双功能性植物源提取物/脂肪族聚酯PBS复合材料的界面作用机理及相容性调控

Based on the drawbacks about toxic, carcinogenic, cannot be recycled and single function of synthetic dyes and inorganic, synthetic organic antibacterial agents, this project intends to apply the plant-derived extracts with common colored compounds into biodegradable materials, which will bring the pharmacological activity of the extracts in full and make it give dyeing and antibacterial bifunctional to aliphatic polyester PBS. At the same time, based on the defects of that the main ingredients in the plant-derived extracts were water-soluble components, controlling the compatibility of the composites in theory is necessary. With adopting flavonoids, anthraquinones and polyhydric phenolic as the representative of hydrophilic plant-derived extracts, the effects of different extracts on the performance of PBS, the same kind of extract but different effective components on the performance of PBS, and the molecular dynamics simulation of the single extracts component with PBS were studied. The proposed is to reveal the interface mechanism of the composites, establish the interface mechanism control guidance for compatibility and achieve compatibility control regulation of extracts and aliphatic polyester in improving the dyeing and antibacterial function of the composites initiative. The technical basis for design and application of the environmentally friendly color antibacterial composites will be provided.

基于合成染料、无机及合成有机抗菌剂有毒、致癌等危害，不可循环利用且功能单一的弊端，本项目拟将普遍存在有色化合物的植物源提取物应用于可生物降解材料，充分发挥提取物的药理活性，赋予脂肪族聚酯PBS染色及抗菌双功能性。同时基于植物源提取物中以水溶性成分为主的缺陷，从理论上对复合材料相容性进行调控成为必然。拟采用黄酮类、蒽醌类以及多元酚类亲水性植物源提取物为代表，通过研究不同种类提取物对PBS性能的影响规律、相同种类提取物不同有效组分对PBS性能的影响规律，结合提取物单一组分与PBS的分子动力学模拟，揭示复合材料的界面作用机理，建立复合材料界面作用机理对相容性的调控指导，实现亲水性植物源提取物与脂肪族聚酯PBS相容性调控对复合材料染色、抗菌功能性的主动提高，为环境友好型彩色抗菌复合材料的设计和应用提供技术依据。

抗菌塑料的开发为保护人类健康树起了一道绿色屏障，但基于合成染料、无机及有机抗菌剂有毒、致癌等危害，本研究将具有染色、抗菌功能性的植物源提取物应用于可生物降解材料，以阐明亲水性植物源提取物/脂肪族聚酯PBS复合材料的界面作用机理并对相容性调控为出发点，建立不同种类提取物与PBS基脂肪族聚酯间的相容性调控规律，实现对染色、抗菌功能性的主动提高。具体工作如下：.对黄酮类、蒽醌类、多元酚类等多种不同化学属的植物源提取物进行了提取，为无定形粉末，对热、对光基本稳定，耐酸碱性优良，其有效活性物质对大肠杆菌的抑制效果大于对金黄色葡萄球菌。将所提取的植物源提取物与PBS共混，不同种类植物源提取物只与PBS进行了共混，且提取物成分中的-OH均作为给电子基与PBS发生了氢键作用。植物源提取物/PBS复合材料的降解速率明显要高于PBS，其抗大肠杆菌的能力同样高于金黄色葡萄球菌。.通过硅烷偶联剂KH-550、钛酸酯偶联剂NDZ-201对不同种类植物源提取物修饰；以壳聚糖（CS）和羟丙基-β-环糊精（H-β-CD）为壁材，植物源提取物为芯材制备微胶囊并与PBS复合；采用乙酰氯、异丁酰氯、苯甲酰氯对植物源提取物化学改性后与PBS制备复合材料，均发现提取物修饰后，修饰物均与复合材料产生了分子间相互作用或化学反应，使得复合材料的界面相容性增强。将所提取的植物源提取物与PBS-OH、PBS-COOH以及其他PBS改性产物（GTA-PBS、Glu-PBS、N-PBS、P-PBS、多羟基PBS）复合，植物源提取物/PBS改性产物的相容性均有不同程度的提高，其染色特性及抗菌功能性有所改善。.不同种类植物源提取物/PBS复合材料体系的内聚能密度均大于400 J/cm3，溶解度参数大于20 (J/cm3)1/2，同样表明不同复合体系中分子之间具有一定的相互作用。各种改性后复合材料的结合能（Eij）良好，混合能（Emix）和Huggins–Flory相互作用参数（χ）更接近于0，体系的相容性更好。分子动力学模拟表明，改性复合体系分子间存在静电能、氢键作用和范德华能，使得复合材料的界面相容性得以提高，其染色和抗菌功能性进一步实现。