In-Situ Polymerization in 3D Ceramic Frameworks for High-Performance Composite Solid Electrolytes

Abstract

In the Battery of Things era, lithium-ion batteries (LIBs) act as the heart of any electronic device, from tiny devices such as earphones and smart pens to electric vehicles (EVs). Unfortunately, current safety issue associated with conventional LIBs originates from the use of flammable liquid electrolytes. Therefore, solid-state batteries (SSBs) using solid-state electrolytes (SSEs) as a potential candidate can address the safety concerns and revive the lithium metal to further increase the energy density of batteries. Among several types of SSEs such as ceramic electrolytes, solid polymer electrolytes, and composite solid electrolytes (CSEs), CSEs are more attractive by combining the advantages of both ceramic and polymer electrolytes. However, CSEs still suffer from insufficient ionic conductivity at room temperature to meet the requirement for high-performance electrolytes. In this study, 3D ceramic porous framework as a continuous lithium-ion conduction pathway as well as a backbone for in-situ polymer penetration was prepared to overcome the challenge. The synergistic effect of the 3D continuous framework, well-organized polymer, and their interphase enabled high-performance SSEs. A solid-state lithium-ion cell composed of 3D-Li6.4La3Zr1.4Ta0.6O12 containing CSE, LiNi0.8Co0.1Mn0.1O2 cathode, and Li metal anode, could operate for 230 cycles by maintaining a high capacity of 118.8 mAh g-1, and showed good rate capability up to 5 C at 30 °C. In addition, a solid-state sodium ion cell composed of 3D-Na3.3Zr1.7La0.3(SiO4)2(PO4) containing CSE, Na3Mg0.05V1.95(PO4)3@C cathode, and Na metal anode achieved a long lifespan of 3000 cycles at 2 C with zero fading and excellent rate capability up to 10 C at 30 °C.