Water-Stable Sulfide Solid Electrolyte Membranes Directly Applicable in All-Solid-State Batteries Enabled by Superhydrophobic Li+-Conducting Protection Layer,Advanced Energy Materials

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Water-Stable Sulfide Solid Electrolyte Membranes Directly Applicable in All-Solid-State Batteries Enabled by Superhydrophobic Li+-Conducting Protection Layer
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2021-12-05 , DOI: 10.1002/aenm.202102348
Jieru Xu _{1,

2,

3,

4} , Yongxing Li _{1,

5} , Pushun Lu _{1,

2,

3,

4} , Wenlin Yan _{1,

2,

3,

4} , Ming Yang _{1,

5} , Hong Li _{1,

2,

3,

4} , Liquan Chen _{1,

2,

3,

4} , Fan Wu _{1,

2,

3,

4,

5}

Affiliation

Sulfide solid electrolytes (SEs) represent one most promising technical routes to realize all-solid-state batteries (ASSBs) due to their high ionic conductivity and low mechanical stiffness. However, the poor air/moisture/water stability of sulfide SEs leads to completely destroyed structure/composition, reduced Li⁺ conductivity, and toxic H₂S release, limiting their practical application in ASSBs. To solve this problem, a universal method applicable to all types of sulfide SEs is developed to realize water-stable sulfide SE membranes, by spray coating a Li⁺-conductive superhydrophobic protection layer with Li_1.4Al_0.4Ti_1.6(PO₄)₃ (LATP) nanoparticles and fluorinated polysiloxane (F-POS) via hydrolysis and condensation of tetraethyl orthosilicate and 1H,1H,2H,2H-perfluorodecyltriethoxysilane molecules. The F-POS@LATP coating layer exhibits excellent superhydrophobicity (water static contact angles > 160°) to resist extreme exposure (direct water jetting), because of its micro-/nanoscale roughness and low surface energy. Moreover, ASSBs using the extreme-condition-exposed modified Li₆PS₅Cl membrane exhibit a reversible capacity of 147.3 mAh g^-1, comparable with the ASSBs using pristine sulfide membranes. The superhydrophobic Li⁺-conducting layer is demonstrated to be an effective protection method for sulfide membranes so that they remain stable and functionable in extreme water exposure conditions, providing a new approach to protect all types of sulfide SEs and other air/moisture/water-sensitive materials without sacrificing electrochemical performance.

中文翻译：

超疏水锂离子导电保护层可直接应用于全固态电池的水稳定硫化物固体电解质膜

硫化物固体电解质（SEs）由于其高离子电导率和低机械刚度是实现全固态电池（ASSB）的一种最有前途的技术路线。然而，硫化物SEs较差的空气/水分/水稳定性导致结构/组成完全破坏，Li ⁺电导率降低和有毒的H ₂ S释放，限制了它们在ASSBs中的实际应用。为了解决这个问题，开发了一种适用于所有类型硫化物 SE 的通用方法，通过喷涂Li _1.4 Al _0.4 Ti _1.6 (PO ₄⁾₃来实现水稳定的硫化物 SE 膜。(LATP) 纳米颗粒和氟化聚硅氧烷 (F-POS) 通过原硅酸四乙酯和 1 H ,1 H ,2 H ,2 H -全氟癸基三乙氧基硅烷分子的水解和缩合。F-POS@LATP 涂层由于其微米/纳米级粗糙度和低表面能而表现出优异的超疏水性（水静态接触角 > 160°）以抵抗极端暴露（直接喷水）。此外，使用暴露在极端条件下的改性 Li ₆ PS ₅ Cl 膜的 ASSB 的可逆容量为 147.3 mAh g ^-1，与使用原始硫化物膜的 ASSB 相当。超疏水的 Li ⁺- 导电层被证明是一种有效的硫化膜保护方法，使它们在极端的水暴露条件下保持稳定和功能，提供了一种新的方法来保护所有类型的硫化物 SEs 和其他空气/水分/水敏感材料而不牺牲电化学性能。

更新日期：2022-01-13

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