Argyrodite Solid Electrolyte-Integrated Ni-Rich Oxide Cathode with Enhanced Interfacial Compatibility for...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• All-solid-state lithium batteries (ASSLBs) offer high energy and safety potential using argyrodite sulfide solid electrolytes.
• Scalable production of ASSLBs is hindered by poor interfacial contact between sulfide electrolytes and cathodes.
• Inferior interfaces impede large-scale commercialization of ASSLBs.

Purpose of the Study:

• To develop a scalable method for improving the interface between sulfide solid electrolytes and Ni-rich oxide cathodes in ASSLBs.
• To investigate the impact of conformal in situ integration on interfacial compatibility and electrochemical performance.
• To demonstrate a proof-of-concept for reliable interfacial design in high-performance ASSLBs.

Main Methods:

• Facile tape casting method for in situ integration of sulfide solid electrolyte onto Ni-rich oxide cathode.
• Fabrication of ASSLBs with integrated electrodes and segregated electrode structures for comparison.
• Electrochemical characterization including discharge capacity, cyclic stability, rate performance, and polarization analysis.

Main Results:

• Conformal in situ integration achieved intimate contact between sulfide electrolyte and Ni-rich cathode.
• Improved solid-solid interfacial compatibility and reduced interfacial reaction resistances were observed.
• ASSLBs with integrated electrodes showed superior discharge capacity, cyclic stability, and rate performance compared to segregated cells.
• Low polarization and fast reaction kinetics were attributed to the advanced interfacial contact.

Conclusions:

• The proposed tape casting method effectively creates a robust interface between sulfide electrolytes and Ni-rich cathodes.
• Enhanced interfacial contact is crucial for achieving high performance in ASSLBs.
• This work provides a viable fabrication strategy for high-performance ASSLBs with improved interfacial design.