Interface Degradation of LaCl3-Based Solid Electrolytes Coupled with Ultrahigh-Nickel Cathodes

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2024-11-25 DOI:10.1021/acs.nanolett.4c0350210.1021/acs.nanolett.4c03502

Ye-Chao Wu, Feng Li, Xiaobin Cheng, Yihong Tan, Xin Huang, Jin-Da Luo, Shu Chen, Ruijun Pan, Yi-Chen Yin*, Zheng Liang* and Hong-Bin Yao*,

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Abstract

Despite competitive compatibility with high-nickel cathodes, chloride solid electrolytes (SEs) still experience inevitable side reactions at the cathode/SE interface, causing capacity decay in all-solid-state lithium batteries (ASSLBs) during cycling. Herein, a three-electrode ASSLB testing device is developed to comprehensively reveal the interface failure mechanisms of the ultrahigh-nickel LiNi_0.92Co_0.05Mn_0.03O₂ (NCM92) cathode paired with LaCl₃-based chloride SE Li_0.447La_0.475Zr_0.059Ta_0.179Cl₃ (LLZTC). Distribution of relaxation time (DRT) analysis clearly shows the ASSLB degradation accompanied by a significant NCM92/LLZTC interface impedance increase, which becomes more pronounced at the higher cutoff charging voltage of 4.8 V vs Li⁺/Li. Furthermore, time-of-flight secondary ion mass spectrometry (ToF-SIMS) and focused ion beam scanning electron microscopy (FIB-SEM) analysis also confirm the deterioration arising from active lattice oxygen and loss of physical contact at the NCM92/LLZTC interface. These findings reveal both electrochemical degradation and physical contact failure at the cathode/SE interface as key causes of the ASSLBs’ capacity decay.

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lacl3基固体电解质与超高镍阴极耦合界面降解研究

尽管氯化物固体电解质（SEs）与高镍阴极具有很强的兼容性，但在阴极/SE界面仍会发生不可避免的副反应，导致全固态锂电池（ASSLBs）在循环过程中容量衰减。为了全面揭示超高镍lini0.92 co0.05 mn0.030 o2 （NCM92）阴极与lacl3基氯离子SE Li0.447La0.475Zr0.059Ta0.179Cl3 （LLZTC）的界面破坏机理，研制了三电极ASSLB测试装置。弛缓时间（DRT）分布分析清楚地表明，ASSLB降解伴随着NCM92/LLZTC界面阻抗的显著增加，在4.8 V vs Li+/Li较高的截止充电电压下更为明显。此外，飞行时间二次离子质谱（ToF-SIMS）和聚焦离子束扫描电镜（FIB-SEM）分析也证实了NCM92/LLZTC界面上活性点阵氧和物理接触损失引起的劣化。这些发现表明，阴极/SE界面的电化学降解和物理接触失效是asslb容量衰减的主要原因。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.