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Although thermoplastic starch (TPS) has been developed to mitigate greenhouse gas emissions and environmental and health-related impacts from plastics, high moisture sensitivity and poor mechanical properties limited its practical applications. Blending TPS with biodegradable polyesters, i.e., poly(lactic acid) (PLA) and poly(butylene succinate-co-butylene adipate) (PBSA), is an alternative approach; however, the compatibility among polymer phases needs to be improved. Here, polyethylene glycol sorbitan monostearate (Tween 60), an amphiphilic surfactant, was proposed to improve the compatibility and performance of the TPS/PLA/PBSA 40/30/30 blend. The concentration of Tween 60 varied in the range of 0.5-2.5 wt%. The blends were fabricated using an extruder through two different melt-mixing routes, i.e., direct mixing and masterbatch mixing, and then converted to film using a blown film extrusion line. Tween 60 could improve compatibility between TPS dispersed phase and PLA/PBSA matrix, resulting in increased tensile strength, extensibility, impact strength, thermal stability, and water vapor and oxygen barrier properties of the ternary blend. In addition, better performance of the blend was obtained from the direct mixing route. Tween 60 could thus be considered a potential compatibilizer for the TPS/PLA/PBSA blend film, which can be further used as a biodegradable packaging material.

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Although thermoplastic starch (TPS) is a good candidate to overcome the limitations of poly(lactic acid) (PLA) due to its relatively low cost and high flexibility, the toughness and barrier properties of PLA/TPS blends are still insufficient for film applications. Therefore, the present work aims to improve the performance of PLA/TPS blend by simultaneous biaxial stretching and partially replacing PLA with poly(butylene adipate-co-terephthalate) (PBAT) for packaging film applications. PLA/TPS and PLA/PBAT/TPS sheets were prepared by melt cast extrusion and simultaneously biaxially stretched to form films. The mechanical, morphological, thermal, and water vapor and oxygen barrier properties and crystallinity of both intermediate sheets and their corresponding stretched films were examined. After stretching, PLA/TPS and PLA/PBAT/TPS blends showed markedly improved extensibility, impact strength, crystallinity, water vapor and oxygen barrier properties, and surface hydrophobicity. The stretched films demonstrated stacked-layer planar morphology, in which their outermost layers were a biodegradable polyester-rich phase. The synergistic effects of simultaneous biaxial stretching and partial replacing PLA with PBAT were extremely impressive for toughness improvement. The stretched films have the potential to replace non-biodegradable plastic packaging films, particularly where good mechanical and barrier properties are required.

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The development and production of thermoplastic starch (TPS) films based on blown film extrusion have been spurred by increasing interest in renewable resources and an alternative solution to meet industrial-scale demand. The chemical structure of the plasticizer and its proportion have a significant effect on the mechanical and barrier properties of TPS films. Therefore, this research aims to evaluate the influence of plasticizer type and content on the performance of TPS blown films. TPS films were prepared by mixing cassava starch with three types of plasticizer, i.e. glycerol, glycerol/xylitol, and glycerol/sorbitol with a weight ratio of 1:1. The quantity of plasticizer varied among 38, 40, and 42 parts per hundred parts of starch. Although TPS films plasticized with the small-sized plasticizer glycerol were easily processed and extensible, the surface stickiness leading to single-wall films, low tensile strength, and poor water vapor barrier properties would limit their use. By replacing glycerol with larger-sized plasticizers such as xylitol or sorbitol, the films exhibited reduced stickiness and separable double walls and showed improved tensile strength, stiffness, and water vapor and oxygen barrier properties. The obtained TPS blown films offer potential applications as edible films for food and pharmaceutical products.

