通过机器学习了解聚合物纳米复合材料中的爬行抑制机制
Entao Yang1, James F Pressly2, Bharath Natarajan3
1Department of Chemical & Biomolecular Engineering, University of Pennsylvania, Philadelphia, PA 19104, USA. rrig@seas.upenn.edu.
Soft matter
|September 27, 2023
概括
接口显著影响纳米复合材料中的聚合物动态. 这项研究将包装效应与其他因素分开,揭示了结构动态关系的改变,而不仅仅是包装,导致纳米粒子附近的动态变慢.
科学领域:
- 材料科学 材料科学 材料科学
- 聚合物物理 聚合物物理
- 计算材料科学科学 计算材料科学
背景情况:
- 了解聚合物纳米复合材料 (PNC) 等复杂材料的界面动力学至关重要,但具有挑战性.
- 虽然局部结构会影响同质系统中的动态,但在异质系统中的界面效应是不太了解的.
- 已知接口会改变分子包装,但它们对动态的影响远远超出了直接接近的范围.
研究的目的:
- 量化区分聚合物包装和其他因素在PNC中纳米粒子表面附近改变动态的作用.
- 通过使用先进的计算和实验方法,研究在接口上的结构和动态之间的关系.
- 根据PNC的静态结构,开发一种基于PNC的爬行行为预测模型.
主要方法:
- 结合分子动力学模拟和实验技术 (例如,爬行合规测量).
- 利用机器学习的结构指标 ("软度") 来分解聚合物动态.
- 从纳米粒子表面距离的函数中分析动力学.
主要成果:
- 在模拟和实验之间实现了良好的质量一致,用于玻璃结构和爬行合规性.
- 将分解的聚合物动力学分为包装依赖的和包装独立的对自由能量障碍的贡献.
- 发现包装依赖和独立障碍在纳米颗粒附近都升高,并且随着应用于应力而降低.
- 证明缓慢的界面动力学是由改变的包装和修改的结构动力学关系引起的.
结论:
- 在聚合物-纳米粒子接口上观察到的缓慢动态不仅仅是由于聚合物包装的差异.
- 材料结构和动力学之间的基本关系的变化起着重要作用.
- 开发的分解方法准确地从静态配置中预测PNC的应变时间爬行曲线.
- 提供了对聚合物-纳米粒子接口的爬行抑制机制的新见解.
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