Multivalent Design of Low-Entropy-Penalty Ion–Dipole Interactions for Dynamic Yet Thermostable Supramolecular Networks,Journal of the American Chemical Society

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Multivalent Design of Low-Entropy-Penalty Ion–Dipole Interactions for Dynamic Yet Thermostable Supramolecular Networks
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-01-31 , DOI: 10.1021/jacs.2c12133
Zhekai Jin ₁ , Tao Chen _{1,

2} , Yuncong Liu ₁ , Wenwen Feng ₁ , Lili Chen ₁ , Chao Wang ₁

Affiliation

Dynamic supramolecular networks are constantly accompanied by thermal instability. The fundamental reason is most reversible noncovalent bonds quickly decay at elevated temperatures and dissociate below 100 °C. Here, in this paper, we realize a reversible ion–dipole interaction with high-temperature stability exceeding 150 °C. The resultant supramolecular network can simultaneously possess mechanical strength of 1.32 MPa (14.8 times that of pristine material), dynamic self-healing capability, and a stable working temperature of up to 200 °C. From the prolonged characteristic relaxation time of 600 s even at 100 °C, our material represents one of the most thermally stable dynamic supramolecular polymers. These remarkable performances are achieved by using a new multivalent yet low-entropy-penalty molecular design. In this way, the noncovalent bond can reach a high enthalpy while minimizing the entropy-dominated thermal dissociations.

中文翻译：

动态但热稳定的超分子网络的低熵损失离子-偶极子相互作用的多价设计

动态超分子网络总是伴随着热不稳定性。根本原因是大多数可逆非共价键在高温下会迅速衰减并在 100 °C 以下解离。在这里，在这篇论文中，我们实现了一种可逆的离子-偶极子相互作用，具有超过 150 °C 的高温稳定性。所得超分子网络可同时具备 1.32 MPa 的机械强度（原始材料的 14.8 倍）、动态自愈能力和高达 200 °C 的稳定工作温度。即使在 100 °C 下，从 600 s 的延长特征弛豫时间来看，我们的材料代表了热稳定性最高的动态超分子聚合物之一。这些卓越的性能是通过使用新的多价但低熵惩罚分子设计实现的。这样，

更新日期：2023-01-31

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