Studies on the alcoholysis of poly(3-hydroxybutyrate) and the synthesis of PHB-b-PLA block copolymer for the preparation of PLA/PHB-b-PLA blends

Don, Trong‐Ming; Liao, Kuo-Hua

doi:10.1007/s10965-017-1432-z

Cited by 16 publications

(10 citation statements)

References 48 publications

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“…The small reduction of the T onset indicates that the thermal stability was not significantly compromised. In the DSC run shown in Figure B, the pure PLA displays a glass temperature ( T g ) at 60.83 °C, a cold crystallization peak at 121.29 °C and a double melting peak of 152.58 and 157.14 °C, which is in good accordance with the literature. ,, The incorporated PHB-di-rub fillers at the various amounts in PLA matrix exhibited a single T g indicating that PHB-di-rub is likely to be miscible in the PLA matrix. ,, Yet, PHB-di-rub might also microphase separate into small domains in the matrix . As more PHB-di-rub filler was added, the overall T g of the biocomposites decreased as shown in Table .…”

Section: Resultssupporting

confidence: 85%

“…22,27,32 The incorporated PHBdi-rub fillers at the various amounts in PLA matrix exhibited a single T g indicating that PHB-di-rub is likely to be miscible in the PLA matrix. 39,49,50 Yet, PHB-di-rub might also microphase separate into small domains in the matrix. 51 As more PHB-dirub filler was added, the overall T g of the biocomposites decreased as shown in Table 1.…”

Section: ■ Results and Discussionmentioning

confidence: 93%

“…This increased free volume between the filler and the matrix, hence increasing the chain mobility of the polymer chains. 50 The incorporation of PHBdi-rub fillers also contributed to an exothermal coldcrystallization peak (T cc ) during the second heating cycle, similar to the neat PLA. This occurrence is resemblance by the sharp T cc peak observed in the initial crystalline PHB-diol.…”

Section: ■ Results and Discussionmentioning

confidence: 98%

See 2 more Smart Citations

Biodegradable PHB-Rubber Copolymer Toughened PLA Green Composites with Ultrahigh Extensibility

Yeo

Muiruri

Tan

et al. 2018

ACS Sustainable Chem. Eng.

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The sustainable biopolymer, poly(lactide) (PLA), has been intensely researched over the past decades because of its excellent biodegradability, renewability, and sustainability. The boundless potential of this sustainable biopolymer could resolve the adverse negative impact caused by the petroleum-based polymers. However, the inherent drawback of PLA such as brittleness, low heat distortion temperature, and slow recrystallization rate narrowed the broad applications in biomedical, automotive, and structural fields. In this study, we successfully synthesized a PHB-based filler (PHB-di-rub) displaying synergetic functions of (1) effective nucleation and (2) extreme toughening of the PLA matrix at only 5% (1.5 wt % PHB content). Remarkably, the storage modulus improves by 15%; tensile elongation extends by 57-fold (300% strain) and toughness by 38-fold while maintaining its original strength and stiffness. Likewise, 10% of PHB-di-rub (3 wt % PHB content) has an even higher improvement with a storage modulus improvement by 32%, elongation by 128-fold (680% strain), and toughness by 84-fold, with a marginal change in strength and stiffness. NMR results confirmed the structure of PHB-di-rub, where PHB acts as the rigid core and the poly(lactide-cocaprolactone) (DLA-co-CL) random copolymer confers the flexibility. DSC, WAXD, and POM display the excellent nucleating ability of PHB-di-rub. SEM shows the morphology of elongated fibrils structure with strong matrix−filler interaction and homogeneous filler dispersion. SAXS, WAXS, and WAXD elucidate the extreme toughening mechanism to be a combination of rubber-induced crazing effect and highly orientated PLA matrix with PHB-di-rub. The Herman's orientation function further quantifies the extreme elongation (680%) owing to the perfect alignment. This highly biodegradable biocomposite with high strength and toughness shows potential in replacing the current petroleum-based polymers, which open up to broader prospects in the biomedical, automotive, and structural application.

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Section: Resultssupporting

confidence: 85%

Section: ■ Results and Discussionmentioning

confidence: 93%

Section: ■ Results and Discussionmentioning

confidence: 98%

See 1 more Smart Citation

Biodegradable PHB-Rubber Copolymer Toughened PLA Green Composites with Ultrahigh Extensibility

Yeo

Muiruri

Tan

et al. 2018

ACS Sustainable Chem. Eng.

