Kirkendall effect-induced uniform stress distribution stabilizes nickel-rich layered oxide cathodes

Ziyao Gao, Chenglong Zhao (), Kai Zhou, Junru Wu, Yao Tian, Xianming Deng, Lihan Zhang, Kui Lin, Feiyu Kang, Lele Peng (), Marnix Wagemaker () and Baohua Li ()
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Ziyao Gao: Tsinghua University
Chenglong Zhao: Tsinghua University
Kai Zhou: Tsinghua University
Junru Wu: Tsinghua University
Yao Tian: Tsinghua University
Xianming Deng: Tsinghua University
Lihan Zhang: Tsinghua University
Kui Lin: Tsinghua University
Feiyu Kang: Tsinghua University
Lele Peng: Tsinghua University
Marnix Wagemaker: Delft University of Technology
Baohua Li: Tsinghua University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Nickel-rich layered oxide cathodes promise ultrahigh energy density but is plagued by the mechanical failure of the secondary particle upon (de)lithiation. Existing approaches for alleviating the structural degradation could retard pulverization, yet fail to tune the stress distribution and root out the formation of cracks. Herein, we report a unique strategy to uniformize the stress distribution in secondary particle via Kirkendall effect to stabilize the core region during electrochemical cycling. Exotic metal/metalloid oxides (such as Al2O3 or SiO2) is introduced as the heterogeneous nucleation seeds for the preferential growth of the precursor. The calcination treatment afterwards generates a dopant-rich interior structure with central Kirkendall void, due to the different diffusivity between the exotic element and nickel atom. The resulting cathode material exhibits superior structural and electrochemical reversibility, thus contributing to a high specific energy density (based on cathode) of 660 Wh kg−1 after 500 cycles with a retention rate of 86%. This study suggests that uniformizing stress distribution represents a promising pathway to tackle the structural instability facing nickel-rich layered oxide cathodes.

Date: 2024
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DOI: 10.1038/s41467-024-45373-1

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