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Temperature-Responsive Formation Cycling Enabling LiF-Rich Cathode-Electrolyte Interphase
Luxi Hong1, Yi Zhang1, Pan Mei1
1Innovation Center for Chemical Science, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, 215123, P. R. China.
Angewandte Chemie (International Ed. in English)
|July 15, 2024
Summary
An additive-free strategy using low-temperature formation cycling creates a LiF-rich cathode electrolyte interphase (CEI) for advanced wide-temperature batteries. This method enhances high-temperature cyclability and low-temperature performance without side reactions.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- Wide-temperature battery performance is crucial for applications requiring operation across diverse thermal conditions.
- Formation of a LiF-rich cathode-electrolyte interphase (CEI) is desirable for stable wide-temperature battery operation.
- Conventional methods using fluorinated additives to form LiF-rich CEI often lead to unwanted side reactions.
Purpose of the Study:
- To develop an additive-free strategy for creating a LiF-rich CEI.
- To investigate the mechanism of LiF-rich CEI formation via low-temperature cycling.
- To evaluate the impact of this CEI on battery performance across a wide temperature range.
Main Methods:
- Low-temperature formation cycling at -5°C using LiNi0.33Mn0.33Co0.33O2 as a model cathode.
- Characterization of the CEI composition using techniques to determine LiF content.
- Electrochemical testing at various temperatures (-20°C to 60°C) to assess battery performance.
- Theoretical simulations to understand the underlying chemical mechanisms.
Main Results:
- Low-temperature cycling at -5°C significantly enhanced LiF content in the CEI (~17.7%) compared to 25°C formation (2.7%).
- The mechanism involves the spontaneous and exothermic decomposition of LiPF6 on the positively charged cathode surface at low temperatures.
- Batteries exhibited improved high-temperature (60°C) cyclability and a 100% capacity enhancement at -20°C (3C rate).
- The strategy was successfully extended to other cathode materials (LiNi0.8Mn0.1Co0.1O2, LiCoO2, LiMn2O4).
Conclusions:
- Additive-free, low-temperature formation cycling is an effective strategy for creating LiF-rich CEI.
- This approach overcomes limitations of conventional methods, avoiding side reactions and improving battery stability.
- The developed method offers a versatile pathway to enhance the performance of wide-temperature batteries.
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