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Poly(3-hydroxybutyrate) (PHB) was blended with medium-chain-length PHAs (mcl-PHAs) for improving its flexibility while nanocellulose (NC) was added as a reinforcing agent. Even and odd-chain-length PHAs, having as main component poly(3-hydroxyoctanoate) (PHO) or poly(3-hydroxynonanoate) (PHN) were synthesized and served as PHB modifiers. The effects of PHO and PHN on the morphology, thermal, mechanical and biodegradation behaviors of PHB were different, especially in the presence of NC. The addition of mcl-PHAs decreased the storage modulus (E') of PHB blends by about 40 %. The further addition of NC mitigated this decrease bringing the E' of PHB/PHO/NC close to that of PHB and having a minor effect on the E' of PHB/PHN/NC. The biodegradability of PHB/PHN/NC was higher than that of PHB/PHO/NC, the latter's being close to that of neat PHB after soil burial for four months. The results showed a complex effect of NC, which enhanced the interaction between PHB and mcl-PHAs and decreased the size of PHO/PHN inclusions (1.9 ± 0.8/2.6 ± 0.9 μm) while increasing the accessibility of water and microorganisms during soil burial. The blown film extrusion test showed the ability of mcl-PHA and NC modified PHB to stretch forming uniform tube and supports the application of these biomaterials in the packaging sector., Competing Interests: Declaration of competing interest The authors declare no conflict of interest., (Copyright © 2023. Published by Elsevier B.V.)

Poly (3-hydroxybutyrate) (PHB) is a valuable bio-based and biodegradable polymer that may substitute common polymers in packaging and biomedical applications provided that the production cost is reduced and some properties improved. Blending PHB with other biodegradable polymers is the most simple and accessible route to reduce costs and to improve properties. This review provides a comprehensive overview on the preparation, properties and application of the PHB blends with other biodegradable polyesters such as medium-chain-length polyhydroxyalkanoates, poly(ε-caprolactone), poly(lactic acid), poly(butylene succinate), poly(propylene carbonate) and poly (butylene adipate-co-terephthalate) or polysaccharides and their derivatives. A special attention has been paid to the miscibility of PHB with these polymers and the compatibilizing methods used to improve the dispersion and interface. The changes in the PHB morphology, thermal, mechanical and barrier properties induced by the second polymer have been critically analyzed in view of industrial application. The biodegradability and recyclability strategies of the PHB blends were summarized along with the processing techniques adapted to the intended application. This review provides the tools for a better understanding of the relation between the micro/nanostructure of PHB blends and their properties for the further development of PHB blends as solutions for biodegradable packaging., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Medium chain-length polyhydroxyalkanoates (mPHAs) are flexible elastomeric biopolymers with valuable properties for biomedical applications like artificial arteries and other medical implants. However, an environmentally friendly and high productivity process together with the tuning of the mechanical and biological properties of mPHAs are mandatory for this purpose. Here, for the first time, a melt processing technique was applied for the preparation of bionanocomposites starting from poly(3-hydroxyoctanoate) (PHO) and bacterial cellulose nanofibers (BC). The incorporation of only 3 wt % BC in PHO improved its thermal stability with 25 °C and reinforced it, increasing the Young's modulus with 76% and the tensile strength with 44%. The percolation threshold calculated with the aspect ratio of the fibers after melt processing was very low and close to 3 wt %. We showed that this bionanocomposite is able to preserve the ductile behavior during storage, no important aging being noted between 3 h and one month after compression-molding. Moreover, this study is the first to investigate the melt processability of PHO nanocomposite for tube extrusion. In addition, biocompatibility study showed no proinflammatory immune response and better cell adhesion for PHO/BC nanocomposite with 3 wt % BC and demonstrated the high feasibility of this bionanocomposite for in vivo application of tissue-engineered blood vessels.

Blending poly(3-hydroxybutyrate) (PHB) with other polymers could be a rapid and accessible solution to overcome some of its drawbacks. In this work, PHB was modified with microfibrillated cellulose (MC) and a thermoplastic polyurethane containing biodegradable segments (PU) by two routes, using a masterbatch and by direct mixing. The PU and MC modifiers improved the thermal stability of PHB by up to 13 °C and slightly decreased its melt viscosity and crystallinity, thus improving the melt processability. The addition of PU in PHB composites led to a decrease in the storage modulus, which did not exceed 20% at room temperature. The hydrolytic degradation in an alkaline environment at 50 °C for 28 days decreased the thermal stability of the composites by 58–65 °C, while the lower mass loss and morphological features showed that the PU modifier delayed the degradation of the PHB composites. The improved thermal stability, melt processability, and lower cost, along with higher flexibility and the possibility of controlling the hydrolytic degradation by the PU content, make the PHB/PU/MC composites obtained by the masterbatch method promising materials for medical and engineering applications. [ABSTRACT FROM AUTHOR]

