Mitigating the Kinetic Hysteresis of Co‐Free Ni‐Rich Cathodes via Gradient Penetration of Nonmagnetic Silicon

Co-free Ni-rich layered oxides are considered a promising cathode material for next-generation Li-ion batteries due to their cost-effectiveness and high capacity. However, they still suffer from the practical challenges of low discharge capacity and poor rate capability due to the hysteresis of Li-ion diffusion kinetics. Herein, based on the regulation of the lattice magnetic frustration, the Li/Ni intermixing defects as the primary origin of kinetic hysteresis are radically addressed via the doping of the nonmagnetic Si element. Meanwhile, by adopting gradient penetration doping, a robust Si-O surface structure with reversible lattice oxygen evolution and low lattice strain is constructed on Co-free Ni-rich cathodes to suppress the formation of surface dense barrier layer. With the remarkably enhanced Li-ion diffusion kinetics in atomic and electrode particle scales, the as-obtained cathodes (LiNi<sub>x</sub>Mn<sub>1-x</sub>Si<sub>0.01</sub>O<sub>2</sub>, 0.6≤x≤0.9) achieve superior performance in discharge capacity, rate capability, and durability. This work highlights the coupling effect of magnetic structure and interfacial chemicals on Li-ion transport properties, and the concept will inspire more researchers to conduct an intensive study.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2024-09-02
DOI
https://doi.org/10.1002/anie.202409764
Citations
14
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
2.92

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article

Mitigating the Kinetic Hysteresis of Co‐Free Ni‐Rich Cathodes via Gradient Penetration of Nonmagnetic Silicon

Yongfu Tang, Yijun Song, Zhijian Qiu, Yongpeng Cui et al.
14 citations
Angewandte Chemie International Edition
Advancements in Battery Materials
2.92
article

Mitigating the Kinetic Hysteresis of Co‐Free Ni‐Rich Cathodes via Gradient Penetration of Nonmagnetic Silicon

Yongfu Tang, Yijun Song, Zhijian Qiu, Yongpeng Cui, Debin Kong, Qingzhong Xue, Lina Ge, Xiaofang Li, Xuejin Li, Wei Dong Xing, Lei Zhu, Zifeng Yan, Jianqiang Zhang, Zhipeng Xie, Li Zhou, Pengyun Liu, Bo Wang
article en
14 citations

Abstract

Co-free Ni-rich layered oxides are considered a promising cathode material for next-generation Li-ion batteries due to their cost-effectiveness and high capacity. However, they still suffer from the practical challenges of low discharge capacity and poor rate capability due to the hysteresis of Li-ion diffusion kinetics. Herein, based on the regulation of the lattice magnetic frustration, the Li/Ni intermixing defects as the primary origin of kinetic hysteresis are radically addressed via the doping of the nonmagnetic Si element. Meanwhile, by adopting gradient penetration doping, a robust Si-O surface structure with reversible lattice oxygen evolution and low lattice strain is constructed on Co-free Ni-rich cathodes to suppress the formation of surface dense barrier layer. With the remarkably enhanced Li-ion diffusion kinetics in atomic and electrode particle scales, the as-obtained cathodes (LiNi<sub>x</sub>Mn<sub>1-x</sub>Si<sub>0.01</sub>O<sub>2</sub>, 0.6≤x≤0.9) achieve superior performance in discharge capacity, rate capability, and durability. This work highlights the coupling effect of magnetic structure and interfacial chemicals on Li-ion transport properties, and the concept will inspire more researchers to conduct an intensive study.

Angewandte Chemie International EditionVol. 63(48)
China University of Petroleum, Beijing (CN), Yanshan University (CN), China University of Petroleum, East China (CN), State Key Laboratory of Heavy Oil (CN)
National Natural Science Foundation of China, China Postdoctoral Science Foundation, Natural Science Foundation of Shandong Province, Fundamental Research Funds for the Central Universities
Openalex Percentile: Top 8%
Advancements in Battery Materials
2.92
DOIOpen Access PDFOpenAlex
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