafter assembled in a pilot roll-to-roll laminating system, where the blown PHA-based film was located as the outer layers while the electrospun antimicrobial hot-tack PHBV layer and the barrier CNC coating were placed as interlayers. The resultant multilayer films, having a final thickness in the 130-150 mu m range, were characterized to ascertain their potential in biodegradable food packaging. The multilayers showed contact transparency, interlayer adhesion, improved barrier to water and limonene vapors, and intermediate mechanical performance. Moreover, the films presented high antimicrobial and antioxidant activities in both open and closed systems for up to 15 days. Finally, the food safety of the multilayers was assessed by migration and cytotoxicity tests, demonstrating that the films are safe to use in both alcoholic and acid food simulants and they are also not cytotoxic for Caco-2 cells.The Spanish Ministry of Science and Innovation (MICI) through the RTI2018-097249-B-C21 program number and the EU H2020 YPACK (reference number 773872) projects funded this research.Figueroa-Lopez, KJ.; Torres-Giner, S.; Angulo, I.; Pardo-Figuerez, M.; Escuin, JM.; Bourbon, AI.; Cabedo, L.... (2020). Development of Active Barrier Multilayer Films Based on Electrospun Antimicrobial Hot-Tack Food Waste Derived Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and Cellulose Nanocrystal Interlayers. Nanomaterials. 10(12):1-24. https://doi.org/10.3390/nano10122356S124101

Development and Characterization of Electrospun Fiber-Based Poly(ethylene- co -vinyl Alcohol) Films of Application Interest as High-Gas-Barrier Interlayers in Food Packaging

In the present study, poly(ethylene-co-vinyl alcohol) with 44 mol % ethylene content (EVOH44) was managed to be processed, for the first time, by electrospinning assisted by the coaxial technology of solvent jacket. In addition to this, different suspensions of cellulose nanocrystals (CNCs), with contents ranging from 0.1 to 1.0 wt %, were also electrospun to obtain hybrid bio-/non-bio nanocomposites. The resultant fiber mats were thereafter optimally annealed to promote interfiber coalescence at 145 °C, below the EVOH44 melting point, leading to continuous transparent fiber-based films. The morphological analysis revealed the successful distribution of CNCs into EVOH44 up to contents of 0.5 wt %. The incorporation of CNCs into the ethylene-vinyl alcohol copolymer caused a decrease in the crystallization and melting temperatures (TC and Tm) of about 12 and 7 °C, respectively, and also crystallinity. However, the incorporation of CNCs led to enhanced thermal stability of the copolymer matrix for a nanofiller content of 1.0 wt %. Furthermore, the incorporation of 0.1 and 0.5 wt % CNCs produced increases in the tensile modulus (E) of ca. 38% and 28%, respectively, but also yielded a reduction in the elongation at break and toughness. The oxygen barrier of the hybrid nanocomposite fiber-based films decreased with increasing the CNCs content, but they were seen to remain high barrier, especially in the low relative humidity (RH) regime, i.e., at 20% RH, showing permeability values lower than 0.6 × 10−20 m3·m·m−2·Pa−1·s−1. In general terms, an optimal balance in physical properties was found for the hybrid copolymer composite with a CNC loading of 0.1 wt %. On the overall, the present study demonstrates the potential of annealed electrospun fiber-based high-barrier polymers, with or without CNCs, to develop novel barrier interlayers to be used as food packaging constituents

Multilayer Film Comprising Polybutylene Adipate Terephthalate and Cellulose Nanocrystals with High Barrier and Compostable Properties

In the present study, a multilayer, high-barrier, thin blown film based on a polybutylene adipate terephthalate (PBAT) blend with polyhydroxyalkanoate (PHA), and composed of four layers including a cellulose nanocrystal (CNC) barrier layer and an electrospun poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) hot-tack layer, was characterized in terms of the surface roughness, surface tension, migration, mechanical and peel performance, barrier properties, and disintegration rate. The results showed that the film exhibited a smooth surface. The overall migration tests showed that the material is suitable to be used as a food contact layer. The addition of the CNC interlayer had a significant effect on the mechanical properties of the system, drastically reducing the elongation at break and, thus, the flexibility of the material. The film containing CNCs and electrospun PHBV hot-tack interlayers exhibited firm but not strong adhesion. However, the multilayer was a good barrier to water vapor (2.4 &plusmn; 0.1 &times; 10&minus;12 kg&middot;m&minus;2&middot;s&minus;1&middot;Pa&minus;1), and especially to oxygen (0.5 &plusmn; 0.3 &times; 10&minus;15 m3&middot;m&minus;2&middot;s&minus;1&middot;Pa&minus;1), the permeance of which was reduced by up to 90% when the CNC layer was added. The multilayer system disintegrated completely in 60 days. All in all, the multilayer system developed resulted in a fully compostable structure with significant potential for use in high-barrier food packaging applications