Probing Blended-Additive-Regulated Interface Chemistry Based on a Dynamic Competition Mechanism in Lithium Metal
Jin Ren1, Han Zhang1, Jiale Wan1
1State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology (HIT), Harbin, China.
Angewandte Chemie (International Ed. in English)
|July 7, 2026
Summary
Developing stable interfaces for high-voltage lithium metal batteries is key. This study reveals how fluoroethylene carbonate (FEC) and lithium difluorophosphate (LiDFP) additives interact, leading to a more robust electrode-electrolyte interphase.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- High-voltage lithium metal batteries require durable electrode-electrolyte interphases for stability.
- Interface chemistry in blended electrolyte additives remains complex and poorly understood.
- Lithium difluorophosphate (LiDFP) is a potential electrolyte additive, but its behavior in mixtures is unclear.
Purpose of the Study:
- To elucidate the interface chemistry in blended-additive electrolytes involving LiDFP.
- To understand the role of fluoroethylene carbonate (FEC) when co-used with LiDFP.
- To develop a mechanism-driven framework for optimizing multi-additive electrolyte systems.
Main Methods:
- Investigated the decomposition pathway of LiDFP using the dynamic competition mechanism (DCM).
- Analyzed interfacial evolution in blended-additive formulations (LiDFP with LiNO3 and FEC).
- Characterized the resulting interphase composition and properties.
Main Results:
- LiNO3 decomposition and LiDFP protonation initially led to harmful H3PO4 and HF accumulation.
- FEC unexpectedly remained undecomposed, modulating the interface by directing H+ adsorption.
- This modulation promoted complete LiDFP decomposition, forming an inorganic-rich interphase (Li3PO4 and LiF).
Conclusions:
- A universal DCM framework was proposed for optimizing multi-additive electrolytes based on additive synergies.
- The study shifts from empirical screening to mechanism-driven design for battery interfaces.
- Insights provide a blueprint for navigating complex interface chemistry in high-voltage batteries.
Keywords:
additive decompositionbi‐electrodes interphasesinterface chemistrylithium metal batterieslocal chemical environmentMore Related Videos
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