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Which Exchange Current Densities Can Be Achieved in Composite Cathodes of Bulk-Type All-Solid-State Batteries? A
Vanessa Miß1, Asvitha Ramanayagam1, Bernhard Roling1
1Department of Chemistry, Philipps-Universität Marburg, Hans-Meerwein-Straße 4, Marburg D-35032, Germany.
ACS Applied Materials & Interfaces
|August 15, 2022
Summary
This study quantifies lithium-ion exchange current densities in all-solid-state lithium batteries. High pressures enhance these densities, rivaling those in liquid electrolyte systems.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Batteries
Background:
- All-solid-state lithium battery performance relies on cathode active material (CAM) and solid electrolyte (SE) particle contact.
- Lithium-ion (Li+) exchange current densities at CAM | SE interfaces are critical but experimentally underexplored.
- Understanding impedance spectra is key to determining Li+ exchange current densities in solid-state batteries.
Purpose of the Study:
- To experimentally determine Li+ exchange current densities at CAM | SE interfaces in bulk-type all-solid-state Li batteries (ASSBs).
- To investigate the influence of different cathode active materials (LiCoO2 and LiNi0.83Mn0.06Co0.11O2) on interfacial performance.
- To elucidate the relationship between interfacial impedance and overall battery performance under varying conditions.
Main Methods:
- Utilized impedance spectroscopy on In-Li | SE | In-Li symmetric cells to isolate anode and anode | separator interfacial impedances.
- Employed composite cathodes with amorphous Li3PS4 + LiI solid electrolyte and single-crystalline CAM particles.
- Varied composite cathode thickness to distinguish ion transport from charge transfer resistance.
Main Results:
- Successfully quantified Li+ exchange current densities for two distinct CAMs within composite cathodes.
- Demonstrated that high stack pressures (400 MPa) significantly enhance Li+ exchange current densities.
- Observed that these enhanced densities can match or surpass those found at CAM | liquid electrolyte interfaces.
Conclusions:
- Experimental determination of Li+ exchange current densities in ASSBs is feasible and crucial for performance understanding.
- Optimizing interfacial contact through applied pressure is a viable strategy to boost ASSB performance.
- Solid-state interfaces can achieve electrochemical performance comparable to traditional liquid electrolyte systems.
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