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Enhancing food preservation and safety using environmentally friendly techniques is urgently needed. The aim of this study was to develop food packaging films using biodegradable poly-L-lactic acid (PLA) as biopolymer and carvacrol (CV) essential oil as an antioxidant/antibacterial agent for the replacement of chemical additives. CV was adsorbed onto natural zeolite (NZ) via a new vacuum adsorption method. The novel nanohybrid CV@NZ with a high CV content contained 61.7%wt. CV. Pure NZ and the CV@NZ nanohybrid were successfully dispersed in a PLA/triethyl citrate (TEC) matrix via a melt extrusion process to obtain PLA/TEC/xCV@NZ and PLA/TEC/xNZ nanocomposite films with 5, 10, and 15%wt CV@NZ or pure NZ content. The optimum resulting film PLA/TEC/10CV@NZ contained 10%wt. CV@NZ and exhibited self-healable properties, 22% higher tensile strength, 40% higher elongation at break, 45% higher water barrier, and 40% higher oxygen barrier than the pure PLA/TEC matrix. This film also had a high CV release content, high CV control release rate as well as 2.15 mg/L half maximal effective concentration (EC50) and 0.27 mm and 0.16 mm inhibition zones against Staphylococcus aureus and Salmonella enterica ssp. enterica serovar Typhimurium, respectively. This film not only succeeded in extending the shelf life of fresh minced pork, as shown by the total viable count measurements in four days but also prevented the lipid oxidation of fresh minced pork and provided higher nutritional values of the minced meat, as revealed by the heme iron content determination. It also had much better and acceptable sensory characteristics than the commercial packaging paper.
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The increasing global concern over plastic waste and its environmental impact has led to a growing interest in the development of sustainable packaging alternatives. This study focuses on the innovative use of expired dairy products as a potential resource for producing edible packaging materials. Expired milk and yogurt were selected as the primary raw materials due to their protein and carbohydrate content. The extracted casein was combined with various concentrations of chitosan, glycerol, and squid ink, leading to the studied samples. Chitosan was chosen due to its appealing characteristics, including biodegradability, and film-forming properties, and casein was utilized for its superior barrier and film-forming properties, as well as its biodegradability and non-toxic nature. Glycerol was used to further improve the flexibility of the materials. The prepared hydrogels were characterized using various instrumental methods, and the findings reveal that the expired dairy-based edible packaging materials exhibited promising mechanical properties comparable to conventional plastic packaging and improved barrier properties with zero-oxygen permeability of the hydrogel membranes, indicating that these materials have the potential to effectively protect food products from external factors that could compromise quality and shelf life.
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Nowadays, increased food safety and decreased food waste are two of the major global interests. Self-healable active packaging materials are an attractive option to achieve such targets. This property is critical for the hygiene and the consumption appropriateness of the food. Polylactic acid is a very promising polymeric matrix that potentially could replace the widely used low-density polyethylene due to its biobased origin and its easy biodegradable nature. The main drawback of this polymeric matrix is its brittle, fragile nature. On the other hand, tetraethyl citrate is a biobased approved food additive which became an attractive option as a plasticizer for industries seeking alternative materials to replace the traditional petrochemically derived compounds. A novel biobased film exhibiting self-healing behavior suitable for food-active packaging was developed during this study. Polylactic acid's brittleness was reduced drastically by incorporating tetraethyl citrate, and a random cut on the original self-repairing film was fully healed after 120 s. The optimum concentration of tetraethyl citrate in the polylactic acid was around 15% v/w with a water/oxygen barrier close to the relevant of polylactic acid and low migration. According to the EC50 parameter, the antioxidant activity was 300% higher than the relevant of pure polylactic acid, while according to the thiobarbituric acid and heme iron parameters, the film resisted lipid oxidation and deterioration. Finally, the total viable count parameter indicates the strong antimicrobial activity of this sample.
