Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells

While high-voltage operation of mid-Ni layered oxide cathodes in full-cell Li-ion batteries is essential for achieving high energy density, it inevitably accelerates electrode degradation, ultimately resulting in capacity loss. However, the underlying degradation mechanisms under high-voltage condit...

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Main Authors: Seungjae Suk, Namgyu Yoo, Youngsu Lee, Jaesub Kwon, Heeju Ahn, Seungsu Yoo, Jaewoon Lee, Haneul Kim, Joongho Bae, Jongwoo Kim, Chiho Jo, Yong-Tae Kim, Kyu-Young Park
Format: Article
Language:English
Published: Taylor & Francis Group 2025-12-01
Series:Science and Technology of Advanced Materials
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Online Access:https://www.tandfonline.com/doi/10.1080/14686996.2025.2502324
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author Seungjae Suk
Namgyu Yoo
Youngsu Lee
Jaesub Kwon
Heeju Ahn
Seungsu Yoo
Jaewoon Lee
Haneul Kim
Joongho Bae
Jongwoo Kim
Chiho Jo
Yong-Tae Kim
Kyu-Young Park
author_facet Seungjae Suk
Namgyu Yoo
Youngsu Lee
Jaesub Kwon
Heeju Ahn
Seungsu Yoo
Jaewoon Lee
Haneul Kim
Joongho Bae
Jongwoo Kim
Chiho Jo
Yong-Tae Kim
Kyu-Young Park
author_sort Seungjae Suk
collection DOAJ
description While high-voltage operation of mid-Ni layered oxide cathodes in full-cell Li-ion batteries is essential for achieving high energy density, it inevitably accelerates electrode degradation, ultimately resulting in capacity loss. However, the underlying degradation mechanisms under high-voltage conditions remain poorly understood. In this study, we reveal that anode slippage – induced by cross-talk-driven surface degradation – is the dominant factor in capacity fade during high-voltage (4.35 or 4.40 V) cycling of single-crystal mid-Ni layered oxide (SC-NCM)/graphite pouch full-cells. Electrochemical and post-mortem analyses show that, although high-voltage operation induces cathode surface degradation, including lattice oxygen loss and phase transitions, its direct impact on capacity loss is relatively minor compared to that of the anode. Instead, anode degradation is primarily caused by cross-talk effects from cathode Ni dissolution, which promote the accumulation of irreversible organic byproducts – such as LiOx and Li2CO3 – within the solid electrolyte interphase (SEI) layer of the graphite anode. This leads to increased resistance and reduced anode electrochemical activity, disrupting electrode balance and accelerating full-cell capacity fade. These findings highlight the critical role of anode degradation in high-voltage operation and emphasize the importance of mitigating cross-talk effects. A comprehensive understanding of cross-talk–induced anode slippage is therefore critical for the rational design of high-voltage mid-Ni full-cell systems with long-term durability.
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spelling doaj-art-855cddecc6524feaa4cfd7610bdecad82025-08-20T02:33:15ZengTaylor & Francis GroupScience and Technology of Advanced Materials1468-69961878-55142025-12-0126110.1080/14686996.2025.2502324Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cellsSeungjae Suk0Namgyu Yoo1Youngsu Lee2Jaesub Kwon3Heeju Ahn4Seungsu Yoo5Jaewoon Lee6Haneul Kim7Joongho Bae8Jongwoo Kim9Chiho Jo10Yong-Tae Kim11Kyu-Young Park12Department of Materials Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Republic of KoreaGraduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang, Republic of KoreaGraduate Institute of Ferrous & Eco Materials Technology (GIFT), Pohang University of Science and Technology University, Pohang, Republic of KoreaDepartment of Materials Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaLG Energy Solution, Research Park, Daejeon, Republic of KoreaDepartment of Materials Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Republic of KoreaDepartment of Materials Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Republic of KoreaWhile high-voltage operation of mid-Ni layered oxide cathodes in full-cell Li-ion batteries is essential for achieving high energy density, it inevitably accelerates electrode degradation, ultimately resulting in capacity loss. However, the underlying degradation mechanisms under high-voltage conditions remain poorly understood. In this study, we reveal that anode slippage – induced by cross-talk-driven surface degradation – is the dominant factor in capacity fade during high-voltage (4.35 or 4.40 V) cycling of single-crystal mid-Ni layered oxide (SC-NCM)/graphite pouch full-cells. Electrochemical and post-mortem analyses show that, although high-voltage operation induces cathode surface degradation, including lattice oxygen loss and phase transitions, its direct impact on capacity loss is relatively minor compared to that of the anode. Instead, anode degradation is primarily caused by cross-talk effects from cathode Ni dissolution, which promote the accumulation of irreversible organic byproducts – such as LiOx and Li2CO3 – within the solid electrolyte interphase (SEI) layer of the graphite anode. This leads to increased resistance and reduced anode electrochemical activity, disrupting electrode balance and accelerating full-cell capacity fade. These findings highlight the critical role of anode degradation in high-voltage operation and emphasize the importance of mitigating cross-talk effects. A comprehensive understanding of cross-talk–induced anode slippage is therefore critical for the rational design of high-voltage mid-Ni full-cell systems with long-term durability.https://www.tandfonline.com/doi/10.1080/14686996.2025.2502324Lithium-ion batteriesanode slippagehigh-voltage cyclingsingle-crystal mid-Ni NCMfull-cellcross-talk
spellingShingle Seungjae Suk
Namgyu Yoo
Youngsu Lee
Jaesub Kwon
Heeju Ahn
Seungsu Yoo
Jaewoon Lee
Haneul Kim
Joongho Bae
Jongwoo Kim
Chiho Jo
Yong-Tae Kim
Kyu-Young Park
Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells
Science and Technology of Advanced Materials
Lithium-ion batteries
anode slippage
high-voltage cycling
single-crystal mid-Ni NCM
full-cell
cross-talk
title Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells
title_full Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells
title_fullStr Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells
title_full_unstemmed Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells
title_short Understanding cross-talk–induced anode slippage in high-voltage mid-Ni NCM/graphite full cells
title_sort understanding cross talk induced anode slippage in high voltage mid ni ncm graphite full cells
topic Lithium-ion batteries
anode slippage
high-voltage cycling
single-crystal mid-Ni NCM
full-cell
cross-talk
url https://www.tandfonline.com/doi/10.1080/14686996.2025.2502324
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