Frömbgen Tom, Zaby Paul, Alizadeh Vahideh, Da Silva Juarez L F, Kirchner Barbara, Lourenço Tuanan C
Mulliken Center for Theoretical Chemistry, University of Bonn, Beringstraße 4, D-53115, Bonn, Germany.
São Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, Brazil.
Chemphyschem. 2025 Apr 14;26(8):e202401048. doi: 10.1002/cphc.202401048. Epub 2025 Feb 18.
Ionic liquids are nowadays investigated with respect to their use as electrolytes for high-performance energy storage materials. In this study, we provide a tutorial on how to calculate dynamic properties such as self-diffusion coefficients, ionic conductivities, transference numbers, as well as ion pair and ion cage dynamics, that all play a role in judging the applicability of ionic liquids as electrolytes. For the case of the ionic liquid , we investigate the performance of different force fields. Amongst them are non-polarizable models employing unity charges, a charge-scaled version of a non-polarizable model, a polarizable model and another non-polarizable model with refined Lennard-Jones parameters. We also study the influence of the system size on the dynamic properties. While all studied force field models capture qualitatively correct trends, only the polarizable force field and the non-polarizable force field with refined Lennard-Jones parameters provide quantitative agreement to reference data, making the latter model very attractive for the reason of lower computational costs.
如今，人们正在研究离子液体作为高性能储能材料电解质的用途。在本研究中，我们提供了一个教程，介绍如何计算诸如自扩散系数、离子电导率、迁移数以及离子对和离子笼动力学等动态性质，这些性质在判断离子液体作为电解质的适用性方面都起着重要作用。对于离子液体 的情况，我们研究了不同力场的性能。其中包括采用单位电荷的非极化模型、非极化模型的电荷缩放版本、极化模型以及另一个具有精细 Lennard-Jones 参数的非极化模型。我们还研究了系统尺寸对动态性质的影响。虽然所有研究的力场模型在定性上都捕捉到了正确的趋势，但只有极化力场和具有精细 Lennard-Jones 参数的非极化力场与参考数据提供了定量一致性，由于计算成本较低，后一种模型非常有吸引力。
