Control of seed formation allows two distinct self-sorting patterns of supramolecular nanofibers
Control of seed formation allows two distinct self-sorting patterns of supramolecular nanofibers
复制标题
DOI：
10.1038/s41467-020-17984-x
复制
发表时间：
2020-08-14
影响因子：
16.6
通讯作者：
Hamachi, Itaru
中科院分区：
文献类型：
--
作者：
Kubota, Ryou;Nagao, Kazutoshi;Hamachi, Itaru
由正交超分子纳米纤维组成的自分类双网络水凝胶作为人工调控的多组分体系引起了人们的关注。自分类纳米纤维网络图案的调控被认为是光电子学等潜在应用的关键，但由于缺乏有用的方法来制备和分析网络图案，因此仍然具有挑战性。在这里，我们描述了通过动态共价肟化学控制种子形成的动力学，选择性地构建两种不同的自分类网络模式，相互穿透和平行。共聚焦成像显示，在脂类纳米纤维存在的情况下，O-苄基羟胺与苯甲醛系结的多肽水凝胶形成了互穿的自分类网络。我们还成功地构建了一个并行的自分类网络，通过使用缓慢的肟基交换反应来减慢种子形成的速度。通过仔细观察，多肽型种子和纳米纤维的形成主要发生在脂类纳米纤维的表面，通过高度动态和热波动的过程。
Self-sorting double network hydrogels comprising orthogonal supramolecular nanofibers have attracted attention as artificially-regulated multi-component systems. Regulation of network patterns of self-sorted nanofibers is considered as a key for potential applications such as optoelectronics, but still challenging owing to a lack of useful methods to prepare and analyze the network patterns. Herein, we describe the selective construction of two distinct self-sorting network patterns, interpenetrated and parallel, by controlling the kinetics of seed formation with dynamic covalent oxime chemistry. Confocal imaging reveals the interpenetrated self-sorting network was formed upon addition of O-benzylhydroxylamine to a benzaldehyde-tethered peptide-type hydrogelator in the presence of lipid-type nanofibers. We also succeed in construction of a parallel self-sorting network through deceleration of seed formation using a slow oxime exchange reaction. Through careful observation, the formation of peptide-type seeds and nanofibers is shown to predominantly occur on the surface of the lipid-type nanofibers via highly dynamic and thermally-fluctuated processes.