Surface Li⁺ /H⁺ exchange engineering for enhancing structural stability and electrochemical performance of lithium-rich manganese-based layered oxides
File(s)
Supplementary information
Accepted version
Author(s)
Type
Journal Article
Abstract
Lithium-rich manganese-based layered oxides (LRO) are promising ultra-high-capacity cathode materials for next-generation lithium-ion batteries but suffer from structural instability, capacity/voltage decay, and poor rate capability. Herein, a novel surface spinel coating strategy is proposed to address these challenges through a citric acid solution treatment followed by thermal annealing. A Li4Mn5O12 spinel coating layer is formed on the cathode material surface via Li+/H+ exchange and structural rearrangement, while preserving the bulk-layered structure. The spinel phase not only suppresses interfacial side reactions and lattice oxygen loss but also establishes 3D Li+ diffusion channels, enhancing kinetics and surface stability. The modified cathode material exhibits remarkable electrochemical improvements with a high-rate capacity of 205.29 mAh g−1 at 5 C, and 86.3% capacity retention after 150 cycles at 1 C, outperforming the untreated LRO. This work provides a scalable surface engineering approach to reconcile the trade-off between high energy density and long-cycle stability in the LRO, advancing their practical viability for high-energy-density batteries.
Date Issued
2025-12-17
Date Acceptance
2025-11-01
Citation
Small, 2025, 21 (50)
ISSN
1613-6810
Publisher
Wiley
Journal / Book Title
Small
Volume
21
Issue
50
Copyright Statement
Copyright © 2025 Wiley-VCH GmbH. This is the author’s accepted manuscript made available under a CC-BY licence in accordance with Imperial’s Research Publications Open Access policy (www.imperial.ac.uk/oa-policy)
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/41195649
Subjects
Li+/H+ exchange
citric acid
lithium‐rich manganese‐based oxides
side reactions
spinel coating
Publication Status
Published
Coverage Spatial
Germany
Article Number
e09446
Date Publish Online
2025-11-06