Kamiyama Yuji, Tamate Ryota, Hiroi Takashi, Samitsu Sadaki, Fujii Kenta, Ueki Takeshi
Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan.
Graduate School of Life Science, Hokkaido University, Kita 10, Nishi 8, Kita-ku, Sapporo, Hokkaido 060-0810, Japan.
Sci Adv. 2022 Oct 21;8(42):eadd0226. doi: 10.1126/sciadv.add0226. Epub 2022 Oct 19.
Highly stretchable and self-healing polymer gels formed solely by physical entanglements of ultrahigh-molecular weight (UHMW) polymers were fabricated through a facile one-step process. Radical polymerization of vinyl monomers in ionic liquids under very low initiator concentration conditions produced UHMW polymers of more than 10 g/mol with nearly 100% yield, resulting in the formation of physically entangled transparent polymer gels. The UHMW gels showed excellent properties, such as high stretchability, high ionic conductivity, and recyclability. Furthermore, the UHMW gel exhibited room temperature self-healing ability without any external stimuli. The tensile experiments and molecular dynamics simulations indicate that the nonequilibrium state of the fractured surfaces and microscopic interactions between the polymer chains and solvents play a vital role in the self-healing ability. This study provides a physical approach for fabricating stretchable and self-healing polymer gels based on UHMW polymers.
通过简便的一步法制备了仅由超高分子量（UHMW）聚合物的物理缠结形成的高拉伸性和自愈合聚合物凝胶。在非常低的引发剂浓度条件下，离子液体中乙烯基单体的自由基聚合产生了分子量超过10 g/mol且产率接近100%的超高分子量聚合物，从而形成了物理缠结的透明聚合物凝胶。超高分子量凝胶表现出优异的性能，如高拉伸性、高离子导电性和可回收性。此外，超高分子量凝胶在没有任何外部刺激的情况下表现出室温自愈合能力。拉伸实验和分子动力学模拟表明，断裂表面的非平衡状态以及聚合物链与溶剂之间的微观相互作用在自愈合能力中起着至关重要的作用。这项研究为基于超高分子量聚合物制备可拉伸和自愈合聚合物凝胶提供了一种物理方法。
