Optimizing NaF-Rich Solid Electrolyte Interphase for Stabilizing Sodium Metal Batteries by Electrolyte Additive,Advanced Functional Materials

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Optimizing NaF-Rich Solid Electrolyte Interphase for Stabilizing Sodium Metal Batteries by Electrolyte Additive
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-04-27 , DOI: 10.1002/adfm.202214195
Chunlei Zhu ₁ , Daxiong Wu ₁ , Zhongsheng Wang ₁ , Huaping Wang ₁ , Jiandong Liu ₁ , Kanglong Guo ₁ , Quanhui Liu ₁ , Jianmin Ma ₁

Affiliation

NaF-rich electrode–electrolyte interphases play crucial roles in determining the cycling stability of sodium metal batteries (SMBs) because of their electronic insulation and mechanical stability. In this work, perfluorobenzene (PFB) is proposed as the additive to contribute the formation of NaF-rich solid electrolyte interphases (SEI). PFB at the periphery of the solvation layer can pull out a part of the EC with the lowest solvation energy by Van der Waals forces, thus allowing more

P F_{6}^{-} ${\bf PF}_{\bf 6}^{\bm{ - }}$

to participate in the Na⁺ solvation layer and form an anion-aggregated solvation sheath, thus promoting the decomposition of

P F_{6}^{-} ${\bf PF}_{\bf 6}^{\bm{ - }}$

to produce NaF. In addition, PFB has a higher highest occupied molecular orbital and lower lowest unoccupied molecular orbital energy level, which also preferentially decomposes to produce NaF at both electrodes. Benefiting from the intensified NaF ratio in SEI, the Na||Na symmetric cells with such an electrolyte achieves a superior cycling life over 350 h at 1 mA cm⁻², and the Na||Na₃V₂(PO₄)₂O₂F batteries also realize ultrahigh cycling performance with 88.8% capacity retention after 500 cycles.

中文翻译：

通过电解质添加剂优化富NaF固体电解质界面以稳定钠金属电池

富含 NaF 的电极-电解质界面由于其电子绝缘性和机械稳定性，在决定钠金属电池 (SMB) 的循环稳定性方面发挥着至关重要的作用。在这项工作中，提出全氟苯（PFB）作为添加剂来促进富含NaF的固体电解质中间相（SEI）的形成。溶剂化层外围的PFB可以通过范德华力将溶剂化能最低的部分EC拉出，从而允许更多

磷 F_{6}^{-} ${\bf PF}_{\bf 6}^{\bm{ - }}$

参与Na ⁺溶剂化层，形成阴离子聚集的溶剂化鞘，从而促进Na + 溶剂化层的分解

磷 F_{6}^{-} ${\bf PF}_{\bf 6}^{\bm{ - }}$

生产NaF。此外，PFB具有较高的最高占据分子轨道和较低的最低未占据分子轨道能级，这也优先在两个电极上分解产生NaF。受益于SEI中增强的NaF比例，具有这种电解质的Na||Na对称电池在1 mA cm ^-2下实现了超过350小时的优异循环寿命，并且Na||Na ₃ V ₂ (PO ₄ ) ₂ O _2F电池还实现了超高的循环性能，500次循环后容量保持率为88.8%。

更新日期：2023-04-27

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