Title
Chemical short-range disorder in lithium oxide cathodes
Author
Wang, Q. (TU Delft RST/Storage of Electrochemical Energy)
Yao, Zhenpeng (Shanghai Jiao Tong University)
Wang, Jianlin (Chinese Academy of Sciences)
Guo, Hao (China Institute of Atomic Energy)
Li, Chao (East China Normal University)
Zhou, Dong (Helmholtz-Zentrum Berlin für Materialen und Energie GmbH)
Bai, Xuedong (Chinese Academy of Sciences)
Li, Hong (Chinese Academy of Sciences)
Li, Baohua (Tsinghua University)
Wagemaker, M. (TU Delft RST/Storage of Electrochemical Energy) 
Zhao, C. (TU Delft RST/Storage of Electrochemical Energy)
Date
2024
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.
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http://resolver.tudelft.nl/uuid:8829a6ee-5c88-43f4-a6fd-5e899fea38cd
DOI
https://doi.org/10.1038/s41586-024-07362-8
Embargo date
2024-11-08
ISSN
0028-0836
Source
Nature: international weekly journal of science, 629 (8011), 341-347
Bibliographical note
Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.
Part of collection
Institutional Repository
Document type
journal article
Rights
© 2024 Q. Wang, Zhenpeng Yao, Jianlin Wang, Hao Guo, Chao Li, Dong Zhou, Xuedong Bai, Hong Li, Baohua Li, M. Wagemaker, C. Zhao