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脂肪族-芳香族共聚酯与纤维素纳米晶体的生物可吸收纳米复合材料的结构与生物相容性

Structure and Biocompatibility of Bioabsorbable Nanocomposites of Aliphatic-Aromatic Copolyester and Cellulose Nanocrystals.

作者信息

Kashani Rahimi Shahab, Aeinehvand Robabeh, Kim Kyoungtae, Otaigbe Joshua U

机构信息

School of Polymers and High Performance Materials, The University of Southern Mississippi , 118 College Drive, Hattiesburg, Mississippi, United States.

Nano-Biopolymers Research Laboratory, Department of Chemical Engineering, College of Engineering, University of Tehran , P.O. Box 11155-4563, Tehran, Iran.

出版信息

Biomacromolecules. 2017 Jul 10;18(7):2179-2194. doi: 10.1021/acs.biomac.7b00578. Epub 2017 Jun 27.

Abstract

Poly(butylene adipate-co-terephthalate) (PBAT) was first chemically modified via free radical grafting with maleic anhydride (MA) and the MA-g-PBAT graft copolymer was then used as a matrix material to obtain cellulose nanocrystal (CNC)-reinforced MA-g-PBAT bionanocomposites via reactive extrusion process to accelerate efforts to develop functional bioabsorbable polymer nanocomposites with improved properties. The molecular structure of the PBAT after chemical modification with maleic anhydride was confirmed by H NMR and FTIR spectroscopy. The morphological observation of the nanocomposites revealed that the CNCs were finely dispersed in the matrix. Thermal analysis of the hybrids showed an improvement of the thermal stability of the nanocomposites upon increasing the CNC content. In addition, it was found that the CNC nucleated crystallization of the PBAT in the nanocomposites. Extensive melt rheological characterization of the nanocomposite samples revealed a significant improvement of the viscoelastic properties of the matrix due to the strong interfacial adhesion of the CNC particles to the PBAT. Further, development of the nonterminal characteristics of the viscoelastic material functions and exhibition of yield stress were correlated with the evolution of a 3D-netowork nanostructure of CNCs in the matrix. This CNC nanostructure was interpreted in the framework of scaling theory of fractal elastic gels, and found to be consistent with the structure of open-porous flocs. Tensile testing of the samples showed considerable improvement in the modulus and ultimate strength of the samples with increasing the CNC content. In addition, a positive shift of the glass transition temperature was found in dynamic mechanical analysis. Finally, in vitro biocompatibility using Thiazolyl blue tetrazolium bromide (MTT) assay and cell adhesion studies with L929 fibroblast cells revealed no cytotoxic effect of CNCs, confirming the biocompatibility of the nanocomposites and the associated significant improvement of cell adhesion, suggesting the potential applicability of this nanocomposite in biomedical and tissue engineering applications.

摘要

聚己二酸丁二醇酯-对苯二甲酸丁二醇酯(PBAT)首先通过与马来酸酐(MA)进行自由基接枝进行化学改性,然后将MA-g-PBAT接枝共聚物用作基体材料,通过反应挤出工艺获得纤维素纳米晶(CNC)增强的MA-g-PBAT生物纳米复合材料,以加速开发具有改进性能的功能性生物可吸收聚合物纳米复合材料的进程。通过1H NMR和FTIR光谱证实了用马来酸酐化学改性后PBAT的分子结构。纳米复合材料的形态观察表明,CNC在基体中分散良好。对杂化物的热分析表明,随着CNC含量的增加,纳米复合材料的热稳定性有所提高。此外,发现CNC在纳米复合材料中使PBAT成核结晶。对纳米复合材料样品进行的广泛熔体流变学表征表明,由于CNC颗粒与PBAT之间的强界面粘附力,基体的粘弹性性能有了显著改善。此外,粘弹性材料功能的非末端特性的发展和屈服应力的表现与基体中CNC的三维网络纳米结构的演变相关。这种CNC纳米结构在分形弹性凝胶的标度理论框架内进行了解释,发现与开孔絮凝物的结构一致。对样品的拉伸测试表明,随着CNC含量的增加,样品的模量和极限强度有了相当大的提高。此外,在动态力学分析中发现玻璃化转变温度有正向偏移。最后,使用噻唑蓝四氮唑溴盐(MTT)测定法进行的体外生物相容性研究以及与L929成纤维细胞的细胞粘附研究表明,CNC没有细胞毒性作用,证实了纳米复合材料的生物相容性以及细胞粘附的显著改善,表明这种纳米复合材料在生物医学和组织工程应用中的潜在适用性。

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