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Biopolymers from Natural Resources

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Polymers 2021, 13(15), 2532; https://doi.org/10.3390/polym13152532 - 30 Jul 2021

Cited by 14 | Viewed by 3178

Abstract

During the last decades, the increasing ecology in the reduction of environmental impact caused by traditional plastics is contributing to the growth of more sustainable plastics with the aim to reduce the consumption of non-renewable resources for their production [...] Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Influence of the Presence of Choline Chloride on the Classical Mechanism of “Gelatinization” of Starch

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Polymers 2021, 13(9), 1509; https://doi.org/10.3390/polym13091509 - 07 May 2021

Cited by 1 | Viewed by 1829

Abstract

The aim of this research is to contribute to a better understanding the destructuration of three native starches and a wheat flour in mixtures of water and choline chloride. Model systems have thus been defined to allow a better approach to hydrothermic transformations [...] Read more.

The aim of this research is to contribute to a better understanding the destructuration of three native starches and a wheat flour in mixtures of water and choline chloride. Model systems have thus been defined to allow a better approach to hydrothermic transformations related to the interactions between choline chloride and starch. We have observed that choline chloride has an impact on the gelatinization of starch which corresponds to the stabilizing salts phenomenon. The depolymerization and dissolution of the starch have also been demonstrated and can there dominate the gelatinization. However, the results obtained in X-ray diffraction by heating cell have shown that the exotherm which appeared was not only related to the depolymerization of the starch, but that a stage of crystalline rearrangement of the starch coexisted with this phenomenon. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Characterization of Novel Biopolymer Blend Mycocel from Plant Cellulose and Fungal Fibers

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Polymers 2021, 13(7), 1086; https://doi.org/10.3390/polym13071086 - 30 Mar 2021

Cited by 15 | Viewed by 2742

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In this study unique blended biopolymer mycocel from naturally derived biomass was developed. Softwood Kraft (KF) or hemp (HF) cellulose fibers were mixed with fungal fibers (FF) in different ratios and the obtained materials were characterized regarding microstructure, air permeability, mechanical properties, and [...] Read more.

In this study unique blended biopolymer mycocel from naturally derived biomass was developed. Softwood Kraft (KF) or hemp (HF) cellulose fibers were mixed with fungal fibers (FF) in different ratios and the obtained materials were characterized regarding microstructure, air permeability, mechanical properties, and virus filtration efficiency. The fibers from screened Basidiomycota fungi Ganoderma applanatum (Ga), Fomes fomentarius (Ff), Agaricus bisporus (Ab), and Trametes versicolor (Tv) were applicable for blending with cellulose fibers. Fungi with trimitic hyphal system (Ga, Ff) in combinations with KF formed a microporous membrane with increased air permeability (>8820 mL/min) and limited mechanical strength (tensile index 9–14 Nm/g). HF combination with trimitic fungal hyphae formed a dense fibrillary net with low air permeability (77–115 mL/min) and higher strength 31–36 Nm/g. The hyphal bundles of monomitic fibers of Tv mycelium and Ab stipes made a tight structure with KF with increased strength (26–43 Nm/g) and limited air permeability (14–1630 mL/min). The blends KF FF (Ga) and KF FF (Tv) revealed relatively high virus filtration capacity: the log₁₀ virus titer reduction values (LRV) corresponded to 4.54 LRV and 2.12 LRV, respectively. Mycocel biopolymers are biodegradable and have potential to be used in water microfiltration, food packaging, and virus filtration membranes. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Upgrading Argan Shell Wastes in Wood Plastic Composites with Biobased Polyethylene Matrix and Different Compatibilizers

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Maria Jorda-Reolid

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Jaume Gomez-Caturla

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Juan Ivorra-Martinez

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Pablo Marcelo Stefani

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Sandra Rojas-Lema

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Luis Quiles-Carrillo

Polymers 2021, 13(6), 922; https://doi.org/10.3390/polym13060922 - 17 Mar 2021

Cited by 23 | Viewed by 2824

Abstract

The present study reports on the development of wood plastic composites (WPC) based on micronized argan shell (MAS) as a filler and high-density polyethylene obtained from sugarcane (Bio-HDPE), following the principles proposed by the circular economy in which the aim is to achieve [...] Read more.

The present study reports on the development of wood plastic composites (WPC) based on micronized argan shell (MAS) as a filler and high-density polyethylene obtained from sugarcane (Bio-HDPE), following the principles proposed by the circular economy in which the aim is to achieve zero waste by the introduction of residues of argan as a filler. The blends were prepared by extrusion and injection molding processes. In order to improve compatibility between the argan particles and the green polyolefin, different compatibilizers and additional filler were used, namely polyethylene grafted maleic anhydride (PE-g-MA 3 wt.-%), maleinized linseed oil (MLO 7.5 phr), halloysite nanotubes (HNTs 7.5 phr), and a combination of MLO and HNTs (3.75 phr each). The mechanical, morphological, thermal, thermomechanical, colorimetric, and wettability properties of each blend were analyzed. The results show that MAS acts as a reinforcing filler, increasing the stiffness of the Bio-HDPE, and that HNTs further increases this reinforcing effect. MLO and PE-g-MA, altogether with HNTs, improve the compatibility between MAS and Bio-HDPE, particularly due to bonds formed between oxygen-based groups present in each compound. Thermal stability was also improved provided by the addition of MAS and HNTs. All in all, reddish-like brown wood plastic composites with improved stiffness, good thermal stability, enhanced compatibility, and good wettability properties were obtained. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Yield and Selectivity Improvement in the Synthesis of Carbonated Linseed Oil by Catalytic Conversion of Carbon Dioxide

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David Alejandro González Martínez

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Enrique Vigueras Santiago

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Susana Hernández López

Polymers 2021, 13(6), 852; https://doi.org/10.3390/polym13060852 - 10 Mar 2021

Cited by 6 | Viewed by 2155

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Carbonation of epoxidized linseed oil (CELO) containing five-membered cyclic carbonate (CC5) groups has been optimized to 95% by reacting epoxidized linseed oil (ELO) with carbon dioxide (CO₂) and tetrabutylammonium bromide (TBAB) as catalysts. The effect of reaction variables (temperature, CO₂ [...] Read more.

