Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions.
Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and Propylene Carbonate as Solvents for Electrolyte Solutions.
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DOI：
10.1007/s41061-018-0187-2
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发表时间：
2018-02-12
期刊：
影响因子：
--
通讯作者：
Rempe SB
中科院分区：
文献类型：
--
作者：
Chaudhari MI;Muralidharan A;Pratt LR;Rempe SB
综述了基于分子模拟的液体碳酸亚乙酯（EC）和碳酸亚丙酯（PC）的研究进展，着重介绍了原子间作用力的简单模型。散装液体的结果进行检查的角度来看，预期的应用程序的电能存储设备的材料。电化学双层电容器的碳纳米管森林和模型固体电解质界面（SEI）层的锂离子电池的基础上的初步结果被认为是作为例子。讨论的基本结果表明，一个经验参数化，非极化力场可以重现实验的EC和PC液体的结构，热力学和介电性能与可接受的精度。更复杂的力场可能包括分子极化率和白金汉模型对原子间重叠排斥的描述，作为对货车德瓦耳斯相互作用的伦纳-琼斯模型的扩展。简单的方法应该是同样成功的应用程序也为EC/PC解决方案中的有机分子离子，但重要的情况下，锂值得特别注意，因为特别强的相互作用，小离子与相邻的溶剂分子。要处理液体EC/PC溶液中的锂离子，我们确定的经验缩放部分电荷离子-溶剂相互作用的相互作用模型。经验调整使用更多基本输入、电子结构计算和从头算分子动力学模拟，以及EC/PC溶液中Li热力学和输运的实验结果。应用这种模型的锂输运机制在玻璃SEI模型强调了这些非平衡材料的长时间尺度的分子动力学研究的优势。
Progress in understanding liquid ethylene carbonate (EC) and propylene carbonate (PC) on the basis of molecular simulation, emphasizing simple models of interatomic forces, is reviewed. Results on the bulk liquids are examined from the perspective of anticipated applications to materials for electrical energy storage devices. Preliminary results on electrochemical double-layer capacitors based on carbon nanotube forests and on model solid-electrolyte interphase (SEI) layers of lithium ion batteries are considered as examples. The basic results discussed suggest that an empirically parameterized, non-polarizable force field can reproduce experimental structural, thermodynamic, and dielectric properties of EC and PC liquids with acceptable accuracy. More sophisticated force fields might include molecular polarizability and Buckingham-model description of inter-atomic overlap repulsions as extensions to Lennard-Jones models of van der Waals interactions. Simple approaches should be similarly successful also for applications to organic molecular ions in EC/PC solutions, but the important case of Li deserves special attention because of the particularly strong interactions of that small ion with neighboring solvent molecules. To treat the Li ions in liquid EC/PC solutions, we identify interaction models defined by empirically scaled partial charges for ion-solvent interactions. The empirical adjustments use more basic inputs, electronic structure calculations and ab initio molecular dynamics simulations, and also experimental results on Li thermodynamics and transport in EC/PC solutions. Application of such models to the mechanism of Li transport in glassy SEI models emphasizes the advantage of long time-scale molecular dynamics studies of these non-equilibrium materials.
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影响因子：
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