Regulating the Electron Distribution of Metal‐Oxygen for Enhanced Oxygen Stability in Li‐rich Layered Cathodes

Abstract: Li‐rich Mn‐based layered oxides (LLO) hold great promise as cathode materials for lithium‐ion batteries (LIBs) due to their unique oxygen redox (OR) chemistry, which enables additional capacity. However, the LLOs face challenges related to the instability of their OR process due to the weak transition metal (TM)‐oxygen bond, leading to oxygen loss and irreversible phase transition that results in severe capacity and voltage decay. Herein, a synergistic electronic regulation strategy of surface and interior structures to enhance oxygen stability is proposed. In the interior of the materials, the local electrons around TM and O atoms may be delocalized by surrounding Mo atoms, facilitating the formation of stronger TM─O bonds at high voltages. Besides, on the surface, the highly reactive O atoms with lone pairs of electrons are passivated by additional TM atoms, which provides a more stable TM─O framework. Hence, this strategy stabilizes the oxygen and hinders TM migration, which enhances the reversibility in structural evolution, leading to increased capacity and voltage retention. This work presents an efficient approach to enhance the performance of LLOs through surface‐to‐interior electronic structure modulation, while also contributing to a deeper understanding of their redox reaction.

Location
Deutsche Nationalbibliothek Frankfurt am Main
Extent
Online-Ressource
Language
Englisch

Bibliographic citation
Regulating the Electron Distribution of Metal‐Oxygen for Enhanced Oxygen Stability in Li‐rich Layered Cathodes ; day:22 ; month:04 ; year:2024 ; extent:10
Advanced science ; (22.04.2024) (gesamt 10)

Creator
Yin, Zijia
Zhao, Jun
Luo, Dong
Chin, Yi‐Ying
Chen, Chien‐Te
Chen, Huaican
Yin, Wen
Tang, Yu
Yang, Tingting
Ren, Jincan
Li, Tianyi
Wiaderek, Kamila M.
Kong, Qingyu
Fan, Jun
Zhu, He
Ren, Yang
Liu, Qi

DOI
10.1002/advs.202307397
URN
urn:nbn:de:101:1-2404231423223.058126193694
Rights
Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
Last update
03.02.20252026, 1:41 AM CET

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Associated

  • Yin, Zijia
  • Zhao, Jun
  • Luo, Dong
  • Chin, Yi‐Ying
  • Chen, Chien‐Te
  • Chen, Huaican
  • Yin, Wen
  • Tang, Yu
  • Yang, Tingting
  • Ren, Jincan
  • Li, Tianyi
  • Wiaderek, Kamila M.
  • Kong, Qingyu
  • Fan, Jun
  • Zhu, He
  • Ren, Yang
  • Liu, Qi

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