Poly (3-hydroxybutyrate) (PHB) is a valuable biopolymer that is produced in industrial quantity but is not widely used in applications due to some drawbacks. The addition of cellulose nanofibers (CNF) as a biofiller in PHB/CNF nanocomposites may improve PHB properties and enlarge its application field. In this work, n-octyltriethoxy silane (OTES), a medium-chain-length alkyl silane, was used to surface chemically modify the CNF (CNF_OTES) to enhance their hydrophobicity and improve their compatibility with PHB. The surface functionalization of CNF and nanodimension were emphasized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, atomic force microscopy, dynamic light scattering, and water contact angle (CA). Surface modification of CNF with OTES led to an increase in thermal stability by 25 °C and more than the doubling of CA. As a result of the higher surface hydrophobicity, the CNF_OTES were more homogeneously dispersed in PHB than unmodified CNF, leading to a PHB nanocomposite with better thermal and mechanical properties. Thus, an increase by 122% of the storage modulus at 25 °C, a slight increase in crystallinity, a better melting processability, and good thermal stability were obtained after reinforcing PHB with CNF_OTES, paving the way for increasing PHB applicability. [ABSTRACT FROM AUTHOR]

Poly(3-hydroxybutyrate) (PHB) is one of the most promising substitutes for the petroleum-based polymers used in the packaging and biomedical fields due to its biodegradability, biocompatibility, good stiffness, and strength, along with its good gas-barrier properties. One route to overcome some of the PHB's weaknesses, such as its slow crystallization, brittleness, modest thermal stability, and low melt strength is the addition of cellulose nanocrystals (CNCs) and the production of PHB/CNCs nanocomposites. Choosing the adequate processing technology for the fabrication of the PHB/CNCs nanocomposites and a suitable surface treatment for the CNCs are key factors in obtaining a good interfacial adhesion, superior thermal stability, and mechanical performances for the resulting nanocomposites. The information provided in this review related to the preparation routes, thermal, mechanical, and barrier properties of the PHB/CNCs nanocomposites may represent a starting point in finding new strategies to reduce the manufacturing costs or to design better technological solutions for the production of these materials at industrial scale. It is outlined in this review that the use of low-value biomass resources in the obtaining of both PHB and CNCs might be a safe track for a circular and bio-based economy. Undoubtedly, the PHB/CNCs nanocomposites will be an important part of a greener future in terms of successful replacement of the conventional plastic materials in many engineering and biomedical applications. [ABSTRACT FROM AUTHOR]

3D printing represents a valuable alternative to traditional processing methods, clearly demonstrated by the promising results obtained in the manufacture of various products, such as scaffolds for regenerative medicine, artificial tissues and organs, electronics, components for the automotive industry, art objects and so on. This revolutionary technique showed unique capabilities for fabricating complex structures, with precisely controlled physical characteristics, facile tunable mechanical properties, biological functionality and easily customizable architecture. In this paper, we provide an overview of the main 3D-printing technologies currently employed in the case of poly (lactic acid) (PLA) and polyhydroxyalkanoates (PHA), two of the most important classes of thermoplastic aliphatic polyesters. Moreover, a short presentation of the main 3D-printing methods is briefly discussed. Both PLA and PHA, in the form of filaments or powder, proved to be suitable for the fabrication of artificial tissue or scaffolds for bone regeneration. The processability of PLA and PHB blends and composites fabricated through different 3D-printing techniques, their final characteristics and targeted applications in bioengineering are thoroughly reviewed. [ABSTRACT FROM AUTHOR]

The fast depletion of fossil fuel reserves, global warming and environmental problems caused by non-biodegradable plastic materials as well as the high toxicity of some synthetic polymers that prevents their use in packaging or medical applications are the main reasons for a greener and more sustainable approach. There is also an imperative demand from the medical sector for more advanced materials with both biocompatibility and specialized functionalities to be used in living systems. High expectations arise from polymers obtained from renewable sources: poly(lactic acid) (PLA), polyhydroxyalkanoates (PHA), poly(butylene succinate) (PBS) and their blends, which are relevant materials for both biomedical and engineering fields. Moreover, bacterial cellulose (BC) has excellent properties and very broad application opportunities. Therefore, considering that these promising biomaterials will play an active role in the future, this review covers the progress made in the study of aliphatic polyesters/BC nanocomposites from the perspective of nanostructure–property relationship. New approaches to obtain aliphatic polyesters/BC nanocomposites with tailored mechanical properties and inherent biocompatibility are also summarized. The updated information from this review will help identifying new directions and strategies to design biocomposites for medical field and other applications. [ABSTRACT FROM AUTHOR]