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首页> 外文期刊>ACS applied materials & interfaces >Impact of cis- versus trans-Configuration of Butylene Carbonate Electrolyte on Microscopic Solid Electrolyte Interphase Formation Processes in Lithium-Ion Batteries
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Impact of cis- versus trans-Configuration of Butylene Carbonate Electrolyte on Microscopic Solid Electrolyte Interphase Formation Processes in Lithium-Ion Batteries

机译：CIS-碳酸丁酯电解液对锂离子电池微观固体电解质间形成过程的影响

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摘要

The solid electrolyte interphase (SEI) film, which consists of the products of reduction reaction of the electrolyte, has a strong influence on the lifetime and safety of Li-ion batteries. Of particular importance when designing SEI films is its strong dependence on the electrolyte solvent. In this study, we focused on geometric isomers cis- and trans-2,3-butylene carbonates (c/t-BC) as model electrolytes. Despite their similar structures and chemical properties, t-BC-based electrolytes have been reported to enable the reversible reaction of graphite anodes [as in ethylene carbonate (EC)], whereas c-BC-based electrolytes cause the exfoliation of graphite [as in propylene carbonate (PC)]. To understand the microscopic origin of the different electrochemical behaviors of t-BC and c-BC, we applied Red Moon simulation to elucidate the microscopic SEI film formation processes. The results revealed that the SEI film formed in c-BC-based electrolytes contains fewer dimerized products, which are primary components of a good SEI film; this lower number of dimerized products can cause reduced film stability. As one of the origins of the decreased dimerization in c-BC, we identified the larger solvation energy of c-BC for the intermediate species and its smaller diffusion constant, which largely diminishes the dimerization. Moreover, the correlation among the Li+ intercalation behavior, nature of the SEI film, and strength of solvation was found to be common for EC/PC and t-BC/c-BC electrolytes, confirming the importance of solvation of the intermediates in the stability of the SEI film. These results suggest that weakening the solvation of the intermediates is one possible way to stabilize the SEI film for better charge-discharge performance.
机译：由电解质还原反应的产品组成的固体电解质相互作用（SEI）膜对锂离子电池的寿命和安全性具有很大的影响。在设计SEI薄膜时特别重要是它对电解质溶剂的强烈依赖。在这项研究中，我们将几何异构体CIS-和反式-2,3-丁烯碳酸丁酯（C / T-BC）为模型电解质。尽管它们具有相似的结构和化学性质，但据报道了T-BC基电解质能够使石墨阳极的可逆反应[如在碳酸亚乙酯（EC）中，而基于C-BC的电解质会导致石墨的剥离[如在碳酸亚丙酯（PC）]。为了了解T-BC和C-BC的不同电化学行为的显微血管来源，我们施加了红月岩仿真以阐明微观SEI膜形成过程。结果表明，在基于C-BC的电解质中形成的SEI膜含有较少的二聚产物，其是良好的SEI膜的主要成分;这种较少的二聚产物数量会导致薄膜稳定性降低。作为C-BC中的降低的起源之一，我们鉴定了C-BC的较大溶剂化能量，用于中间物质及其较小的扩散常数，其在很大程度上减少了二聚化。此外，发现SEI膜的性质，SEI膜的性质和溶剂强度的相关性对于EC / PC和T-BC / C-BC电解质常见，证实了中间体在稳定性中溶解的重要性SEI电影。这些结果表明，削弱中间体的溶解是稳定SEI膜以更好地放电性能的一种可能方法。

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