Oligo[2]catenane That Is Robust at Both the Microscopic and Macroscopic Scales,Journal of the American Chemical Society

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Oligo[2]catenane That Is Robust at Both the Microscopic and Macroscopic Scales
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-04-13 , DOI: 10.1021/jacs.3c00221
Ruixue Bai ₁ , Zhaoming Zhang ₁ , Weishuai Di ₂ , Xue Yang ₁ , Jun Zhao ₁ , Hao Ouyang ₁ , Guoquan Liu ₁ , Xinhai Zhang ₁ , Lin Cheng ₁ , Yi Cao ₂ , Wei Yu ₁ , Xuzhou Yan ₁

Affiliation

Polycatenanes are extremely attractive topological architectures on account of their high degrees of conformational freedom and multiple motion patterns of the mechanically interlocked macrocycles. However, exploitation of these peculiar structural and dynamic characteristics to develop robust catenane materials is still a challenging goal. Herein, we synthesize an oligo[2]catenane that showcases mechanically robust properties at both the microscopic and macroscopic scales. The key feature of the structural design is controlling the force-bearing points on the metal-coordinated core of the [2]catenane moiety that is able to maximize the energy dissipation of the oligo[2]catenane via dissociation of metal-coordination bonds and then activation of sequential intramolecular motions of circumrotation, translation, and elongation under an external force. As such, at the microscopic level, the single-molecule force spectroscopy measurement exhibits that the force to rupture dynamic bonds in the oligo[2]catenane reaches a record high of 588 ± 233 pN. At the macroscopic level, our oligo[2]catenane manifests itself as the toughest catenane material ever reported (15.2 vs 2.43 MJ/m³). These fundamental findings not only deepen the understanding of the structure-property relationship of poly[2]catenanes with a full set of dynamic features but also provide a guiding principle to fabricate high-performance mechanically interlocked catenane materials.

中文翻译：

在微观和宏观尺度上都很稳健的寡 [2] 链烷

聚链烷是极具吸引力的拓扑结构，因为它们具有高度的构象自由度和机械互锁大环的多种运动模式。然而，利用这些特殊的结构和动力学特性来开发坚固的链烷材料仍然是一个具有挑战性的目标。在此，我们合成了一种低聚 [2] 链烷，它在微观和宏观尺度上都具有机械稳健的特性。结构设计的关键特征是控制 [2] 链烷部分金属配位核上的受力点，能够通过以下途径最大化低聚 [2] 链烷的能量耗散金属配位键的解离，然后在外力作用下激活连续的分子内旋转、平移和伸长运动。因此，在微观水平上，单分子力谱测量表明，破坏寡 [2] 链烷中动态键的力达到创纪录的 588 ± 233 pN。在宏观层面上，我们的低聚 [2] 链烷表现为有史以来最坚韧的链烷材料（15.2对2.43 MJ/m ³）。这些基本发现不仅加深了对具有全套动态特征的聚 [2] 链烷的结构-性能关系的理解，而且为制造高性能机械互锁链烷材料提供了指导原则。

更新日期：2023-04-13

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