Classical and reactive molecular dynamics: Principles and applications in combustion and energy systems
Classical and reactive molecular dynamics: Principles and applications in combustion and energy systems
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DOI：
10.1016/j.pecs.2023.101084
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发表时间：
2023-07
影响因子：
29.5
通讯作者：
Q. Mao;Muye Feng;X. Jiang;Yihua Ren;K. Luo;A. V. van Duin
中科院分区：
文献类型：
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作者：
Q. Mao;Muye Feng;X. Jiang;Yihua Ren;K. Luo;A. V. van Duin
在过去的60年里，分子动力学（MD）已经发展成为一种无处不在的、通用的和强大的计算方法，用于生物学、化学、生物医学和物理学等科学分支的基础研究。近几十年来，在快速发展的超级计算技术的推动下，MD已经进入工程领域，作为材料特性、物理化学过程的第一原理预测方法，甚至作为设计工具。这些发展具有深远的影响，本文首次涵盖了燃烧和能源系统的MD，包括气/液/固燃料氧化、热解、催化燃烧、非均相燃烧、电化学、纳米颗粒合成、传热、相变和流体力学等主题。首先，系统地描述了MD方法的理论框架，涵盖了经典和反应性MD。重点是反应性力场（ReaxFF） MD的发展，它使化学反应能够在MD框架内进行模拟，利用量子化学计算和/或实验数据进行力场训练。其次，详细介绍了MD仿真的数值方法、边界条件、后处理和计算成本。接下来是对经典MD方法和反应MD方法在燃烧和能量系统中的应用进行评述。结果表明，ReaxFF MD已成功应用于气体/液体/固体燃料的热解和/或氧化，揭示了详细的能量变化和化学途径。此外，从原子的角度来看，纳米颗粒的催化反应、烟尘形成和火焰合成等复杂的物理化学动力学过程清晰可见。流动，传热和相变现象也仔细审查了MD模拟。在原子水平上研究了纳米尺度过程的前所未有的细节，如液滴碰撞，燃料液滴蒸发，以及亚临界和超临界条件下的二氧化碳捕获和储存。最后，在新兴计算平台、机器学习和多尺度建模的背景下，讨论了燃烧和能源系统的原子模拟的前景。
Molecular dynamics (MD) has evolved into a ubiquitous, versatile and powerful computational method for fundamental research in science branches such as biology, chemistry, biomedicine and physics over the past 60 years. Powered by rapidly advanced supercomputing technologies in recent decades, MD has entered the engineering domain as a first-principle predictive method for material properties, physicochemical processes, and even as a design tool. Such developments have far-reaching consequences, and are covered for the first time in the present paper, with a focus on MD for combustion and energy systems encompassing topics like gas/liquid/solid fuel oxidation, pyrolysis, catalytic combustion, heterogeneous combustion, electrochemistry, nanoparticle synthesis, heat transfer, phase change, and fluid mechanics. First, the theoretical framework of the MD methodology is described systemically, covering both classical and reactive MD. The emphasis is on the development of the reactive force field (ReaxFF) MD, which enables chemical reactions to be simulated within the MD framework, utilizing quantum chemistry calculations and/or experimental data for the force field training. Second, details of the numerical methods, boundary conditions, post-processing and computational costs of MD simulations are provided. This is followed by a critical review of selected applications of classical and reactive MD methods in combustion and energy systems. It is demonstrated that the ReaxFF MD has been successfully deployed to gain fundamental insights into pyrolysis and/or oxidation of gas/liquid/solid fuels, revealing detailed energy changes and chemical pathways. Moreover, the complex physico-chemical dynamic processes in catalytic reactions, soot formation, and flame synthesis of nanoparticles are made plainly visible from an atomistic perspective. Flow, heat transfer and phase change phenomena are also scrutinized by MD simulations. Unprecedented details of nanoscale processes such as droplet collision, fuel droplet evaporation, and CO2capture and storage under subcritical and supercritical conditions are examined at the atomic level. Finally, the outlook for atomistic simulations of combustion and energy systems is discussed in the context of emerging computing platforms, machine learning and multiscale modelling.