Facile fabrication of solution-processed solid-electrolytes for high-energy-density all-solid-state-batteries by...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• All-solid-state lithium-ion batteries (ASSBs) offer enhanced safety and high capacity compared to conventional lithium-ion batteries (LIBs).
• Solid electrolytes (SEs) in ASSBs achieve ionic conductivity comparable to liquid electrolytes, but fabrication challenges persist.
• Slurry processing of SEs can lead to detrimental reactions with polar solvents used in composite electrodes.

Purpose of the Study:

• To investigate an efficient infiltration process for SE slurry into composite LIB electrodes (NCM622).
• To develop a scalable, solution-based fabrication method for high-energy-density ASSBs.
• To overcome fabrication challenges associated with sulfide-based SEs and conventional electrode structures.

Main Methods:

• Studied SE slurry infiltration into NCM622 composite LIB electrodes using a scalable solution-based approach.
• Optimized processing temperatures above the boiling point of ethanol to facilitate SE molecule movement via convective flow during solvent vaporization.
• Utilized composite electrodes with mixed active material particle sizes to enhance pore filling and electrode density.

Main Results:

• Achieved efficient and even distribution of LPSCl SE within the porous electrode structures.
• Demonstrated improved initial discharge capacity of ASSBs to 177 mAh/g with LPSCl SE-infiltrated NCM622 electrodes.
• Showcased excellent ASSB performance at high electrode loading (17 mg/cm²), rivaling conventional LIBs.

Conclusions:

• The developed scalable solution-based infiltration method is effective for fabricating high-performance ASSBs.
• Optimized processing conditions enhance SE infiltration and electrode density, leading to superior electrochemical performance.
• This approach presents a viable pathway for producing competitive high-energy-density ASSBs for demanding applications.