Imaging-Based Study on Control Factors over Self-Sorting of Supramolecular Nanofibers Formed from Peptide- and Lipid-type Hydrogelators
Imaging-Based Study on Control Factors over Self-Sorting of Supramolecular Nanofibers Formed from Peptide- and Lipid-type Hydrogelators
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DOI：
10.1021/acs.bioconjchem.8b00260
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发表时间：
2018-06-01
影响因子：
4.7
通讯作者：
Hamachi, Itaru
中科院分区：
文献类型：
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作者：
Kubota, Ryou;Liu, Shuang;Hamachi, Itaru
多组分自组装是智能软材料构建的一个迷人的策略。其中，包含自分选纳米纤维的超分子水凝胶由于其合理地并入刺激响应性而最近引起了显著的关注。然而，已经有有限的调查的关键因素控制的自我排序现象。在这里，我们描述了一种基于成像的方法来评估控制肽和脂质型水凝胶因子形成自分选纳米纤维的因素。我们筛选了一个小的库，水凝胶因子具有不同的化学性质，通过直接可视化的自组装行为，通过使用共聚焦激光扫描显微镜。我们的系统研究确定了影响纳米纤维自分选行为的两个重要因素：（i）水凝胶因子的表面电荷;和（ii）肽型水凝胶因子侧链的疏水性。我们确定，相同的净/表面电荷的水凝胶因子和侧链上的肽型水凝胶因子具有较低的疏水性是优选的。这些发现，结合先前报道的动力学因素，被用来设计和成功地制备由超分子纳米纤维从肽和脂质型水凝胶因子和阳离子有机铑络合物组成的三组分正交自组装。研究结果对基于自分选现象的智能软材料的设计具有一定的指导意义。
Multicomponent self-assembly is a fascinating strategy for the construction of smart soft materials. Among them, supramolecular hydrogels comprising self-sorting nanofibers have recently attracted significant attention owing to their rationally incorporated stimulus responsiveness. However, there have been limited investigations of the crucial factors that control the self-sorting phenomena. Here, we describe an imaging-based approach to evaluate the factors that control the formation of self-sorting nanofibers from peptide- and lipid-type hydrogelators. We screened a small library of hydrogelators with distinct chemical properties by direct visualization of their self-assembly behavior by using confocal laser scanning microscopy. Our systematic research identified two important factors that influence the self-sorting behavior of nanofibers: (i) the surface charge of the hydrogelators; and (ii) the hydrophobicity of the side chain on the peptide-type hydrogelators. We determined that the same net/surface charge on the hydrogelators and side chains with a lower hydrophobicity on the peptide-type hydrogelators were preferred. These findings, in combination with the previously reported kinetic factors, were used to design and successfully prepare a three-component orthogonal self-assembly composed of supramolecular nanofibers from peptide- and lipid-type hydrogelators and a cationic organorhodium complex. Our findings would be beneficial for the design of intelligent soft materials based on self-sorting phenomena.