Architecturally Inspired Lattice Engineering Enables Long-Life Ultra-High Nickel Cathodes

Longhao Cao; Denghui Ma; Yun Liu; Cancan Peng; Yinghan Shao; Yiyao Xiao; Xiaosong Zhang; Jing Zhang; Said Amzil; Wanli Wei; Ziyin Guo; Guang Li; Binjie Hu; Ya Jun Cheng; Lai Chen; Yonggao Xia

doi:10.1002/adfm.202520093

Architecturally Inspired Lattice Engineering Enables Long-Life Ultra-High Nickel Cathodes

Longhao Cao
, Denghui Ma
, Yun Liu
, Cancan Peng
, Yinghan Shao
, Yiyao Xiao
, Xiaosong Zhang
, Jing Zhang
, Said Amzil
, Wanli Wei
, Ziyin Guo
, Guang Li
, Binjie Hu^*
, Ya Jun Cheng
, Lai Chen
, Yonggao Xia^*

^*此作品的通讯作者

CAS - Ningbo Institute of Material Technology and Engineering
The University of Nottingham Ningbo China
Ningbo University of Technology
Beijing Institute of Technology
University of California Merced
Hohai University Changzhou
University of Chinese Academy of Sciences

科研成果: 期刊稿件 › 文章 › 同行评审

2 引用（Scopus）

摘要

Using state-of-the-art ultra-high nickel (UHN) layered oxides (LiNi_xCo_yMn_1-x-yO₂, x≥0.9) as battery cathodes is expected to push the boundaries of energy density. However, their structural instability, particularly the H2–H3 phase transition, drives rapid capacity fading. Here, a structural modulation strategy inspired by architectural mechanics is presented: a simple candle soot coating followed by thermal annealing induces a mortise-like disordered surface phase and stabilizing “Ni²⁺ columns” within Ni94 cathode. These features synergistically suppress intergranular stress and mitigate the H2–H3 phase transition. As a result, 4.5V-Graphite||Ni94 pouch cell retains 80.2% of their capacity after 2000 cycles. STEM and operando electrochemical analysis, supported by DFT calculations, reveal the role of “Ni²⁺ columns” in stabilizing the layered framework. This work introduces a novel approach to lattice engineering in ultra-high nickel cathodes, offering a practical pathway toward long-life, cobalt-lean lithium-ion batteries.

源语言	英语
文章编号	e20093
期刊	Advanced Functional Materials
卷	36
期	21
DOI	https://doi.org/10.1002/adfm.202520093
出版状态	已出版 - 12 3月 2026
已对外发布	是

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title = "Architecturally Inspired Lattice Engineering Enables Long-Life Ultra-High Nickel Cathodes",

abstract = "Using state-of-the-art ultra-high nickel (UHN) layered oxides (LiNixCoyMn1-x-yO2, x≥0.9) as battery cathodes is expected to push the boundaries of energy density. However, their structural instability, particularly the H2–H3 phase transition, drives rapid capacity fading. Here, a structural modulation strategy inspired by architectural mechanics is presented: a simple candle soot coating followed by thermal annealing induces a mortise-like disordered surface phase and stabilizing “Ni2+ columns” within Ni94 cathode. These features synergistically suppress intergranular stress and mitigate the H2–H3 phase transition. As a result, 4.5V-Graphite||Ni94 pouch cell retains 80.2\% of their capacity after 2000 cycles. STEM and operando electrochemical analysis, supported by DFT calculations, reveal the role of “Ni2+ columns” in stabilizing the layered framework. This work introduces a novel approach to lattice engineering in ultra-high nickel cathodes, offering a practical pathway toward long-life, cobalt-lean lithium-ion batteries.",

keywords = "architectural inspiration, high voltage, long cycle, phase transition, ultra-high nickel",

author = "Longhao Cao and Denghui Ma and Yun Liu and Cancan Peng and Yinghan Shao and Yiyao Xiao and Xiaosong Zhang and Jing Zhang and Said Amzil and Wanli Wei and Ziyin Guo and Guang Li and Binjie Hu and Cheng, \{Ya Jun\} and Lai Chen and Yonggao Xia",

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year = "2026",

month = mar,

day = "12",

doi = "10.1002/adfm.202520093",

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T1 - Architecturally Inspired Lattice Engineering Enables Long-Life Ultra-High Nickel Cathodes

AU - Cao, Longhao

AU - Ma, Denghui

AU - Liu, Yun

AU - Peng, Cancan

AU - Shao, Yinghan

AU - Xiao, Yiyao

AU - Zhang, Xiaosong

AU - Zhang, Jing

AU - Amzil, Said

AU - Wei, Wanli

AU - Guo, Ziyin

AU - Li, Guang

AU - Hu, Binjie

AU - Cheng, Ya Jun

AU - Chen, Lai

AU - Xia, Yonggao

PY - 2026/3/12

Y1 - 2026/3/12

N2 - Using state-of-the-art ultra-high nickel (UHN) layered oxides (LiNixCoyMn1-x-yO2, x≥0.9) as battery cathodes is expected to push the boundaries of energy density. However, their structural instability, particularly the H2–H3 phase transition, drives rapid capacity fading. Here, a structural modulation strategy inspired by architectural mechanics is presented: a simple candle soot coating followed by thermal annealing induces a mortise-like disordered surface phase and stabilizing “Ni2+ columns” within Ni94 cathode. These features synergistically suppress intergranular stress and mitigate the H2–H3 phase transition. As a result, 4.5V-Graphite||Ni94 pouch cell retains 80.2% of their capacity after 2000 cycles. STEM and operando electrochemical analysis, supported by DFT calculations, reveal the role of “Ni2+ columns” in stabilizing the layered framework. This work introduces a novel approach to lattice engineering in ultra-high nickel cathodes, offering a practical pathway toward long-life, cobalt-lean lithium-ion batteries.

AB - Using state-of-the-art ultra-high nickel (UHN) layered oxides (LiNixCoyMn1-x-yO2, x≥0.9) as battery cathodes is expected to push the boundaries of energy density. However, their structural instability, particularly the H2–H3 phase transition, drives rapid capacity fading. Here, a structural modulation strategy inspired by architectural mechanics is presented: a simple candle soot coating followed by thermal annealing induces a mortise-like disordered surface phase and stabilizing “Ni2+ columns” within Ni94 cathode. These features synergistically suppress intergranular stress and mitigate the H2–H3 phase transition. As a result, 4.5V-Graphite||Ni94 pouch cell retains 80.2% of their capacity after 2000 cycles. STEM and operando electrochemical analysis, supported by DFT calculations, reveal the role of “Ni2+ columns” in stabilizing the layered framework. This work introduces a novel approach to lattice engineering in ultra-high nickel cathodes, offering a practical pathway toward long-life, cobalt-lean lithium-ion batteries.

KW - architectural inspiration

KW - high voltage

KW - long cycle

KW - phase transition

KW - ultra-high nickel

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DO - 10.1002/adfm.202520093

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SN - 1616-301X

VL - 36

JO - Advanced Functional Materials

JF - Advanced Functional Materials

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ER -

Architecturally Inspired Lattice Engineering Enables Long-Life Ultra-High Nickel Cathodes

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