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纳米受限聚合限制了无滞后凝胶中的裂纹扩展。

Nanoconfined polymerization limits crack propagation in hysteresis-free gels.

作者信息

Li Weizheng, Wang Xiaoliang, Liu Ziyang, Zou Xiuyang, Shen Zhihao, Liu Dong, Li Lingling, Guo Yu, Yan Feng

机构信息

Jiangsu Engineering Laboratory of Novel Functional Polymeric Materials, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies College of Chemistry, Suzhou Key Laboratory of Soft Material and New Energy, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China.

School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China.

出版信息

Nat Mater. 2024 Jan;23(1):131-138. doi: 10.1038/s41563-023-01697-9. Epub 2023 Oct 26.

Abstract

Consecutive mechanical loading cycles cause irreversible fatigue damage and residual strain in gels, affecting their service life and application scope. Hysteresis-free hydrogels within a limited deformation range have been created by various strategies. However, large deformation and high elasticity are inherently contradictory attributes. Here we present a nanoconfined polymerization strategy for producing tough and near-zero-hysteresis gels under a large range of deformations. Gels are prepared through in situ polymerization within nanochannels of covalent organic frameworks or molecular sieves. The nanochannel confinement and strong hydrogen bonding interactions with polymer segments are crucial for achieving rapid self-reinforcement. The rigid nanostructures relieve the stress concentration at the crack tips and prevent crack propagation, enhancing the ultimate fracture strain (17,580 ± 308%), toughness (87.7 ± 2.3 MJ m) and crack propagation strain (5,800%) of the gels. This approach provides a general strategy for synthesizing gels that overcome the traditional trade-offs of large deformation and high elasticity.

摘要

连续的机械加载循环会导致凝胶中出现不可逆的疲劳损伤和残余应变,从而影响其使用寿命和应用范围。通过各种策略已制备出在有限变形范围内无滞后现象的水凝胶。然而,大变形和高弹性本质上是相互矛盾的特性。在此,我们提出一种纳米受限聚合策略,用于在大范围变形下制备坚韧且近乎零滞后的凝胶。凝胶是通过在共价有机框架或分子筛的纳米通道内原位聚合制备的。纳米通道限制以及与聚合物链段的强氢键相互作用对于实现快速自增强至关重要。刚性纳米结构减轻了裂纹尖端的应力集中并防止裂纹扩展,提高了凝胶的极限断裂应变(17580±308%)、韧性(87.7±2.3 MJ·m)和裂纹扩展应变(5800%)。这种方法为合成凝胶提供了一种通用策略,克服了大变形和高弹性之间传统的权衡。

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