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The incorporation of halloysite clay nanotubes (HNTs) into thermoplastic starch/poly(butylene adipate-co-terephthalate) (TPS/PBAT) blends has been investigated with the aim of improving the compatibility and properties of the matrix. TPS/PBAT/HNTs nano-biocomposites with different TPS/PBAT weight fractions and HNTs contents were elaborated using a melt blending process, and their morphology and properties were investigated. The TPS80/PBAT20 and TPS20/PBAT80 blends exhibited dispersed phases of small droplets of PBAT or TPS, respectively, whereas the TPS50/PBAT50 blend presented a more homogeneous structure. Elongation at break of the TPS/PBAT/HNTs biocomposites with 5 wt% of HNTs significantly increased with increasing PBAT proportion, i.e., 6.5 %, 41.3 %, and 351.5 % for the composites based on TPS80/PBAT20, TPS50/PBAT50, and TPS20/PBAT80, respectively. The incorporation of 5 wt% of HNTs improved compatibility and increased Young's modulus of the TPS80/PBAT20, TPS50/PBAT50, and TPS20/PBAT80 blends approx. 350 %, 142 %, and 18 %, respectively. These results demonstrate that HNTs are promising nanofillers to improve properties of TPS-based blends.

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Nano-biocomposites based on halloysite nanoclay and potato starch were elaborated by melt blending with different polyol plasticizers such as glycerol, sorbitol or a mixture of both. The effects of the type of plasticizer and clay content on potato starch/halloysite nano-biocomposites were studied. SEM analyses combined with ATR-FTIR results showed that a high content of sorbitol had a negative effect on the dispersion of the halloysite nanoclay in the starchy matrix. XRD results demonstrated that incorporation of halloysite nanoclay into glycerol-plasticized starch systems clearly led to the formation of a new crystalline structure. The addition of halloysite nanoclay improved the thermal stability and decreased the moisture absorption of the nano-biocomposites, whatever the type of plasticizer used. Halloysite addition led to more pronounced improvement in mechanical properties for glycerol plasticized system compared to nanocomposites based on sorbitol and glycerol/sorbitol systems with a 47% increase in tensile strength for glycerol-plasticized starch compared to 10.5% and 11% for sorbitol and glycerol/sorbitol systems, respectively. The use of a mixture of polyols was found to be a promising way to optimize the mechanical properties of these starch-based nanocomposites.

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Fabrication of starch-based edible film using blown film extrusion is challenging and interesting because this process provides continuous operation with shorter production time and lower energy consumption, is less labor intensive, and results in higher productivity than the conventional solution casting technique. Previously, we reported on the preparation and some properties of thermoplastic starch/chitosan (TPS/CTS) blown films; however, their morphological characteristics and barrier properties had not yet been elucidated. The present work thus aims to investigate the effect of chitosan (0.37-1.45%) on morphological characteristics, water vapor and oxygen barrier properties as well as hydrophilicity of the TPS and TPS/CTS films. The relationship between morphological characteristics and properties of the films was also discussed. Scanning electron microscopy (SEM), confocal laser scanning microscopy (CLSM) and X-ray photoelectron spectroscopy (XPS) confirmed the distribution and deposition of chitosan on the film surface. The existence of chitosan on the surface imparted the improved water vapor and oxygen barrier properties and the reduced surface hydrophilicity to the film. The results suggest that this biodegradable bio-based TPS/CTS film could potentially be used as an edible film for food and pharmaceutical applications.

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The objective of the present work was to improve blown film extrusion processability and properties of thermoplastic starch (TPS) film by incorporating plasticized chitosan, with a content of 0.37-1.45%. The effects of chitosan on extrusion processability and melt flow ability of TPS, as well as that on appearance, optical properties, thermal properties, viscoelastic properties and tensile properties of the films were investigated. The possible interactions between chitosan and starch molecules were evaluated by FTIR and XRD techniques. Chitosan and starch molecules could interact via hydrogen bonds, as confirmed from the blue shift of OH bands and the reduction of V-type crystal formation. Although the incorporation of chitosan caused decreased extensibility and melt flow ability, as well as increased yellowness and opacity, the films possessed better extrusion processability, increased tensile strength, rigidity, thermal stability and UV absorption, as well as reduced water absorption and surface stickiness. The obtained TPS/chitosan-based films offer real potential application in the food industry, e.g. as edible films.

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