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Synergistic Bulk-Surface Modulation Stabilizing LiCoO2 at 4.65 V via Zr-Pillaring and In Situ Lattice-Matching
Guanming Yang1, Jianhang Cui1, Bingwu Zhou1
1School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, P. R. China.
Angewandte Chemie (International Ed. in English)
|August 7, 2026
Summary
This study enhances lithium cobalt oxide (LCO) batteries for higher energy density. A novel Zr-pillaring and LiCoPO4 coating strategy stabilizes LCO, improving cycling stability for advanced lithium-ion battery applications.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Lithium cobalt oxide (LiCoO2, LCO) is crucial for high-energy lithium-ion batteries.
- High-voltage operation (>4.55 V) causes LCO degradation (phase transition, oxygen loss, Co dissolution).
Purpose of the Study:
- To develop a synergistic bulk-surface modification to stabilize LCO at 4.65 V.
- To enhance the structural integrity and electrochemical performance of LCO cathodes.
Main Methods:
- Combined Zr-pillaring (LZCO) and in situ LiCoPO4 coating (LZCO@P).
- Employed density functional theory (DFT) to understand stabilization mechanisms.
- Investigated interfacial engineering via P-O tetrahedral formation.
Main Results:
- LZCO@P demonstrated 80.8% capacity retention after 1000 cycles at 1 C (3.5-4.65 V).
- Achieved 91.2% retention after 1000 cycles at 3 C (3.5-4.65 V).
- A pouch cell showed 92.3% retention after 160 cycles at 1 C (3.0-4.6 V).
Conclusions:
- Synergistic bulk-surface modification effectively stabilizes LCO at high voltages.
- Zr-pillaring expands the band gap, suppressing oxygen redox activity.
- LiCoPO4 coating enhances adhesion and reduces surface reactivity, improving cycling stability.
