In situ inorganic conductive network formation in high-voltage single-crystal Ni-rich cathodes

Xinming Fan, Xing Ou (), Wengao Zhao (), Yun Liu, Bao Zhang, Jiafeng Zhang, Lianfeng Zou, Lukas Seidl, Yangzhong Li, Guorong Hu, Corsin Battaglia and Yong Yang ()
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Xinming Fan: Central South University
Xing Ou: Central South University
Wengao Zhao: Empa, Swiss Federal Laboratories for Materials Science and Technology
Yun Liu: Central South University
Bao Zhang: Central South University
Jiafeng Zhang: Central South University
Lianfeng Zou: Pacific Northwest National Laboratory
Lukas Seidl: Empa, Swiss Federal Laboratories for Materials Science and Technology
Yangzhong Li: National Supercomputing Center in Shenzhen, Shenzhen
Guorong Hu: Central South University
Corsin Battaglia: Empa, Swiss Federal Laboratories for Materials Science and Technology
Yong Yang: Xiamen University, Xiamen

Nature Communications, 2021, vol. 12, issue 1, 1-13

Abstract: Abstract High nickel content in LiNixCoyMnzO2 (NCM, x ≥ 0.8, x + y + z = 1) layered cathode material allows high specific energy density in lithium-ion batteries (LIBs). However, Ni-rich NCM cathodes suffer from performance degradation, mechanical and structural instability upon prolonged cell cycling. Although the use of single-crystal Ni-rich NCM can mitigate these drawbacks, the ion-diffusion in large single-crystal particles hamper its rate capability. Herein, we report a strategy to construct an in situ Li1.4Y0.4Ti1.6(PO4)3 (LYTP) ion/electron conductive network which interconnects single-crystal LiNi0.88Co0.09Mn0.03O2 (SC-NCM88) particles. The LYTP network facilitates the lithium-ion transport between SC-NCM88 particles, mitigates mechanical instability and prevents detrimental crystalline phase transformation. When used in combination with a Li metal anode, the LYTP-containing SC-NCM88-based cathode enables a coin cell capacity of 130 mAh g−1 after 500 cycles at 5 C rate in the 2.75-4.4 V range at 25 °C. Tests in Li-ion pouch cell configuration (i.e., graphite used as negative electrode active material) demonstrate capacity retention of 85% after 1000 cycles at 0.5 C in the 2.75-4.4 V range at 25 °C for the LYTP-containing SC-NCM88-based positive electrode.

Date: 2021
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DOI: 10.1038/s41467-021-25611-6

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