Carbonation of epoxidized linseed oil (CELO) containing five-membered cyclic carbonate (CC5) groups has been optimized to 95% by reacting epoxidized linseed oil (ELO) with carbon dioxide (CO₂) and tetrabutylammonium bromide (TBAB) as catalysts. The effect of reaction variables (temperature, CO₂ pressure, and catalyst concentration) on the reaction parameters (conversion, carbonation and selectivity) in an autoclave system was investigated. The reactions were monitored, and the products were characterized by Fourier Transform Infrared Spectroscopy (FT-IR), carbon-13 nuclear magnetic resonance (¹³C-NMR) and proton nuclear magnetic resonance (¹H-NMR) spectroscopies. The results showed that when carrying out the reaction at high temperature (from 90 °C to 120 °C) and CO₂ pressure (60–120 psi), the reaction’s conversion improves; however, the selectivity of the reaction decreases due to the promotion of side reactions. Regarding the catalyst, increasing the TBAB concentration from 2.0 to 5.0 w/w% favors selectivity. The presence of a secondary mechanism is based on the formation of a carboxylate ion, which was formed due to the interaction of CO₂ with the catalyst and was demonstrated through ¹³C-NMR and FT-IR. The combination of these factors makes it possible to obtain the largest conversion (96%), carbonation (95%), and selectivity (99%) values reported until now, which are obtained at low temperature (90 °C), low pressure (60 psi) and high catalyst concentration (5.0% TBAB). Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Development and Characterization of Weft-Knitted Fabrics of Naturally Occurring Polymer Fibers for Sustainable and Functional Textiles

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Polymers 2021, 13(4), 665; https://doi.org/10.3390/polym13040665 - 23 Feb 2021

Cited by 12 | Viewed by 2620

Abstract

This study focuses on the potential uses in textiles of fibers of soy protein (SP) and chitin, which are naturally occurring polymers that can be obtained from agricultural and food processing by-products and wastes. The as-received natural fibers were first subjected to a [...] Read more.

This study focuses on the potential uses in textiles of fibers of soy protein (SP) and chitin, which are naturally occurring polymers that can be obtained from agricultural and food processing by-products and wastes. The as-received natural fibers were first subjected to a three-step manufacturing process to develop yarns that were, thereafter, converted into fabrics by weft knitting. Different characterizations in terms of physical properties and comfort parameters were carried out on the natural fibers and compared to waste derived fibers of coir and also conventional cotton and cotton-based fibers, which are widely used in the textile industry. The evaluation of the geometry and mechanical properties revealed that both SP and chitin fibers showed similar fineness and tenacity values than cotton, whereas coir did not achieve the expected properties to develop fabrics. In relation to the moisture content, it was found that the SP fibers outperformed the other natural fibers, which could successfully avoid variations in the mechanical performance of their fabrics as well as impair the growth of microorganisms. In addition, the antimicrobial activity of the natural fibers was assessed against different bacteria and fungi that are typically found on the skin. The obtained results indicated that the fibers of chitin and also SP, being the latter functionalized with biocides during the fiber-formation process, showed a high antimicrobial activity. In particular, reductions of up to 100% and 60% were attained for the bacteria and fungi strains, respectively. Finally, textile comfort was evaluated on the weft-knitted fabrics of the chitin and SP fibers by means of thermal and tactile tests. The comfort analysis indicated that the thermal resistance of both fabrics was similar to that of cotton, whereas their air permeability was higher, particularly for chitin due to its higher fineness, which makes these natural fibers very promising for summer clothes. Both the SP and chitin fabrics also presented relatively similar values of fullness and softness than the pure cotton fabric in terms of body feeling and richness. However, the cotton/polyester fabric was the only one that achieved a good range for uses in winter-autumn cloths. Therefore, the results of this work demonstrate that non-conventional chitin and SP fibers can be considered as potential candidates to replace cotton fibers in fabrics for the textile industry due to their high comfort and improved sustainability. Furthermore, these natural fibers can also serve to develop novel functional textiles with antimicrobial properties. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Preparation and Characterization of a New Polymeric Multi-Layered Material Based K-Carrageenan and Alginate for Efficient Bio-Sorption of Methylene Blue Dye

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Polymers 2021, 13(3), 411; https://doi.org/10.3390/polym13030411 - 28 Jan 2021

Cited by 18 | Viewed by 1880

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The current study highlights a novel bio-sorbent design based on polyelectrolyte multi-layers (PEM) biopolymeric material. First layer was composed of sodium alginate and the second was constituted of citric acid and k-carrageenan. The PEM system was crosslinked to non-woven cellulosic textile material. Resulting [...] Read more.

The current study highlights a novel bio-sorbent design based on polyelectrolyte multi-layers (PEM) biopolymeric material. First layer was composed of sodium alginate and the second was constituted of citric acid and k-carrageenan. The PEM system was crosslinked to non-woven cellulosic textile material. Resulting materials were characterized using FT-IR, SEM, and thermal analysis (TGA and DTA). FT-IR analysis confirmed chemical interconnection of PEM bio-sorbent system. SEM features indicated that the microspaces between fibers were filled with layers of functionalizing polymers. PEM exhibited higher surface roughness compared to virgin sample. This modification of the surface morphology confirmed the stability and the effectiveness of the grafting method. Virgin cellulosic sample decomposed at 370 °C. However, PEM samples decomposed at 250 °C and 370 °C, which were attributed to the thermal decomposition of crosslinked sodium alginate and k-carrageenan and cellulose, respectively. The bio-sorbent performances were evaluated under different experimental conditions including pH, time, temperature, and initial dye concentration. The maximum adsorbed amounts of methylene blue are 124.4 mg/g and 522.4 mg/g for the untreated and grafted materials, respectively. The improvement in dye sorption evidenced the grafting of carboxylate and sulfonate groups onto cellulose surface. Adsorption process complied well with pseudo-first-order and Langmuir equations. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Production and Properties of Lignin Nanoparticles from Ethanol Organosolv Liquors—Influence of Origin and Pretreatment Conditions

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Polymers 2021, 13(3), 384; https://doi.org/10.3390/polym13030384 - 26 Jan 2021

Cited by 15 | Viewed by 1943

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Despite major efforts in recent years, lignin as an abundant biopolymer is still underutilized in material applications. The production of lignin nanoparticles with improved properties through a high specific surface area enables easier applicability and higher value applications. Current precipitation processes often show [...] Read more.

