Long-Range Cationic Disordering Induces two Distinct Degradation Pathways in Co-Free Ni-Rich Layered Cathodes

© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH..

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 Li1-m (Ni0.94 Al0.06 )1+m O2 (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.

Medienart:

E-Artikel

Erscheinungsjahr:

2023

Erschienen:

2023

Enthalten in:

Zur Gesamtaufnahme - volume:62

Enthalten in:

Angewandte Chemie (International ed. in English) - 62(2023), 12 vom: 13. März, Seite e202214880

Sprache:

Englisch

Beteiligte Personen:

Hua, Weibo [VerfasserIn]
Zhang, Jilu [VerfasserIn]
Wang, Suning [VerfasserIn]
Cheng, Yi [VerfasserIn]
Li, Hang [VerfasserIn]
Tseng, Jochi [VerfasserIn]
Wu, Zhonghua [VerfasserIn]
Shen, Chong-Heng [VerfasserIn]
Dolotko, Oleksandr [VerfasserIn]
Liu, Hao [VerfasserIn]
Hung, Sung-Fu [VerfasserIn]
Tang, Wei [VerfasserIn]
Li, Mingtao [VerfasserIn]
Knapp, Michael [VerfasserIn]
Ehrenberg, Helmut [VerfasserIn]
Indris, Sylvio [VerfasserIn]
Guo, Xiaodong [VerfasserIn]

Links:

Volltext

Themen:

Cationic Disordering
Degradation Pathways
Journal Article
Lattice Distortion
Ni-Rich Cathodes
Surface Reconstruction

Anmerkungen:

Date Completed 06.03.2023

Date Revised 06.03.2023

published: Print-Electronic

Citation Status PubMed-not-MEDLINE

doi:

10.1002/anie.202214880

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM350574146