Revealing the degradation pathways of layered Li-rich oxide cathodes
Liu, Zhimeng ; Zeng, Yuqiang ; Tan, Junyang ; Wang, Hailong ; Zhu, Yudong ; Geng, Xin ; Guttmann, Peter ; Hou, Xu LU
; Yang, Yang
LU
and Xu, Yunkai
, et al.
(2024)
In Nature Nanotechnology
19(12).
p.1821-1830
- Abstract
Layered lithium-rich transition metal oxides are promising cathode candidates for high-energy-density lithium batteries due to the redox contributions from transition metal cations and oxygen anions. However, their practical application is hindered by gradual capacity fading and voltage decay. Although oxygen loss and phase transformation are recognized as primary factors, the structural deterioration, chemical rearrangement, kinetic and thermodynamic effects remain unclear. Here we integrate analysis of morphological, structural and oxidation state evolution from individual atoms to secondary particles. By performing nanoscale to microscale characterizations, distinct structural change pathways associated with intraparticle... (More)
Layered lithium-rich transition metal oxides are promising cathode candidates for high-energy-density lithium batteries due to the redox contributions from transition metal cations and oxygen anions. However, their practical application is hindered by gradual capacity fading and voltage decay. Although oxygen loss and phase transformation are recognized as primary factors, the structural deterioration, chemical rearrangement, kinetic and thermodynamic effects remain unclear. Here we integrate analysis of morphological, structural and oxidation state evolution from individual atoms to secondary particles. By performing nanoscale to microscale characterizations, distinct structural change pathways associated with intraparticle heterogeneous reactions are identified. The high level of oxygen defects formed throughout the particle by slow electrochemical activation triggers progressive phase transformation and the formation of nanovoids. Ultrafast lithium (de)intercalation leads to oxygen-distortion-dominated lattice displacement, transition metal ion dissolution and lithium site variation. These inhomogeneous and irreversible structural changes are responsible for the low initial Coulombic efficiency, and ongoing particle cracking and expansion in the subsequent cycles.
(Less)
- author
- Liu, Zhimeng
; Zeng, Yuqiang
; Tan, Junyang
; Wang, Hailong
; Zhu, Yudong
; Geng, Xin
; Guttmann, Peter
; Hou, Xu
LU
; Yang, Yang
LU
and Xu, Yunkai
, et al. (More)
- Liu, Zhimeng
; Zeng, Yuqiang
; Tan, Junyang
; Wang, Hailong
; Zhu, Yudong
; Geng, Xin
; Guttmann, Peter
; Hou, Xu
LU
; Yang, Yang
LU
; Xu, Yunkai
; Cloetens, Peter
; Zhou, Dong
; Wei, Yinping
; Lu, Jun
; Li, Jie
; Liu, Bilu
; Winter, Martin
; Kostecki, Robert
; Lin, Yuanjing
and He, Xin
(Less)
- publishing date
- 2024-12
- type
- Contribution to journal
- publication status
- published
- in
- Nature Nanotechnology
- volume
- 19
- issue
- 12
- pages
- 10 pages
- publisher
- Nature Publishing Group
- external identifiers
-
- pmid:39223255
- scopus:85202965515
- ISSN
- 1748-3387
- DOI
- 10.1038/s41565-024-01773-4
- language
- English
- LU publication?
- no
- additional info
- Publisher Copyright: © The Author(s), under exclusive licence to Springer Nature Limited 2024.
- id
- 401a5f28-c29d-4138-a45f-0f682dcd78a2
- date added to LUP
- 2025-12-05 22:19:27
- date last changed
- 2025-12-20 00:15:39
@article{401a5f28-c29d-4138-a45f-0f682dcd78a2,
abstract = {{<p>Layered lithium-rich transition metal oxides are promising cathode candidates for high-energy-density lithium batteries due to the redox contributions from transition metal cations and oxygen anions. However, their practical application is hindered by gradual capacity fading and voltage decay. Although oxygen loss and phase transformation are recognized as primary factors, the structural deterioration, chemical rearrangement, kinetic and thermodynamic effects remain unclear. Here we integrate analysis of morphological, structural and oxidation state evolution from individual atoms to secondary particles. By performing nanoscale to microscale characterizations, distinct structural change pathways associated with intraparticle heterogeneous reactions are identified. The high level of oxygen defects formed throughout the particle by slow electrochemical activation triggers progressive phase transformation and the formation of nanovoids. Ultrafast lithium (de)intercalation leads to oxygen-distortion-dominated lattice displacement, transition metal ion dissolution and lithium site variation. These inhomogeneous and irreversible structural changes are responsible for the low initial Coulombic efficiency, and ongoing particle cracking and expansion in the subsequent cycles.</p>}},
author = {{Liu, Zhimeng and Zeng, Yuqiang and Tan, Junyang and Wang, Hailong and Zhu, Yudong and Geng, Xin and Guttmann, Peter and Hou, Xu and Yang, Yang and Xu, Yunkai and Cloetens, Peter and Zhou, Dong and Wei, Yinping and Lu, Jun and Li, Jie and Liu, Bilu and Winter, Martin and Kostecki, Robert and Lin, Yuanjing and He, Xin}},
issn = {{1748-3387}},
language = {{eng}},
number = {{12}},
pages = {{1821--1830}},
publisher = {{Nature Publishing Group}},
series = {{Nature Nanotechnology}},
title = {{Revealing the degradation pathways of layered Li-rich oxide cathodes}},
url = {{http://dx.doi.org/10.1038/s41565-024-01773-4}},
doi = {{10.1038/s41565-024-01773-4}},
volume = {{19}},
year = {{2024}},
}