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Revisiting the High-Entropy Paradigm for Ni-Rich Cathodes: Dopant-Induced Surface Engineering as the Key to Stability
Hyewon Lee1, Jin Ho Bang1,2
1Department of Applied Chemistry, Center for Bionano Intelligence Education and Research, Hanyang University ERICA, Ansan, Gyeonggi-do, 15588, Republic of Korea.
Small (Weinheim an Der Bergstrasse, Germany)
|December 31, 2025
Summary
Dopant chemistry, not entropy, is key for high-performance lithium-ion battery cathodes. Tailoring specific elements creates stable surface phases, enhancing cycling stability for next-generation batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- High-entropy doping stabilizes high-nickel layered cathodes for lithium-ion batteries.
- The precise contribution of configurational entropy versus dopant chemistry to performance enhancement is unclear.
Purpose of the Study:
- To systematically differentiate the roles of configurational entropy and dopant chemistry in Co-free, Ni-rich cathodes.
- To identify the primary drivers of electrochemical performance and cycling stability.
Main Methods:
- Comparative analysis of cathodes with identical entropy but different dopant compositions (W-Nb-Mg vs. Zr-Ti-Mg).
- Investigation of effects of increased elemental composition on entropy and properties.
- Characterization of surface phase formation and cathode-electrolyte interphase.
Main Results:
- Dopant chemistry significantly outweighs configurational entropy in determining electrochemical performance.
- W/Nb/Mg-doped cathodes show superior cycling stability due to a passivating rock-salt surface phase and robust LiF-rich interphase.
- Increased entropy (W-Nb-Mg-Zr-Ti-Al) improved bulk mechanical properties and suppressed phase transitions but offered minimal cycling gains.
Conclusions:
- Specific dopant chemistry is paramount for high-performance cathodes, even in high-entropy strategies.
- A chemically informed doping approach focusing on stable surface phase engineering is more effective than maximizing entropy.
- This strategy offers a rational pathway toward durable next-generation lithium-ion battery cathodes.
Keywords:
dopant effecthigh‐Ni layered cathodeshigh‐entropy cathodesinterfacial stabilitysurface phase evolutionMore Related Videos
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