High-voltage poly (ethylene oxide) all-solid-state lithium batteries enabled by high-concentration interfacial layer

IF 11 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Rare Metals Pub Date : 2025-07-31 DOI:10.1007/s12598-025-03464-y

Hao-Tong Li, Geng-Chen Wang, Zi-Hu Kang, Yue Zheng, Ning-Ning Wu, Xia Tao

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引用次数: 0

Abstract

Poly (ethylene oxide) (PEO) solid electrolytes hold great promise in all-solid-state lithium batteries (ASSLBs) with high-energy and safety capabilities. However, the PEO electrolyte is hardly resistant to degrade electrochemically at high voltages (>4 V) in ASSLBs. Herein, we design and prepare a highly efficient and stable PEO-based solid electrolyte (denoted as PEO-L/DT-PEO) applied to high-voltage ASSLBs, in which the Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO)-containing PEO (PEO-L) serves as a bulk of the electrolyte and the PEO with dual-salts (LiDFOB and high-concentration LiTFSI) forms an ultrathin coating layer (DT-PEO) covering on PEO-L. With 3% coating layer, the PEO-L/DT-PEO electrolyte exhibits an enhanced decomposition potential (> 4.9 V vs. Li/Li⁺) originating from the high concentration of LiTFSI as well as renders Al foil current collector high anticorrosion by the introduction of LiDFOB. Upon coupling with high-voltage NCM811 cathode, the DT-PEO efficiently suppresses the interfacial degradation kinetics between electrolyte and cathode, and slows down the irreversible phase change of NCM811. The assembled PEO-L/DT-PEO-based Li/NCM811 battery exhibits an excellent cycling stability of remaining 63.0% after 400 cycles at a cutoff voltage of 4.2 V as well as an initial discharge specific capacity of 164.5 mAh g⁻¹ at a rate of 0.4C. This work offers a facile and feasible strategy to overcoming interface decomposition of the PEO electrolyte matching perfectly with high-voltage cathode for high-performance ASSLBs.

Graphical abstract

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高浓度界面层使高压聚环氧乙烷全固态锂电池成为可能

聚环氧乙烷（PEO）固体电解质具有高能量和安全性能，在全固态锂电池（asslb）中具有很大的前景。然而，在asslb中，PEO电解质在高压（>4 V）下很难抵抗电化学降解。本文设计并制备了一种用于高压asslb的高效稳定的PEO基固体电解质（记为PEO- l /DT-PEO），其中含Li6.4La3Zr1.4Ta0.6O12 （LLZTO）的PEO （PEO- l）作为主体电解质，PEO与双盐（LiDFOB和高浓度LiTFSI）形成超薄涂层（DT-PEO）覆盖在PEO- l上。当涂层层数为3%时，PEO-L/DT-PEO电解质的分解电位（> 4.9 V vs. Li/Li+）因高浓度的LiTFSI而增强，并通过引入LiDFOB使Al箔集流器具有较高的耐腐蚀性。与高压NCM811阴极耦合后，DT-PEO有效抑制了电解质与阴极之间的界面降解动力学，减缓了NCM811的不可逆相变。组装的PEO-L/ dt - peo基Li/NCM811电池在4.2 V的截止电压下，在400次循环后的剩余率为63.0%，在0.4C的速率下，初始放电比容量为164.5 mAh g−1。这项工作为克服高性能assb中PEO电解质与高压阴极完美匹配的界面分解提供了一种简单可行的策略。图形抽象

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来源期刊

Rare Metals 工程技术-材料科学：综合

CiteScore

12.10

自引率

12.50%

发文量

2919

审稿时长

2.7 months

期刊介绍： Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.