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The use of natural raw substances for food preservation could provide a great contribution to food waste reduction, circular economy enhancement, and green process application widening. Recent studies indicated that the use of porous materials as adsorbents for natural essential oils provided nanohybrids with excellent antioxidant and antimicrobial properties. Following this trend in this work, a thymol oil (TEO) rich SBA-15 nanohybrid was prepared and characterized physiochemically with various techniques. This TEO@SBA-15 nanohybrid, along with the pure SBA-15, was extruded with low-density polyethylene (LDPE) to develop novel active packaging films. Results indicated that TEO loading was higher than other porous materials reported recently, and the addition of both pure SBA-15 and TEO@SBA-15 to the LDPE increased the water/oxygen barrier. The film with the higher thyme-oil@SBA-15 nanohybrid content exhibited a slower release kinetic. The antioxidant activity of the final films ignited after 48 h, was in the range of 60-70%, and was almost constant for 7 days. Finally, all tests indicated a sufficient improvement by the addition of thyme-oil@SBA-15 nanohybrids in the pure LDPE matrix and the concentration of wt. 10% of such nanocarriers provided the optimum final LDPE/10TEO@SBE-15 active packaging film. This material could be a potential future product for active packaging applications.
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Carvacrol is well documented for its antibacterial and antioxidant effects. However, its high volatility has directed researchers toward nanoencapsulation technology according to bioeconomy and sustainability trends. This study examined and compared free carvacrol (FC), carvacrol microemulsion (MC), carvacrol microemulsion busted with chitosan (MMC), and carvacrol nanoemulsions (NC) as active coatings on extending minced pork meat shelf life at 4 ± 1 °C for 9 days, focusing on microbiological, physiochemical, and sensory characteristics. The research involved pre-characterizing droplet sizes, evaluating antioxidants, and determining antibacterial efficacy. The results demonstrated that NC with a 21 nm droplet size exhibited the highest antioxidant and antibacterial activity. All coatings succeeded in extending the preservation of fresh minced pork meat in comparison to the free carvacrol sample (FC). The NC coating showed the highest extension of minced pork meat preservation and maintained meat freshness for 9 days, with a lower TBARs of 0.736 mg MDA/Kg, and effectively reduced mesophilic, lactic acid, and psychotrophic bacterial counts more significantly by 1.2, 2, and 1.3 log, respectively, as compared to FC. Sensory assessments confirmed the acceptability of NC and MCC coatings. Overall, the carvacrol-based nanoemulsion can be considered a novel antioxidant and antimicrobial active coating due to its demonstrated higher efficacy in all the examined tests performed.
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Chondroitin sulfate (ChS), chitosan (Chi), and fish gelatin (FG), which are byproducts of a fish-treatment small enterprise, were incorporated with glycerol (Gly) to obtain dense hydrogel membranes with reduced brittleness, candidates for dressing in wound healing applications. The mechanical properties of all samples were studied via Dynamic Mechanical Analysis (DMA) and tensile tests while their internal structure was characterized using Attenuated Total Reflectance-Fourier Transform Infrared Spectroscopy (ATR-FTIR) and X-ray Diffraction (XRD) instruments. Their surface morphology was analyzed by ThermoGravimetric Analysis (TGA) method, while their water permeability was estimated via Water Vapor Transmission Rate (WVTR) measurements. Wettability and degradation rate measurements were also carried out. Characterization results indicated that secondary interactions between the natural polymers and the plasticizer create the hydrogel membranes. The samples were amorphous due to the high concentration of plasticizer and the amorphous nature of the natural polymers. The integration of ChS led to decreased decomposition temperature in comparison with the glycerol-free sample, and all the materials had dense structures. Finally, the in vitro endothelial cell attachment studies indicate that the hydrogel membranes successfully support the attachment and survival of primary on the hydrogel membranes and could be appropriate for external application in wound healing applications as dressings.
