Chemical short-range disorder in lithium oxide cathodes

Qidi Wang (), Zhenpeng Yao, Jianlin Wang, Hao Guo, Chao Li, Dong Zhou, Xuedong Bai, Hong Li (), Baohua Li (), Marnix Wagemaker () and Chenglong Zhao ()
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Qidi Wang: Delft University of Technology
Zhenpeng Yao: Shanghai Jiao Tong University
Jianlin Wang: Chinese Academy of Sciences
Hao Guo: China Institute of Atomic Energy
Chao Li: East China Normal University
Dong Zhou: Helmholtz-Zentrum Berlin für Materialien und Energie
Xuedong Bai: Chinese Academy of Sciences
Hong Li: Chinese Academy of Sciences
Baohua Li: Tsinghua University
Marnix Wagemaker: Delft University of Technology
Chenglong Zhao: Delft University of Technology

Nature, 2024, vol. 629, issue 8011, 341-347

Abstract: Abstract Ordered layered structures serve as essential components in lithium (Li)-ion cathodes1–3. However, on charging, the inherently delicate Li-deficient frameworks become vulnerable to lattice strain and structural and/or chemo-mechanical degradation, resulting in rapid capacity deterioration and thus short battery life2,4. Here we report an approach that addresses these issues using the integration of chemical short-range disorder (CSRD) into oxide cathodes, which involves the localized distribution of elements in a crystalline lattice over spatial dimensions, spanning a few nearest-neighbour spacings. This is guided by fundamental principles of structural chemistry and achieved through an improved ceramic synthesis process. To demonstrate its viability, we showcase how the introduction of CSRD substantially affects the crystal structure of layered Li cobalt oxide cathodes. This is manifested in the transition metal environment and its interactions with oxygen, effectively preventing detrimental sliding of crystal slabs and structural deterioration during Li removal. Meanwhile, it affects the electronic structure, leading to improved electronic conductivity. These attributes are highly beneficial for Li-ion storage capabilities, markedly improving cycle life and rate capability. Moreover, we find that CSRD can be introduced in additional layered oxide materials through improved chemical co-doping, further illustrating its potential to enhance structural and electrochemical stability. These findings open up new avenues for the design of oxide cathodes, offering insights into the effects of CSRD on the crystal and electronic structure of advanced functional materials.

Date: 2024
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DOI: 10.1038/s41586-024-07362-8

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