Revealing the degradation pathways of layered Li-rich oxide cathodes

Liu, Zhimeng1; Zeng, Yuqiang2,3; Tan, Junyang4,5; Wang, Hailong1,2; Zhu, Yudong6; Geng, Xin1; Guttmann, Peter7; Hou, Xu8,9; Yang, Yang10,11; Xu, Yunkai12; Cloetens, Peter11; Zhou, Dong13; Wei, Yinping4,5; Lu, Jun12; Li, Jie8,9,14; Liu, Bilu4,5; Winter, Martin8,9; Kostecki, Robert3; Lin, Yuanjing2; He, Xin1,15

2024-09-01

10.1038/s41565-024-01773-4

NATURE NANOTECHNOLOGY   影响因子和分区

1748-3387

1748-3395

["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.","This work employs nano- to microscale characterization to identify different structural change pathways associated with non-homogeneous reactions within the particles, and explores differences in the failure mechanisms of lithium-rich transition metal oxide materials at different current densities."]

SCI ; EI

英语

通讯

Shenzhen Science and Technology Program[RCYX20231211090432060] ; Sichuan Science and Technology Program[2023NSFSC1131] ; Shenzhen Stable Support Plan Program for Higher Education Institutions Research Program[20231120094333001] ; Major Research Plan of the National Natural Science Foundation of China[92372207]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:001302955200002

NATURE PORTFOLIO

Web of Science

1.Sichuan Univ, Sch Chem Engn, Chengdu, Peoples R China
2.Southern Univ Sci & Technol, Sch Microelect, Shenzhen, Peoples R China
3.Lawrence Berkeley Natl Lab, Energy Storage & Distributed Resources Div, Berkeley, CA USA
4.Tsinghua Univ, Tsinghua Berkeley Shenzhen Inst, Shenzhen Geim Graphene Ctr, Shenzhen, Peoples R China
5.Tsinghua Univ, Inst Mat Res, Shenzhen Int Grad Sch, Shenzhen, Peoples R China
6.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen Key Lab Full Spectral Solar Elect Generat, Shenzhen, Peoples R China
7.Helmholtz Zentrum Berlin, Xray Microscopy Grp, Berlin, Germany
8.Univ Munster, Forschungszentrum Julich GmbH, Helmholtz Inst Munster HI MS, IEK 12, Munster, Germany
9.Univ Munster, MEET Battery Res Ctr, Munster, Germany
10.ESRF European Synchrotron Radiat Facil, Grenoble, France
11.Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY USA
12.Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou, Peoples R China
13.Inst Adv Sci Facil, Shenzhen 518000, Peoples R China
14.Politecn Milan, Dept Energy, Milan, Italy
15.Sichuan Univ, Coll Elect Engn, Chengdu, Peoples R China

Liu, Zhimeng,Zeng, Yuqiang,Tan, Junyang,et al. Revealing the degradation pathways of layered Li-rich oxide cathodes[J]. NATURE NANOTECHNOLOGY,2024.

Liu, Zhimeng.,Zeng, Yuqiang.,Tan, Junyang.,Wang, Hailong.,Zhu, Yudong.,...&He, Xin.(2024).Revealing the degradation pathways of layered Li-rich oxide cathodes.NATURE NANOTECHNOLOGY.

Liu, Zhimeng,et al."Revealing the degradation pathways of layered Li-rich oxide cathodes".NATURE NANOTECHNOLOGY (2024).