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“…Up to now, there have been many efforts by the scientific community to address these drawbacks and both chemical and physical approaches have been used for modulating PHB’s thermal and mechanical properties. Examples of chemical approaches already reported in the literature are copolymerization, − internal plasticization, , and grafting. , Common physical approaches are blending, − external plasticization, , and the use of nucleating agents and fillers. , One of the most interesting approaches from an industrial viewpoint is plasticization. Plasticizers comprise one of the major additive industries in the world due to their effectiveness in tuning polymer flexibility and improving processability. , A general rule is that plasticizers decrease polymer–polymer intra- and intermolecular interactions by filling the space between polymer chains, thus increasing the free volume, which leads to a decrease in the glass transition temperature. , Plasticizers can be classified as internal or external plasticizers. , The copolymerization of hydroxybutyrate (HB) and hydroxyvalerate (HV) to form poly(hydroxybutyrate- co -valerate) (PHBV) is a well-known approach to modulate the thermal and mechanical properties of PHB because the HV monomeric units act as internal plasticizers.…”

Section: Introductionmentioning

confidence: 99%

Plasticization of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) with an Oligomeric Polyester: Miscibility and Effect of the Microstructure and Plasticizer Distribution on Thermal and Mechanical Properties

2021

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In the last few decades, many efforts have been made to make poly(3-hydroxybutyrate) (PHB) and its copolymers more suitable for industrial production and large-scale use. Plasticization, especially using biodegradable oligomeric plasticizers, has been one of the strategies for this purpose. However, PHB and its copolymers generally present low miscibility with plasticizers. An understanding of the plasticizer distribution between the mobile and rigid amorphous phases and how this influences thermal, mechanical, and morphological properties remains a challenge. Herein, formulations of poly(hydroxybutyrate-co-valerate) (PHBV) plasticized with an oligomeric polyester based on lactic acid, adipic acid, and 1,2-propanediol (PLAP) were prepared by melt extrusion. The effects of the PLAP content on the processability, miscibility, and microstructure of the semicrystalline PHBV and on the thermal, morphological, and mechanical properties of the formulations were investigated. The compositions of the mobile and rigid amorphous phases of the PHBV/PLAP formulations were easily estimated by combining dynamic mechanical data and the Fox equation, which showed a heterogeneous distribution of PLAP in these two phases. An increase in the PLAP mass fraction in the formulations led to progressive changes in the composition of the amorphous phases, an increase of both crystalline lamellae and interlamellar layer thickness, and a decrease in the melting and glass transition temperatures as well as the PHBV stiffness. The Flory–Huggins interaction parameter varied with the formulation composition in the range of −0.299 to −0.081. The critical PLAP mass fraction of 0.37 obtained from thermodynamic data is close to the value estimated from dynamic mechanical analysis (DMA) data and the Fox equation. The mechanical properties showed a close relationship with the distribution of PLAP in the rigid and mobile amorphous phases as well as with the microstructure of the crystalline phase of PHBV in the formulations.

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“…Thermoplastic elastomers based on PLA, mainly triblock copolymers or multiblock copolymers, can be prepared. The prepolymers reported as flexible segments include polyethylene glycol (PEG) [28][29][30], polycaprolactone (PCL) [31,32], poly (3-hydroxybutyrate) (PHB) [33][34][35], polyethylene oxide (PEO) [36][37][38][39], poly (1,3-trimethylene carbonate) (PTMC) [40], polydimethylsiloxane (PDMS) [41,42] and so on. In lowmolecular weight block copolymers, the addition of chain extender or coupling agent can further improve their molecular weight, resulting in multi-block TPU.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of PLA-based thermoplastic elastomer and study on preparation and properties of PLA-based shape memory polymers

Fan

Weng

et al. 2019

Mater. Res. Express

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As a new functional polymer material, shape memory polymer (SMP) has many advantages, and can be widely used in medical devices, textiles, aerospace and other fields. For thermal response SMPs, temporary deformation can be stored under external force above T g with a rapid cooling down to below T g or T m , and when heated again to the critical temperature point, they return to their original shape. In this paper, shape memory poly (lactic acid) (PLA) block copolymers were prepared from a chain extension reaction of PLA with poly(ε-caprolactone) diol (PCL-OH). Using hexamethylene diisocyanate (HDI) as a chain extender, the molecular weight of the prepolymer could be greatly increased by melt chain extension. Polylactic acid thermoplastic elastomer (PLAE) synthesized by chain extension reaction is soft and tough, similar to thermoplastic polyurethane (TPU). Polylactic acid-based shape memory polymers with good shape memory properties can be obtained by blending PLAE with PLA. The shape memory property test showed that the polylactic acid-based shape memory polymer was successfully prepared, and the recovery rate of the polylactic acid-based shape memory polymer could reach to approximately 80%. Besides, we also did thermal and microstructural analysis of the blend material. Due to their good biocompatibility and biodegradability, PLAE and PLA/PLAE will have potential applications in biomedical implant materials, engineering plastics, and textiles.

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Studies on the alcoholysis of poly(3-hydroxybutyrate) and the synthesis of PHB-b-PLA block copolymer for the preparation of PLA/PHB-b-PLA blends

Cited by 16 publications

References 48 publications

Biodegradable PHB-Rubber Copolymer Toughened PLA Green Composites with Ultrahigh Extensibility

Biodegradable PHB-Rubber Copolymer Toughened PLA Green Composites with Ultrahigh Extensibility

Plasticization of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) with an Oligomeric Polyester: Miscibility and Effect of the Microstructure and Plasticizer Distribution on Thermal and Mechanical Properties

Synthesis of PLA-based thermoplastic elastomer and study on preparation and properties of PLA-based shape memory polymers

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