网络结构对自由基聚合合成凝胶断裂行为影响的分子模拟

IF 5.2 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-03-19 DOI:10.1021/acs.macromol.4c02875

Tsutomu Furuya, Tsuyoshi Koga

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引用次数: 0

摘要

近年来，一些研究小组报道了用高单体和低交联剂浓度的自由基聚合法合成具有多缠结的高强度凝胶。为了阐明这种高强凝胶的增韧机理，采用粗粒度分子动力学模拟方法研究了自由基聚合合成凝胶的断裂行为。模拟结果定性地再现了报告的实验结果；高单体和低交联剂浓度形成的凝胶由于交联而具有少量的弹性有效链，但有许多聚合物纠缠，并且在不牺牲剪切模量的情况下具有高韧性。在韧性凝胶中，结构变化抑制了聚合物链在延伸方向上的取向和应力集中。网络结构与断裂行为的关系分析表明，交联点之间的链长和缠结数对凝胶的韧性有重要影响。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Molecular Simulation of Effects of Network Structure on Fracture Behavior of Gels Synthesized by Radical Polymerization

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Molecular Simulation of Effects of Network Structure on Fracture Behavior of Gels Synthesized by Radical Polymerization

The synthesis of high-strength gels with many entanglements by radical polymerization with high monomer and low cross-linker concentrations has recently been reported by several groups. In order to elucidate the toughening mechanism of such high-strength gels, the fracture behavior of gels synthesized by radical polymerization is studied by a coarse-grained molecular dynamics simulation. The simulation results qualitatively reproduce the reported experimental results; the gels formed with high monomer and low cross-linker concentrations have a small number of elastically effective chains due to cross-linking, but many polymer entanglements, and exhibit high toughness without sacrificing the shear modulus. In the tough gels, the structural changes that suppress the orientation of the polymer chains in the elongation direction and stress concentration are confirmed. Analysis of the relationship between network structure and fracture behavior reveals that the chain length between cross-linking points and the number of entanglements are important for the toughness of the gels.

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.