Multiphase blends of poly(lactic acid) (PLA), ethylene-methyl acrylate-glycidyl methacrylate (EMA-GMA) terpolymer, and a series of renewable poly(ether-b-amide) elastomeric copolymer (PEBA) were fabricated through reactive melt blending in an effort to improve the toughness of the PLA. Supertoughened PLA blend showing impact strength of ∼500 J/m with partial break impact behavior was achieved at an optimized blending ratio of 70 wt % PLA, 20 wt % EMA-GMA, and 10 wt % PEBA. Miscibility and thermal behavior of the binary blends PLA/PEBA and PLA/EMA-GMA, and the multiphase blends were also investigated through differential scanning calorimetric (DSC) and dynamic mechanical analysis (DMA). Phase morphology and fracture surface morphology of the blends were studied through scanning electron microscopy (SEM) and atomic force microscopy (AFM) to understand the strong corelation between the morphology and its significant effect on imparting tremendous improvement in toughness. A unique "multiple stacked structure" with partial encapsulation of EMA-GMA and PEBA minor phases was observed for the PLA/EMA-GMA/PEBA (70/20/10) revealing the importance of particular blend composition in enhancing the toughness. Toughening mechanism behind the supertoughened PLA blends have been established by studying the impact fractured surface morphology at different zones of fracture. Synergistic effect of good interfacial adhesion and interfacial cavitations followed by massive shear yielding of the matrix was believed to contribute to the enormous toughening effect observed in these multiphase blends.
A ternary blend of entirely biodegradable polymers, namely polylactide (PLA), poly(3-hydroxybutyrate-co-hydroxyvalerate) (PHBV), and poly(butylene succinate) (PBS), was first melt-compounded in an effort to prepare novel fully biodegradable materials with an excellent balance of properties. The miscibility, morphology, thermal behavior, mechanical properties, and thermal resistance of the blends were investigated. DMA analysis revealed that PHBV and PLA showed some limited miscibility with each other, but PBS is immiscible with PLA or PHBV. Minor phase-separated structure was observed from SEM for all the blends composition except PHBV/PLA/PBS 60/30/10 blend, which formed a typical mixture of core-shell morphology. The morphologies were verified by analysis of the spreading coefficients. Excellent stiffness-toughness balance was achieved by ternary blends of PLA, PHBV, and PBS. Significant enhancement of the toughness and flexibility of PLA was achieved by the incorporation of PBS and PHBV without sacrificing the strength apparently. Both the stiffness and toughness were improved for PHBV in the ternary blends with PHBV as matrix. The crystallization of the PLA and PBS were enhanced by presence of PHBV in the blends, while the crystallization of PHBV was confined by PLA and PBS phases. Moreover, the thermal resistances and melt flow properties of the materials were also studied by analysis of the heat deflection temperature (HDT) and melt flow index (MFI) value in the work.
Poly(lactic acid) (PLA), one of the widely studied renewable resource based biopolymers, has yet to gain a strong commercial standpoint because of certain property limitations. This work is a successful attempt in achieving PLA biocomposites that showed concurrent improvements in impact strength and heat deflection temperature (HDT). Biocomposites were fabricated from a super toughened ternary blend of PLA, poly(ether-b-amide) elastomeric copolymer and ethylene-methyl acrylate-glycidyl methacrylate and miscanthus fibers. The effects of varying the processing parameters and addition of various nucleating agents were investigated. Crystallinity was controlled by optimizing the mold temperature and cycle time of the injection process. With the addition of 1 wt % aromatic sulfonate derivative (Lak-301) as a nucleating agent at a mold temperature of 110 °C, PLA biocomposites exhibited dramatic reduction in crystallization half time to 1.3 min with crystallinity content of 42%. Mechanical and thermal properties assessment for these biocomposites revealed a 4-fold increase in impact strength compared to neat PLA. The HDT of PLA biocomposites increased to 85 °C from 55 °C compared to neat PLA. Crystallization behavior was studied in detail using differential scanning calorimetry and was supported with observations from wide-angle X-ray diffraction profiles and polarized optical microscopy. The presence of a nucleating agent did not alter the crystal structure of PLA; however, a significant difference in spherulite size, crystallization rate and content was observed. Fracture surface morphology and distribution of nucleating agent in the PLA biocomposites were investigated through scanning electron microscopy.
