Soluble and Processable Single-Crystalline Cationic Polymers,Journal of the American Chemical Society

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Soluble and Processable Single-Crystalline Cationic Polymers
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-09 , DOI: 10.1021/jacs.3c02266
Yang Liu _{1,

2} , Xin-Ru Guan _{1,

2} , Duan-Chao Wang _{1,

2} , J Fraser Stoddart _{1,

2,

3,

4} , Qing-Hui Guo _{1,

2}

Affiliation

Single-crystal-to-single-crystal (SCSC) polymerization offers an effective protocol for the environmentally friendly preparation of polymer single crystals (PSCs) with extremely high crystallinity and very large molecular weights. Single-crystal X-ray diffraction (SCXRD) serves as a powerful technique for the in-depth characterization of their structures at a molecular level. Hence, a fundamental understanding of the structure–property relationships of PSCs is within our reach. Most of the reported PSCs, however, suffer from poor solubility, a property which hampers their post-functionalization and solution processability when it comes to practical applications. Here, we report soluble and processable PSCs with rigid polycationic backbones by taking advantage of an ultraviolet-induced topochemical polymerization from an elaborately designed monomer that results in a multitude of photoinduced [2 + 2] cycloadditions. The high crystallinity and excellent solubility of the resulting polymeric crystals enable their characterization both in the solid state by X-ray crystallography and electron microscopy and in the solution phase by NMR spectroscopy. The topochemical polymerization follows first-order reaction kinetics to a first approximation. Post-functionalization of the PSCs by anion exchange renders them super-hydrophobic materials for water purification. Solution processability endows PSCs with excellent gel-like rheological properties. This research represents a major step towards the controlled synthesis and full characterization of soluble single-crystalline polymers, which may find application in the fabrication of PSCs with many different functions.

中文翻译：

可溶且可加工的单晶阳离子聚合物

单晶到单晶（SCSC）聚合为环境友好地制备具有极高结晶度和极大分子量的聚合物单晶（PSC）提供了有效的方案。单晶 X 射线衍射 (SCXRD) 是在分子水平上深入表征其结构的强大技术。因此，我们可以对 PSC 的结构-性能关系有一个基本的了解。然而，大多数报道的PSC都存在溶解度差的问题，这一特性在实际应用中阻碍了它们的后功能化和溶液加工性。这里，我们报告了具有刚性聚阳离子主链的可溶性和可加工的 PSC，通过利用精心设计的单体的紫外线诱导的拓扑化学聚合，导致大量光诱导的 [2 + 2] 环加成。所得聚合物晶体的高结晶度和优异的溶解度使其能够通过 X 射线晶体学和电子显微镜在固态下以及通过 NMR 光谱在溶液相中进行表征。拓扑化学聚合遵循一级反应动力学至一级近似。通过阴离子交换对 PSC 进行后功能化，使其成为用于水净化的超疏水材料。溶液加工性赋予 PSC 优异的凝胶状流变性能。

更新日期：2023-06-09

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