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Lithium/Sulfur Cell Discharge Mechanism: An Original Approach for Intermediate Species Identification

Barchasz, Céline ; Molton, Florian ; Duboc, Carole ; Leprêtre, Jean-Claude ; Patoux, Sébastien ; Alloin, Fannie

Analytical chemistry (Washington), 2012-05, Vol.84 (9), p.3973-3980 [Periódico revisado por pares]

Washington, DC: American Chemical Society

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  • Título:
    Lithium/Sulfur Cell Discharge Mechanism: An Original Approach for Intermediate Species Identification
  • Autor: Barchasz, Céline ; Molton, Florian ; Duboc, Carole ; Leprêtre, Jean-Claude ; Patoux, Sébastien ; Alloin, Fannie
  • Assuntos: Analytical chemistry ; Chemical precipitation ; Chemical Sciences ; Chemistry ; Chromatographic methods and physical methods associated with chromatography ; Chromatography ; Electrochemical methods ; Electrodes ; Electrolytes ; Exact sciences and technology ; Other chromatographic methods ; Spectrometric and optical methods ; Ultraviolet radiation
  • É parte de: Analytical chemistry (Washington), 2012-05, Vol.84 (9), p.3973-3980
  • Notas: ObjectType-Article-1
    SourceType-Scholarly Journals-1
    ObjectType-Feature-2
    content type line 23
  • Descrição: The lithium/sulfur battery is a promising electrochemical system that has a high theoretical capacity of 1675 mAh g–1, but its discharge mechanism is well-known to be a complex multistep process. As the active material dissolves during cycling, this discharge mechanism was investigated through the electrolyte characterization. Using high-performance liquid chromatography, UV–visible absorption, and electron spin resonance spectroscopies, we investigated the electrolyte composition at different discharge potentials in a TEGDME-based electrolyte. In this study, we propose a possible mechanism for sulfur reduction consisting of three steps. Long polysulfide chains are produced during the first reduction step (2.4–2.2 V vs Li+/Li), such as S8 2– and S6 2–, as evidenced by UV and HPLC data. The S3 •– radical can also be found in solution because of a disproportionation reaction. S4 2– is produced during the second reduction step (2.15–2.1 V vs Li+/Li), thus pointing out the gradual decrease of the polysulfide chain lengths. Finally, short polysulfide species, such as S3 2–, S2 2–, and S2–, are produced at the end of the reduction process, i.e., between 2.1 and 1.9 V vs Li+/Li. The precipitation of the poorly soluble and insulating short polysulfide compounds was evidenced, thus leading to the positive electrode passivation and explaining the early end of discharge.
  • Editor: Washington, DC: American Chemical Society
  • Idioma: Inglês
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