Polylactide (PLA) was melt blended with a biodegradable hyperbranched poly(ester amide) (HBP) to enhance its flexibility and toughness without sacrificing comprehensive performance. The advantage of using HBP was due to its unique spherical shape, low melt viscosity, and abundant functional end groups together with its easy access. Rheological measurement showed that blending PLA with as little as 2.5% HBP resulted in a 40% reduction of melt viscosity. The glass transition temperature (T g) of PLA in the blends decreased slightly with the increase of HBP content, indicating partial miscibility which resulted from intermolecular interactions via H-bonding. The H-bonding involving CO of PLA with OH and NH of HBP was evidenced by FTIR analysis for the first time. The HBP component, as a heterogeneous nucleating agent, accelerated the crystallization rate of PLA. Remarkably, with the increase of HBP content, the elongation at break of PLA blends dramatically increased without severe loss in tensile strength, even the tensile strength increased within 10% content of HBP. The stress−strain curves and the SEM photos of impact-fractured surface showed the material changed from brittle to ductile failure with the addition of HBP. Reasonable interfacial adhesion via H-bonding and finely dispersed particulate structure of HBP in PLA were proposed to be responsible for the improved mechanical properties.
The study of structural and functional magnetic resonance imaging data has greatly benefitted from the development of sophisticated and efficient algorithms aimed at automating and optimizing the analysis of brain data. We address, in the context of the segmentation of brain from non-brain tissue (i.e., brain extraction, also known as skull-stripping), the tension between the increased theoretical and clinical interest in patient data, and the difficulty of conventional algorithms to function optimally in the presence of gross brain pathology. Indeed, because of the reliance of many algorithms on priors derived from healthy volunteers, images with gross pathology can severely affect their ability to correctly trace the boundaries between brain and non-brain tissue, potentially biasing subsequent analysis. We describe and make available an optimized brain extraction script for the pathological brain (optiBET) robust to the presence of pathology. Rather than attempting to trace the boundary between tissues, optiBET performs brain extraction by (i) calculating an initial approximate brain extraction; (ii) employing linear and non-linear registration to project the approximate extraction into the MNI template space; (iii) back-projecting a standard brain-only mask from template space to the subject’s original space; and (iv) employing the back-projected brain-only mask to mask-out non-brain tissue. The script results in up to 94% improvement of the quality of extractions over those obtained with conventional software across a large set of severely pathological brains. Since optiBET makes use of freely available algorithms included in FSL, it should be readily employable by anyone having access to such tools.
Hydrogels are soft materials used in an array of biomedical applications. However, the in situ formation of hydrogels at target sites, particularly in dynamic in vivo environments, usually requires a prolonged gelation time and results in poor adhesion. These limitations cause considerable loss of both hydrogel mass and encapsulated therapeutic cargoes, thereby compromising treatment outcomes. Here, we report the development of a hydrogel based on thiourea-catechol reaction to enhance the bioadhesion. Compared with classical bioadhesive hydrogels, our hydrogels show enhanced mechanical properties, exceedingly short curing time, and pH-independent gelation with a much lower oxidant concentration. We further report the robust adhesion of our hydrogels to acidic gastric tissues and easy delivery to the porcine stomach via endoscopy. The delivered hydrogels adhered to ulcer sites in vivo for at least 48 hours. Hydrogel treatment of gastric ulcers in rodent and porcine models accelerated ulcer healing by suppressing inflammation and promoting re-epithelization and angiogenesis. The improved retention of proregenerative growth factors and reduced exposure to external catabolic factors after hydrogel application may contribute to the observed therapeutic outcomes. Our findings reveal a promising biomaterial-based approach for treating gastrointestinal diseases.
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