Despite major efforts in recent years, lignin as an abundant biopolymer is still underutilized in material applications. The production of lignin nanoparticles with improved properties through a high specific surface area enables easier applicability and higher value applications. Current precipitation processes often show poor yields, as a portion of the lignin stays in solution. In the present work, lignin was extracted from wheat straw, spruce, and beech using ethanol organosolv pretreatment at temperatures from 160–220 °C. The resulting extracts were standardized to the lowest lignin content and precipitated by solvent-shifting to produce lignin micro- and nanoparticles with mean hydrodynamic diameters from 67.8 to 1156.4 nm. Extracts, particles and supernatant were analyzed on molecular weight, revealing that large lignin molecules are precipitated while small lignin molecules stay in solution. The particles were purified by dialysis and characterized on their color and antioxidant activity, reaching ASC equivalents between 19.1 and 50.4 mg/mg. This work gives detailed insight into the precipitation process with respect to different raw materials and pretreatment severities, enabling better understanding and optimization of lignin nanoparticle precipitation. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Carboxymethyl Bacterial Cellulose from Nata de Coco: Effects of NaOH

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Pornchai Rachtanapun

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Pensak Jantrawut

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Warinporn Klunklin

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Kittisak Jantanasakulwong

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Yuthana Phimolsiripol

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Polymers 2021, 13(3), 348; https://doi.org/10.3390/polym13030348 - 22 Jan 2021

Cited by 36 | Viewed by 5193

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Bacterial cellulose from nata de coco was prepared from the fermentation of coconut juice with Acetobacter xylinum for 10 days at room temperature under sterile conditions. Carboxymethyl cellulose (CMC) was transformed from the bacterial cellulose from the nata de coco by carboxymethylation using [...] Read more.

Bacterial cellulose from nata de coco was prepared from the fermentation of coconut juice with Acetobacter xylinum for 10 days at room temperature under sterile conditions. Carboxymethyl cellulose (CMC) was transformed from the bacterial cellulose from the nata de coco by carboxymethylation using different concentrations of sodium hydroxide (NaOH) and monochloroacetic acid (MCA) in an isopropyl (IPA) medium. The effects of various NaOH concentrations on the degree of substitution (DS), chemical structure, viscosity, color, crystallinity, morphology and the thermal properties of carboxymethyl bacterial cellulose powder from nata de coco (CMCn) were evaluated. In the carboxymethylation process, the optimal condition resulted from NaOH amount of 30 g/100 mL, as this provided the highest DS value (0.92). The crystallinity of CMCn declined after synthesis but seemed to be the same in each condition. The mechanical properties (tensile strength and percentage of elongation at break), water vapor permeability (WVP) and morphology of CMCn films obtained from CMCn synthesis using different NaOH concentrations were investigated. The tensile strength of CMCn film synthesized with a NaOH concentration of 30 g/100 mL increased, however it declined when the amount of NaOH concentration was too high. This result correlated with the DS value. The highest percent elongation at break was obtained from CMCn films synthesized with 50 g/100 mL NaOH, whereas the elongation at break decreased when NaOH concentration increased to 60 g/100 mL. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Improving the Tensile and Tear Properties of Thermoplastic Starch/Dolomite Biocomposite Film through Sonication Process

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Polymers 2021, 13(2), 274; https://doi.org/10.3390/polym13020274 - 15 Jan 2021

Cited by 19 | Viewed by 2742

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In this work, dolomite filler was introduced into thermoplastic starch (TPS) matrix to form TPS-dolomite (TPS-DOL) biocomposites. TPS-DOL biocomposites were prepared at different dolomite loadings (1 wt%, 2 wt%, 3 wt%, 4 wt% and 5 wt%) and by using two different forms of [...] Read more.

In this work, dolomite filler was introduced into thermoplastic starch (TPS) matrix to form TPS-dolomite (TPS-DOL) biocomposites. TPS-DOL biocomposites were prepared at different dolomite loadings (1 wt%, 2 wt%, 3 wt%, 4 wt% and 5 wt%) and by using two different forms of dolomite (pristine (DOL(P) and sonicated dolomite (DOL(U)) via the solvent casting technique. The effects of dolomite loading and sonication process on the mechanical properties of the TPS-DOL biocomposites were analyzed using tensile and tear tests. The chemistry aspect of the TPS-DOL biocomposites was analyzed using Fourier transform infrared spectroscopy (FTIR) and X-Ray Diffraction (XRD) analysis. According to the mechanical data, biocomposites with a high loading of dolomite (4 and 5 wt%) possess greater tensile and tear properties as compared to the biocomposites with a low loading of dolomite (1 and 2 wt%). Furthermore, it is also proved that the TPS-DOL(U) biocomposites have better mechanical properties when compared to the TPS-DOL(P) biocomposites. Reduction in the dolomite particle size upon the sonication process assisted in its dispersion and distribution throughout the TPS matrix. Thus, this led to the improvement of the tensile and tear properties of the biocomposite. Based on the findings, it is proven that the sonication process is a simple yet beneficial technique in the production of the TPS-dolomite biocomposites with improved tensile and tear properties for use as packaging film. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Synthesis, Characterization, and Application of Carboxymethyl Cellulose from Asparagus Stalk End

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Warinporn Klunklin

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Kittisak Jantanasakulwong

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Yuthana Phimolsiripol

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Polymers 2021, 13(1), 81; https://doi.org/10.3390/polym13010081 - 28 Dec 2020

Cited by 49 | Viewed by 4226

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Cellulose from Asparagus officinalis stalk end was extracted and synthesized to carboxymethyl cellulose (CMC_as) using monochloroacetic acid (MCA) via carboxymethylation reaction with various sodium hydroxide (NaOH) concentrations starting from 20% to 60%. The cellulose and CMC_as were characterized by the [...] Read more.

