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Mitigating Diffusion-Induced Intragranular Cracking in Single-Crystal LiNi0.5Mn1.5O4 via Extended Solid-Solution
Hyeonsol Shin1, Agwu Ndukwe2, Taemin Kim1
1Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
Angewandte Chemie (International Ed. in English)
|February 4, 2025
Summary
Magnesium doping in single-crystal lithium nickel manganese oxide cathodes significantly reduces cracking and volume change. This enhances mechanical integrity and battery durability by suppressing internal stress during lithium diffusion.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Single-crystal cathodes offer resistance to intergranular cracking but suffer from intragranular cracking.
- The mechanisms driving intragranular cracking in these materials are not fully understood.
Purpose of the Study:
- To investigate the effect of magnesium doping on mitigating crack formation in single-crystal LiNi0.5Mn1.5O4 (Mg-SC-LNMO) cathodes.
- To understand the role of magnesium in improving the mechanical and electrochemical properties of these cathodes.
Main Methods:
- Extended solid-solution reactions were employed for magnesium doping.
- Electrochemical performance testing and continuum modeling were utilized.
- Characterization focused on structural integrity and lithium-ion diffusion.
Main Results:
- Magnesium doping reduced volume change by nearly 50% and suppressed two-phase reactions.
- The lithium-ion diffusion coefficient was effectively doubled.
- Continuum modeling confirmed reduced internal stress due to magnesium's structural support.
Conclusions:
- Magnesium doping enhances the mechanical robustness of single-crystal LNMO cathodes.
- This strategy improves electrochemical performance and durability for next-generation lithium-ion batteries.
- The findings offer insights into designing mechanically stable single-crystal battery materials.
