聚轮烷动态共价网络中机械拓扑和化学交换的协同效应

IF 7 2区 材料科学 Q2 CHEMISTRY, PHYSICAL
Bitgaram Kim, Moonseok Jang, Zekai Wang and Ji-Hun Seo*, 
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引用次数: 0

摘要

虽然动态共价网络(DCNs)作为可再加工热固性材料受到越来越多的关注,但其力学和动力学行为需要进一步优化。大多数现有的方法依赖于化学调整键交换反应;然而,网络的拓扑设计,特别是通过机械互锁键(MIBs)的集成,还没有系统地探索。在这项研究中,我们通过设计非滑动(固定)和滑动(含PR)聚合物的网络来研究基于聚轮烷(PR)的MIBs对乙烯基聚氨酯DCNs的可重构性和机械性能的影响。基于pr的系统根据其直接或间接参与胺交换反应进一步分类。将pr加入DCNs可显著提高弛豫动力学、可再加工性和韧性。其中,具有直接参与键交换的氨基化PR的DPRam网络具有最低的活化能(85.3 kJ mol-1)、最高的韧性保持(94.8%)、最佳的后处理能力和最快的形状恢复。这些优点归功于可滑动拓扑结构和动态共价反应性的协同结合。本研究强调了将pr集成到结构设计策略中以推进拓扑适应性、高性能DCN系统的潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Synergistic Effects of Mechanical Topology and Chemical Exchange in Dynamic Covalent Networks Incorporated with Polyrotaxane

Synergistic Effects of Mechanical Topology and Chemical Exchange in Dynamic Covalent Networks Incorporated with Polyrotaxane

While dynamic covalent networks (DCNs) have garnered increasing attention as reprocessable thermosets, their mechanical and dynamic behaviors need further optimization. Most existing approaches rely on chemically tuning bond exchange reactions; however, the topological design of the network, particularly through the integration of mechanically interlocked bonds (MIBs), has not been systematically explored. In this study, we investigate the impact of polyrotaxane (PR)-based MIBs on the reconfigurability and mechanical performance of vinylogous urethane-based DCNs by designing networks with non-sliding (fixed) and sliding (PR-containing) polymers. The PR-based systems are further categorized according to their direct or indirect participation in amine exchange reactions. Incorporating PRs into DCNs significantly enhanced relaxation dynamics, reprocessability, and toughness. Among them, the DPRam network, featuring aminated PR capable of directly participating in the bond exchange, shows the lowest activation energy (85.3 kJ mol–1), the highest toughness retention (94.8%), the best reprocessing ability, and the fastest shape recovery. These advantages are attributed to the synergistic combination of slidable topology and dynamic covalent reactivity. This study highlights the potential of integrating PRs into a structural design strategy to advance topologically adaptive, high-performance DCN systems.

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来源期刊
Chemistry of Materials
Chemistry of Materials 工程技术-材料科学:综合
CiteScore
14.10
自引率
5.80%
发文量
929
审稿时长
1.5 months
期刊介绍: The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.
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