12 μm-Thick Sintered Garnet Ceramic Skeleton Enabling High-Energy-Density Solid-State Lithium Metal Batteries

摘要

Ultrathin composite solid-state electrolytes (CSSEs) demonstrate greatpromise in high-energy-density solid-state batteries due to their ultrathinthickness and good adaptability to lithium metal anodes. However, uncontrolleddendrite growth and performance deterioration caused by the aggregationof inorganic powder restrict the practical application of ultrathin CSSEs.Herein, a flexible, self-supporting Li_(6.5)La_3Zr_(1.5)Ta_(0.5)O_(12) (LLZO) ceramic skeletonis prepared by the tape-casting method. Subsequently, a 12 μm-thick CSSEwith a 3D interconnection structure is achieved through in situ UV curing ofethoxylated trimethylolpropane triacrylate (ETPTA) in a ceramic skeleton (CSCSSE).This design includes a sintered LLZO ceramic, which can avoid theuneven distribution of the inorganic phase and regulate ion migration. Meanwhile,the cross-linked ETPTA polymer electrolyte contributes to lower interfacialimpedance. In addition, the continuous two-phase interface can also providea fast transmission channel for Li+. As a result, CS-CSSE demonstrates superiorLi+ transference number (0.83) and ionic conductivity (1.19 × 10-3 S cm~(-1)at 25℃. As-prepared LiLiNi_(0.83)Co_(0.12)Mn_(0.05)O_2 batteries exhibit high dischargespecific capacities of 185.4 mAh g~（-1） at 0.1 C and average coulombic efficiencygreater than 99. The pouch cells exhibit high energy densities of376 Wh Kg（-1） and 1186 Wh L~（-1）. This work provides new insights into theapplication of ceramics to high-energy-density solid-state batteries.