Cellulose from Asparagus officinalis stalk end was extracted and synthesized to carboxymethyl cellulose (CMC_as) using monochloroacetic acid (MCA) via carboxymethylation reaction with various sodium hydroxide (NaOH) concentrations starting from 20% to 60%. The cellulose and CMC_as were characterized by the physical properties, Fourier Transform Infrared spectroscopy (FTIR), Differential scanning calorimetry (DSC), Scanning electron microscopy (SEM) and X-ray diffraction (XRD). In addition, mechanical properties of CMC_as films were also investigated. The optimum condition for producing CMC_as was found to be 30% of NaOH concentration for the carboxymethylation reaction, which provided the highest percent yield of CMC_as at 44.04% with the highest degree of substitution (DS) at 0.98. The melting point of CMC_as decreased with increasing NaOH concentrations. Crystallinity of CMC_as was significantly deformed (p < 0.05) after synthesis at a high concentration. The L* value of the CMC_as was significantly lower at a high NaOH concentration compared to the cellulose. The highest tensile strength (44.59 MPa) was found in CMC_as film synthesized with 40% of NaOH concentration and the highest percent elongation at break (24.99%) was obtained in CMC_as film treated with 30% of NaOH concentration. The applications of asparagus stalk end are as biomaterials in drug delivery system, tissue engineering, coating, and food packaging. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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The Effect of Halloysite Nanotubes on the Fire Retardancy Properties of Partially Biobased Polyamide 610

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Lourdes Sanchez-Nacher

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Luis Quiles-Carrillo

Polymers 2020, 12(12), 3050; https://doi.org/10.3390/polym12123050 - 19 Dec 2020

Cited by 10 | Viewed by 2029

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The main objective of the work reported here was the analysis and evaluation of halloysite nanotubes (HNTs) as natural flame retardancy filler in partially biobased polyamide 610 (PA610), with 63% of carbon from natural sources. HNTs are naturally occurring clays with a nanotube-like [...] Read more.

The main objective of the work reported here was the analysis and evaluation of halloysite nanotubes (HNTs) as natural flame retardancy filler in partially biobased polyamide 610 (PA610), with 63% of carbon from natural sources. HNTs are naturally occurring clays with a nanotube-like shape. PA610 compounds containing 10%, 20%, and 30% HNT were obtained in a twin-screw co-rotating extruder. The resulting blends were injection molded to create standard samples for fire testing. The incorporation of the HNTs in the PA610 matrix leads to a reduction both in the optical density and a significant reduction in the number of toxic gases emitted during combustion. This improvement in fire properties is relevant in applications where fire safety is required. With regard to calorimetric cone results, the incorporation of 30% HNTs achieved a significant reduction in terms of the peak values obtained of the heat released rate (HRR), changing from 743 kW/m² to about 580 kW/m² and directly modifying the shape of the characteristic curve. This improvement in the heat released has produced a delay in the mass transfer of the volatile decomposition products, which are entrapped inside the HNTs’ lumen, making it difficult for the sample to burn. However, in relation to the ignition time of the samples (TTI), the incorporation of HNTs reduces the ignition start time about 20 s. The results indicate that it is possible to obtain polymer formulations with a high renewable content such as PA610, and a natural occurring inorganic filler in the form of a nanotube, i.e., HNTs, with good flame retardancy properties in terms of toxicity, optical density and UL94 test. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Hydroxypropyl Methylcellulose E15: A Hydrophilic Polymer for Fabrication of Orodispersible Film Using Syringe Extrusion 3D Printer

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Warintorn Ruksiriwanich

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Pensak Jantrawut

Polymers 2020, 12(11), 2666; https://doi.org/10.3390/polym12112666 - 12 Nov 2020

Cited by 22 | Viewed by 4387

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Extrusion-based 3D printing technology is a relatively new technique that has a potential for fabricating pharmaceutical products in various dosage forms. It offers many advantages over conventional manufacturing methods, including more accurate drug dosing, which is especially important for the drugs that require [...] Read more.

Extrusion-based 3D printing technology is a relatively new technique that has a potential for fabricating pharmaceutical products in various dosage forms. It offers many advantages over conventional manufacturing methods, including more accurate drug dosing, which is especially important for the drugs that require exact tailoring (e.g., narrow therapeutic index drugs). In this work, we have successfully fabricated phenytoin-loaded orodispersible films (ODFs) through a syringe extrusion 3D printing technique. Two different grades of hydroxypropyl methylcellulose (HPMC E5 and HPMC E15) were used as the film-forming polymers, and glycerin and propylene glycol were used as plasticizers. The 3D-printed ODFs were physicochemically characterized and evaluated for their mechanical properties and in vitro disintegration time. Then, the optimum printed ODFs showing good mechanical properties and the fastest disintegration time were selected to evaluate their drug content and dissolution profiles. The results showed that phenytoin-loaded E15 ODFs demonstrated superior properties when compared to E5 films. It demonstrated a fast disintegration time in less than 5 s and rapidly dissolved and reached up to 80% of drug release within 10 min. In addition, it also exhibited drug content uniformity within United States Pharmacopeia (USP) acceptable range and exhibited good mechanical properties and flexibility with low puncture strength, low Young’s modulus and high elongation, which allows ease of handling and application. Furthermore, the HPMC E15 printing dispersions with suitable concentrations at 10% w/v exhibited a non-Newtonian (shear-thinning) pseudoplastic behavior along with good extrudability characteristics through the extrusion nozzle. Thus, HPMC E15 can be applied as a 3D printing polymer for a syringe extrusion 3D printer. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Methyl Methacrylate (MMA) Treatment of Empty Fruit Bunch (EFB) to Improve the Properties of Regenerated Cellulose Biocomposite Films

