论文标题
了解金属表面上的高温化学反应
Understanding High-Temperature Chemical Reactions on Metal Surfaces
论文作者
论文摘要
金属表面上的化学反应在各种过程中很重要，例如异质催化和纳米结构生长。在中等或较低的温度下，这些反应通常遵循最小能量路径和温度效应，可以通过谐波振荡器模型合理地描述。在接近底物熔点的高温下，表面反应的一般行为仍然难以捉摸。在这项研究中，通过将碳氢化合物物种吸附在Cu上（111）作为模型系统并进行由机器学习潜力提供动力的广泛的分子动力学模拟，我们确定了几种重要的高温效应，包括局部化学环境，表面原子迁移率和底物热膨胀。它们以不同的方式影响高温表面反应的不同方面。这些结果加深了我们对高温反应的理解。
Chemical reactions on metal surfaces are important in various processes such as heterogeneous catalysis and nanostructure growth. At moderate or lower temperatures, these reactions generally follow the minimum energy path and temperature effects can be reasonably described by a harmonic oscillator model. At a high temperature approaching the melting point of the substrate, general behaviors of surface reactions remain elusive. In this study, by taking hydrocarbon species adsorbed on Cu(111) as a model system and performing extensive molecular dynamics simulations powered by machine learning potentials, we identify several important high-temperature effects, including local chemical environment, surface atom mobility, and substrate thermal expansion. They affect different aspects of a high-temperature surface reaction in different ways. These results deepen our understanding of high-temperature reactions.
