Enabling high energy lithium metal batteries via single-crystal Ni-rich cathode material co-doping strategy

Xing Ou, Tongchao Liu, Wentao Zhong, Xinming Fan (), Xueyi Guo, Xiaojing Huang, Liang Cao, Junhua Hu, Bao Zhang, Yong S. Chu, Guorong Hu, Zhang Lin, Mouad Dahbi, Jones Alami, Khalil Amine (), Chenghao Yang () and Jun Lu ()
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Xing Ou: School of Environment and Energy, South China University of Technology
Tongchao Liu: Argonne National Laboratory
Wentao Zhong: School of Environment and Energy, South China University of Technology
Xinming Fan: Central South University
Xueyi Guo: Central South University
Xiaojing Huang: Brookhaven National Laboratory
Liang Cao: School of Environment and Energy, South China University of Technology
Junhua Hu: Zhengzhou University
Bao Zhang: Central South University
Yong S. Chu: Brookhaven National Laboratory
Guorong Hu: Central South University
Zhang Lin: Central South University
Mouad Dahbi: Mohammed VI Polytechnic University
Jones Alami: Mohammed VI Polytechnic University
Khalil Amine: Argonne National Laboratory
Chenghao Yang: School of Environment and Energy, South China University of Technology
Jun Lu: Argonne National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract High-capacity Ni-rich layered oxides are promising cathode materials for secondary lithium-based battery systems. However, their structural instability detrimentally affects the battery performance during cell cycling. Here, we report an Al/Zr co-doped single-crystalline LiNi0.88Co0.09Mn0.03O2 (SNCM) cathode material to circumvent the instability issue. We found that soluble Al ions are adequately incorporated in the SNCM lattice while the less soluble Zr ions are prone to aggregate in the outer SNCM surface layer. The synergistic effect of Al/Zr co-doping in SNCM lattice improve the Li-ion mobility, relief the internal strain, and suppress the Li/Ni cation mixing upon cycling at high cut-off voltage. These features improve the cathode rate capability and structural stabilization during prolonged cell cycling. In particular, the Zr-rich surface enables the formation of stable cathode-electrolyte interphase, which prevent SNCM from unwanted reactions with the non-aqueous fluorinated liquid electrolyte solution and avoid Ni dissolution. To prove the practical application of the Al/Zr co-doped SNCM, we assembled a 10.8 Ah pouch cell (using a 100 μm thick Li metal anode) capable of delivering initial specific energy of 504.5 Wh kg−1 at 0.1 C and 25 °C.

Date: 2022
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DOI: 10.1038/s41467-022-30020-4

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