(De)lithiation mechanism of Li/SeSx (x = 0-7) batteries determined by in situ synchrotron x-ray diffraction and X-ray absorption spectroscopy

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

  • Yanjie Cui
  • Ali Abouimrane
  • Jun Lu
  • Trudy Bolin
  • Wei Weng
  • Chengjun Sun
  • Victor A. Maroni
  • Steve M. Heald
  • Khalil Amine

Detail(s)

Original languageEnglish
Pages (from-to)8047-8056
Journal / PublicationJournal of the American Chemical Society
Volume135
Issue number21
Publication statusPublished - 29 May 2013
Externally publishedYes

Abstract

Electrical energy storage for transportation has gone beyond the limit of converntional lithium ion batteries currently. New material or new battery system development is an alternative approach to achieve the goal of new high-energy storage system with energy densities 5 times or more greater. A series of SeSx-carbon (x = 0-7) composite materials has been prepared and evaluated as the positive electrodes in secondary lithium cells with ether-based electrolyte. In situ synchrotron high-energy X-ray diffraction was utilized to investigate the crystalline phase transition during cell cycling. Complementary, in situ Se K-edge X-ray absorption near edge structure analysis was used to track the evolution of the Se valence state for both crystalline and noncrystalline phases, including amorphous and electrolyte-dissolved phases in the (de)lithiation process. On the basis of these results, a mechanism for the (de)lithiation process is proposed, where Se is reduced to the polyselenides, Li2Sen (n ≥ 4), Li2Se2, and Li2Se sequentially during the lithiation and Li2Se is oxidized to Se through Li2Sen (n ≥ 4) during the delithiation. In addition, X-ray photoelectron spectroscopy and electrochemical impedance spectroscopy demonstrated the reversibility of the Li/Se system in ether-based electrolyte and the presence of side products in the carbonate-based electrolytes. For Li/SeS2 and Li/SeS7 cells, Li 2Se and Li2S are the discharged products with the presence of Se only as the crystalline phase in the end of charge. © 2013 American Chemical Society.

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Citation Format(s)

(De)lithiation mechanism of Li/SeSx (x = 0-7) batteries determined by in situ synchrotron x-ray diffraction and X-ray absorption spectroscopy. / Cui, Yanjie; Abouimrane, Ali; Lu, Jun et al.

In: Journal of the American Chemical Society, Vol. 135, No. 21, 29.05.2013, p. 8047-8056.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review