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We report the production of BC gels by Komagataeibacter sucrofermentans in synthetic (Hestrin and Schramm; HS) and natural media (raisin finishing side-stream extracts; RFSE), and their in situ modification by natural zeolite (Zt) and activated carbon (AC) nanostructures (NSs) carrying thyme oil (Th). The NS content for optimum BC yield was 0.64 g/L for both Zt-Th (2.56 and 1.47 g BC/L in HS and RFSE, respectively), and AC-Th (1.78 and 0.96 g BC/L in HS and RFSE, respectively). FTIR spectra confirmed the presence of NS and Th in the modified BCs, which, compared to the control, had reduced specific surface area (from 5.7 to 0.2-0.8 m2/g), average pore diameter (from 264 to 165-203 Å), cumulative pore volume (from 0.084 to 0.003-0.01 cm3/g), crystallinity index (CI) (from 72 to 60-70%), and crystallite size (from 78 to 72-76%). These values (except CI and CS), slightly increased after the use of the BC films as antimicrobial coatings on white cheese for 2 months at 4 °C. Tensile properties analysis showed that the addition of NSs resulted in a decrease of elasticity, tensile strength, and elongation at break values. The best results regarding an antimicrobial effect as cheese coating were obtained in the case of the RFSE/AC-Th BC.
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Biomass exploitation is a global trend due to the circular economy and the environmentally friendly spirit. Numerous applications are now based on the use of biomass-derived products. Hydrogen sulfide (H2S) is a highly toxic and environmentally hazardous gas which is emitted from various processes. Thus, the efficient removal of this toxic hazardous gas following cost-effective processes is an essential requirement. In this study, we present the synthesis and characterization of biomass-derived activated carbon/zinc oxide (ZnO@AC) composites from different biomass sources as potential candidates for H2S sorption. The synthesis involved a facile method for activated carbon production via pyrolysis and chemical activation of biomass precursors (spent coffee, Aloe-Vera waste leaves, and corncob). Activated carbon production was followed by the incorporation of zinc oxide nanoparticles into the porous carbon matrix using a simple melt impregnation method. The synthesized ZnO@AC composites were characterized using X-ray diffraction (XRD), infrared spectroscopy (IR), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), and nitrogen porosimetry. The H2S removal performance of the ZnO@AC composites was evaluated through sorption experiments using a handmade apparatus. Our findings demonstrate that the Aloe-Vera-, spent coffee-, and corncob-derived composites exhibit superior H2S sorption capacity up to 106 mgH2S/gads., 66 mgH2S/gads., and 47 mgH2S/gads., respectively.
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A notable application of polymeric nanocomposites is the design of water vapor permeable (WVP) membranes. "Breathable" membranes can be created by the incorporation of micro/nanofillers, such as CaCO3, that interrupt the continuity of the polymeric phase and when subjected to additional uniaxial or biaxial stretching this process leads to the formation of micro/nanoporous structures. Among the candidate nanofillers, carbon nanotubes (CNTs) have demonstrated excellent intrinsic WVP properties. In this study, chemically modified MWCNTs with oligo olefin-type groups (MWCNT-g-PP) are incorporated by melt processes into a PP matrix; a ß-nucleating agent (ß-ΝA) is also added. The crystallization behavior of the nanocomposite films is evaluated by differential scanning calorimetry (DSC) and X-ray diffraction (XRD). The WVP performance of the films is assessed via the "wet" cup method. The nanohybrid systems, incorporating both MWCNT-g-PP and ß-NA, exhibit enhanced WVP compared to films containing only MWCNT-g-PP or ß-NA. This improvement can be attributed to the significant increase in the growth of α-type crystals taking place at the edges of the CNTs. This increased crystal growth exerts a form of stress on the metastable ß-phase, thereby expanding the initial microporosity. In parallel, the coexistence of the inherently water vapor-permeable CNTs, further enhances the water vapor permeability reaching a specific water vapor transmission rate (Sp.WVTR) of 5500 µm.g/m2.day in the hybrid composite compared to 1000 µm.g/m2.day in neat PP. Notably, the functionalized MWCNT-g-PP used as nanofiller in the preparation of the "breathable" PP films demonstrated no noteworthy cytotoxicity levels within the low concentration range used, an important factor in terms of sustainability.
