Activating Anionic Redox of Li-Rich Mn-Based Layered Oxide in All-Solid-State Batteries by Tailoring the Cathode...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Lithium-rich manganese-based layered oxides (LRMOs) are key for high-energy-density lithium-ion batteries.
• Liquid electrolytes limit LRMO cycle life due to gas release and manganese dissolution.
• All-solid-state batteries (ASSBs) offer a potential solution, but require stable interfaces and efficient ion transport.

Purpose of the Study:

• To investigate the impact of monolithic LRMO particle microstructure on ASSB performance.
• To activate anionic redox and improve lithium-ion kinetics in LRMO cathodes for ASSBs.
• To demonstrate a strategy for enhancing LRMO capacity and cycle life in ASSBs.

Main Methods:

• Utilized monolithic LRMO particles without surface modification.
• Fabricated and tested LRMO-based cathodes within an all-solid-state battery architecture.
• Characterized electrochemical performance, focusing on capacity and Li+ diffusion.

Main Results:

• Achieved a high capacity of 268.4 mAh g⁻¹ with monolithic LRMO particles.
• Demonstrated significantly enhanced oxygen redox activation compared to polycrystalline LRMOs.
• Observed improved cathode-electrolyte contact and shortened Li+ diffusion pathways.

Conclusions:

• Monolithic LRMO particle design is crucial for activating anionic redox in ASSBs.
• Tailoring cathode microstructure offers a viable path to high-performance LRMO-based ASSBs.
• This approach overcomes limitations of conventional LRMOs in solid-state battery applications.