High Energy Density Solid‐State Lithium Metal Batteries Enabled by In Situ Polymerized Integrated Ultrathin Solid Electrolyte/Cathode

Abstract

Solid‐state batteries (SSBs) are regarded as the most promising next‐generation energy storage devices due to their potential to achieve higher safety performance and energy density. However, the troubles in the preparation of ultrathin solid‐state electrolytes (SEs) as well as the resultant compromise in mechanical strength greatly limit the safety application of SSBs. Herein, a novel in situ polymerized integrated ultrathin SE/cathode design is developed. The ultrathin ceramic layer supported on the cathode serves not only as a rigid scaffold to prevent direct contact between the cathode and anode but also as active inorganic fillers to enhance the mechanical properties of in situ polymerized SE film. The unique Li‐ion coordination environments as well as the Li hopping mechanism profoundly promote fast ion transport in composite SEs. The in situ polymerized SEs simultaneously achieve the balance in ultrathin thickness (10 µm), fast ion transport (0.65 mS cm−1), superior Young's modulus (66.8 GPa), and excellent interface contact. The pouch cells with practical Li||LiNi0.8Co0.1Mn0.1O2 configuration achieve an ultrahigh volumetric energy density of 1018 Wh L−1 and safety performance. The in situ polymerized integrated ultrathin SE/cathode design exhibits great promise for the practical application of SSBs with high energy density and safety performance.

Development of 2D Framework Structures-Based Solid-State Electrolytes with Fast Ion-Transport Channels Using Ionic Liquids Encapsulated in 2D-LiMNT Frameworks

“…With higher energy density and excellent cycle life compared to other energy storage devices, lithium-ion secondary batteries are playing an increasingly important role in electronic digital products and new energy vehicle systems. − However, conventional lithium-ion secondary batteries contain a large amount of flammable organic liquid electrolytes, which is prone to safety issues; meanwhile, their energy density is close to the theoretical upper limit. , Solid-state lithium metal batteries (SSLMBs) are considered the most promising next-generation energy storage batteries because of their use of a high-energy-density lithium metal anode instead of a conventional graphite anode and solid-state electrolytes (SSEs) that suppress lithium dendrites instead of conventional separators and flammable liquid electrolytes and improve safety. − …”