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Salmah Husseinsyah

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Nur Liyana Izyan Zailuddin

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Polymers 2020, 12(11), 2618; https://doi.org/10.3390/polym12112618 - 06 Nov 2020

Cited by 5 | Viewed by 1882

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The empty fruit bunch (EFB) regenerated cellulose (RC) biocomposite films for packaging application were prepared using ionic liquid. The effects of EFB content and methyl methacrylate (MMA) treatment of the EFB on the mechanical and thermal properties of the RC biocomposite were studied. [...] Read more.

The empty fruit bunch (EFB) regenerated cellulose (RC) biocomposite films for packaging application were prepared using ionic liquid. The effects of EFB content and methyl methacrylate (MMA) treatment of the EFB on the mechanical and thermal properties of the RC biocomposite were studied. The tensile strength and modulus of elasticity of the MMA treated RC biocomposite film achieved a maximum value when 2 wt% EFB was used for the regeneration process. The treated EFB RC biocomposite films also possess higher crystallinity index. The morphology analysis indicated that the RC biocomposite film containing MMA treated EFB exhibits a smoother and more homogeneous surface compared to the one containing the untreated EFB. The substitution of the –OH group of the EFB cellulose with the ester group of the MMA resulted in greater dissolution of the EFB in the ionic liquid solvent, thus improving the interphase bonding between the filler and matrix phase of the EF RC biocomposite. Due to this factor, thermal stability of the EFB RC biocomposite also successfully improved. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Biodegradable Starch/Chitosan Foam via Microwave Assisted Preparation: Morphology and Performance Properties

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Polymers 2020, 12(11), 2612; https://doi.org/10.3390/polym12112612 - 06 Nov 2020

Cited by 14 | Viewed by 3406 | Correction

Abstract

The effects of chitosan (CTS) as the reinforcing phase on the properties of potato starch (PS)-based foams were studied in this work. The formic acid solutions of CTS and PS were uniformly mixed in a particular ratio by blending and then placed in [...] Read more.

The effects of chitosan (CTS) as the reinforcing phase on the properties of potato starch (PS)-based foams were studied in this work. The formic acid solutions of CTS and PS were uniformly mixed in a particular ratio by blending and then placed in a mold made of polytetrafluoroethylene for microwave treatment to form starch foam. The results showed that the molecular weight and concentration of CTS could effectively improve the density and compressive properties of starch-based foams. Furthermore, orthogonal experiments were designed, and the results showed that when the molecular weight of CTS in foams is 4.4 × 10⁵, the mass fraction is 4 wt%, and the mass ratio of CTS–PS is 3/4.2; the compressive strength of foams is the highest at approximately 1.077 mPa. Furthermore, Fourier transform infrared spectroscopy analysis demonstrated the interaction between starch and CTS, which confirmed that the compatibility between CTS and PS is excellent. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Natural Inspired Carboxymethyl Cellulose (CMC) Doped with Ammonium Carbonate (AC) as Biopolymer Electrolyte

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Mohd Ibnu Haikal Ahmad Sohaimy

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Mohd Ikmar Nizam Mohamad Isa

Polymers 2020, 12(11), 2487; https://doi.org/10.3390/polym12112487 - 26 Oct 2020

Cited by 16 | Viewed by 2565

Abstract

Green and safer materials in energy storage technology are important right now due to increased consumption. In this study, a biopolymer electrolyte inspired from natural materials was developed by using carboxymethyl cellulose (CMC) as the core material and doped with varied ammonium carbonate [...] Read more.

Green and safer materials in energy storage technology are important right now due to increased consumption. In this study, a biopolymer electrolyte inspired from natural materials was developed by using carboxymethyl cellulose (CMC) as the core material and doped with varied ammonium carbonate (AC) composition. X-ray diffraction (XRD) shows the prepared CMC-AC electrolyte films exhibited low crystallinity content, X_c (~30%) for sample AC7. A specific wavenumber range between 900–1200 cm⁻¹ and 1500–1800 cm⁻¹ was emphasized in Fourier transform infrared (FTIR) testing, as this is the most probable interaction to occur. The highest ionic conductivity, σ of the electrolyte system achieved was 7.71 × 10⁻⁶ Scm⁻¹ and appeared greatly dependent on ionic mobility, µ and diffusion coefficient, D. The number of mobile ions, η, increased up to the highest conducting sample (AC7) but it became less prominent at higher AC composition. The transference measurement, t_ion showed that the electrolyte system was predominantly ionic with sample AC7 having the highest value (t_ion = 0.98). Further assessment also proved that the H⁺ ion was the main conducting species in the CMC-AC electrolyte system, which presumably was due to protonation of ammonium salt onto the complexes site and contributed to the overall ionic conductivity enhancement. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Biocomposites Based on Plasticized Wheat Flours: Effect of Bran Content on Thermomechanical Behavior

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Polymers 2020, 12(10), 2248; https://doi.org/10.3390/polym12102248 - 29 Sep 2020

Cited by 4 | Viewed by 1972

Abstract

In the present work, the effect of different bran content on the overall thermomechanical behavior of plasticized wheat flours (thermoplastic wheat flour; TPWF) was investigated. Refined flour (F0) with negligible bran fiber content, F1 flour (whole grain flour, 20% wt. bran), F3 (50% [...] Read more.

