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Enhanced Electrochemical Performance of Disordered Rocksalt Cathodes Enabled by a Graphite Conductive Additive
Shripad Patil1,2, Krishna Prasad Koirala3, Matthew J Crafton4,5
1Bredesen Center for Interdisciplinary Research and Education, University of Tennessee Knoxville, Knoxville, Tennessee 37996, United States.
ACS Applied Materials & Interfaces
|August 11, 2023
Summary
Reducing carbon content in cobalt-free cation-disordered rocksalt (DRX) cathodes is key for better Li-ion batteries. Graphite additives significantly improve performance by creating protective coatings and stable conductive networks.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Cobalt-free cation-disordered rocksalt (DRX) cathodes offer high theoretical capacities for next-generation Li-ion batteries.
- High carbon content (up to 30 wt%) is typically required for DRX cathodes, negatively impacting energy density.
- Understanding carbon's role is crucial for optimizing DRX cathode performance and reducing carbon loading.
Purpose of the Study:
- To investigate the influence of carbon microstructure and loading (10-20 wt%) on DRX cathode performance.
- To identify pathways for reducing electrode carbon content while maintaining or improving battery performance.
- To elucidate the mechanisms behind performance variations in DRX cathodes with different carbon additives.
Main Methods:
- Fabrication of DRX cathodes (Li1.2Mn0.5Ti0.3O1.9F0.1) with varying carbon additives (graphite, C65, ketjenblack) at 10-20 wt% loading.
- Electrochemical testing including cycling performance and rate capability assessments.
- Material characterization using a suite of tools to analyze electrode microstructure and surface properties.
Main Results:
- DRX cathodes with conventional disordered carbons (C65, ketjenblack) showed rapid capacity fade due to unstable interfaces.
- Electrodes with 10 wt% graphite exhibited superior cycling performance (∼260 mA h/g, 85% retention after 50 cycles) and rate capability (∼135 mA h/g at 1000 mA/g).
- Graphite addition led to uniform surface coatings and homogeneous dispersion, enhancing electronic conductivity and stability.
Conclusions:
- Graphite's superior performance in DRX cathodes is attributed to protective surface coatings and robust conductive networks.
- Reducing carbon content to 10 wt% using graphite is a viable strategy to enhance DRX cathode energy density and stability.
- Further optimization through alternative graphitic coating methods is recommended for improved DRX cathode performance.
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