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Improvement of Polymer Mechanical Behaviors by Introducing [2]Rotaxane Units with Intra- and Intermolecular Hydrogen Bonds
Macromolecules ( IF 5.1 ) Pub Date : 2024-08-16 , DOI: 10.1021/acs.macromol.4c00150 Lang He 1 , Jialin Wei 1 , Zibin Zhang 1 , Ning Shentu 1 , Jiao Wang 2, 3 , Jiaxi Yu 1 , Zhiqiang Ren 4 , Jiyong Liu 2, 3 , Guangfeng Li 2, 3 , Feihe Huang 2, 3 , Shijun Li 1
Macromolecules ( IF 5.1 ) Pub Date : 2024-08-16 , DOI: 10.1021/acs.macromol.4c00150 Lang He 1 , Jialin Wei 1 , Zibin Zhang 1 , Ning Shentu 1 , Jiao Wang 2, 3 , Jiaxi Yu 1 , Zhiqiang Ren 4 , Jiyong Liu 2, 3 , Guangfeng Li 2, 3 , Feihe Huang 2, 3 , Shijun Li 1
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Rotaxanes have demonstrated great potential in the development of smart materials owing to their attractive dynamic and movable properties. However, it remains a significant challenge to construct polymers with outstanding mechanical performance by the introduction of rotaxane units. Here, we synthesized several pillar[5]arene-based [2]rotaxanes by condensation reaction of 1-naphthyl isocyanate and alkyl diamines and introduced them into covalent polymers through ring-opening metathesis polymerization. The rigid and bulky pillar[5]arene units, sliding motions of rotaxane moieties, and intra- and intermolecular hydrogen bonds between urea groups endow the polymers with excellent mechanical properties (PR4: Young’s modulus = 360.1 ± 32.1 MPa, yield stress = 14.2 ± 0.1 MPa, stress at break = 14.8 ± 0.6 MPa, and toughness = 67.8 ± 2.0 MJ/m3). Moreover, the mechanical properties of PR4 could be weakened and strengthened by the introduction of Ac– and Cl–, respectively, showing their abundant regulable features. These findings provide novel insights into the preparation of advanced supramolecular materials with enhanced mechanical properties.
中文翻译：
通过引入具有分子内和分子间氢键的[2]轮烷单元改善聚合物机械性能
轮烷由于其有吸引力的动态和可移动特性，在智能材料的开发中显示出巨大的潜力。然而，通过引入轮烷单元构建具有优异机械性能的聚合物仍然是一个重大挑战。在这里，我们通过1-萘基异氰酸酯和烷基二胺的缩合反应合成了几种基于柱[5]芳烃的[2]轮烷，并通过开环复分解聚合将它们引入到共价聚合物中。刚性大的柱[5]芳烃单元、轮烷部分的滑动以及脲基之间的分子内和分子间氢键赋予聚合物优异的机械性能（ PR4 ：杨氏模量= 360.1 ± 32.1 MPa，屈服应力= 14.2 ± 0.1 MPa，断裂应力= 14.8 ± 0.6 MPa，韧性= 67.8 ± 2.0 MJ/m 3 ）。此外， Ac-和Cl-的引入可以分别减弱和增强PR4的力学性能，显示出其丰富的可调节特性。这些发现为制备具有增强机械性能的先进超分子材料提供了新的见解。
更新日期：2024-08-16
中文翻译：
通过引入具有分子内和分子间氢键的[2]轮烷单元改善聚合物机械性能
轮烷由于其有吸引力的动态和可移动特性，在智能材料的开发中显示出巨大的潜力。然而，通过引入轮烷单元构建具有优异机械性能的聚合物仍然是一个重大挑战。在这里，我们通过1-萘基异氰酸酯和烷基二胺的缩合反应合成了几种基于柱[5]芳烃的[2]轮烷，并通过开环复分解聚合将它们引入到共价聚合物中。刚性大的柱[5]芳烃单元、轮烷部分的滑动以及脲基之间的分子内和分子间氢键赋予聚合物优异的机械性能（ PR4 ：杨氏模量= 360.1 ± 32.1 MPa，屈服应力= 14.2 ± 0.1 MPa，断裂应力= 14.8 ± 0.6 MPa，韧性= 67.8 ± 2.0 MJ/m 3 ）。此外， Ac-和Cl-的引入可以分别减弱和增强PR4的力学性能，显示出其丰富的可调节特性。这些发现为制备具有增强机械性能的先进超分子材料提供了新的见解。
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