Department of Chemistry, University of Cincinnati, Cincinnati, Ohio 45221, USA.
J Chem Phys. 2017 Oct 28;147(16):161710. doi: 10.1063/1.4992788.
Research on fundamental interactions in Li-ion batteries is accelerating due to the importance of developing batteries with enhanced energy and power densities while maintaining safety. Improving electrode materials and controlling the formation of the solid electrolyte interphase during the first battery charge have been the main focus areas for research. Ion-solvent interactions in the electrolyte are also of great importance in tuning solvation and transport properties, however. Here we present ab initio density functional theory simulations of a Li ion in ethylene and propylene carbonates. The aim is to obtain a detailed analysis of local solvation structure and solvent polarization near the ion and in the bulk. The results indicate the significance of molecular polarization for developing accurate solvation models. The simulations illustrate the substantial differences between ion solvation in water and in organic materials.
由于开发具有更高能量和功率密度同时保持安全性的电池的重要性，锂离子电池中基础相互作用的研究正在加速。改善电极材料和控制电池首次充电时固体电解质中间相的形成一直是研究的主要重点领域。然而，电解质中的离子-溶剂相互作用对于调节溶剂化和输运性质也非常重要。在这里，我们提出了在乙烯和丙烯碳酸酯中的锂离子的从头算密度泛函理论模拟。目的是获得对离子附近和本体中局部溶剂化结构和溶剂极化的详细分析。结果表明分子极化对于开发准确的溶剂化模型的重要性。模拟说明了离子在水中和有机材料中的溶剂化的显著差异。
