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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On the extraction of cellulose nanowhiskers from food by-products and their comparative reinforcing effect on a polyhydroxybutyrate-co-valerate polymer

The present work reports on the characterization of cellulose nanowhiskers (CNW) extracted from three different food by-products, i.e., wheat straw (WSCNW), Brewers spent grains (BGCNW) and olive pomace (OPCNW), by using an optimized hydrolysis method similar to that developed to extract bacterial cellulose nanowhiskers (BCNW). WSCNW and BGCNW were seen to present optimal properties, with aspect ratio, crystallinity and thermal stability values comparable to those of BCNW. Additionally, the optimized hydrolysis treatment led to extraction yields higher than those previously reported for food by-products. The CNW were subsequently incorporated into a commercial polyhydroxybutyrate-co-valerate polymer (PHBV) by solution casting, and the produced nanocomposites were characterized. Although the addition of BGCNW and WSCNW was advantageous in terms of mechanical performance in comparison with OPCNW, no significant enhancement of the pure PHBV mechanical properties was reported because of the low nanofiller loadings used and the inherent difficulty of achieving a high degree of dispersion by the casting method. Interestingly, BGCNW and WSCNW presented reduced moisture sensitivity as compared with BCNW, leading to greater barrier performance and resulting in oxygen permeability reductions up to 26 % with WSCNW and 44 % with BGCNW.Noelle Peutat, on leave from the University of Grenoble in France, is acknowledged for her great dedication and support in the experimental work. M. Martinez-Sanz would like to thank the Spanish Ministry of Education for FPU Grant 1484. The authors acknowledge financial support from the EU FP7 ECOBIOCAP Project. The Electronic Microscopy Department in the SCIE from the University of Valencia is acknowledged for the support with SEM and TEM analyses. The Portuguese authors also acknowledge support from the FCT (Portuguese Foundation for Science and Technology) through strategic project PEst-OE/EQB/LA0023/2013

Melt processability, characterization, and antibacterial activity of compression-molded green composite sheets made of poly(3-hydroxybutyrate-co-3-hydroxyvalerate) reinforced with coconut fibers impregnated with oregano essential oil

New packaging materials based on green composite sheets consisting of poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) and coconut fibers (CFs) were obtained by twin-screw extrusion (TSE) followed by compression molding. The effect of varying the CF weight content, i.e. 1, 3, 5, and 10wt.-%, and the screw speed during melt processing, i.e. 75, 150, and 225rpm, on both the aspect ratio and dispersion of the fibers was analyzed and related to the properties of the compression-molded sheets. Finally, the CFs were impregnated with oregano essential oil (OEO) by an innovative spray coating methodology and then incorporated into PHBV at the optimal processing conditions. The functionalized green composite sheets presented bacteriostatic effect against Staphylococcus aureus from fiber contents as low as 3wt.-%. Therefore, the here-prepared CFs can be successfully applied as natural vehicles to entrap extracts and develop green composites of high interest in active food packaging to provide protection and shelf life extension.This research was funded by the EU H2020 project YPACK (reference number 773872), the Spanish Ministry of Economy and Competitiveness (MINECO) project AGL2015-63855-C2-1-R, the Portuguese Foundation for Science and Technology (FCT) under the scope of the strategic funding of UID/BIO/04469/2013 unit and COMPETE 2020 (POCI-01-0145-FEDER-006684), and the BioTecNorte operation (NORTE-01-0145-FEDER-000004) funded by the European Regional Development Fund (ERDF) under the scope of Norte2020 – Programa Operacional Regional do Norte. Prof. Sergio Torres-Giner wants to thank the European Cooperation in Science and Technology (COST) Action FP1405, ActInPak, for financial support during his Short Term Scientific Mission (STSM) at the University of Minho.info:eu-repo/semantics/publishedVersio

Electrospinning for healthcare: recent advancements

Electrospinning is a simple route to generate polymer-based fibres with diameters on the nano- to micron-scale. It has been very widely explored in biomedical science for applications including drug delivery systems, diagnostic imaging, theranostics, and tissue engineering. This extensive literature reveals that a diverse range of functional components including small molecule drugs, biologics, and nanoparticles can be incorporated into electrospun fibres, and it is possible to prepare materials with complex compartmentalised architectures. This perspective article briefly introduces the electrospinning technique before considering its potential applications in biomedicine. Particular attention is paid to the translation of electrospinning to the clinic, including the need to produce materials at large scale and the requirement to do so under Good Manufacturing Practice conditions. We finish with a summary of the key current challenges and future perspectives

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 of active bio-based multilayer systems: encapsulation of cinnamaldehyde and their physicochemical characterization

[Excerpt] In this work, different multilayer structures, using a polyhydroxybutyrate-co-valerate film with a valerate content of 8% (PHBV8) as support, were developed aiming the development of active bio-based multilayer systems. An interlayer based on zein nanofibers with and without cinnamaldehyde were electrospun in the PHBV8 film and three multilayer systems were developed: 1) without an outer layer; 2) using a PHBV8 film as outer layer; and 3) using an alginate-based film as outer layer. Their physico-chemical properties were evaluated through: water vapour and oxygen permeabilities and colour measurements, Fourier Transform Infrared Spectroscopy (FTIR) and thermal analyses. Results showed that the presence of different outer layers affected the water vapour permeability and transparency of the multilayer films. (...

Use of electrospinning to develop antimicrobial biodegradable multilayer systems: encapsulation of cinnamaldehyde and their physicochemical characterization

In this work, three active bio-based multilayer structures, using a polyhydroxybutyrate-co-valerate film with a valerate content of 8 % (PHBV8) as support, were developed. To this end, a zein interlayer with or without cinnamaldehyde (CNMA) was directly electrospun onto one side of the PHBV8 film and the following systems were developed: (1) without an outer layer; (2) using a PHBV8 film as outer layer; and (3) using an alginate-based film as outer layer. These multilayer structures were characterized in terms of water vapour and oxygen permeabilities, transparency, intermolecular arrangement and thermal properties. The antimicrobial activity of the active bio-based multilayer systems and the release of CNMA in a food simulant were also evaluated. Results showed that the presence of different outer layers reduced the transport properties and transparency of the multilayer films. The active bio-based multilayer systems showed antibacterial activity against Listeria monocytogenes being the multilayer structure prepared with CNMA and PHBV outer layers (PHBV + zein/CNMA + PHBV) the one that showed the greater antibacterial activity. The release of CNMA depended on the multilayer structures, where both Fick's and Case II transport-polymer relaxation explained the release of CNMA from the multilayer systems.Acknowledgments: Miguel A. Cerqueira (SFRH/BPD/72753/2010) andAnaI.Bourbon(SFRH/BD/73178/2010)arerecipientofafellowship from the Fundação para a Ciência e Tecnologia (FCT, POPH-QREN and FSE Portugal). J.L. Castro-Mayorga is supported by the Administrative Department of Science, Technology and Innovation (Colciencias) of Colombian Government. M. J. Fabra is a recipient of a Ramon y Cajal contract (RyC-2014-158) from the Spanish Ministry of Economy and Competitiveness. This study was supported by the Portuguese Foundation for Science and Technology (FCT) under the scope of the strategic funding of UID/BIO/04469/2013 unit and COMPETE 2020 (POCI-01-0145-FEDER-006684) and of the Project RECI/BBB-EBI/ 0179/2012 (FCOMP-01-0124-FEDER-027462). The support of EU Cost Action MP1206 is gratefully acknowledged