Elucidating and Mitigating High-Voltage Degradation Cascades in Cobalt-Free LiNiO2 Lithium-Ion Battery Cathodes
- Authors
- Park, Kyu-Young; Zhu, Yizhou; Torres-Castanedo, Carlos G.; Jung, Hee Joon; Luu, Norman S.; Kahvecioglu, Ozge; Yoo, Yiseul; Seo, Jung-Woo T.; Downing, Julia R.; Lim, Hee-Dae; Bedzyk, Michael J.; Wolverton, Christopher; Hersam, Mark C.
- Issue Date
- Jan-2022
- Publisher
- WILEY-V C H VERLAG GMBH
- Keywords
- graphene coating; lithium battery; lithium nickel oxide; oxygen evolution; stacking faults
- Citation
- ADVANCED MATERIALS, v.34, no.3, pp.1 - 11
- Indexed
- SCIE
SCOPUS
- Journal Title
- ADVANCED MATERIALS
- Volume
- 34
- Number
- 3
- Start Page
- 1
- End Page
- 11
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/186241
- DOI
- 10.1002/adma.202106402
- ISSN
- 0935-9648
- Abstract
- LiNiO2 (LNO) is a promising cathode material for next-generation Li-ion batteries due to its exceptionally high capacity and cobalt-free composition that enables more sustainable and ethical large-scale manufacturing. However, its poor cycle life at high operating voltages over 4.1 V impedes its practical use, thus motivating efforts to elucidate and mitigate LiNiO2 degradation mechanisms at high states of charge. Here, a multiscale exploration of high-voltage degradation cascades associated with oxygen stacking chemistry in cobalt-free LiNiO2, is presented. Lattice oxygen loss is found to play a critical role in the local O3-O1 stacking transition at high states of charge, which subsequently leads to Ni-ion migration and irreversible stacking faults during cycling. This undesirable atomic-scale structural evolution accelerates microscale electrochemical creep, cracking, and even bending of layers, ultimately resulting in macroscopic mechanical degradation of LNO particles. By employing a graphene-based hermetic surface coating, oxygen loss is attenuated in LNO at high states of charge, which suppresses the initiation of the degradation cascade and thus substantially improves the high-voltage capacity retention of LNO. Overall, this study provides mechanistic insight into the high-voltage degradation of LNO, which will inform ongoing efforts to employ cobalt-free cathodes in Li-ion battery technology.
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