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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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  This version of the article has been accepted for publication, after peer review (when applicable) and is subject to Springer Nature’s AM terms of use, but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online at: http://dx.doi.org/10.1007/s10008-024-05886-7

Keyword: All-solid-state battery, argyrodite, halogen-rich, high capacity, solid electrolyte

Date published: 2024-04-04

Publisher: Springer Science and Business Media LLC

Journal:

• Journal of Solid State Electrochemistry (ISSN: 14330768) p. 4409-4417

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Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5091

First published URL: https://doi.org/10.1007/s10008-024-05886-7

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Updated at: 2025-04-09 08:30:14 +0900

Published on MDR: 2025-04-08 21:53:58 +0900