Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries

Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries

The widespread adoption of Li-ion batteries in energy storage and power applications necessitates advancements in energy density, safety, and reliability. All-solid-state Li-ion batteries (SSBs) are a promising direction. This study investigates the interfacial behavior of LiNi0.83Co0.14Mn0.03O2 (NC...

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Bibliographic Details
Main Authors: Jing Wang, Yi Zhang, Yingchun Lyu, Tu Lan, Bing Han, Yitong Guo, Zexi Yang, Jingjing Zhou, Shangqian Zhao, Rong Yang, Shigang Lu
Format: Article
Language:English
Published: Elsevier 2025-10-01
Series:Next Materials
Subjects:
Ni rich NCM
Solid electrolyte interface
Halide electrolyte
All solid-state batteries
Online Access:http://www.sciencedirect.com/science/article/pii/S2949822825004496
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Summary:The widespread adoption of Li-ion batteries in energy storage and power applications necessitates advancements in energy density, safety, and reliability. All-solid-state Li-ion batteries (SSBs) are a promising direction. This study investigates the interfacial behavior of LiNi0.83Co0.14Mn0.03O2 (NCM83)/Li3InCl6 (LIC) SSBs at high potentials (≥4.3 V) before and after cycling. AC impedance analysis reveals increased interfacial impedance at high potentials, particularly during constant-current/constant-voltage charging, indicating interfacial instability. High-resolution transmission electron microscopy (HR-TEM) identifies a 5 nm rock-salt phase on NCM83 at 4.3 V, thickening to 12 nm at 4.5 V, accompanied by a 15 nm lattice distortion layer. X-ray absorption spectroscopy (XAS) confirms Ni3 + /4 + reduction to Ni2+, correlating with rock-salt phase formation. X-ray photoelectron spectroscopy (XPS) detects Cl and In oxides on LIC at 4.5 V, suggesting interfacial reactions. Scanning electron microscopy (SEM) reveals cracks at the NCM83/LIC interface and within the LIC electrolyte, causing interfacial contact loss and structural degradation. In situ X-ray diffraction (XRD) attributes this to volume changes during H2–H3 phase transitions in NCM83. As a result, there are interfacial reactions at high potentials and interfacial contact loss during cycling. Electrode-dense structure damage of NCM83 in LIC-based SSBs leads to accelerated electrochemical performance degradation at high potentials.
ISSN:2949-8228

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