Argyrodite 基电解质的高空气稳定性和优异的锂金属相容性可实现卓越的全固态锂金属电池,Advanced Functional Materials

当前位置： X-MOL 学术 › Adv. Funct. Mater. › 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.)

Argyrodite 基电解质的高空气稳定性和优异的锂金属相容性可实现卓越的全固态锂金属电池
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-05-26 , DOI: 10.1002/adfm.202203858
Hong Liu ₁ , Qisi Zhu ₁ , Chao Wang ₁ , Guoxu Wang ₁ , Yuhao Liang ₁ , Dabing Li ₁ , Lei Gao ₁ , Li‐Zhen Fan ₁

Affiliation

用于全固态锂金属电池（ASSLMBs）的硫化物固体电解质（SSEs）由于其超高的离子电导率和良好的机械加工性而受到越来越多的关注。然而，目前的SSEs普遍存在锂金属相容性差和空气稳定性差的问题，严重阻碍了它们在ASSLMBs的实际应用。在此，首次通过 Bi, O 共掺杂 Li ₆ PS ₅ Cl 合成了新型的基于 Argyrodite 的 Li ₆₊₂_x P ₁₋_x Bi _x S _5−1.5_x O _1.5_x Cl SSE 。通过调整掺杂浓度，优化后的 Li _6.04 P _0.98 Bi_0.02 S _4.97 O _0.03 Cl 具有超高的离子电导率（3.4 × 10 ^-3 S cm ^-1）。此外，这种电解质在暴露于潮湿空气和氯苯后表现出出色的结构稳定性，表现出令人赞叹的空气稳定性和溶剂稳定性。通过进行第一性原理密度泛函理论计算，可以深刻理解氧化物掺杂 SSE 增强空气稳定性的机制。此外，Li _6.04 P _0.98 Bi _0.02 S _4.97 O _0.03 Cl 电解液引发了 Li 负极界面上的铋合金在降低锂^离子扩散能垒和提高界面相容性方面发挥着至关重要的作用，导致锂对称电池具有 1.1 mA cm ^-2的超高临界电流密度和出色的循环稳定性。因此，配备原始或空气暴露 Li _6.04 P _0.98 Bi _0.02 S _4.97 O _0.03 Cl 的 ASSLMB 可以在室温下提供令人满意的放电比容量。

"点击查看英文标题和摘要"

High Air Stability and Excellent Li Metal Compatibility of Argyrodite-Based Electrolyte Enabling Superior All-Solid-State Li Metal Batteries

Sulfide solid electrolytes (SSEs) for all-solid-state Li metal batteries (ASSLMBs) are attracting increasing attention due to their ultrahigh ionic conductivity and good machinability. However, current SSEs generally suffer from inferior Li metal compatibility and poor air-stability, which severely impede their practical applications for ASSLMBs. Herein, novel argyrodite-based SSEs of Li₆₊₂_xP₁₋_xBi_xS_5−1.5_xO_1.5_xCl are synthesized via the Bi, O co-doping the Li₆PS₅Cl for the first time. By adjusting the concentrations of dopant, the optimized Li_6.04P_0.98Bi_0.02S_4.97O_0.03Cl presents an ultrahigh ionic conductivity (3.4 × 10⁻³ S cm⁻¹). Moreover, such electrolyte displays splendid structural stability after exposure to humid air and chlorobenzene, demonstrating admirable air-stability and solvent-stability. The mechanism of the enhanced air-stability of oxide-doped SSEs is profoundly understood by conducting first-principles density functional theory calculations. In addition, the Li_6.04P_0.98Bi_0.02S_4.97O_0.03Cl electrolyte triggers the generation of LiBi alloy at the anode interface, which plays a crucial role in reducing Li⁺ diffusion energy barriers and improving interfacial compatibility, leading to an ultrahigh critical current density of 1.1 mA cm⁻² and splendid cyclic stability in Li symmetric cell. As a result, ASSLMBs equipped with either pristine or air-exposed Li_6.04P_0.98Bi_0.02S_4.97O_0.03Cl can deliver satisfying discharge specific capacity at room temperature.

更新日期：2022-05-26

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