聚合物烧结过程中的非均相缠结分布及缠结与结晶的相互作用：分子动力学模拟

IF 5.2 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-04-14 DOI:10.1021/acs.macromol.5c00070

Ran Chen, Shengming Jiang, Chuanfu Luo, Xiaoniu Yang

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引用次数: 0

摘要

利用大尺度分子动力学模拟研究了重缠结和结晶过程中沿链的缠结分布。用缠结长度Ne与头指数的关系来表征缠结分布的非均匀性。结果表明，在重纠缠过程中，纠缠的发展是不均匀的。纠缠长度的宽双峰分布进一步支持了这一点。此外，在等温结晶过程中，缠结沿链分布的非均质性增强。这归因于非均相解缠过程，其中链倾向于在链端段解缠和结晶。在结晶过程中，Ne先降低到一定程度，然后又显著升高。Ne的初始还原是由于结晶过程中链刚度的增加和链的持续膨胀和扩散。此外，还研究了纠缠重构对晶体形态的影响。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Heterogeneous Entanglement Distribution during Polymer Sintering and the Interplay of Entanglement with Crystallization: Molecular Dynamics Simulations

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Heterogeneous Entanglement Distribution during Polymer Sintering and the Interplay of Entanglement with Crystallization: Molecular Dynamics Simulations

The entanglement distribution along a chain during re-entanglement and crystallization is investigated using large-scale molecular dynamics simulations. The dependence of the entanglement length, N_e, on the bead index is used to characterize the heterogeneity of the entanglement distribution. The results reveal that entanglements develop heterogeneously during re-entanglement. This is further supported by the broad bimodal distribution of the entanglement length. Furthermore, there is enhanced heterogeneity in the entanglement distribution along the chain during isothermal crystallization. This is ascribed to the heterogeneous disentanglement process, where chains prefer to disentangle and crystallize at chain-end segments. During crystallization, N_e decreases to a certain extent, followed by a significant increase. The initial reduction in N_e is attributed to increased chain rigidity and the continuous chain expansion and diffusion during crystallization. Additionally, the influence of entanglement reconstruction on crystal morphology is investigated.

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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.