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The necessity of reducing the greenhouse effect by decreasing the carbon dioxide fingerprint directed the food packaging technology to use biobased raw materials. Alginates, which are derived from brown algae species, are one of the most promising biobased biopolymers for the development of edible active coatings capable of protecting food from oxidation/bacterial spoilage. In this study, sodium alginate, which was plasticized with glycerol and mixed with a biobased thymol/natural halloysite nanohybrid, was used to develop novel edible active coatings. Nanocomposite coatings were also developed in this project by mixing pure halloysite with sodium alginate/glycerol matrix and were used as reference material for comparison reasons. Instrumental analysis indicated a higher compatibility of a thymol/halloysite nanohybrid with a sodium alginate/glycerol matrix compared to pure halloysite with a sodium alginate/glycerol matrix. Increased compatibility resulted in improved tensile properties, water/oxygen barrier properties, and total antioxidant activity. These edible active coatings were applied to traditional Greek spread cheese and showed a reduction in the mesophilic microbial population over one log10 unit (cfu/g) compared to uncoated cheese. Moreover, the reduction in the mesophilic microbial population increased with the increase in halloysite and thymol content, indicating such sodium alginate/glycerol/thymol/halloysite hydrogels as promising edible active coatings for dairy products.
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Nowadays, the global trends of bioeconomy and sustainability require the use of biobased raw materials in all scientific and application fields to reduce the global carbon dioxide fingerprint [...].
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Currently, food saving, a circular economy, and zero environmental fingerprints are of major interest. Scientific efforts for enhanced food preservation using "green" methods have been intensified. Even though chemicals could achieve such targets effectively, the global trend against the "greenhouse effect" suggests the use of environmentally friendly biobased materials for this purpose. In this study, the promising biopolymer chitosan is incorporated with the promising biodegradable polymer polyvinyl alcohol to produce an improved biopolymeric matrix. This biodegradable biopolymer was further mixed homogeneously with 15% thymol/nano-zeolite nanohybrid material. The properties of the final developed film were improved compared to the relevant values of chitosan/polyvinyl alcohol film. The mechanical properties were enhanced significantly, i.e., there was a 34% increase in Young's modulus and a 4.5% increase in the ultimate tensile strength, while the antioxidant activity increased by 53.4%. The antibacterial activity increased by 134% for Escherichia coli, 87.5% for Staphylococcus aureus, 32% for Listeria monocytogenes, and 9% for Salmonella enterica. The water vapor diffusion coefficient and the oxygen permeability coefficient decreased to -51% and -74%, respectively, and thus, the water vapor and oxygen barrier increased significantly. The active pads were used in strawberries, and the antimicrobial activity evaluation against the mold of fungi was carried out. The visual evaluation shows that the active pads could extend the shelf life duration of strawberries.
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Τhe replacement of food packaging additives and preservatives with bio-based antioxidant/antibacterial compounds has been a common practice in recent years following the trend of bioeconomy and nanotechnology. Such bio-additives are often enclosed in nanocarriers for a controlled release process. Following this trend in this work, a thymol (TO)-rich activated carbon (AC) nanohybrid was prepared and characterized physicochemically with various techniques. This TO@AC nanohybrid, along with the pure activated carbon, was extruded with low-density polyethylene (LDPE) to develop novel active packaging films. The codenames used in this paper were LDPE/xTO@AC and LDPE/xAC for the nanohybrid and the pure activated carbon, respectively. X-ray diffractometry, Fourier-transform infrared spectroscopy, and scanning electron microscopy measurements showed high dispersity of both the TO@AC nanohybrid and the pure AC in the LDPE matrix, resulting in enhanced mechanical properties. The active film with 15 wt.% of the TO@AC nanohybrid (LDPE/15TO@AC) exhibited a 230% higher water/vapor barrier and 1928% lower oxygen permeability than the pure LDPE film. For this active film, the highest antioxidant activity referred to the DPPH assay (44.4%), the lowest thymol release rate (k2 ≈ 1.5 s-1), and the highest antibacterial activity were recorded, resulting in a 2-day extension of fresh pork fillets' shelf-life.
