Wang Yongming, Liu Guoquan, Zhao Jun, Zhang Zhaoming, Zhang Hao, Ding Yi, Zhang Xinhai, Liu Zhu, Yu Wei, Yan Xuzhou
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Angew Chem Int Ed Engl. 2024 Oct 14;63(42):e202409705. doi: 10.1002/anie.202409705. Epub 2024 Sep 12.
Adhesives have been widely used to splice and repair materials to meet practical needs of humanity for thousands of years. However, developing robust adhesives with balanced adhesive and cohesive properties still remains a challenging task. Herein, we report the design and preparation of a robust mechanically interlocked [an]daisy chain network (MIN) adhesive by orthogonal integration of mechanical bonds and 2-ureido-4[1H]-pyrimidone (UPy) H-bonding in a single system. Specifically, the UPy moiety plays a dual role: it allows the formation of a cross-linked network and engages in multivalent interactions with the substrate for strong interfacial bonding. The mechanically interlocked [an]daisy chain, serving as the polymeric backbone of the adhesive, is able to effectively alleviate applied stress and uphold network integrity through synergistic intramolecular motions, and thus significantly improves the cohesive performance. Comparative analysis with the control made of the same quadruple H-bonding network but with non-interlocked [an]daisy chain backbones demonstrates that our MIN possesses superior adhesion properties over a wide temperature range. These findings not only contribute to a deep understanding of the structure-property relationship between microscopic mechanical bond motions and macroscopic adhesive properties but also provide a valuable guide for optimizing design principles of robust adhesives.
数千年来，粘合剂已被广泛用于拼接和修复材料，以满足人类的实际需求。然而，开发具有平衡粘合性和内聚性的强力粘合剂仍然是一项具有挑战性的任务。在此，我们报告了一种强力机械互锁雏菊链网络（MIN）粘合剂的设计与制备，该粘合剂通过在单一体系中机械键与2-脲基-4[1H]-嘧啶酮（UPy）氢键的正交整合而成。具体而言，UPy部分发挥双重作用：它允许形成交联网络，并与基材进行多价相互作用以实现强界面粘合。作为粘合剂聚合物主链的机械互锁雏菊链能够通过协同分子内运动有效缓解施加的应力并维持网络完整性，从而显著提高内聚性能。与由相同四重氢键网络但无互锁雏菊链主链制成的对照物进行的对比分析表明，我们的MIN在很宽的温度范围内具有优异的粘合性能。这些发现不仅有助于深入理解微观机械键运动与宏观粘合性能之间的结构-性能关系，还为优化强力粘合剂设计原则提供了有价值的指导。
