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Published on: May 14, 2019
Revisiting Carbonate Additives through Dynamic Regulation of Cathode Electric Double Layers
Qi Yu1, Kaixiang Ren1, Xinchun Song1
1School of Materials Science and Engineering, Anhui University of Technology, Maanshan243002, China.
Vinylene carbonate (VC) and fluoroethylene carbonate (FEC) stabilize high-voltage lithium metal batteries by forming protective interphases and dynamically regulating the electric double layer (EDL). This prevents electrolyte decomposition on NCM811 cathodes, with FEC offering superior durability.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- High-voltage lithium metal batteries (LMBs) require stable electrolytes.
- Carbonate additives like vinylene carbonate (VC) and fluoroethylene carbonate (FEC) are crucial for electrolyte stabilization.
- Current understanding focuses on static film formation by these additives.
Purpose of the Study:
- To reassess the functions of VC and FEC at high-voltage NCM811 cathodes.
- To investigate the dynamic roles of VC and FEC beyond simple film formation.
- To elucidate the mechanism of electrolyte stabilization in high-voltage LMBs.
Main Methods:
- In-situ electrochemical surface-enhanced Raman spectroscopy (EC-SERS).
- Theoretical calculations.
- Systematic electrochemical evaluation.
Main Results:
- VC and FEC contribute to cathode electrolyte interphase (CEI) formation.
- These additives dynamically regulate the cathode-side electric double layer (EDL).
- They suppress electrolyte decomposition by reducing potential sensitivity and limiting solvent/PF6- enrichment near the NCM811 surface.
- FEC forms a more durable LiF-rich organic-inorganic hybrid interphase compared to VC.
Conclusions:
- VC and FEC exhibit a novel EDL-regulation mechanism in high-voltage LMBs.
- This EDL regulation is key to preventing continuous electrolyte decomposition.
- Findings provide guidance for designing advanced electrolytes for high-voltage LMBs.
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