Ionic transport properties of lithium polysulfides within poly(ethylene-oxide) homopolymer electrolytes - Archive ouverte HAL
Article Dans Une Revue Electrochimica Acta Année : 2024

Ionic transport properties of lithium polysulfides within poly(ethylene-oxide) homopolymer electrolytes

Résumé

Lithium-sulfur (Li-S) batteries are attractive due to their high theoretical specific energy density, nonetheless, their upscaling and widespread adaptation have been hampered by issues such as the dissolution and shuttling of lithium polysulfides species (Li$_2$S$_x$, 2 ≤x ≤8) from the positive electrode through the electrolyte to the negative electrode. The electrolyte medium is thus a decisive factor in tackling the lithium polysulfide shuttle mechanism. In this study, the thermodynamical, structural, and ionic transport properties of Li$_2$S$_x$ within poly(ethylene-oxide), PEO, a solid-polymer electrolyte that can potentially be used in all-solid-state Li-S batteries have been investigated. Results from thermodynamical, infrared spectroscopy and XRD characterizations show that Li$_2$S$_8$ solubilizes better in PEO homopolymer compared to Li$_2$S$_4$ salt. In terms of ionic transport properties, the diffusion measurements via electrochemical methodologies also demonstrate that PEO can slow down the shuttling speed of S$_8$$^2$$^−$ and S$_4$$^2$$^−$ by almost two orders of magnitude compared to a conventional liquid electrolyte such as DOL/DME. Long-chain polysulfides in PEO homopolymer show more pronounced shuttling than the short-chain polysulfide. These findings may guide the design of adapted solid polymer electrolytes that can be used as binders or electrolyte separators for all-solid-state Li-S batteries.
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hal-04546068 , version 1 (15-04-2024)

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Ernest Ahiavi, Priscillia Soudant, Didier Devaux, Renaud Bouchet. Ionic transport properties of lithium polysulfides within poly(ethylene-oxide) homopolymer electrolytes. Electrochimica Acta, 2024, 488, pp.144202. ⟨10.1016/j.electacta.2024.144202⟩. ⟨hal-04546068⟩
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