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In Situ Surface Reaction for the Preparation of High-Performance Li-Rich Mn-Based Cathode Materials with Integrated
Zihao Su1,2, Zhihao Guo1,2, Haoyu Xie1,2
1Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu 610041, P. R. China.
ACS Applied Materials & Interfaces
|July 17, 2024
Summary
Surface functionalization of Li-rich Mn-based cathode materials using a simple NaBF4 treatment significantly boosts initial Coulombic efficiency and structural stability for advanced Li-ion batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Solid State Chemistry
Background:
- Li-rich Mn-based cathode materials (LLOs) exhibit high energy density but suffer from low initial Coulombic efficiency (ICE), poor rate capability, and structural instability.
- Existing methods struggle to address these limitations simultaneously, hindering their practical application in high-performance batteries.
Purpose of the Study:
- To develop a facile surface functionalization strategy for LLOs to overcome their inherent drawbacks.
- To enhance the electrochemical performance, particularly ICE and structural integrity, of LLOs for next-generation lithium-ion batteries.
Main Methods:
- A two-step fabrication process involving liquid-stage NaBF4 treatment followed by in situ sintering.
- Density functional theory (DFT) calculations to elucidate the underlying mechanisms of structural and electronic modifications.
Main Results:
- The treatment successfully introduced oxygen vacancies (OV), spinel structures, and doping of Na, B, and F into the LLO structure.
- Enhanced electrical conductivity, suppressed lattice oxygen activity, and improved structural stability due to strong B-O bonding preventing transition metal migration.
- Achieved a high ICE of 90.29% and excellent capacity retention (89.94% after 100 cycles at 1C), along with increased operating voltage.
Conclusions:
- The developed surface functionalization method effectively addresses key challenges in LLOs, leading to significantly improved electrochemical performance.
- This approach offers a promising strategy for designing high-energy-density cathode materials for advanced lithium-ion batteries.
