Design Rules for Selecting Fluorinated Linear Organic Solvents for Li Metal Batteries,The Journal of Physical Chemistry Letters

当前位置： X-MOL 学术 › J. Phys. Chem. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Design Rules for Selecting Fluorinated Linear Organic Solvents for Li Metal Batteries
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-06-17 , DOI: 10.1021/acs.jpclett.1c01522
Yumin Zhang ₁ , Venkatasubramanian Viswanathan _{1,

2}

Affiliation

Fluorinated linear organic solvents have great potential in improving the safety and lifetime of next-generation Li metal batteries. However, this group of solvents is underexplored. Here, we investigate the molecular and interfacial reactivity properties of seven partially and fully fluorinated linear carbonates designed based on conventional solvents. Using density functional theory, we find the highest occupied molecular orbital levels decrease with increasing substitution of the fluorinated functional groups, implying that fluorination, to a first approximation, improves the stability toward high voltage cathodes. On the basis of the simulated decomposition mechanisms and statistical analyses, we find that a fluorinated linear carbonate with partial fluorination at the methyl component is more accessible in terms of degradation and LiF nascence formation, leading to a potentially LiF-rich solid electrolyte interphase (SEI). The molecular design concepts and the computational techniques presented are transferable to ester and ether systems, facilitating the navigation in a large chemical design space.

中文翻译：

锂金属电池氟化线性有机溶剂选择设计规则

含氟线性有机溶剂在提高下一代锂金属电池的安全性和寿命方面具有巨大潜力。然而，这组溶剂尚未得到充分探索。在这里，我们研究了基于常规溶剂设计的七种部分和完全氟化的直链碳酸酯的分子和界面反应性。使用密度泛函理论，我们发现最高占据的分子轨道水平随着氟化官能团取代度的增加而降低，这意味着氟化在第一近似值上提高了对高压阴极的稳定性。在模拟分解机制和统计分析的基础上，我们发现在甲基组分部分氟化的氟化直链碳酸酯在降解和 LiF 新生形成方面更容易获得，从而导致潜在的富含 LiF 的固体电解质中间相 (SEI)。所呈现的分子设计概念和计算技术可转移到酯和醚系统，促进在大型化学设计空间中的导航。

更新日期：2021-06-24

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南