In:
Angewandte Chemie, Wiley, Vol. 135, No. 12 ( 2023-03-13)
Abstract:
Ni‐rich layered oxides are one of the most attractive cathode materials in high‐energy‐density lithium‐ion batteries, their degradation mechanisms are still not completely elucidated. Herein, we report a strong dependence of degradation pathways on the long‐range cationic disordering of Co‐free Ni‐rich Li 1− m (Ni 0.94 Al 0.06 ) 1+ m O 2 (NA). Interestingly, a disordered layered phase with lattice mismatch can be easily formed in the near‐surface region of NA particles with very low cation disorder (NA‐LCD, m ≤0.06) over electrochemical cycling, while the layered structure is basically maintained in the core of particles forming a “core–shell” structure. Such surface reconstruction triggers a rapid capacity decay during the first 100 cycles between 2.7 and 4.3 V at 1 C or 3 C. On the contrary, the local lattice distortions are gradually accumulated throughout the whole NA particles with higher degrees of cation disorder (NA‐HCD, 0.06≤ m ≤0.15) that lead to a slow capacity decay upon cycling.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v135.12
DOI:
10.1002/ange.202214880
Language:
English
Publisher:
Wiley
Publication Date:
2023
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