Ultrastable cathodes enabled by compositional and structural dual-gradient design

Tongchao Liu (), Lei Yu, Junxiang Liu, Alvin Dai, Tao Zhou, Jing Wang, Weiyuan Huang, Luxi Li, Matthew Li, Tianyi Li, Xiaojing Huang, Xianghui Xiao, Mingyuan Ge, Lu Ma, Zengqing Zhuo, Rachid Amine, Yong S. Chu, Wah-Keat Lee, Jianguo Wen and Khalil Amine ()
Additional contact information
Tongchao Liu: Argonne National Laboratory
Lei Yu: Argonne National Laboratory
Junxiang Liu: Argonne National Laboratory
Alvin Dai: Argonne National Laboratory
Tao Zhou: Argonne National Laboratory
Jing Wang: Argonne National Laboratory
Weiyuan Huang: Argonne National Laboratory
Luxi Li: Argonne National Laboratory
Matthew Li: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Xiaojing Huang: Brookhaven National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Mingyuan Ge: Brookhaven National Laboratory
Lu Ma: Brookhaven National Laboratory
Zengqing Zhuo: Lawrence Berkeley National Laboratory
Rachid Amine: Argonne National Laboratory
Yong S. Chu: Brookhaven National Laboratory
Wah-Keat Lee: Brookhaven National Laboratory
Jianguo Wen: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory

Nature Energy, 2024, vol. 9, issue 10, 1252-1263

Abstract: Abstract Cathodes for next-generation batteries are pressed for higher voltage operation (≥4.5 V) to achieve high capacity with long cyclability and thermal tolerance. Current cathodes fail to meet these requirements owing to structural and electrochemical strains at high voltages, leading to fast capacity fading. Here we present a cathode with a coherent architecture ranging from ordered to disordered frameworks with concentration gradient and controllable Ni oxidation activities, which can overcome voltage ceilings imposed by existing cathodes. This design enables simultaneous high-capacity and high-voltage operation at 4.5 V without capacity fading, and up to 4.7 V with negligible capacity decay. Multiscale diffraction and imaging techniques reveal the disordered surface is electrochemically and structurally indestructible, preventing surface parasitic reactions and phase transitions. Structural coherence from ordering to disordering limits lattice parameter changes, mitigating lattice strain and enhancing morphological integrity. The dual-gradient design also notably improves thermal stability, driving the advancement of high-performance cathode materials.

Date: 2024
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DOI: 10.1038/s41560-024-01605-8

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