Molecular-level structural modification is a well-established approach to impart advanced functionality to materials that continues to be the focus of research and development in both academic and industrial laboratories. Here, we report the synthesis of an ordered two-dimensional (2D) poly[2]catenate from the simultaneous self-assembly of two organic ligands and a metal salt by the formation of catenate links using metal coordination and imine condensation reactions. Subsequent chemical reduction of the imine bonds generated the corresponding demetallized poly[2]catenane, which was found to have greater non-rigid-body-like character than the poly[2]catenate as a result of the increased internal dynamics of the mechanical bonds and resulted in an 8-fold increase in elasticity. This synthetic approach allowed for the efficient incorporation of mechanically interlocked molecules (MIMs) within a 2D ordered structure and demonstrated their importance in improving the physical properties of materials by accessing molecular degrees of freedom that cannot be achieved by other means.

中文翻译：

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通过串联形成二维共价有机框架


分子级结构改性是一种行之有效的方法，可以赋予材料先进的功能，并且仍然是学术和工业实验室研究和开发的重点。在这里，我们报告了通过使用金属配位和亚胺缩合反应形成链酸酯连接，由两个有机配体和金属盐同时自组装合成有序二维（2D）聚[2]链酸酯。随后亚胺键的化学还原生成了相应的脱金属聚[2]链烯，由于机械键的内部动力学增加，人们发现它比聚[2]链酸酯具有更大的非刚性体特征并导致弹性增加8倍。这种合成方法可以将机械互锁分子（MIM）有效地结合到二维有序结构中，并证明了它们在通过获得其他方法无法实现的分子自由度来改善材料物理性能方面的重要性。