Construction of Stable Li2O-Rich Solid Electrolyte Interphase for Practical PEO-Based Li-Metal Batteries,Advanced Energy Materials

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Construction of Stable Li2O-Rich Solid Electrolyte Interphase for Practical PEO-Based Li-Metal Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-12-15 , DOI: 10.1002/aenm.202302587
Jiahui Zhang _{1,

2} , Siyuan Li ₁ , Xinyang Wang ₁ , Shulan Mao _{1,

2} , Junze Guo ₁ , Zeyu Shen _{1,

2} , Jiale Mao _{1,

2} , Qian Wu _{1,

2} , Kang Shen ₃ , Hao Cheng _{1,

2} , Yuanzhong Tan ₃ , Yingying Lu _{1,

2}

Affiliation

Polyethylene oxide (PEO)-based solid polymer electrolytes (SPE) have garnered recognition as highly promising candidates for advanced lithium-metal batteries. However, the practical application of PEO-based SPE is hindered by its low critical current density (CCD) resulting from undesired dendrite growth. In this study, a PEO-based SPE that exhibits an ultra-high CCD (4 mA cm⁻²) is presented and enhanced lithium ionic conductivity through the incorporation of small amounts of P₂S₅ (PS). The crystalline Li₂O-rich and P/S-containing solid electrolyte interphase (SEI) is revealed by cryo-electron microscope (cryo-EM) and Time of flight secondary ion mass spectrometry (TOF-SIMS), which inhibits dendrite growth and adverse reactions between SPE and reductive lithium, thus offering a spherical growth behavior for dendrite-free lithium metal anode. Consequently, utilizing the PS-integrated SPE, a Li-Li symmetric cell demonstrates reduced resistance during operation, enabling stable cycles exceeding 200 hours at 0.5 mA cm⁻² and 0.5 mAh cm⁻², a stringent test condition for PEO-based electrolytes. Moreover, a Li/SPE/LiFePO₄ (LFP) pouch cell exhibits 80% capacity retention after 100 cycles with 50 µm Li and 30 µm PEO electrolyte, showcasing its potential for practical applications.

中文翻译：

实用PEO基锂金属电池稳定富Li2O固体电解质界面的构建

基于聚环氧乙烷（PEO）的固体聚合物电解质（SPE）已被认为是先进锂金属电池的极有前景的候选材料。然而，基于 PEO 的 SPE 的实际应用受到不良枝晶生长导致的低临界电流密度 (CCD) 的阻碍。在这项研究中，提出了一种基于PEO的SPE，它具有超高CCD（4 mA cm ^-2），并通过掺入少量的P ₂ S ₅ (PS)来增强锂离子电导率。通过冷冻电子显微镜 (cryo-EM) 和飞行时间二次离子质谱 (TOF-SIMS) 揭示了富含 Li ₂ O 且含有 P/S 的晶体电解质界面 (SEI)，它抑制了枝晶的生长，并抑制了枝晶的生长。 SPE 和还原性锂之间发生不良反应，从而为无枝晶的锂金属负极提供球形生长行为。因此，利用PS集成SPE，Li-Li对称电池在运行过程中表现出较低的电阻，从而能够在0.5 mA cm ^-2和0.5 mAh cm ^-2下稳定循环超过200小时，这是基于PEO的电解质的严格测试条件。此外，Li/SPE/LiFePO ₄ (LFP) 软包电池在使用 50 µm Li 和 30 µm PEO 电解质的 100 次循环后表现出 80% 的容量保持率，展示了其实际应用的潜力。

更新日期：2023-12-15

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