Mechanochemistry of an Interlocked Poly[2]catenane: From Single Molecule to Bulk Gel,CCS Chemistry

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Mechanochemistry of an Interlocked Poly[2]catenane: From Single Molecule to Bulk Gel
CCS Chemistry ( IF 9.4 ) Pub Date : 2019-10-21 , DOI: 10.31635/ccschem.019.201900043
Hao Xing ₁ , Zhandong Li ₂ , Wenbo Wang ₁ , Peiren Liu ₁ , Junkai Liu ₃ , Yu Song ₂ , Zi Liang Wu ₄ , Wenke Zhang ₂ , Feihe Huang ₁

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Mechanically interlocked molecules (MIMs) are prototypical molecular machines with parts that enable controlled, large-amplitude movement with one component positioned relative to another. Incorporating MIMs into polymeric matrices is promising for the designing of functional materials with unprecedented properties. However, the central issue is the challenges involved with establishing the mechanistic linkage between the single-molecule and the bulk material. Herein, we explore the mechanochemical properties and energetic details of a linear poly[2] catenane with strong intercomponent hydrogen bonding (IHB) revealed by single-molecule force spectroscopy. Our results showed that the individual linear poly[2]catenane chain exhibited typical sawtooth pattern, corresponding to the reversible unlocking and relocking transitions under external force or upon stimulations to dissociate or re-form the strong IHB. Furthermore, when a poly[2]catenane-based polymer gel was prepared using a thiol–ene click reaction between thiol-ended poly[2] catenane and a low-molecule-weight cross-linker, the resultant gel showed excellent mechanical adaptability and dynamic properties, which correlated well with the molecular-level observations. The unique poly[2]catenane structure also contributed to the gel formation with an extraordinary IHB-mediated swelling behavior and shape memory property. Thus our present results demonstrate the functioning of bulk material in a linear tandem manner from the behavior of a single molecule, a finding which should be applicable to other systems with versatile properties and promising applications.

中文翻译：

联锁的聚[2]环烷的机械化学：从单分子到本体凝胶

机械互锁分子（MIM）是典型的分子机器，其零件使一个组件相对于另一个组件处于可控制的大振幅运动。将MIM并入聚合物基体对于设计具有前所未有性能的功能材料很有希望。但是，中心问题是在单分子和散装材料之间建立机械连接所涉及的挑战。在本文中，我们探索了通过单分子力谱揭示的具有强组分间氢键（IHB）的线性聚[2]链烷的力学化学性质和高能细节。我们的结果表明，单个线性聚[2]链烷烃链表现出典型的锯齿形，对应于在外力作用下或在刺激下解离或重新形成强IHB的可逆解锁和重新锁定转变。此外，当使用巯基封端的聚[2]链烯和低分子量交联剂之间的噻吩-烯点击反应制备聚[2]环戊烷基聚合物凝胶时，所得凝胶显示优异的机械适应性和动态特性，与分子水平的观察结果很好地相关。独特的聚[2]环戊烷结构还促进了凝胶的形成，具有非凡的IHB介导的溶胀行为和形状记忆特性。因此，我们目前的结果证明了单个分子的行为以线性串联的方式作用于散装材料，

更新日期：2020-06-24

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