One-pot construction of microcomponent supramolecular materials comprising self-sorted supramolecular architechtures of DNA and semi-artificial g;ycopeptides.
One-pot construction of microcomponent supramolecular materials comprising self-sorted supramolecular architechtures of DNA and semi-artificial g;ycopeptides.
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由 DNA 和半人工糖肽自排序超分子结构组成的微组分超分子材料的一锅法构建。
DOI：
10.1021/acsabm.0c01316
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
M. Ikeda.
中科院分区：
文献类型：
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作者：
S. L. Higashi;K. M. Hirosawa;K. G. N. Suzuki;K. Matsuura;M. Ikeda.
多组分超分子材料是由具有独特自分类行为的多个超分子结构组成的，由于其具有复杂的功能和层次结构，例如：活细胞。然而，应用超分子系统设计来设计多元超分子结构之间的自分类行为仍然具有挑战性。在此，我们证明了热退火诱导的多个单链DNA和单个半人工糖肽（GP）的一锅组装导致了整体自分类超分子纳米结构（ssSNs）的快速形成，包括GP超分子纳米带被DNA瓦状纳米管包围。荧光成像显示了通过正交分子组装工艺形成的每个超分子纳米结构。此外，光漂白后的荧光恢复（FRAP）揭示了在瓦片纳米管形成之前，DNA瓦片与GP超分子纳米结构之间在中尺度水平上存在可逆的吸引相互作用，这对于集成sns的形成至关重要。此外，我们发现整合性纳米结构保留了其生物刺激反应性，因此每个超分子纳米结构都可以选择性地降解。最后，在前人研究成果的基础上，我们成功构建了由三元超分子结构（GP超分子纳米结构、DNA瓦片纳米管和DNA微球）组成的复杂软纳米材料。
Multicomponent supramolecular materials, which comprise plural supramolecular architectures that exhibit distinct self-sorting behaviors, are receiving increasing attention because they can be implemented with sophisticated functions and hierarchical structures,e.g., living cells. Nevertheless, the application of supramolecular system design to engineer self-sorting behaviors among plural supramolecular architectures remains challenging. Herein, we show that the thermal annealing-induced one-pot assembly of multiple single-stranded DNAs and a single semi-artificial glycopeptide (GP) results in the emergent formation ofintegrativeself-sorted supramolecular nanostructures (ssSNs) consisting of a GP supramolecular nanoribbon surrounded by DNA tile-nanotubes. Fluorescence imaging revealed the formation of each supramolecular nanostructure through orthogonal molecular assembling processes. Moreover, the fluorescence recovery after photobleaching (FRAP) disclosed the presence of reversible attractive interactions between the DNA tile, prior to the formation of the tile-nanotube, and the GP supramolecular nanostructures at the mesoscale level, which are crucial for the formation of theintegrativessSNs. Further, we revealed that theintegrativessSNs retain their biostimuli responsiveness so that each supramolecular nanostructure can be selectively degraded. Finally, we successfully constructed a complex soft nanomaterial composed of ternary supramolecular architectures (a GP supramolecular nanostructure, DNA tile-nanotube, and DNA microsphere) based on the present as well as previous findings.