Resolving atomic-scale phase transformation and oxygen loss mechanism in ultrahigh-nickel layered cathodes for cobalt-free lithium-ion batteries
Abstract
Doped LiNiO2 has recently become one of the most promising cathode materials for its high specific energy, long cycle life, and reduced cobalt content. Despite this, the degradation mechanism of LiNiO2 and its derivatives still remains elusive. Here, by combining in situ electron microscopy and first-principles calculations, we elucidate the atomic-level chemomechanical degradation pathway of LiNiO2-derived cathodes. We uncover that the O1 phase formed at high voltages acts as a preferential site for rock-salt transformation via a two-step pathway involving cation mixing and shear along (003) planes. Moreover, electron tomography reveals that planar cracks nucleated simultaneously from particle interior and surface propagate along the [100] direction on (003) planes, accompanied by concurrent structural degradation in a discrete manner. Our results provide an in-depth understanding of the degradation mechanism of LiNiO2-derived cathodes, pointing out the concept that suppressing O1 phase and oxygen loss is the key in stabilizing LiNiO2 for developing next-generation high-energy cathode materials.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1774682
- Alternate Identifier(s):
- OSTI ID: 1807946; OSTI ID: 1811467
- Report Number(s):
- BNL-221807-2021-JAAM; BNL-221952-2021-JAAM
Journal ID: ISSN 2590-2385; S2590238521001193; PII: S2590238521001193
- Grant/Contract Number:
- AC02-06CH11357; SC0012704; SC0021204; EE0008444
- Resource Type:
- Published Article
- Journal Name:
- Matter (Online)
- Additional Journal Information:
- Journal Name: Matter (Online) Journal Volume: 4 Journal Issue: 6; Journal ID: ISSN 2590-2385
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; layered cathode; lithium-ion batteries; structural degradation; cracks; phase transformation; oxygen loss; in-situ; electron tomography; transmission electron microscopy; electron tomography transmission electron microscopy
Citation Formats
Wang, Chunyang, Han, Lili, Zhang, Rui, Cheng, Hao, Mu, Linqin, Kisslinger, Kim, Zou, Peichao, Ren, Yang, Cao, Penghui, Lin, Feng, and Xin, Huolin L. Resolving atomic-scale phase transformation and oxygen loss mechanism in ultrahigh-nickel layered cathodes for cobalt-free lithium-ion batteries. United States: N. p., 2021.
Web. doi:10.1016/j.matt.2021.03.012.
Wang, Chunyang, Han, Lili, Zhang, Rui, Cheng, Hao, Mu, Linqin, Kisslinger, Kim, Zou, Peichao, Ren, Yang, Cao, Penghui, Lin, Feng, & Xin, Huolin L. Resolving atomic-scale phase transformation and oxygen loss mechanism in ultrahigh-nickel layered cathodes for cobalt-free lithium-ion batteries. United States. https://doi.org/10.1016/j.matt.2021.03.012
Wang, Chunyang, Han, Lili, Zhang, Rui, Cheng, Hao, Mu, Linqin, Kisslinger, Kim, Zou, Peichao, Ren, Yang, Cao, Penghui, Lin, Feng, and Xin, Huolin L. Tue .
"Resolving atomic-scale phase transformation and oxygen loss mechanism in ultrahigh-nickel layered cathodes for cobalt-free lithium-ion batteries". United States. https://doi.org/10.1016/j.matt.2021.03.012.
@article{osti_1774682,
title = {Resolving atomic-scale phase transformation and oxygen loss mechanism in ultrahigh-nickel layered cathodes for cobalt-free lithium-ion batteries},
author = {Wang, Chunyang and Han, Lili and Zhang, Rui and Cheng, Hao and Mu, Linqin and Kisslinger, Kim and Zou, Peichao and Ren, Yang and Cao, Penghui and Lin, Feng and Xin, Huolin L.},
abstractNote = {Doped LiNiO2 has recently become one of the most promising cathode materials for its high specific energy, long cycle life, and reduced cobalt content. Despite this, the degradation mechanism of LiNiO2 and its derivatives still remains elusive. Here, by combining in situ electron microscopy and first-principles calculations, we elucidate the atomic-level chemomechanical degradation pathway of LiNiO2-derived cathodes. We uncover that the O1 phase formed at high voltages acts as a preferential site for rock-salt transformation via a two-step pathway involving cation mixing and shear along (003) planes. Moreover, electron tomography reveals that planar cracks nucleated simultaneously from particle interior and surface propagate along the [100] direction on (003) planes, accompanied by concurrent structural degradation in a discrete manner. Our results provide an in-depth understanding of the degradation mechanism of LiNiO2-derived cathodes, pointing out the concept that suppressing O1 phase and oxygen loss is the key in stabilizing LiNiO2 for developing next-generation high-energy cathode materials.},
doi = {10.1016/j.matt.2021.03.012},
journal = {Matter (Online)},
number = 6,
volume = 4,
place = {United States},
year = {Tue Jun 01 00:00:00 EDT 2021},
month = {Tue Jun 01 00:00:00 EDT 2021}
}
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