Engineering a redox-active interface for highly reversible aluminum anode-based practical all-solid-state lithium...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Aluminum anodes are promising for all-solid-state lithium batteries (ASSLBs) due to high capacity.
• Practical application is limited by mechanochemical failure, sluggish kinetics, and low reversibility.

Purpose of the Study:

• To engineer a stable and efficient interface for aluminum anodes in ASSLBs.
• To overcome the limitations of aluminum anodes for practical battery applications.

Main Methods:

• Constructed a redox-active interface on Al anodes via electrochemical activation of Li5.4PS4.4Cl1.6 sulfide electrolyte.
• Utilized theoretical modeling to establish Li+ binding energy difference (ΔE) as a descriptor for interfacial stability.

Main Results:

• The engineered interface accelerated Li+ transport and enhanced interfacial stability.
• Aluminum anodes achieved near-theoretical capacity and exceptional reversibility.
• ASSLBs demonstrated over 1000 cycles under demanding conditions (low N/P ratio, high loading, high current density).

Conclusions:

• The redox-interface strategy significantly enhances the performance and stability of aluminum anodes in ASSLBs.
• This approach offers a viable pathway for cost-effective, high-energy-density ASSLBs.
• The study sets a new benchmark for practical ASSLB operations.