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Toughened Bimodal Cathodes for All-Solid-State Batteries via Controlled Interfacial Heterogeneity
Junhee Kang1, Hong Rim Shin1, Jonghyeok Yun1
1Division of Materials Science and Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul 04763, Republic of Korea.
ACS Applied Materials & Interfaces
|October 24, 2025
Summary
Bimodal cathodes in all-solid-state batteries improve packing density but can fail due to particle cracking. Adding a nanolayer prevents this failure, enabling stable cycling for high-energy-density batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- All-solid-state batteries (ASSBs) face energy density limitations due to heavy solid electrolytes.
- Bimodal cathodes, using mixed particle sizes, are proposed to increase cathode packing density.
Purpose of the Study:
- Investigate fracture-induced failure mechanisms in bimodal cathodes.
- Determine requirements for high-performance, long-cycling ASSBs.
- Enhance the stability of bimodal cathodes in sulfide-based ASSBs.
Main Methods:
- Fabrication and electrochemical cycling of unimodal and bimodal cathodes (LiNi0.88Co0.09Al0.03O2/Li6PS5Cl).
- Microstructural characterization, impedance analysis, and mechanical simulations.
- Application of Li2ZrO3 nanolayer to mitigate interfacial issues.
Main Results:
- Bimodal cathodes show higher packing density and conductivity but suffer rapid capacity decline.
- Failure attributed to cracking in larger active material particles caused by interfacial heterogeneity.
- Li2ZrO3 nanolayer effectively suppressed particle cracking and improved cycling stability.
Conclusions:
- Interfacial heterogeneity is a critical factor causing mechanical failure in bimodal cathodes.
- Mitigating interfacial reactions is essential for stable cycling of high-energy-density ASSBs.
- Nanolayer coating offers a viable strategy to enhance the durability of bimodal cathodes.
