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首页> 外文期刊>Chemistry: A European journal >Main-chain linear polyrotaxanes: Synthesis, characterization, and conformational modulation
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Main-chain linear polyrotaxanes: Synthesis, characterization, and conformational modulation

机译：主链线性聚轮烷：合成，表征和构象调制

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摘要

Two functional main-chain linear polyrotaxanes, one a covalent polymeric chain that threads through many macrocycles (P1) and the other a poly[n]rotaxane chain that is composed of many repeating rotaxane units (P2), were synthesized by employing strong crown-ether/ammonium-based (DB24C8/DBA) host-guest interactions and click chemistry. Energy transfer between the wheel and axle units in both polyrotaxanes was used to provide insight into the conformational information of their resulting polyrotaxanes. Steady-state and time-resolved spectroscopy were performed to understand the conformation differences between polymers P1 and P2 in solution. Additional investigations by using dynamic/static light scattering and atomic force microscopy illustrated that polymer P1 was unbending and had a rigid rod-like structure, whilst polymer P2 was curved and flexible. This flexible topology facilitated the self-assembly of polymer P2 into relatively large ball-shaped particles. In addition, the energy transfer between the wheel and axle units was controlled by the addition of specific anions or base. The anion-induced energy enhancement was attributed to a change in electrostatic interactions between the polymer chains. The base-driven molecular shuttle broke the DB24C8/DBA host-guest interactions. These results confirm that both intra- and intermolecular electrostatic interactions are crucial for modulating conformational topology, which determines the assembly of polyrotaxanes in solution.
机译：两种功能性主链线性聚轮烷，一种是通过多个大环（P1）穿过的共价聚合物链，另一种是由许多重复的轮烷单元（P2）组成的聚[n]轮烷链，方法是使用强冠基于醚/铵（DB24C8 / DBA）的主客互动和单击化学。两种聚轮烷中的轮轴单元之间的能量转移被用来深入了解其所得聚轮烷的构象信息。进行稳态和时间分辨光谱分析以了解溶液中聚合物P1和P2之间的构象差异。使用动态/静态光散射和原子力显微镜进行的其他研究表明，聚合物P1弯曲且具有刚性杆状结构，而聚合物P2则弯曲且具有柔性。这种灵活的拓扑结构有助于将聚合物P2自组装为相对较大的球形颗粒。此外，通过添加特定的阴离子或碱来控制轮轴单元之间的能量传递。阴离子诱导的能量增强归因于聚合物链之间静电相互作用的变化。碱基驱动的分子穿梭破坏了DB24C8 / DBA宿主-客体的相互作用。这些结果证实，分子内和分子间静电相互作用对于调节构象拓扑至关重要，而构象拓扑决定了溶液中聚轮烷的组装。

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