In the present work, the effect of different bran content on the overall thermomechanical behavior of plasticized wheat flours (thermoplastic wheat flour; TPWF) was investigated. Refined flour (F0) with negligible bran fiber content, F1 flour (whole grain flour, 20% wt. bran), F3 (50% wt. bran) and F2 (F1:F3, 50:50) film samples were realized by extrusion process. The effect of TPWF blending with two different biopolymers (polycaprolactone and poly butyrate adipate terephthalate), combined with the presence of citric acid as compatibilizer was also considered. Results from FESEM analysis and tensile characterization demonstrated that PCL was able to reach improved compatibility with the plasticized flour fraction at intermediate bran content (F2 based formulation) when 25% wt. of biopolymeric phase was added. Additionally, it was proved that improvements can be achieved in both thermal and mechanical performance when higher shear rate (120 rpm) and low temperature profiles (T_set2 = 130–135–140 °C) are selected. Disintegrability of the TPWF basic formulations in compositing conditions within 21 days was also confirmed; at the same time, an absence of any phytotoxic event of compost itself was registered. The obtained results confirmed the suitability of these materials, realized by adding different bran contents, to mechanically compete with bioplastics obtained by using purified starches. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Encapsulation Effect on the In Vitro Bioaccessibility of Sacha Inchi Oil (Plukenetia volubilis L.) by Soft Capsules Composed of Gelatin and Cactus Mucilage Biopolymers

by

María Carolina Otálora

,

Robinson Camelo

,

Andrea Wilches-Torres

,

Agobardo Cárdenas-Chaparro

and

Jovanny A. Gómez Castaño

Polymers 2020, 12(9), 1995; https://doi.org/10.3390/polym12091995 - 02 Sep 2020

Cited by 6 | Viewed by 3168

Abstract

Sacha inchi (Plukenetia volubilis L.) seed oil is a rich source of polyunsaturated fatty acids (PUFAs) that are beneficial for human health, whose nutritional efficacy is limited because of its low water solubility and labile bioaccessibility (compositional integrity). In this work, the [...] Read more.

Sacha inchi (Plukenetia volubilis L.) seed oil is a rich source of polyunsaturated fatty acids (PUFAs) that are beneficial for human health, whose nutritional efficacy is limited because of its low water solubility and labile bioaccessibility (compositional integrity). In this work, the encapsulation effect, using blended softgels of gelatin (G) and cactus mucilage (CM) biopolymers, on the PUFAs’ bioaccessibility of P. volubilis seed oil was evaluated during in vitro simulated digestive processes (mouth, gastric, and intestinal). Gas chromatography–mass spectrometry (GC–MS) and gas chromatography with a flame ionization detector (GC–FID) were used for determining the chemical composition of P. volubilis seed oil both before and after in vitro digestion. The most abundant compounds in the undigested samples were α-linolenic, linoleic, and oleic acids with 59.23, 33.46, and 0.57 (g/100 g), respectively. The bioaccessibility of α-linolenic, linoleic, and oleic acid was found to be 1.70%, 1.46%, and 35.8%, respectively, along with the presence of some oxidation products. G/CM soft capsules are capable of limiting the in vitro bioaccessibility of PUFAs because of the low mucilage ratio in their matrix, which influences the enzymatic hydrolysis of gelatin, thus increasing the release of the polyunsaturated content during the simulated digestion. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Cutin from Solanum Myriacanthum Dunal and Solanum Aculeatissimum Jacq. as a Potential Raw Material for Biopolymers

by

Mayra Beatriz Gómez-Patiño

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Rosa Estrada-Reyes

,

María Elena Vargas-Diaz

and

Daniel Arrieta-Baez

Polymers 2020, 12(9), 1945; https://doi.org/10.3390/polym12091945 - 28 Aug 2020

Cited by 2 | Viewed by 2518

Abstract

Plant cuticles have attracted attention because they can be used to produce hydrophobic films as models for novel biopolymers. Usually, cuticles are obtained from agroresidual waste. To find new renewable natural sources to design green and commercially available bioplastics, fruits of S. aculeatissimum [...] Read more.

Plant cuticles have attracted attention because they can be used to produce hydrophobic films as models for novel biopolymers. Usually, cuticles are obtained from agroresidual waste. To find new renewable natural sources to design green and commercially available bioplastics, fruits of S. aculeatissimum and S. myriacanthum were analyzed. These fruits are not used for human or animal consumption, mainly because the fruit is composed of seeds. Fruit peels were object of enzymatic and chemical methods to get thick cutins in good yields (approximately 77% from dry weight), and they were studied by solid-state resonance techniques (CPMAS ¹³C NMR), attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR), atomic force microscopy (AFM) and direct injection electrospray ionization mass spectrometry (DIESI-MS) analytical methods. The main component of S. aculeatissimum cutin is 10,16-dihydroxypalmitic acid (10,16-DHPA, 69.84%), while S. myriacanthum cutin besides of 10,16-DHPA (44.02%); another two C18 monomers: 9,10,18-trihydroxy-octadecanoic acid (24.03%) and 18-hydroxy-9S,10R-epoxy-octadecanoic acid (9.36%) are present. The hydrolyzed cutins were used to produce films demonstrating that both cutins could be a potential raw material for different biopolymers. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Controlled Release, Disintegration, Antioxidant, and Antimicrobial Properties of Poly (Lactic Acid)/Thymol/Nanoclay Composites

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,

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María Carmen Garrigós

Polymers 2020, 12(9), 1878; https://doi.org/10.3390/polym12091878 - 20 Aug 2020

Cited by 21 | Viewed by 2475

Abstract

Nano-biocomposite films based on poly (lactic acid) (PLA) were prepared by adding thymol (8 wt.%) and a commercial montmorillonite (D43B) at different concentrations (2.5 and 5 wt.%). The antioxidant, antimicrobial, and disintegration properties of all films were determined. A kinetic study was carried [...] Read more.

