Constructing Superionic Heterointerface via Multiphase Engineering to Achieve Stable Oxyhalide-Based All-Solid-State...

Area of Science:

• Materials Science
• Electrochemistry
• Solid-State Chemistry

Background:

• Amorphous oxyhalides are attractive solid-state electrolytes (SSEs) for all-solid-state batteries (ASSBs) due to their stability and deformability.
• However, their practical application is limited by low room-temperature ionic conductivity and interfacial reactions with cathodes.

Purpose of the Study:

• To enhance Li+ transport and interfacial stability in amorphous lithium oxyhalides for ASSBs.
• To investigate the effect of incorporating ZrB2 and ZrN on the properties of amorphous Li2O-ZrCl4 (LZCO) matrix.

Main Methods:

• A facile multiphase regulation strategy was employed by incorporating ZrB2 and ZrN into an amorphous 1.3Li2O-ZrCl4 (LZCO) matrix.
• The resulting composite material (LZCOBN0.1) was characterized for its ionic conductivity and electrochemical performance in ASSBs.

Main Results:

• The incorporation of ZrB2 and ZrN created superionic heterointerfaces and a more continuous Li+ conduction network, increasing ionic conductivity to 2.41 mS cm-1.
• ASSBs utilizing LZCOBN0.1 exhibited a high initial capacity (210 mAh g-1) and excellent cycling stability, retaining 82.7% capacity after 2000 cycles.
• The multiphase architecture mitigated interfacial side reactions and improved interface compatibility.

Conclusions:

• Phase engineering via multiphase regulation is a viable strategy for developing high-performance amorphous oxyhalide-based SSEs.
• The developed LZCOBN0.1 composite demonstrates significant potential for practical ASSB applications.