Tailoring hetero-precursor transformation for simultaneous surface-coating and subsurface-doping of Ni-rich layered oxide cathodes

Junfan Zhang; Ran Wang; Kunkun Guo; Mohan Yang; Zenan Zhao; Jing Wang; Qi Liu; Lai Chen; Ning Li; Yuefeng Su; Feng Wu; Guoqiang Tan

doi:10.1016/j.cej.2025.162307

Tailoring hetero-precursor transformation for simultaneous surface-coating and subsurface-doping of Ni-rich layered oxide cathodes

Junfan Zhang, Ran Wang, Kunkun Guo, Mohan Yang, Zenan Zhao, Jing Wang^*, Qi Liu, Lai Chen, Ning Li, Yuefeng Su, Feng Wu, Guoqiang Tan

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

Alleviating surface/interface microstructural degradation of Ni-rich layered oxides is critical for enhancing safety and cycle-life of high-energy Li-ion batteries. Here we report a one-pot hetero-precursor transformation method by directly calcining Ni_0.9Co_0.1O@AlPO₄ with LiOH. Li₃PO₄ surface-coating and Li(Ni_0.9Co_0.1)_1-_xAl_xO₂ subsurface-doping layers are formed onto LiNi_0.9Co_0.1O₂ simultaneously, yielding a compact LiNi_0.9Co_0.1O₂-Li(Ni_0.9Co_0.1)_1-_xAl_xO₂-Li₃PO₄ heterostructure. This cathode architectural design exploits advantages of both surface-coating and elemental-doping, whereas Pnmb Li₃PO₄ acts as the surface protection and fast Li-ion conductor, and Fm3m Li (Ni_0.9Co_0.1)_1-_xAl_xO₂ serves as the subsurface stabilizer and Li-ion conductive bridge. Such surface/subsurface engineering significantly enhances structural and chemical stability and electrical properties of the LiNi_0.9Co_0.1O₂ cathode, enabling promising electrochemical performance. Notably, in a LiNi_0.9Co_0.1O₂//Si-C full-cell, the obtained cathode exhibits a high initial reversible capacity of 195.2 mAh g⁻¹ and an excellent cycling retention of 88.2 % at 1.0C over 300cycles. This simultaneous synthesis stratege accompanied with the simple and scalable hetero-precursor transformation approach provides new design paradigm for cathode surface engineering of advanced Li-ion batteries.

Original language	English
Article number	162307
Journal	Chemical Engineering Journal
Volume	512
DOIs	https://doi.org/10.1016/j.cej.2025.162307
Publication status	Published - 15 May 2025

Keywords

Cathode engineering
Li-ion batteries
Ni-rich layered oxides
Precursor transformation
Subsurface-doping
Surface-coating

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10.1016/j.cej.2025.162307

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@article{e0bfaf7e10404560a9e27a94f895908f,

title = "Tailoring hetero-precursor transformation for simultaneous surface-coating and subsurface-doping of Ni-rich layered oxide cathodes",

abstract = "Alleviating surface/interface microstructural degradation of Ni-rich layered oxides is critical for enhancing safety and cycle-life of high-energy Li-ion batteries. Here we report a one-pot hetero-precursor transformation method by directly calcining Ni0.9Co0.1O@AlPO4 with LiOH. Li3PO4 surface-coating and Li(Ni0.9Co0.1)1-xAlxO2 subsurface-doping layers are formed onto LiNi0.9Co0.1O2 simultaneously, yielding a compact LiNi0.9Co0.1O2-Li(Ni0.9Co0.1)1-xAlxO2-Li3PO4 heterostructure. This cathode architectural design exploits advantages of both surface-coating and elemental-doping, whereas Pnmb Li3PO4 acts as the surface protection and fast Li-ion conductor, and Fm3m Li (Ni0.9Co0.1)1-xAlxO2 serves as the subsurface stabilizer and Li-ion conductive bridge. Such surface/subsurface engineering significantly enhances structural and chemical stability and electrical properties of the LiNi0.9Co0.1O2 cathode, enabling promising electrochemical performance. Notably, in a LiNi0.9Co0.1O2//Si-C full-cell, the obtained cathode exhibits a high initial reversible capacity of 195.2 mAh g−1 and an excellent cycling retention of 88.2 % at 1.0C over 300cycles. This simultaneous synthesis stratege accompanied with the simple and scalable hetero-precursor transformation approach provides new design paradigm for cathode surface engineering of advanced Li-ion batteries.",

keywords = "Cathode engineering, Li-ion batteries, Ni-rich layered oxides, Precursor transformation, Subsurface-doping, Surface-coating",

author = "Junfan Zhang and Ran Wang and Kunkun Guo and Mohan Yang and Zenan Zhao and Jing Wang and Qi Liu and Lai Chen and Ning Li and Yuefeng Su and Feng Wu and Guoqiang Tan",

note = "Publisher Copyright: {\textcopyright} 2025 Elsevier B.V.",

year = "2025",

month = may,

day = "15",

doi = "10.1016/j.cej.2025.162307",

language = "English",

volume = "512",

journal = "Chemical Engineering Journal",

issn = "1385-8947",

publisher = "Elsevier B.V.",

}

TY - JOUR

T1 - Tailoring hetero-precursor transformation for simultaneous surface-coating and subsurface-doping of Ni-rich layered oxide cathodes

