Abstract A novel polyviologen-based molecular architecture was developed via the step-growth polymerization of a hydroxyl-substituted aryl dihydrazide with a water soluble viologen-dialdehyde in water under acidic conditions. When polymerized in the presence of π-electron rich aromatic templates, the reaction mixture underwent hydrogelation. The templates were found to facilitate monomer-monomer as well as monomer-polymer preorganization during polymerization via donor-acceptor charge transfer interactions. Following polymerization, the templates effectively served as post-synthetic non-covalent cross linkers connecting the hydrogel network. The chemical structures of the polymers and molecular recognition between the reacting species were investigated in solution using 1H NMR, while donor-acceptor charge transfer interactions were investigated using UV-vis absorption spectroscopy. We also report the hydrochromic behavior of the templated and non-templated polymers. The surface morphology of the polymers was characterized using scanning electron microscopy, which revealed the formation of sheet-like structures. The new hydrogels developed in this work represents an interesting example of materials comprised of reversible dynamic covalent bonds and reversible non-covalent crosslinking interactions occurring between the electron-rich aryl templates and the electron-deficient bipyridinium units.

中文翻译：

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通过供体-受体相互作用对基于动态共价多紫精的超分子结构进行模板辅助水凝胶化

摘要 通过羟基取代的芳基二酰肼与水溶性紫罗碱-二醛在酸性条件下的逐步增长聚合，开发了一种新型的基于多紫精的分子结构。当在富含 π 电子的芳香族模板存在下聚合时，反应混合物发生水凝胶化。发现模板在聚合过程中通过供体-受体电荷转移相互作用促进单体-单体以及单体-聚合物的预组织。聚合后，模板有效地充当连接水凝胶网络的合成后非共价交联剂。聚合物的化学结构和反应物种之间的分子识别在溶液中使用 1H NMR 进行了研究，而供体-受体电荷转移相互作用则使用紫外-可见吸收光谱进行研究。我们还报告了模板化和非模板化聚合物的水致变色行为。使用扫描电子显微镜表征聚合物的表面形态，这揭示了片状结构的形成。在这项工作中开发的新水凝胶代表了一个有趣的材料例子，该材料由可逆动态共价键和在富电子芳基模板和缺电子联吡啶单元之间发生的可逆非共价交联相互作用组成。这揭示了片状结构的形成。在这项工作中开发的新水凝胶代表了一个有趣的材料例子，该材料由可逆动态共价键和发生在富电子芳基模板和缺电子联吡啶单元之间的可逆非共价交联相互作用组成。这揭示了片状结构的形成。在这项工作中开发的新水凝胶代表了一个有趣的材料例子，该材料由可逆动态共价键和在富电子芳基模板和缺电子联吡啶单元之间发生的可逆非共价交联相互作用组成。