ICGM, Université de Montpellier, CNRS, ENSCM, 34095Montpellier, France.
Réseau sur le Stockage Electrochimique de l'Energie (RS2E), FR CNRS3459, Hub de l'Energie, 80039Amiens, France.
J Chem Theory Comput. 2023 Feb 14;19(3):1023-1034. doi: 10.1021/acs.jctc.2c00926. Epub 2023 Jan 24.
Classical molecular dynamics (MD) simulations of electrolyte systems are important to gain insight into the atom-scale properties that determine the battery-relevant performance. The recent Tinker-HP software release enables efficient and accurate MD simulations with the AMOEBA polarizable force field. In this work, we developed a procedure to construct a universal AMOEBA model for the solvent family of glymes (glycol methyl ethers), which involves a refinement scheme for valence parameters by fitting the AMOEBA-derived atomic forces to those computed at the DFT level. The refined AMOEBA model provides a good description of both local and nonlocal properties in terms of the spectroscopic response of glyme molecules, as well as the liquid glyme density and dielectric constant. In addition, the complexation energies of alkali and alkaline-earth metal cations with tetraglyme molecules obtained from AMOEBA calculations are in good agreement with DFT results, demonstrating the suitability of the developed AMOEBA model for an accurate simulation of glyme-based battery electrolytes. We also expect the procedure to be transferable to the development of AMOEBA models for other battery electrolyte systems.
经典的电解质体系分子动力学（MD）模拟对于深入了解决定电池相关性能的原子尺度性质非常重要。最近发布的 Tinker-HP 软件可以使用 AMOEBA 极化力场进行高效、准确的 MD 模拟。在这项工作中，我们开发了一种构建用于糖醚（乙二醇甲基醚）溶剂族的通用 AMOEBA 模型的方法，其中涉及通过将 AMOEBA 衍生的原子力拟合到在 DFT 水平上计算出的原子力来改进价参数的方案。改进后的 AMOEBA 模型很好地描述了糖醚分子的光谱响应以及液体糖醚密度和介电常数的局部和非局部性质。此外，通过 AMOEBA 计算得到的碱金属和碱土金属阳离子与四甘醇分子的络合能与 DFT 结果非常吻合，这表明所开发的 AMOEBA 模型非常适合用于准确模拟基于糖醚的电池电解质。我们还期望该程序可转移到用于其他电池电解质体系的 AMOEBA 模型的开发。
