Modeling assisted synthesis of Zr-doped Li3-xIn1-xZrxCl6 with ultrahigh ionic conductivity for lithium-ion batteries

All-solid-state lithium-ion batteries (ASSLBs) are an important milestone for the future of energy storage because of their capability of impressive energy density and outstanding safety. However, oxide and sulfide solid-state electrolytes (SSEs) suffer from either low ionic conductivity or poor chemical stability. In contrast, halide-based SSEs, are promising as candidate materials owing to high conductivity, good stability, and broad cathode compatibility. Though element doping of the SSEs is an effective and common approach to further improve their electrochemical properties, dopant exploration and optimization through solely experimental trials are both costly and time-consuming. For this aspect, computational simulations for dopant element and concentration screening are adopted in this research and zirconium is selected as a suitable dopant for Li3InCl6. The synthesized Li2.75In0.75Zr0.25Cl6 exhibited Li ionic conductivity of 5.82 x 10(-3) S cm(-1) at room temperature, which is the highest among reported halide SSEs. The ASSLB formed with Li2CoO2-Li2.75In0.75Zr0.25Cl6-Li/In delivers a high initial capacity of 129.3 mAh center dot g(-1). Conclusively, this work provides an effective approach which combines computational modeling and experimental verification for the development of halide SSEs with improved stability and conductivity. The successful design approach and compelling results provide further possibilities and capabilities in future SSE research.

Automated summary

All-solid-state lithium-ion batteries (ASSLBs) are considered crucial for future energy storage due to their high energy density and exceptional safety. However, current solid-state electrolytes (SSEs), such as oxides and sulfides, suffer from limited ionic conductivity or chemical stability. In contrast, halide-based SSEs show promise as they possess high conductivity, stability, and compatibility with cathode materials. This research utilizes computational simulations and experimental verification to identify zirconium as a suitable dopant for Li3InCl6, resulting in the highest reported ionic conductivity among halide SSEs at 5.82 x 10(-3) S cm(-1) at room temperature. The synthesized Li2.75In0.75Zr0.25Cl6 is then used in an ASSLB, which exhibits a high initial capacity of 129.3 mAh center dot g(-1). Overall, this work showcases an effective approach for the development of halide SSEs with improved stability and conductivity through the integration of computational modeling and experimental validation.