AU - Zhang, Junfan

AU - Wang, Ran

AU - Guo, Kunkun

AU - Yang, Mohan

AU - Zhao, Zenan

AU - Wang, Jing

AU - Liu, Qi

AU - Chen, Lai

AU - Li, Ning

AU - Su, Yuefeng

AU - Wu, Feng

AU - Tan, Guoqiang

PY - 2025/5/15

Y1 - 2025/5/15

N2 - Alleviating surface/interface microstructural degradation of Ni-rich layered oxides is critical for enhancing safety and cycle-life of high-energy Li-ion batteries. Here we report a one-pot hetero-precursor transformation method by directly calcining Ni0.9Co0.1O@AlPO4 with LiOH. Li3PO4 surface-coating and Li(Ni0.9Co0.1)1-xAlxO2 subsurface-doping layers are formed onto LiNi0.9Co0.1O2 simultaneously, yielding a compact LiNi0.9Co0.1O2-Li(Ni0.9Co0.1)1-xAlxO2-Li3PO4 heterostructure. This cathode architectural design exploits advantages of both surface-coating and elemental-doping, whereas Pnmb Li3PO4 acts as the surface protection and fast Li-ion conductor, and Fm3m Li (Ni0.9Co0.1)1-xAlxO2 serves as the subsurface stabilizer and Li-ion conductive bridge. Such surface/subsurface engineering significantly enhances structural and chemical stability and electrical properties of the LiNi0.9Co0.1O2 cathode, enabling promising electrochemical performance. Notably, in a LiNi0.9Co0.1O2//Si-C full-cell, the obtained cathode exhibits a high initial reversible capacity of 195.2 mAh g−1 and an excellent cycling retention of 88.2 % at 1.0C over 300cycles. This simultaneous synthesis stratege accompanied with the simple and scalable hetero-precursor transformation approach provides new design paradigm for cathode surface engineering of advanced Li-ion batteries.

AB - Alleviating surface/interface microstructural degradation of Ni-rich layered oxides is critical for enhancing safety and cycle-life of high-energy Li-ion batteries. Here we report a one-pot hetero-precursor transformation method by directly calcining Ni0.9Co0.1O@AlPO4 with LiOH. Li3PO4 surface-coating and Li(Ni0.9Co0.1)1-xAlxO2 subsurface-doping layers are formed onto LiNi0.9Co0.1O2 simultaneously, yielding a compact LiNi0.9Co0.1O2-Li(Ni0.9Co0.1)1-xAlxO2-Li3PO4 heterostructure. This cathode architectural design exploits advantages of both surface-coating and elemental-doping, whereas Pnmb Li3PO4 acts as the surface protection and fast Li-ion conductor, and Fm3m Li (Ni0.9Co0.1)1-xAlxO2 serves as the subsurface stabilizer and Li-ion conductive bridge. Such surface/subsurface engineering significantly enhances structural and chemical stability and electrical properties of the LiNi0.9Co0.1O2 cathode, enabling promising electrochemical performance. Notably, in a LiNi0.9Co0.1O2//Si-C full-cell, the obtained cathode exhibits a high initial reversible capacity of 195.2 mAh g−1 and an excellent cycling retention of 88.2 % at 1.0C over 300cycles. This simultaneous synthesis stratege accompanied with the simple and scalable hetero-precursor transformation approach provides new design paradigm for cathode surface engineering of advanced Li-ion batteries.

KW - Cathode engineering

KW - Li-ion batteries

KW - Ni-rich layered oxides

KW - Precursor transformation

KW - Subsurface-doping

KW - Surface-coating

UR - http://www.scopus.com/inward/record.url?scp=105002283444&partnerID=8YFLogxK

U2 - 10.1016/j.cej.2025.162307

DO - 10.1016/j.cej.2025.162307

M3 - Article

AN - SCOPUS:105002283444

SN - 1385-8947

VL - 512

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

M1 - 162307

ER -

Tailoring hetero-precursor transformation for simultaneous surface-coating and subsurface-doping of Ni-rich layered oxide cathodes

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Keywords

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