A Hierarchical Model To Understand the Processing of Polysaccharides/Protein-Based Films in Ionic Liquids
A Hierarchical Model To Understand the Processing of Polysaccharides/Protein-Based Films in Ionic Liquids
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DOI：
10.1021/acs.biomac.8b00903
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发表时间：
2018-10-01
影响因子：
6.2
通讯作者：
Salas-de la Cruz, David
中科院分区：
文献类型：
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作者：
Hadadi, Amnah;Whittaker, John W.;Salas-de la Cruz, David
近年来，来自丰富和可再生资源的生物材料在医学和材料科学方面显示出潜力。在这项研究中，我们结合联合收割机的理论建模，分子动力学模拟，和几个实验技术，以了解再生纤维素/丝，甲壳素/丝，和壳聚糖/丝为基础的生物复合材料后，在离子液体中溶解和再生水。我们提出了一种新的理论模型，该模型将复合材料的微观结构与其整体性能相关联。我们依赖于建模非交联的生物聚合物，目前层状结构，如β-片层，我们成功地预测这些生物分子的混合物的结构，热，和机械性能。我们的模型和实验表明，纯物质在所选溶剂中的溶解度可用于调节生物聚合物共混物的结晶度的量，如通过衰减全反射傅里叶变换红外光谱法（ATR-FTIR）测量的。热重分析（TGA）表明，混合生物复合材料的分解温度相比，其纯对应物降低，根据我们的理论预测。通过扫描电子显微镜（SEM）进一步表征材料的形态，并根据共混物显示不同的暴露表面积。最后，进行差示扫描量热法（DSC）来表征材料中的残留水含量，这对于解释水中的再生过程至关重要。作为该模型的最后测试，我们比较我们的模型的预测杨氏模量与现有的数据在文献中。该模型正确地再现实验中观察到的杨氏模量的变化，由于在生物聚合物共混物中的丝的浓度。
In recent years, biomaterials from abundant and renewable sources have shown potential in medicine and materials science alike. In this study, we combine theoretical modeling, molecular dynamics simulations, and several experimental techniques to understand the regeneration of cellulose/silk-, chitin/silk-, and chitosan/silk-based biocomposites after dissolution in ionic liquid and regeneration in water. We propose a novel theoretical model that correlates the composite's microscopic structure to its bulk properties. We rely on modeling non-cross-linked biopolymers that present layer-like structures such as beta-sheets and we successfully predict structural, thermal, and mechanical properties of a mixture of these biomolecules. Our model and experiments show that the solubility of the pure substance in the chosen solvent can be used to modulate the amount of crystallinity of the biopolymer blend, as measured by attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR). Thermogravimetric analysis (TGA) shows that the decomposition temperature of the blended biocomposites compared to their pure counterparts is reduced in accordance with our theoretical predictions. The morphology of the material is further characterized through scanning electron microscopy (SEM) and shows differently exposed surface area depending on the blend. Finally, differential scanning calorimetry (DSC) is performed to characterize the residual water content in the material, essential for explaining the regeneration process in water. As a final test of the model, we compare our model's prediction of the Young's modulus with existing data in the literature. The model correctly reproduces experimental trends observed in the Young's modulus due to varying the concentration of silk in the biopolymer blend.