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A Self-Healing Crystal That Repairs Multiple Cracks
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-09-18 , DOI: 10.1021/jacs.4c09334 Javed R Pathan 1 , Haripriya Balan 1 , Patrick Commins 2 , Arthi Ravi 1 , Marieh B Al-Handawi 2 , Ian Cheng-Yi Hou 2 , Panče Naumov 2, 3, 4, 5 , Kana M Sureshan 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-09-18 , DOI: 10.1021/jacs.4c09334 Javed R Pathan 1 , Haripriya Balan 1 , Patrick Commins 2 , Arthi Ravi 1 , Marieh B Al-Handawi 2 , Ian Cheng-Yi Hou 2 , Panče Naumov 2, 3, 4, 5 , Kana M Sureshan 1
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We report both cracking and self-healing in crystals occurring during a thermal phase transition, followed by a topochemical polymerization. A squaramide-based monomer was designed where the azide and alkyne units of adjacent molecules are positioned favorably for a topochemical click reaction. The monomer undergoes spontaneous single-crystal-to-single-crystal (SCSC) polymerization at room temperature via regiospecific 1,3-dipolar cycloaddition, yielding the corresponding triazole-linked polymer in a few days. When heated at 60 °C, the polymerization completes in a SCSC manner in 24 h. Upon continuous heating from room temperature to 110 °C, the monomer crystals develop multiple cracks, and they self-heal immediately. The cracking occurs due to a thermal phase transition, as evidenced by differential scanning calorimetry (DSC). The cracks heal either upon further heating or upon cooling of the crystals due to the topochemical polymerization or reversal of the phase transition, respectively. Increasing the heating rate leads to the formation of longer and wider cracks, which also heal instantaneously. The self-healed crystals retained their integrity and the crystal structure of the self-healed crystals was analyzed by single-crystal X-ray diffraction. The quality of the self-healed crystals and their diffraction ability conform to those of the completely reacted crystals at room temperature or at 60 °C without developing cracks. This work demonstrates a novel mechanism for self-healing of molecular crystals that could expand the horizon of these materials for a plethora of applications.
中文翻译：
一种可修复多处裂缝的自愈晶体
我们报道了在热相变期间发生的晶体开裂和自修复，然后是拓扑化学聚合。设计了一种基于方酰胺的单体，其中相邻分子的叠氮化物和炔烃单元位于有利于拓扑化学点击反应的位置。单体在室温下通过区域特异性 1,3-偶极环加成反应自发地从单晶到单晶 （SCSC） 聚合，在几天内产生相应的三唑-连接聚合物。当在 60 °C 下加热时，聚合在 24 小时内以 SCSC 方式完成。从室温持续加热到 110 °C 后，单体晶体会产生多条裂纹，并立即自我修复。裂纹是由于热相变而发生的，差示扫描量热法 （DSC） 证明了这一点。裂纹在进一步加热或冷却晶体时愈合，分别是由于拓扑化学聚合或相变的反转。提高加热速度会导致形成更长更宽的裂缝，这些裂缝也会立即愈合。自修复的晶体保持了其完整性，并通过单晶 X 射线衍射分析了自修复晶体的晶体结构。自修复晶体的质量及其衍射能力与室温或 60 °C 下完全反应的晶体的质量和衍射能力一致，不会产生裂纹。这项工作展示了一种分子晶体自愈的新机制，可以扩大这些材料的应用范围，用于多种应用。
更新日期：2024-09-18
中文翻译：
一种可修复多处裂缝的自愈晶体
我们报道了在热相变期间发生的晶体开裂和自修复，然后是拓扑化学聚合。设计了一种基于方酰胺的单体，其中相邻分子的叠氮化物和炔烃单元位于有利于拓扑化学点击反应的位置。单体在室温下通过区域特异性 1,3-偶极环加成反应自发地从单晶到单晶 （SCSC） 聚合，在几天内产生相应的三唑-连接聚合物。当在 60 °C 下加热时，聚合在 24 小时内以 SCSC 方式完成。从室温持续加热到 110 °C 后，单体晶体会产生多条裂纹，并立即自我修复。裂纹是由于热相变而发生的，差示扫描量热法 （DSC） 证明了这一点。裂纹在进一步加热或冷却晶体时愈合，分别是由于拓扑化学聚合或相变的反转。提高加热速度会导致形成更长更宽的裂缝，这些裂缝也会立即愈合。自修复的晶体保持了其完整性，并通过单晶 X 射线衍射分析了自修复晶体的晶体结构。自修复晶体的质量及其衍射能力与室温或 60 °C 下完全反应的晶体的质量和衍射能力一致，不会产生裂纹。这项工作展示了一种分子晶体自愈的新机制，可以扩大这些材料的应用范围，用于多种应用。
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