Solid-State Lithium Metal Battery of Low Capacity Fade Enabled by a Composite Electrolyte with Sulfur-Containing Oligomers

A solid-state lithium metal battery of low capacity fade is acquired using the electrolyte membrane of a polyurethane-acrylate-thiocarbonate (PUAT) oligomer, macromolecules, lithium salt, and an oxide additive. Two types of composite electrolytes have been prepared: the free-standing electrolyte (PUAT-FS) and the electrode-coated electrolyte (PUAT-EC). Featuring a less PUAT content and a finer granular size, PUAT-FS is less ion-conductive than PUAT-EC; 0.44 mS cm^-1 in contrast to 0.51 mS cm^-1 at room temperature. Nonetheless, the lithium iron phosphate battery of PUAT-FS is far superior to that of PUAT-EC in terms of cycling stability. When cycled at 0.1C and room temperature, the PUAT-FS battery reaches a maximum discharge capacity of 169.7 mAh g^-1 at its 20th cycle and decreases to 141.0 mAh g^-1 at the 500th cycle, 83.1% retention. The capacity fading rate of the PUAT-FS battery is 0.034% per cycle at 0.1C, significantly less than that of the PUAT-EC battery, 0.138% per cycle. Other maximum capacities and fading rates of the PUAT-FS battery are 152.5 mAh g^-1 and 0.050% per cycle at 0.2C in 800 cycles and 126.1 mAh g^-1 and 0.051% per cycle at 0.5C in 1000 cycles. These features of a low fading rate and high capacity are attributed to a balanced ratio of oligomer to macromolecule (1:1 w/w) in the free-standing electrolyte and the sulfur-containing oligomer.