Recent developments in molecular mechanics modelling of metal catalyst surfaces with interfaces to complex ad-layers or bulk liquids enable the study of 10 nm scale systems by molecular dynamics simulations of up to microseconds. Therein, electronic polarization as otherwise benchmarked by quantum calculations is mimicked via atom-centered partial charges that are adjusted dynamically to account for changes in local environment. Apart from thermal fluctuations, this encompasses molecule association and dissociation processes as well as externally applied voltage. Here, we elaborate the concept of employing the charge equilibration method to the molecular dynamics simulation of solid catalysts, namely metal surfaces and substrate-supported metal nanoparticles. This showcases the association of reactants and their interplay with local charge polarization upon co-adsorption of ionic liquids or application of external voltage – thus paving the way to understanding complex interfaces in (electro-)catalysis from molecular dynamics simulation.

中文翻译：

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通过分子动力学模拟评估具有离子液体层 (SCILL) 的固体催化剂：局部电荷极化的作用


具有复杂广告层或散装液体界面的金属催化剂表面分子力学建模的最新进展使得能够通过高达微秒的分子动力学模拟来研究 10 nm 尺度的系统。其中，电子极化（以量子计算为基准）是通过以原子为中心的部分电荷来模拟的，这些部分电荷会动态调整以适应局部环境的变化。除了热波动之外，这还包括分子缔合和解离过程以及外部施加的电压。在这里，我们详细阐述了采用电荷平衡方法对固体催化剂（即金属表面和基底负载的金属纳米粒子）进行分子动力学模拟的概念。这展示了反应物的关联及其在离子液体共吸附或施加外部电压时与局部电荷极化的相互作用，从而为从分子动力学模拟理解（电）催化中的复杂界面铺平了道路。