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Uniformization of Electron Distribution at Grain Boundaries via Work Function Adjusting Interlayer to Prevent
Jeewon Lee1, Heebae Kim1, Young Pyo Jeon2
1Department of Chemical and Biological Engineering, and Institute of Chemical Processes, College of Engineering, Seoul National University, Gwanak-ro 1, Gwanak-gu, Seoul, 08826, Republic of Korea.
Small (Weinheim an Der Bergstrasse, Germany)
|March 10, 2025
Summary
Preventing lithium-filament formation in all-solid-state lithium metal batteries is crucial for safety. Uniformizing work functions at the microstructure interfaces using a LiF interlayer significantly suppresses filament growth and enhances battery stability.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- All-solid-state lithium metal batteries (ASSLMBs) require safe operation, with lithium-filament formation being a major safety concern.
- Understanding the electronic properties of inorganic solid-electrolytes (ISEs) is critical for mitigating lithium-filament formation.
- Localized current reduction of Li-ions at grain boundaries in ISEs is a primary driver of filament growth.
Purpose of the Study:
- To elucidate the mechanism of lithium-filament formation in ISEs.
- To investigate the role of work function differences at microstructural interfaces in filament nucleation.
- To develop a strategy for suppressing lithium-filament formation and enhancing ASSLMB safety.
Main Methods:
- Investigated work function differences between grain interiors (LLZO) and grain boundaries (LixAlOy) in ISEs.
- Introduced a thin lithium fluoride (LiF) interlayer to uniformize work functions across the microstructure.
- Utilized laser-induced breakdown spectroscopy (LIBS) for surface and cross-section imaging to identify filament formation.
Main Results:
- Confirmed work function differences (≈4.2 eV vs. ≈4.32 eV) drive localized Li-ion reduction at grain boundaries.
- Demonstrated that a LiF interlayer (≈4.08 eV) effectively uniformizes work functions, suppressing localized currents and Li-filament formation.
- Observed a five-fold increase in critical current density in Li-symmetrical cells with the LiF interlayer, indicating enhanced electrochemical stability.
Conclusions:
- The study reveals that work function heterogeneity at ISE microstructural interfaces is the root cause of Li-filament formation.
- Microstructure interface engineering by uniformizing electronic properties is essential for safe and stable ASSLMBs.
- The LiF interlayer presents a viable strategy for enhancing the safety and performance of next-generation solid-state batteries.
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