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Abstract：
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 of integrative self-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 the integrative ssSNs. Further, we revealed that the integrative ssSNs 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.
摘要：
多组分超分子材料,它们包含多个表现出不同自分类行为的超分子结构，受到越来越多的关注，因为它们可以用复杂的功能和层次结构来实现，例如，活细胞。然而，应用超分子系统设计在多个超分子结构中设计自分类行为仍然具有挑战性。在这里，我们表明，多个单链DNA和单个半人工糖肽（GP）的热退火诱导的一锅组装导致了整合的自分选超分子纳米结构（ssSNs）的突然形成，该结构由GP超分子纳米带组成被DNA瓦片纳米管包围。荧光成像揭示了通过正交分子组装过程形成每个超分子纳米结构。此外，光漂白后的荧光恢复（FRAP）揭示了DNA瓦片之间存在可逆的吸引相互作用，在形成瓦片纳米管之前，和中尺度水平的GP超分子纳米结构，这对于整合ssSN的形成至关重要。Further,我们发现，整合的ssSNs保留了它们的生物刺激响应性，因此每个超分子纳米结构可以被选择性地降解。最后,我们成功构建了由三元超分子结构组成的复杂软纳米材料(GP超分子纳米结构，DNA瓦片纳米管，和DNA微球）基于当前以及先前的发现。
