Three-Dimensional High-Efficiency Superlithiophilic Interface Toward Air-Stable Garnet-Based All-Solid-State Lithium...

Area of Science:

• Materials Science
• Electrochemistry
• Solid-State Chemistry

Background:

• Garnet-type solid-state electrolytes like Li6.4La3Zr1.4Ta0.6O12 (LLZTO) show promise for all-solid-state lithium metal batteries (ASSLMBs).
• Poor air stability and uneven Li/LLZTO contact hinder ASSLMB development.

Purpose of the Study:

• To improve the air stability of LLZTO electrolytes.
• To create a stable and uniform lithium metal-LLZTO interface for high-performance ASSLMBs.

Main Methods:

• Fabrication of a porous LLZTO (PLLZTO) using sodium dodecyl benzene sulfonate (SDBS) and HNO3 etching.
• Construction of a 3D ionic conductor interface (LNO@PLLZTO) via in situ reaction with lithium, graphene oxide quantum dots, and LiNO3.
• Assembly and testing of ASSLMBs with a polyethylene oxide (PEO)-based functional layer.

Main Results:

• Enhanced air stability for PLLZTO (storage > 7 days).
• Achieved low interfacial impedance (4 Ω cm²) and high critical current density (1.5 mA cm⁻²) for Li|LNO@PLLZTO|Li.
• Demonstrated stable cycling for 3000 h at 0.2 mA cm⁻² and 92% capacity retention after 250 cycles at 1 C in assembled ASSLMBs.

Conclusions:

• The developed method significantly improves LLZTO air stability.
• An ultra-lithiophilic interface is achieved, crucial for high-performance ASSLMBs.
• This work provides a foundation for practical, high-performance ASSLMBs.