Salt Concentration Control of Polysulfide Dissolution, Diffusion, and Reactions in Lithium–Sulfur Battery Electrolytes
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| Title: | Salt Concentration Control of Polysulfide Dissolution, Diffusion, and Reactions in Lithium–Sulfur Battery Electrolytes |
|---|---|
| Authors: | Luong, Nguyen Ngoc Tan, 1995, Kottarathil, Aginmariya, 1998, Wieczorek, W, Johansson, Patrik, 1969 |
| Source: | Nästa generations batterier ACS Applied Energy Materials. 8(21):15830-15837 |
| Subject Terms: | polysulfides, Li−S, DFT, battery, operandoRaman spectroscopy, electrolytes |
| Description: | Lithium–sulfur (Li–S) batteries suffer from the dissolution of sulfur and polysulfide (PS) species in the electrolyte, leading to capacity loss, instability, and a shortened lifespan. While highly concentrated electrolytes have been explored to address this issue, the underlying mechanisms of S/PS dissolution and subsequent diffusion, particularly concerning the specific behavior of long- and short-chain PSs under varying states of charge (SOC), remain poorly understood. We here employ operando Raman spectroscopy to semiquantitatively monitor PS solubility and migration across a wide range of LiTFSI concentrations in DME:DOL (1:1, v/v). We find that both PS dianions (S 4–8 2– ) and trisulfur radicals (S 3 •– ) decrease at the lithium anode with increasing electrolyte salt concentration (0.3–7.0 m), indicating reduced solubility and slower transport. Notably, the concentration of S 3 •– decreases more rapidly than that of its parent PS S 6 2– , suggesting less favorable radical formation pathways in highly concentrated electrolytes, potentially due to Li–TFSI–PS adduct formation. These changes result from shifts in the local solvation structure at high salt concentration, thereby controlling the solubility, transport, and chemical pathways of polysulfides in the electrolyte. By providing the real-time dynamics of long- and short-chain PSs, this work advances the mechanistic understanding of PSs in order to provide valuable insight for further improvement of Li–S battery performance. |
| File Description: | electronic |
| Access URL: | https://research.chalmers.se/publication/549301 https://research.chalmers.se/publication/549301/file/549301_Fulltext.pdf |
| Database: | SwePub |
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| Items | – Name: Title Label: Title Group: Ti Data: Salt Concentration Control of Polysulfide Dissolution, Diffusion, and Reactions in Lithium–Sulfur Battery Electrolytes – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Luong%2C+Nguyen+Ngoc+Tan%22">Luong, Nguyen Ngoc Tan</searchLink>, 1995<br /><searchLink fieldCode="AR" term="%22Kottarathil%2C+Aginmariya%22">Kottarathil, Aginmariya</searchLink>, 1998<br /><searchLink fieldCode="AR" term="%22Wieczorek%2C+W%22">Wieczorek, W</searchLink><br /><searchLink fieldCode="AR" term="%22Johansson%2C+Patrik%22">Johansson, Patrik</searchLink>, 1969 – Name: TitleSource Label: Source Group: Src Data: <i>Nästa generations batterier ACS Applied Energy Materials</i>. 8(21):15830-15837 – Name: Subject Label: Subject Terms Group: Su Data: <searchLink fieldCode="DE" term="%22polysulfides%22">polysulfides</searchLink><br /><searchLink fieldCode="DE" term="%22Li−S%22">Li−S</searchLink><br /><searchLink fieldCode="DE" term="%22DFT%22">DFT</searchLink><br /><searchLink fieldCode="DE" term="%22battery%22">battery</searchLink><br /><searchLink fieldCode="DE" term="%22operandoRaman+spectroscopy%22">operandoRaman spectroscopy</searchLink><br /><searchLink fieldCode="DE" term="%22electrolytes%22">electrolytes</searchLink> – Name: Abstract Label: Description Group: Ab Data: Lithium–sulfur (Li–S) batteries suffer from the dissolution of sulfur and polysulfide (PS) species in the electrolyte, leading to capacity loss, instability, and a shortened lifespan. While highly concentrated electrolytes have been explored to address this issue, the underlying mechanisms of S/PS dissolution and subsequent diffusion, particularly concerning the specific behavior of long- and short-chain PSs under varying states of charge (SOC), remain poorly understood. We here employ operando Raman spectroscopy to semiquantitatively monitor PS solubility and migration across a wide range of LiTFSI concentrations in DME:DOL (1:1, v/v). We find that both PS dianions (S 4–8 2– ) and trisulfur radicals (S 3 •– ) decrease at the lithium anode with increasing electrolyte salt concentration (0.3–7.0 m), indicating reduced solubility and slower transport. Notably, the concentration of S 3 •– decreases more rapidly than that of its parent PS S 6 2– , suggesting less favorable radical formation pathways in highly concentrated electrolytes, potentially due to Li–TFSI–PS adduct formation. These changes result from shifts in the local solvation structure at high salt concentration, thereby controlling the solubility, transport, and chemical pathways of polysulfides in the electrolyte. By providing the real-time dynamics of long- and short-chain PSs, this work advances the mechanistic understanding of PSs in order to provide valuable insight for further improvement of Li–S battery performance. – Name: Format Label: File Description Group: SrcInfo Data: electronic – Name: URL Label: Access URL Group: URL Data: <link linkTarget="URL" linkTerm="https://research.chalmers.se/publication/549301" linkWindow="_blank">https://research.chalmers.se/publication/549301</link><br /><link linkTarget="URL" linkTerm="https://research.chalmers.se/publication/549301/file/549301_Fulltext.pdf" linkWindow="_blank">https://research.chalmers.se/publication/549301/file/549301_Fulltext.pdf</link> |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1021/acsaem.5c02378 Languages: – Text: English PhysicalDescription: Pagination: PageCount: 8 StartPage: 15830 Subjects: – SubjectFull: polysulfides Type: general – SubjectFull: Li−S Type: general – SubjectFull: DFT Type: general – SubjectFull: battery Type: general – SubjectFull: operandoRaman spectroscopy Type: general – SubjectFull: electrolytes Type: general Titles: – TitleFull: Salt Concentration Control of Polysulfide Dissolution, Diffusion, and Reactions in Lithium–Sulfur Battery Electrolytes Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Luong, Nguyen Ngoc Tan – PersonEntity: Name: NameFull: Kottarathil, Aginmariya – PersonEntity: Name: NameFull: Wieczorek, W – PersonEntity: Name: NameFull: Johansson, Patrik IsPartOfRelationships: – BibEntity: Dates: – D: 01 M: 01 Type: published Y: 2025 Identifiers: – Type: issn-print Value: 25740962 – Type: issn-locals Value: SWEPUB_FREE – Type: issn-locals Value: CTH_SWEPUB Numbering: – Type: volume Value: 8 – Type: issue Value: 21 Titles: – TitleFull: Nästa generations batterier ACS Applied Energy Materials Type: main |
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