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Sustainability, the circular economy, and the "greenhouse" effect have led the food packaging industry to use naturally available bio-compounds. The integration of such compounds in packaging films increases food safety and extends food shelf-life. The development of an active/antioxidant packaging film based on the widely commercially used low-density polyethylene, natural zeolite, and Thymol, a natural extract from thyme oil, is presented in this work. The obtained active films were characterized using X-Ray Diffraction, Fourier-Transform Infrared Spectroscopy, Scanning Electron Microscopy, and Differential Scanning Calorimetry techniques. The tensile strength, water-oxygen barrier properties, and total antioxidant activity were measured. Low-density polyethylene incorporated with Thymol@Natural Zeolite at a proportion of 15 wt% was the most promising material and was used as film to wrap-up pork fillets. The thiobarbituric acid (TBA) method and heme iron measurements indicated a delayed lipids oxidation using this film. A linear correlation between the TBA method and heme iron values seems to be established, which could result in a fast method to determine the degree of lipid oxidation in pork fillets. Finally, a two-stage diffusion process during Thymol release was observed, and the values of the diffusion coefficient was 2.09 × 10-7 and 1.21 × 10-8 cm2/s for each stage. The applied pseudo-second sorption model provided a rate constant k2 = 0.01647 (s-1). These results indicate the strong potential of such films to be used as food packaging materials free of E-number preservatives.
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A new era is rising in food packaging and preservation, with a consequent focus on transition to "greener" and environmentally friendly techniques. The environmental problems that are emerging nowadays impose use of natural materials for food packaging applications, replacement of chemical preservatives with natural organic extractions, such as essential oils, and targeting of new achievements, such as further extension of food shelf-life. According to this new philosophy, most of the used materials for food packaging should be recyclable, natural or bio-based, and/or edible. The aim of this work was to investigate use and efficiency of a novel food packaging developed based on commercial LDPE polymer incorporated with natural material halloysite impregnated with natural extract of thyme oil. Moreover, a direct correlation between the stiff TBARS method and the easiest heme iron measurements method was scanned to test food lesions easier and faster. The result of this study was development of the LDPE/10TO@HNT film, which contains the optimum amount of a hybrid nanostructure and is capable to be used as an efficient active food packaging film. Furthermore, a linear correlation seems to connect the TBARS and heme iron measurements.
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The concept of this study is the replacement of previous fossil-based techniques for food packaging and food shelf-life extension, with novel more green processes and materials following the spirit of circular economy and the global trend for environmentally positive fingerprints. A novel adsorption process to produce thymol-halloysite nanohybrids is presented in this work. The high dispersion of this thymol-halloysite nanostructure in chitosan biopolymer is one of the goals of this study. The incorporation of this biodegradable matrix with poly-vinyl-alcohol produced a very promising food-packaging film. Mechanical, water-oxygen barrier, antimicrobial, and antioxidant properties were measured. Transparency levels were also tested using a UV-vis instrument. Moreover, the developed films were tested in-vivo for the preservation and the extension of the shelf-life of kiwi fruits. In all cases, results indicated that the increased fraction of thymol from thyme oil significantly enhances the antimicrobial and antioxidant activity of the prepared chitosan-poly-vinyl- alcohol gel. The use of the halloysite increases the mechanical and water-oxygen barrier properties and leads to a control release process of thymol which extends the preservation and the shelf-life of kiwi fruits. Finally, the results indicated that the halloysite improves the properties of the chitosan/poly-vinyl-alcohol films, and the thymol makes them further advantageous.
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This study presents, the development of a green method to produce rich in thymol natural zeolite (TO@NZ) nanostructures. This material was used to prepare sodium-alginate/glycerol/xTO@NZ (ALG/G/TO@NZ) nanocomposite active films for the packaging of soft cheese to extend its shelf-life. Differential scanning calorimetry (DSC), X-ray analysis (XRD), scanning electron microscopy (SEM), and Fourier-transform infrared spectroscopy (FTIR) instruments were used for the characterization of such nanostructures and films, to identify the thymol adsorbed amount, to investigate the thermal behaviour, and to confirm the dispersion of nanostructure powder into the polymer matrix. Water vapor transmission rate, oxygen permeation analyzer, tensile measurements, antioxidant measurements, and antimicrobial measurements were used to estimate the film's water and oxygen barrier, mechanical properties, nanostructure's nanoreinforcement activity, antioxidant and antimicrobial activity. The findings from the study revealed that ALG/G/TO@NZ nanocomposite film could be used as an active packaging film for foods with enhanced, mechanical properties, oxygen and water barrier, antioxidant and antimicrobial activity, and it is capable of extending food shelf-life.
