Department of Engineering and Technology of Polymers, Faculty of Chemistry, Wrocław University of Science and Technology, Wyb. Wyspiańskiego 27, 50-370 Wrocław, Poland.
Department of Mechanics, Materials and Biomedical Engineering, Faculty of Mechanical Engineering, Wroclaw University of Science and Technology, Wyb. Wyspiańskiego 27, 50-370 Wrocław, Poland.
Int J Mol Sci. 2020 Sep 13;21(18):6711. doi: 10.3390/ijms21186711.
Novel biocomposites of poly(L-lactide) (PLLA) and poly(l-lactide-co-glycolide) (PLLGA) with 10 wt.% of surface-modified hydroxyapatite particles, designed for applications in bone tissue engineering, are presented in this paper. The surface of hydroxyapatite (HAP) was modified with polyethylene glycol by using l-lysine as a linker molecule. The modification strategy fulfilled two important goals: improvement of the adhesion between the HAP surface and PLLA and PLLGA matrices, and enhancement of the osteological bioactivity of the composites. The surface modifications of HAP were confirmed by attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR), TGA, and elemental composition analysis. The influence of hydroxyapatite surface functionalization on the thermal and in vitro biological properties of PLLA- and PLLGA-based composites was investigated. Due to HAP modification with polyethylene glycol, the glass transition temperature of PLLA was reduced by about 24.5 °C, and melt and cold crystallization abilities were significantly improved. These achievements were scored based on respective shifting of onset of melt and cold crystallization temperatures and 1.6 times higher melt crystallization enthalpy compared with neat PLLA. The results showed that the surface-modified HAP particles were multifunctional and can act as nucleating agents, plasticizers, and bioactive moieties. Moreover, due to the presented surface modification of HAP, the crystallinity degree of PLLA and PLLGA and the polymorphic form of PLLA, the most important factors affecting mechanical properties and degradation behaviors, can be controlled.
本文介绍了一种新型的聚（L-丙交酯）（PLLA）和聚（L-丙交酯-共-乙交酯）（PLLGA）的生物复合材料，其中含有 10wt%的经过表面改性的羟基磷灰石（HAP）颗粒，设计用于骨组织工程应用。HAP 的表面通过赖氨酸作为连接分子与聚乙二醇进行了改性。这种改性策略实现了两个重要目标：改善 HAP 表面与 PLLA 和 PLLGA 基质之间的粘附力，以及增强复合材料的骨生物活性。通过衰减全反射傅里叶变换红外光谱（ATR-FTIR）、热重分析（TGA）和元素组成分析证实了 HAP 的表面改性。研究了 HAP 表面功能化对基于 PLLA 和 PLLGA 的复合材料的热性能和体外生物性能的影响。由于 HAP 与聚乙二醇的改性，PLLA 的玻璃化转变温度降低了约 24.5°C，熔融和冷结晶能力得到了显著提高。这些成就是基于熔融和冷结晶起始温度的相应偏移以及比纯 PLLA 高 1.6 倍的熔融结晶焓来衡量的。结果表明，表面改性的 HAP 颗粒具有多功能性，可以作为成核剂、增塑剂和生物活性基团。此外，由于 HAP 的表面改性，PLLA 和 PLLGA 的结晶度和 PLLA 的多晶型形式，这些是影响机械性能和降解行为的最重要因素，可以得到控制。
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