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Published on: November 11, 2013
Deciphering Kinetic Principles of Dual-Anion Electrolytes for Extreme Fast-Charging Lithium-Ion Batteries
Hongpeng Gao1,2, Nicholas Solan2, Luqi Zhang2
1Program of Materials Science and Engineering, University of California San Diego, La Jolla, California, USA.
Optimizing lithium-ion battery electrolytes with dual-anions enhances extreme fast-charging performance. This strategy improves interfacial stability and battery lifespan by creating robust electrode-electrolyte interfaces.
Area of Science:
- Materials Science
- Electrochemistry
- Chemical Engineering
Background:
- Tailoring Li+ solvation is key for lithium-ion battery (LIB) performance during extreme fast-charging (XFC).
- Increased Li-anion pairing influences the formation of inorganic-rich electrode-electrolyte interfaces (EEIs).
Purpose of the Study:
- To propose an anion-screening guideline for optimizing dual-anion electrolytes.
- To investigate mechanisms in dual-anion systems for carbonate and ester solvents.
- To address challenges like interfacial instability, lithium plating, and structural degradation in LIBs.
Main Methods:
- Developed an anion-screening guideline based on bulk electrolyte transport, desolvation energy, and interfacial kinetics.
- Employed integrated computational and experimental studies.
- Investigated dual-anion electrolytes in carbonate (dimethyl carbonate) and ester (methyl propionate) solvents.
Main Results:
- Optimized dual-anion systems form partially ion-paired solvation structures and robust anion-derived EEIs.
- LiNi0.6Mn0.2Co0.2 || graphite pouch cells with PF6-/TFSI- in dimethyl carbonate retained >85% capacity after 500 cycles at 4C.
- Ester-based electrolytes showed 94% capacity retention after 500 cycles and 83% after 1000 cycles at 4C.
- Improvements linked to reduced charge-transfer impedance due to enriched inorganic fluorides and sulfates at the interface.
Conclusions:
- Dual-anion electrolytes provide a promising pathway for fast-charging, high-energy-density LIBs.
- The proposed anion-screening framework aids in regulating electrolyte composition for enhanced battery performance.
- Achieved robust electrode-electrolyte interfaces crucial for stable operation under extreme fast-charging conditions.
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