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The global turn from the linear to the circular economy imposes changes in common activities such as food packaging. The use of biodegradable materials such as polyvinyl alcohol, natural raw materials such as clays, and food byproducts such as chitosan to develop novel food packaging films attracts the interest of industrial and institutional research centers. In this study, novel hybrid nanostructures were synthesized via the growth of zinc oxide nanorods on the surface of two nanoclays. The obtained nanostructures were incorporated with chitosan/polyvinyl alcohol composite either as nanoreinforcement or as an active agent to develop packaging films. The developed films were characterized via XRD, FTIR, mechanical, water-vapor diffusion, water sorption, and oxygen permeability measurements. Antimicrobial activity measurements were carried out against four different pathogen microorganisms. XRD indicated the formation of an intercalated nanocomposite structure for both types of nanoclays. Furthermore, improved tensile, water/oxygen barrier, and antimicrobial properties were recorded for all films compared to the pure chitosan/polyvinyl alcohol film. Overall, the results indicated that the use of the bio-based developed films led to an extension of food shelf life and could be used as novel active food packaging materials. Among them, the most promising film was the 6% wt. ZnO@halloysite.
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Today, the use of natural biodegradable materials in the production processes is more and more adopted by industry to achieve cyclic economy targets and to improve environmental and human health indexes. Active packaging is the latest trend for food preservation. In this work, nanostructures were prepared by incorporation of thyme oil with natural natrium-montmorillonite and organo-montmorillonite with two different techniques, direct impregnation and the green evaporation-adsorption process. Such nanostructures were mixed with poly-L-lactic-acid for the first time via an extrusion molding process to develop a new packaging film. Comparisons of morphological, mechanical, and other basic properties for food packaging were carried out via XRD, FTIR, TG, SEM/EDS, oxygen and water vapor permeation, and antimicrobial and antioxidant activity for the first time. Results showed that poly-L-lactic-acid could be modified with clays and essential oils to produce improved active packaging films. The final product exhibits food odor prevention characteristics and shelf-life extension capabilities, and it could be used for active packaging. The films based on OrgMt clay seems to be more promising, while the thyme oil addition improves their behavior as active packaging. The PLLA/3%TO@OrgMt and PLLA/5%TO@OrgMt films were qualified between the tested samples as the most promising materials for this purpose.
Assuntos
Antioxidantes/química , Bentonita/química , Embalagem de Alimentos , Membranas Artificiais , Nanoestruturas/química , Óleos de Plantas/química , Poliésteres/química , Sódio/química , Timol/química , Thymus (Planta)/química , Anti-Infecciosos , Fenômenos Químicos , Fenômenos Mecânicos , Nanoestruturas/ultraestrutura , Análise EspectralRESUMO
In this study, CuMt and TiMt montmorillonites were produced via an ion-exchange process with Cu+ and Ti4+ ions. These nanostructured materials were characterized with X-ray diffraction (XRD) and fourier transform infrared spectroscopy (FTIR) measurements and added as nanoreinforcements and active agents in chitosan (CS)/poly-vinyl-alcohol (PVOH)-based packaging films. The developed films were characterized by XRD and FTIR measurements. The antimicrobial, tensile, and oxygen/water-barrier measurements for the evaluation of the packaging performance were carried out to the obtained CS/PVOH/CuMt and CS/PVOH/TiMt films. The results of this study indicated that CS/PVOH/CuMt film is a stronger intercalated nanocomposite structure compared to the CS/PVOH/TiMt film. This fact reflected higher tensile strength and water/oxygen-barrier properties. The antibacterial activity of these films was tested against four food pathogenic bacteria: Escherichia coli, Staphylococcus aureus, Salmonella enterica and Listeria monocytogenes. Results showed that in most cases, the antibacterial activity was generated by the CuMt and TiMt nanostructures. Thus, both CS/PVOH/CuMt and CS/PVOH/TiMt films are nanocomposite candidates with very good perspectives for future applications on food edible active packaging.