Gerrits Nick
Gorlaeus Laboratories, Leiden Institute of Chemistry, Leiden University, Leiden, Netherlands.
Front Chem. 2024 Oct 9;12:1481235. doi: 10.3389/fchem.2024.1481235. eCollection 2024.
The dissociation of methane is not only an important reaction step in catalytic processes, but also of fundamental interest. Dynamical effects during the dissociative chemisorption of methane on metal surfaces cause significant differences in computed reaction rates, compared to what is predicted by typical transition state theory (TST) models. It is clear that for a good understanding of the catalytic activation of methane dynamical simulations are required. In this paper, a general blueprint is provided for performing dynamical simulations of the dissociative chemisorption of methane on metal surfaces, by employing either the quasi-classical trajectory or ring polymer molecular dynamics approach. If the computational setup is constructed with great care-since results can be affected considerably by the setup - chemically accurate predictions are achievable. Although this paper concerns methane dissociation, the provided blueprint is, so far, applicable to the dissociative chemisorption of most molecules.
甲烷的解离不仅是催化过程中的一个重要反应步骤，而且具有重要的基础研究意义。与典型的过渡态理论（TST）模型预测的结果相比，甲烷在金属表面解离化学吸附过程中的动力学效应导致计算出的反应速率存在显著差异。显然，为了深入理解甲烷的催化活化过程，需要进行动力学模拟。本文提供了一个通用蓝图，用于通过准经典轨迹或环聚合物分子动力学方法对甲烷在金属表面的解离化学吸附进行动力学模拟。由于计算设置会对结果产生很大影响，因此如果精心构建计算设置，就可以实现化学精度的预测。尽管本文关注的是甲烷解离，但到目前为止，所提供的蓝图适用于大多数分子的解离化学吸附。
