生物活性香菇多糖衍生物表面修饰聚氨酯材料的研究
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摘要
生物医用高分子材料是一类可对有机体组织进行修复、替代与再生,具有特殊功能作用的新型高技术合成高分子材料,不仅技术含量和经济价值高,而且对人类的健康生活和社会发展具有极其重大的意义,它已渗入到医学和生命科学的各个部门并应用于临床的诊断与治疗。
对于医用高分子材料而言,材料的生物相容性至关重要,而在不改变材料本体性质的前提下实施表面修饰是一种重要而相对实用的手段之一。本研究首先从香菇子实体中提取香菇多糖,分别对其进行羧甲基和硫酸酯衍生化修饰,再将其固定到聚氨酯基材表面改善其生物相容性,并研究了通过不同方法将香菇多糖衍生物固定在聚氨酯基材表面后其表面性能的变化。
本工作首先对聚氨酯基材表面进行氨基化,然后通过层层自组装的方法将带正电荷的壳聚糖和带负电荷的香菇多糖硫酸酯固定在官能化后的聚氨酯基材表面。水接触角测试表明经表面修饰后的聚氨酯亲水性得到明显提高,并且组装层具有较好的稳定性；通过蛋白吸附测试表明表面修饰后的聚氨酯材料具有良好的排斥蛋白质非特异性吸附的能力,纤维蛋白原的吸附量与未修饰聚氨酯相比下降了81%；通过抗菌活性测试可知,表面修饰后的聚氨酯材料具有一定抑制绿脓杆菌的效果,其抗菌率为57.6%；此外,L-929小鼠成纤维细胞能够较好地在修饰后的聚氨酯材料表面生长繁殖。
对于聚氨酯材料表面层层自组装香菇多糖硫酸酯和纳米银粒子的修饰,首先对表面氨基化的聚氨酯基材在带负电荷的香菇多糖硫酸酯溶液和带正电荷的PEI-AgNO3溶液中进行层层自组装,自组装五个双分子层后,再通过NaBH4的还原作用将Ag+还原为Ag0,从而得到表面带有纳米银粒子和香菇多糖硫酸酯的聚氨酯材料。经表面修饰后的材料表面对纤维蛋白原的吸附量下降了41%,对大肠杆菌的抑菌率为63%。
本研究通过层层自组装和化学接枝的方法采用香菇多糖衍生物对生物医用高分子材料进行表面修饰,该研究将对利用真菌多糖及其衍生物进行医用高分子材料表面修饰的研究,以及制备具有特殊生物活性的新型医用高分子材料的研究提供了新的方法和思路。
Biomedical polymer material is one of advanced hi-tech materials which have special functions on repairation, replacement and regeneration of organic tissues. It has not only highly economic values but also has great applications to human health and society development.
Biocompatibility is one of the most important characteristic of biomedical polymer material. Surface modification is an important and useful method to improve the surface properties but not damage the bulk properties of the material. In this study, lentinan extracted from shiitake mushroom was sulfated and carboxymethylated to afford two water-soluble polysaccharides, respectively. Then, the lentinan derivatives were immobilized onto the surface of polyurethane by different methods.
Positively charged amino groups were introduced to the surface of polyurethane. Then, positively charged chitosan and negatively charged lentinan sulfate were alternatively deposited onto polyurethane surface through layer-by-layer self-assembly technique. The results showed that the water contact angle decreased gradually during the progressive buildup of the polyelectrolyte multilayers, and reached a steady value after five bilayers were assembled. At the same time, the fibrinogen adsorption decreased 80% and reached a steady value after five bilayers. In addition, the modified PU possessed antibacterial activity against Pseudomonas aeruginosa, the number of viable bacteria on the modified surface decreased by 57%.
PEI-AgNO3 and lentinan sulfate were alternatively deposited onto polyurethane surface through layer-by-layer self-assembly technique. Then, a composite film containing Ag nanoparticals was obtained through the reducion reaction between Ag ions and NaBH4. The adsorption of fibrinogen decreased 41%, compared with unmodified polyurethane. In addition, the modified PU possessed antibacterial activity against Escherichia coli.