Nano-biocomposite films based on poly (lactic acid) (PLA) were prepared by adding thymol (8 wt.%) and a commercial montmorillonite (D43B) at different concentrations (2.5 and 5 wt.%). The antioxidant, antimicrobial, and disintegration properties of all films were determined. A kinetic study was carried out to evaluate the thymol release from the polymer matrix into ethanol 10% (v/v) as food simulant. The nanostructured networks formed in binary and ternary systems were of interest in controlling the release of thymol into the food simulant. The results indicated that the diffusion of thymol through the PLA matrix was influenced by the presence of the nanoclay. Disintegration tests demonstrated that the incorporation of both additives promoted the breakdown of the polymer matrix due to the presence of the reactive hydroxyl group in the thymol structure and ammonium groups in D43B. Active films containing thymol and D43B efficiently enhanced the antioxidant activity (inhibition values higher than 77%) of the nano-biocomposites. Finally, the addition of 8 wt.% thymol and 2.5 wt.% D43B significantly increased the antibacterial activity against Escherichia coli and Staphylococcus aureus 8325-4, resulting in a clear advantage to improve the shelf-life of perishable packaged food. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Design and Preparation of Polysulfide Flexible Polymers Based on Cottonseed Oil and Its Derivatives

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and

Polymers 2020, 12(9), 1858; https://doi.org/10.3390/polym12091858 - 19 Aug 2020

Cited by 4 | Viewed by 2373

Abstract

Polysulfide-derived polymers with a controllable density and mechanical strength were designed and prepared successfully using bio-based cottonseed oil (CO) and its derivatives, including fatty acid of cottonseed oil (COF) and sodium soap of cottonseed oil (COS). The reaction features of CO, COF and [...] Read more.

Polysulfide-derived polymers with a controllable density and mechanical strength were designed and prepared successfully using bio-based cottonseed oil (CO) and its derivatives, including fatty acid of cottonseed oil (COF) and sodium soap of cottonseed oil (COS). The reaction features of CO, COF and COS for polysulfide polymers were investigated and compared. Based on the free radical addition mechanism, COF reacts with sulfur to generate serials of polysulfide-derived polymers. COF strongly influences the density and tensile strength of these polymer composites. Whereas COS was not involved in the reaction with sulfur, as a filler, it could increase the density and tensile strength of polysulfide-derived polymers. Moreover, the results showed that these samples had an excellent reprocessability and recyclability. These polysulfide-based polymers, with an adjustable density and mechanical strength based on CO and derivatives, could have potential applications as bio-based functional supplementary additives. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Effect of Iignocellulosic Nanoparticles Extracted from Yerba Mate (Ilex paraguariensis) on the Structural, Thermal, Optical and Barrier Properties of Mechanically Recycled Poly(lactic acid)

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Joaquín Martínez Urreaga

Polymers 2020, 12(8), 1690; https://doi.org/10.3390/polym12081690 - 29 Jul 2020

Cited by 13 | Viewed by 2617

Abstract

In this work, yerba mate nanoparticles (YMNs) were extracted from Ilex paraguairiencis yerba mate wastes and further used to improve the overall performance of mechanically recycled PLA (PLAR). Recycled PLA was obtained by melt reprocessing PLA subjected to an accelerated ageing process, which [...] Read more.

In this work, yerba mate nanoparticles (YMNs) were extracted from Ilex paraguairiencis yerba mate wastes and further used to improve the overall performance of mechanically recycled PLA (PLAR). Recycled PLA was obtained by melt reprocessing PLA subjected to an accelerated ageing process, which involved photochemical, thermal and hydrothermal ageing steps, as well as a final demanding washing step. YMNs (1 and 3 wt. %) were added to the PLAR during the melt reprocessing step and further processed into films. The main goal of the development of PLAR-YMNs bionanocomposites was to increase the barrier properties of recycled PLA, while showing good overall performance for food packaging applications. Thus, optical, structural, thermal, mechanical and barrier properties were evaluated. The incorporation of YMNs led to transparent greenish PLAR-based films with an effective blockage of harmful UV radiation. From the backbone FTIR stretching region (bands at 955 and 920 cm⁻¹), it seems that YMNs favor the formation of crystalline domains acting as nucleating agents for PLAR. The morphological investigations revealed the good dispersion of YMNs in PLAR when they are used in the lowest amount of 1 wt. %, leading to bionanocomposites with improved mechanical performance. Although the addition of high hydrophilic YMNs increased the water vapor transmission, the addition of 1 wt. % of YMNs enhanced the oxygen barrier performance of the produced bionanocomposite films. These results show that the synergistic revalorization of post-consumer PLA and nanoparticles obtained from agri-food waste is a potential way for the production of promising packaging materials that meet with the principles of the circular economy. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Cucumis metuliferus Fruit Extract Loaded Acetate Cellulose Coatings for Antioxidant Active Packaging

by

Marina Patricia Arrieta

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,

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,

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Carol López de Dicastillo

Polymers 2020, 12(6), 1248; https://doi.org/10.3390/polym12061248 - 29 May 2020

Cited by 21 | Viewed by 3377

Abstract

A new active coating was developed by using Cucumis metuliferus fruit extract as antioxidant additive with the aim of obtaining an easy way to functionalize low-density polyethylene (LDPE) films for food packaging applications. Thus, an extraction protocol was first optimized to determine the [...] Read more.

