Targeted Functionalization of Cyclic Ether Solvents for Controlled Reactivity in High-Voltage Lithium Metal Batteries,ACS Energy Letters

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Targeted Functionalization of Cyclic Ether Solvents for Controlled Reactivity in High-Voltage Lithium Metal Batteries
ACS Energy Letters ( IF 19.3 ) Pub Date : 2023-06-27 , DOI: 10.1021/acsenergylett.3c01004
Yan Zhao ₁ , Tianhong Zhou ₁ , Dominika Baster ₂ , Mario El Kazzi ₂ , Jang Wook Choi ₃ , Ali Coskun ₁

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Understanding the degradation pathways and reactivity of electrolytes is the key to address the shortcomings of conventional electrolytes and to develop new electrolytes for high-voltage lithium metal batteries (LMBs). Accordingly, while 1,3-dioxolane (DOL) exhibits desired features such as good compatibility with Li metal, low viscosity, and high ionic conductivity, it suffers from poor oxidation stability, mainly from its ring-opening polymerization. In an effort to control the reactivity of DOL by tuning its electronic properties, we introduced methyl and trifluoromethyl groups to the ethyl moiety of DOL and developed 4-methyl-1,3-dioxolane (MDOL) and 4-(trifluoromethyl)-1,3-dioxolane (TFDOL) as solvents, respectively. Whereas the MDOL-based electrolyte exhibited serious side reactions toward metallic Li, the TFDOL-based electrolyte showed oxidation stability up to 5.0 V. Moreover, the inorganic-rich solid electrolyte interphase induced by the weak solvation power of TFDOL along with high oxidation stability enabled a robust cycling stability in a Li|NCM811 full cell (20 μm Li foil, N/P ratio of 2.5).

中文翻译：

环醚溶剂的靶向功能化以控制高压锂金属电池的反应性

了解电解质的降解途径和反应性是解决传统电解质缺点和开发用于高压锂金属电池（LMB）的新型电解质的关键。因此，虽然1,3-二氧戊环（DOL）表现出所需的特性，例如与锂金属的良好相容性、低粘度和高离子电导率，但其氧化稳定性较差，主要是由于其开环聚合。为了通过调节 DOL 的电子特性来控制 DOL 的反应性，我们将甲基和三氟甲基引入到 DOL 的乙基部分，并开发了 4-甲基-1,3-二氧戊环 (MDOL) 和 4-(三氟甲基)-1， 3-二氧戊环（TFDOL）分别作为溶剂。鉴于 MDOL 基电解质对金属锂表现出严重的副反应，

更新日期：2023-06-27

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