The results of this foundation research have scientific significance and application value. These works have scientific significance and application value for preparing biocompatible materials with specific bioactivity, such as antibacterial, antitumor, or antiviral bioactivity.
对于医用高分子材料而言,材料的生物相容性至关重要,而在不改变材料本体性质的前提下实施表面修饰是一种重要而相对实用的手段之一。本研究首先从香菇子实体中提取香菇多糖,分别对其进行羧甲基和硫酸酯衍生化修饰,再将其固定到聚氨酯基材表面改善其生物相容性,并研究了通过不同方法将香菇多糖衍生物固定在聚氨酯基材表面后其表面性能的变化。
本工作首先对聚氨酯基材表面进行氨基化,然后通过层层自组装的方法将带正电荷的壳聚糖和带负电荷的香菇多糖硫酸酯固定在官能化后的聚氨酯基材表面。水接触角测试表明经表面修饰后的聚氨酯亲水性得到明显提高,并且组装层具有较好的稳定性；通过蛋白吸附测试表明表面修饰后的聚氨酯材料具有良好的排斥蛋白质非特异性吸附的能力,纤维蛋白原的吸附量与未修饰聚氨酯相比下降了81%；通过抗菌活性测试可知,表面修饰后的聚氨酯材料具有一定抑制绿脓杆菌的效果,其抗菌率为57.6%；此外,L-929小鼠成纤维细胞能够较好地在修饰后的聚氨酯材料表面生长繁殖。
对于聚氨酯材料表面层层自组装香菇多糖硫酸酯和纳米银粒子的修饰,首先对表面氨基化的聚氨酯基材在带负电荷的香菇多糖硫酸酯溶液和带正电荷的PEI-AgNO3溶液中进行层层自组装,自组装五个双分子层后,再通过NaBH4的还原作用将Ag+还原为Ag0,从而得到表面带有纳米银粒子和香菇多糖硫酸酯的聚氨酯材料。经表面修饰后的材料表面对纤维蛋白原的吸附量下降了41%,对大肠杆菌的抑菌率为63%。
本研究通过层层自组装和化学接枝的方法采用香菇多糖衍生物对生物医用高分子材料进行表面修饰,该研究将对利用真菌多糖及其衍生物进行医用高分子材料表面修饰的研究,以及制备具有特殊生物活性的新型医用高分子材料的研究提供了新的方法和思路。
Biomedical polymer material is one of advanced hi-tech materials which have special functions on repairation, replacement and regeneration of organic tissues. It has not only highly economic values but also has great applications to human health and society development.
Biocompatibility is one of the most important characteristic of biomedical polymer material. Surface modification is an important and useful method to improve the surface properties but not damage the bulk properties of the material. In this study, lentinan extracted from shiitake mushroom was sulfated and carboxymethylated to afford two water-soluble polysaccharides, respectively. Then, the lentinan derivatives were immobilized onto the surface of polyurethane by different methods.
Positively charged amino groups were introduced to the surface of polyurethane. Then, positively charged chitosan and negatively charged lentinan sulfate were alternatively deposited onto polyurethane surface through layer-by-layer self-assembly technique. The results showed that the water contact angle decreased gradually during the progressive buildup of the polyelectrolyte multilayers, and reached a steady value after five bilayers were assembled. At the same time, the fibrinogen adsorption decreased 80% and reached a steady value after five bilayers. In addition, the modified PU possessed antibacterial activity against Pseudomonas aeruginosa, the number of viable bacteria on the modified surface decreased by 57%.
PEI-AgNO3 and lentinan sulfate were alternatively deposited onto polyurethane surface through layer-by-layer self-assembly technique. Then, a composite film containing Ag nanoparticals was obtained through the reducion reaction between Ag ions and NaBH4. The adsorption of fibrinogen decreased 41%, compared with unmodified polyurethane. In addition, the modified PU possessed antibacterial activity against Escherichia coli.
The results of this foundation research have scientific significance and application value. These works have scientific significance and application value for preparing biocompatible materials with specific bioactivity, such as antibacterial, antitumor, or antiviral bioactivity.
引文
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