Li₇La₃Zr₂O₁₂ sheet-based framework for high-performance lithium–sulfur hybrid quasi-solid battery

Applications of lithium batteries are challenged by their unsatisfactory safety profiles. Solid-state batteries present a very promising solution to overcome the safety issues, but their performance requires major improvement. Hybrid quasi-solid electrolyte (HQSE), comprising solid and liquid components, has emerged as a practical compromise for safer and high-performance Li batteries. Li–S system is one of the most promising Li battery candidates; however, the performance of Li–S hybrid quasi-solid battery still needs to be further enhanced. Herein, a new HQSE design comprising Li₇La₃Zr₂O₁₂ sheet-based solid framework imbibed with liquid electrolyte is applied to Li–S battery. The liquid-infused 3D architecture allows fast Li ion mobility and low interfacial resistance. It is also compatible with Li metal, highly processable, unleakable, and thermally stable. These attributes result in a high-performance Li–S hybrid quasi-solid system with a very good safety profile. The novel HQSE design also demonstrates improved anodic stability, which is very promising for high-voltage cathodes. The excellent performance, enhanced safety, and broad applicability of our sheet-based LLZO HQSE set the path for applications in other types of Li batteries to achieve both safe and high-performance energy storage systems.