Abstract
All-solid-state lithium-ion batteries are a promising next-generation technology because they have higher energy densities than their liquid-electrolyte counterparts. Halogen-rich argyrodite, specifically Li5.4(PS4)(S0.4Cl1.0Br0.6), was recently shown to have higher ionic conductivities compared with those of other argyrodite-like sulfides. Although the Li5.4(PS4)(S0.4Cl1.0Br0.6) in Li | Li5.4(PS4)(S0.4Cl1.0Br0.6) | Li(Ni0.8Co0.1Mn0.1)O2–Li5.4(PS4)(S0.4Cl1.0Br0.6) batteries have shown good electrochemical stability, the low discharge capacity limits the application of the battery. In continuation, this study examined the potential of a carbon additive for altering the electronic conductivity of the cathode and enhancing the capacity of Li | Li5.4(PS4)(S0.4Cl1.0Br0.6) | Li(Ni0.8Co0.1Mn0.1)O2–Li5.4(PS4)(S0.4Cl1.0Br0.6) batteries. After a 50-cycle charge/discharge, the carbon additive (0.1 C) enhanced the discharge capacity from 3.1 to 167 mAh/g, resulted in a capacity retention rate and coulombic efficiency of 95.4% and 99.9% when using 0.1 C and 0.5 C, respectively, and increased the resistance of the battery from 53 to 56 Ω. Therefore, the all-solid-state battery employing high-ion-conductive Li5.4(PS4)(S0.4Cl1.0Br0.6) and a carbon-modified cathode showed improved capacity. This study provides a proven framework for developing all-solid-state batteries employing halogen-rich argyrodite (Li7-α(PS4)(S2-αXα); α > 1) with enhanced ionic conductivities.
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Naoya Masuda performed all syntheses, electrochemical measurements, and analyses. The paper was written by Naoya Masuda and Kiyoshi Kobayashi with input from Futoshi Utsuno and Naoaki Kuwata.
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Masuda, N., Kobayashi, K., Utsuno, F. et al. Enhanced capacity of all-solid-state battery comprising LiNbO3-coated Li(Ni0.8Co0.1Mn0.1)O2 Cathode, Li5.4(PS4)(S0.4Cl1.0Br0.6) solid electrolyte and lithium metal anode. J Solid State Electrochem (2024). https://doi.org/10.1007/s10008-024-05886-7
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DOI: https://doi.org/10.1007/s10008-024-05886-7