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Effect of Block Length and Stereocomplexation on the Thermally Processable Poly(ε-caprolactone) and Poly(Lactic acid) Block Copolymers for Biomedical Applications
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2019-10-30 00:00:00 , DOI: 10.1021/acsapm.9b00789 Neha Mulchandani 1 , Arvind Gupta 1 , Kazunari Masutani 2 , Sachin Kumar 3 , Shinichi Sakurai 2 , Yoshiharu Kimura 2 , Vimal Katiyar 1
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2019-10-30 00:00:00 , DOI: 10.1021/acsapm.9b00789 Neha Mulchandani 1 , Arvind Gupta 1 , Kazunari Masutani 2 , Sachin Kumar 3 , Shinichi Sakurai 2 , Yoshiharu Kimura 2 , Vimal Katiyar 1
Affiliation
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The current research concentrates on the synthesis of linear block copolymers with their backbone consisting of hard and soft segments, that is, poly(L-lactic acid) (PLLA)/ poly(D-lactic acid) (PDLA) and poly(ε-caprolactone) (PCL), with the detailed investigation of the effect of block length on the thermal, mechanical, and crystallization behavior followed by their processing and biocompatibility evaluation. In the current work, sequential ring opening polymerization has been employed wherein PCL is used as a macroinitiator for the synthesis of diblock (PCL-PDLA and PCL-PLLA) and stereotriblock copolymers (PCL-PLLA-PDLA) of targeted molecular weight, which is confirmed by 1H NMR spectroscopy. The block length of PCL, in the case of diblock copolymer, is fixed; however, that of PLLA or PDLA is varied, and the enantiomeric blends thereof are made to achieve the merits of stereocomplexation. The length of the individual blocks is the same in the case of stereotriblock copolymer. The presence of two crystalline domains is manifested from differential scanning calorimetry and thermogravimertric analysis. An interesting improvement in the mechanical properties is observed upon increasing the block length of PDLA/PLLA in the block copolymer system which may be ascribed to the confined crystalliztion of PCL in the microdomain structure. Additionally, the synthesized materials are found to support the adhesion of MG-63 (human bone osteoscarcoma) cells as determined from in vitro studies indicating their potential in bone repair and regeneration. Further, the block copolymers possessing superior mechanical properties are thermally processed by injection molding to fabricate representative orthopedic fixation devices such as cancellous and cortical bone screws. Eventually, the thermo-mechanical stability of the cancellous bone screw made from the synthesized block copolymer is presented as compared to that made from the commercial PLA at the sterilization temperature of the biomedical devices.
中文翻译：
嵌段长度和立体配合对生物医学应用可热加工的聚（ε-己内酯）和聚（乳酸）嵌段共聚物的影响
当前的研究集中在线性嵌段共聚物的合成上，这些骨架的骨架由硬链段和软链段组成，即聚（L-乳酸）（PLLA）/聚（D-乳酸）（PDLA）和聚（ε-己内酯）（PCL），并详细研究了嵌段长度对热，机械和结晶行为的影响，然后对其加工和生物相容性进行了评估。在当前工作中，已采用顺序开环聚合，其中将PCL用作大分子引发剂，以合成目标分子量的二嵌段（PCL-PDLA和PCL-PLLA）和立体三嵌段共聚物（PCL-PLLA-PDLA）。由1确认1 H NMR光谱。在二嵌段共聚物的情况下，PCL的嵌段长度是固定的；然而，PLLA或PDLA的那些是变化的，并且制备其对映体共混物以实现立体复合的优点。在立体三嵌段共聚物的情况下，各个嵌段的长度是相同的。差示扫描量热法和热重分析法表明存在两个晶域。通过增加嵌段共聚物体系中PDLA / PLLA的嵌段长度，可以观察到机械性能的有趣改善，这可以归因于PCL在微区结构中的有限结晶。此外，从体外测定，发现合成材料可支持MG-63（人骨骨肉瘤）细胞的粘附研究表明它们在骨骼修复和再生中的潜力。此外，通过注射成型对具有优异机械性能的嵌段共聚物进行热处理，以制造代表性的骨科固定装置，例如松质和皮质骨螺钉。最终，与在生物医学装置的灭菌温度下由市售PLA制成的松质骨螺钉相比，呈现了由合成的嵌段共聚物制成的松质骨螺钉的热机械稳定性。
更新日期：2019-10-30
中文翻译：
嵌段长度和立体配合对生物医学应用可热加工的聚（ε-己内酯）和聚（乳酸）嵌段共聚物的影响
当前的研究集中在线性嵌段共聚物的合成上，这些骨架的骨架由硬链段和软链段组成，即聚（L-乳酸）（PLLA）/聚（D-乳酸）（PDLA）和聚（ε-己内酯）（PCL），并详细研究了嵌段长度对热，机械和结晶行为的影响，然后对其加工和生物相容性进行了评估。在当前工作中，已采用顺序开环聚合，其中将PCL用作大分子引发剂，以合成目标分子量的二嵌段（PCL-PDLA和PCL-PLLA）和立体三嵌段共聚物（PCL-PLLA-PDLA）。由1确认1 H NMR光谱。在二嵌段共聚物的情况下，PCL的嵌段长度是固定的；然而，PLLA或PDLA的那些是变化的，并且制备其对映体共混物以实现立体复合的优点。在立体三嵌段共聚物的情况下，各个嵌段的长度是相同的。差示扫描量热法和热重分析法表明存在两个晶域。通过增加嵌段共聚物体系中PDLA / PLLA的嵌段长度，可以观察到机械性能的有趣改善，这可以归因于PCL在微区结构中的有限结晶。此外，从体外测定，发现合成材料可支持MG-63（人骨骨肉瘤）细胞的粘附研究表明它们在骨骼修复和再生中的潜力。此外，通过注射成型对具有优异机械性能的嵌段共聚物进行热处理，以制造代表性的骨科固定装置，例如松质和皮质骨螺钉。最终，与在生物医学装置的灭菌温度下由市售PLA制成的松质骨螺钉相比，呈现了由合成的嵌段共聚物制成的松质骨螺钉的热机械稳定性。
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