Activity-driven polymer knotting for macromolecular topology engineering

IF 12.5 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Science Advances Pub Date : 2024-11-29 DOI:10.1126/sciadv.adr0716
Jia-Xiang Li, Song Wu, Li-Li Hao, Qun-Li Lei, Yu-Qiang Ma
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Abstract

Macromolecules can gain special properties by adopting knotted conformations, but engineering knotted macromolecules is a challenging task. Here, we unexpectedly find that knots can be efficiently generated in active polymer systems. When one end of an actively reptative polymer is anchored, it undergoes continual self-knotting as a result of intermittent giant conformation fluctuations and the outward reptative motion. Once a knot is formed, it migrates to the anchoring point due to a nonequilibrium ratchet effect. Moreover, when the active polymer is grafted on a passive polymer, it can function as a self-propelling soft needle to either transfer its own knots or directly braid knots on the passive polymer. We further show that these active needles can create intermolecular bridging knots between two passive polymers. Our finding highlights the nonequilibrium effects in modifying the dynamic pathways of polymer systems, which have potential applications in macromolecular topology engineering.

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高分子拓扑工程中活性驱动的聚合物打结。
采用打结构象可以使大分子获得特殊的性能,但打结大分子的工程设计是一项具有挑战性的任务。在这里,我们意外地发现,结可以有效地在活性聚合物体系中产生。当活性复制聚合物的一端被锚定时,由于间歇性的巨大构象波动和向外复制运动,它会经历持续的自结。一旦结形成,由于非平衡棘轮效应,它就会迁移到锚固点。此外,当活性聚合物接枝到被动聚合物上时,它可以像一个自推进的软针一样转移自己的结或直接在被动聚合物上编织结。我们进一步表明,这些活性针可以在两个被动聚合物之间产生分子间桥接结。我们的发现强调了非平衡效应在改变聚合物体系动态路径中的作用,这在大分子拓扑工程中具有潜在的应用前景。
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来源期刊
Science Advances
Science Advances 综合性期刊-综合性期刊
CiteScore
21.40
自引率
1.50%
发文量
1937
审稿时长
29 weeks
期刊介绍: Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.
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