Hang Yingjie, Ma Jie, Li Siyuan, Zhang Xiaoyi, Liu Bing, Ding Zhaozhao, Lu Qiang, Chen Hong, Kaplan David L
College of Chemistry, Chemical Engineering and Materials Science & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215123, People's Republic of China.
Department of Burns, Gansu Provincial Hospital, Lanzhou 730000, People's Republic of China.
ACS Biomater Sci Eng. 2019 Jun 10;5(6):2762-2768. doi: 10.1021/acsbiomaterials.9b00369. Epub 2019 May 8.
Chemical modifications used with silk materials can be challenging due to heterogeneous reactions, in part due to the assembly state of the protein chains. Here, we assess factors that determine the efficiency of chemical modifications with silk materials. Unlike other natural macromolecules, silk presents changeable self-assembled or aggregation states in aqueous solution, which affect the chemical reactions based on reactive group distribution or accessibility. To confirm this hypothesis, silk nanofibers in various conformation and aggregation states in solution were exposed to the same reaction conditions. Amorphous silk nanofibers provided improved control for consistent chemical modification outcomes, while silk nanofibers with control of structure could be utilized to generate bifunctional materials through multiple chemical modifications. The results of the chemical modifications demonstrated that control of the conformational transitions of silk nanofibers provided a feasible strategy for developing multifunctional silk materials with improved chemical outcomes.
由于反应的不均匀性,部分原因是蛋白质链的组装状态,丝绸材料的化学修饰具有挑战性。在这里,我们评估了决定丝绸材料化学修饰效率的因素。与其他天然大分子不同,丝绸在水溶液中呈现可变的自组装或聚集状态,这会影响基于反应基团分布或可及性的化学反应。为了证实这一假设,将溶液中处于各种构象和聚集状态的丝绸纳米纤维暴露于相同的反应条件下。无定形丝绸纳米纤维为一致的化学修饰结果提供了更好的控制,而具有结构可控性的丝绸纳米纤维可用于通过多次化学修饰生成双功能材料。化学修饰的结果表明,控制丝绸纳米纤维的构象转变为开发具有更好化学效果的多功能丝绸材料提供了一种可行的策略。