A new active coating was developed by using Cucumis metuliferus fruit extract as antioxidant additive with the aim of obtaining an easy way to functionalize low-density polyethylene (LDPE) films for food packaging applications. Thus, an extraction protocol was first optimized to determine the total phenolic compounds and the antioxidant activity of CM. The aqueous CM antioxidant extract was then incorporated into cellulose acetate (CA) film-forming solution in different concentrations (1, 3 and 5 wt.%) to be further coated in corona-treated LDPE to obtain LDPE/CA-CM bilayer systems. CA and CA-CM film-forming solutions were successfully coated onto the surface of LDPE, showing good adhesion in the final bilayer structure. The optical, microstructural, thermal, mechanical and oxygen barrier performance, as well as the antioxidant activity, were evaluated. The active coating casted onto the LDPE film did not affect the high transparency of LDPE and improved the oxygen barrier performance. The antioxidant effectiveness of bilayer packaging was confirmed by release studies of Cucumis metuliferus from the cellulose acetate layer to a fatty food simulant. Finally, the LDPE/CA-CM active materials were also tested for their application in minimally processed fruits, and they demonstrated their ability to reduce the oxidation process of fresh cut apples. Thus, the obtained results suggest that CA-CM-based coating can be used to easily introduce active functionality to typically used LDPE at industrial level and enhance its oxygen barrier, without affecting the high transparency, revealing their potential application in the active food packaging sector to extend the shelf-life of packaged food by prevention of lipid oxidation of fatty food or by prevention fruit browning. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Manufacturing and Properties of Binary Blend from Bacterial Polyester Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) and Poly(caprolactone) with Improved Toughness

by

Juan Ivorra-Martinez

,

Isabel Verdu

,

Octavio Fenollar

,

Lourdes Sanchez-Nacher

,

Rafael Balart

and

Luis Quiles-Carrillo

Polymers 2020, 12(5), 1118; https://doi.org/10.3390/polym12051118 - 14 May 2020

Cited by 16 | Viewed by 3237

Abstract

Polyhydroxyalkanoates (PHAs) represent a promising group of bacterial polyesters for new applications. Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBH) is a very promising bacterial polyester with potential uses in the packaging industry; nevertheless, as with many (almost all) bacterial polyesters, PHBH undergoes secondary crystallization (aging) which [...] Read more.

Polyhydroxyalkanoates (PHAs) represent a promising group of bacterial polyesters for new applications. Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBH) is a very promising bacterial polyester with potential uses in the packaging industry; nevertheless, as with many (almost all) bacterial polyesters, PHBH undergoes secondary crystallization (aging) which leads to an embrittlement. To overcome or minimize this, in the present work a flexible petroleum-derived polyester, namely poly(ε-caprolactone), was used to obtain PHBH/PCL blends with different compositions (from 0 to 40 PCL wt %) using extrusion followed by injection moulding. The thermal analysis of the binary blends was studied by means of differential scanning calorimetry (DSC) and thermogravimetry (TGA). Both TGA and DSC revealed immiscibility between PHBH and PCL. Mechanical dynamic thermal analysis (DMTA) allowed a precise determination of the glass transition temperatures (T_g) as a function of the blend composition. By means of field emission scanning electron microscopy (FESEM), an internal structure formed by two phases was observed, with a PHBH-rich matrix phase and a finely dispersed PCL-rich phase. These results confirmed the immiscibility between these two biopolymers. However, the mechanical properties obtained through tensile and Charpy tests, indicated that the addition of PCL to PHBH considerably improved toughness. PHBH/PCL blends containing 40 PCL wt % offered an impact resistance double that of neat PHBH. PCL addition also contributed to a decrease in brittleness and an improvement in toughness and some other ductile properties. As expected, an increase in ductile properties resulted in a decrease in some mechanical resistant properties, e.g., the modulus and the strength (in tensile and flexural conditions) decreased with increasing wt % PCL in PHBH/PCL blends. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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Open AccessArticle

Development and Characterization of Sustainable Composites from Bacterial Polyester Poly(3-Hydroxybutyrate-co-3-hydroxyhexanoate) and Almond Shell Flour by Reactive Extrusion with Oligomers of Lactic Acid

by

Juan Ivorra-Martinez

,

Jose Manuel-Mañogil

,

Teodomiro Boronat

,

Lourdes Sanchez-Nacher

,

Rafael Balart

and

Luis Quiles-Carrillo

Polymers 2020, 12(5), 1097; https://doi.org/10.3390/polym12051097 - 11 May 2020

Cited by 18 | Viewed by 2561

Abstract

Eco-efficient Wood Plastic Composites (WPCs) have been obtained using poly(hydroxybutyrate-co-hexanoate) (PHBH) as the polymer matrix, and almond shell flour (ASF), a by-product from the agro-food industry, as filler/reinforcement. These WPCs were prepared with different amounts of lignocellulosic fillers (wt %), namely 10, 20 [...] Read more.

Eco-efficient Wood Plastic Composites (WPCs) have been obtained using poly(hydroxybutyrate-co-hexanoate) (PHBH) as the polymer matrix, and almond shell flour (ASF), a by-product from the agro-food industry, as filler/reinforcement. These WPCs were prepared with different amounts of lignocellulosic fillers (wt %), namely 10, 20 and 30. The mechanical characterization of these WPCs showed an important increase in their stiffness with increasing the wt % ASF content. In addition, lower tensile strength and impact strength were obtained. The field emission scanning electron microscopy (FESEM) study revealed the lack of continuity and poor adhesion among the PHBH-ASF interface. Even with the only addition of 10 wt % ASF, these green composites become highly brittle. Nevertheless, for real applications, the WPC with 30 wt % ASF is the most attracting material since it contributes to lowering the overall cost of the WPC and can be manufactured by injection moulding, but its properties are really compromised due to the lack of compatibility between the hydrophobic PHBH matrix and the hydrophilic lignocellulosic filler. To minimize this phenomenon, 10 and 20 phr (weight parts of OLA-Oligomeric Lactic Acid per one hundred weight parts of PHBH) were added to PHBH/ASF (30 wt % ASF) composites. Differential scanning calorimetry (DSC) suggested poor plasticization effect of OLA on PHBH-ASF composites. Nevertheless, the most important property OLA can provide to PHBH/ASF composites is somewhat compatibilization since some mechanical ductile properties are improved with OLA addition. The study by thermomechanical analysis (TMA), confirmed the increase of the coefficient of linear thermal expansion (CLTE) with increasing OLA content. The dynamic mechanical characterization (DTMA), revealed higher storage modulus, E’, with increasing ASF. Moreover, DTMA results confirmed poor plasticization of OLA on PHBH-ASF (30 wt % ASF) composites, but interesting compatibilization effects. Full article

(This article belongs to the Special Issue Biopolymers from Natural Resources)

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