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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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
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Online Access:http://www.sciencedirect.com/science/article/pii/S2949822825004496
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author Jing Wang
Yi Zhang
Yingchun Lyu
Tu Lan
Bing Han
Yitong Guo
Zexi Yang
Jingjing Zhou
Shangqian Zhao
Rong Yang
Shigang Lu
author_facet Jing Wang
Yi Zhang
Yingchun Lyu
Tu Lan
Bing Han
Yitong Guo
Zexi Yang
Jingjing Zhou
Shangqian Zhao
Rong Yang
Shigang Lu
author_sort Jing Wang
collection DOAJ
description 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.
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spelling doaj-art-2ed2f4a8b7674018b26bb9a7b463d18c2025-08-23T04:50:16ZengElsevierNext Materials2949-82282025-10-01910093110.1016/j.nxmate.2025.100931Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteriesJing Wang0Yi Zhang1Yingchun Lyu2Tu Lan3Bing Han4Yitong Guo5Zexi Yang6Jingjing Zhou7Shangqian Zhao8Rong Yang9Shigang Lu10Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai 200444, ChinaNational Power Battery Innovation Center, Beijing 100088, ChinaMaterials Genome Institute, Shanghai University, Shanghai 200444, ChinaMaterials Genome Institute, Shanghai University, Shanghai 200444, ChinaInstitute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai 200444, ChinaInstitute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai 200444, ChinaMaterials Genome Institute, Shanghai University, Shanghai 200444, ChinaMaterials Genome Institute, Shanghai University, Shanghai 200444, ChinaChina Automotive Battery Research Institute Co. Ltd., Beijing 100088, ChinaChina Automotive Battery Research Institute Co. Ltd., Beijing 100088, ChinaInstitute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai 200444, China; Corresponding author.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.http://www.sciencedirect.com/science/article/pii/S2949822825004496Ni rich NCMSolid electrolyte interfaceHalide electrolyteAll solid-state batteries
spellingShingle Jing Wang
Yi Zhang
Yingchun Lyu
Tu Lan
Bing Han
Yitong Guo
Zexi Yang
Jingjing Zhou
Shangqian Zhao
Rong Yang
Shigang Lu
Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries
Next Materials
Ni rich NCM
Solid electrolyte interface
Halide electrolyte
All solid-state batteries
title Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries
title_full Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries
title_fullStr Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries
title_full_unstemmed Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries
title_short Electrochemical performance and interfacial stability in Ni-rich NCM/ halide solid state batteries
title_sort electrochemical performance and interfacial stability in ni rich ncm halide solid state batteries
topic Ni rich NCM
Solid electrolyte interface
Halide electrolyte
All solid-state batteries
url http://www.sciencedirect.com/science/article/pii/S2949822825004496
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