用于聚氯乙烯脱氢氯化建模的非晶格动力学蒙特卡罗（KMC）-分子动力学（MD）综合框架

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science Pub Date : 2024-11-14 DOI:10.1016/j.ces.2024.120928

Feranmi V. Olowookere, C. Heath Turner

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引用次数: 0

摘要

本研究采用三维非晶格动力学蒙特卡洛-分子动力学（KMC-MD）模拟框架[Comp. Mat. Sci. 229, 112421 (2023)]，以原子分辨率和实验时间尺度（103 - 106 秒）研究聚氯乙烯（PVC）在氢氧化钠（NaOH）中的脱氢氯化/共轭转化。通过我们的框架，可以研究受各种溶剂（丙酮、乙二醇、三甘醇、四氢呋喃和生物衍生溶剂）影响的竞争反应途径和分子尺度变化，以及不同分子量分布、NaOH 浓度和温度的影响。该算法在 KMC 阶段模拟键的断裂和形成，而 MD 阶段则专门用于 PVC-NaOH 溶剂体系的弛豫和热化。该框架使我们能够捕捉到传统微观动力学模型无法捕捉到的重要构型方面（混合、关联、聚类等），并有可能使我们在实验时间尺度上进行基准测试。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

An integrated off-lattice kinetic Monte Carlo (KMC)-molecular dynamics (MD) framework for modeling polyvinyl chloride dehydrochlorination

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An integrated off-lattice kinetic Monte Carlo (KMC)-molecular dynamics (MD) framework for modeling polyvinyl chloride dehydrochlorination

In this study, a three-dimensional off-lattice kinetic Monte Carlo-Molecular Dynamics (KMC-MD) simulation framework [Comp. Mat. Sci. 229, 112421 (2023)] is used to investigate the dehydrochlorination/conjugation transformation of polyvinyl chloride (PVC) in sodium hydroxide (NaOH) with atomistic resolutions at experimental timescales (10³ – 10⁶ s). Our framework enables an examination of the competing reaction pathways and molecular-scale changes influenced by various solvents (acetone, ethylene glycol, triethylene glycol, tetrahydrofuran, and bio-derived solvents), as well as the influence of varying molecular weight distributions, NaOH concentrations, and temperatures. The algorithm simulates bond cleavage and formation during the KMC stages, whereas the MD stage is dedicated to the relaxation and thermalization of the PVC-NaOH-solvent system. The framework allows us to capture important configurational aspects (mixing, correlations, clustering, etc.) that are not accessible with a traditional microkinetic model, and it potentially allows us to perform benchmarking at experimental timescales

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来源期刊

Chemical Engineering Science 工程技术-工程：化工

CiteScore

7.50

自引率

8.50%

发文量

1025

审稿时长

50 days

期刊介绍： Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.