Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based...

Area of Science:

• Materials Science
• Electrochemistry
• Battery Technology

Background:

• All-solid-state lithium metal batteries (ASSLMBs) offer enhanced safety and energy density over conventional Li-ion batteries.
• Interfacial reactions between solid-state electrolytes (SSEs) and Li metal anodes hinder ASSLMB stability and cycle life.
• Understanding these interfaces is crucial for designing effective interlayer materials, but direct observation is challenging.

Purpose of the Study:

• To develop a computational framework for identifying stable interlayer materials for ASSLMBs.
• To screen potential interlayer materials compatible with both lithium metal and solid-state electrolytes.
• To experimentally validate the performance of promising interlayer candidates.

Main Methods:

• Development of a database-supported high-throughput screening (DSHTS) framework.
• Utilizing first-principle simulations to predict material stability and compatibility.
• Experimental testing of identified interlayers in symmetric and full ASSLMB cells.

Main Results:

• The DSHTS framework identified Li3OCl as a promising interlayer material for Li3InCl6 SSEs.
• ASSLMBs with a Li3OCl interlayer demonstrated significantly improved cycling stability and capacity retention compared to conventional interlayers.
• A Li|Li3OCl|Li3InCl6|LiCoO2 full cell achieved 76.36% capacity retention after 1000 cycles, outperforming a control cell.

Conclusions:

• The developed DSHTS framework is effective for discovering stable and compatible interlayer materials for ASSLMBs.
• Li3OCl shows great potential as an interlayer to mitigate interfacial issues and enhance the performance of ASSLMBs.
• This approach accelerates the design of next-generation solid-state batteries.