Molybdenum polysulfide chalcogels as high-capacity, anion-redox-driven electrode materials for Li-ion batteries

Vicky V.T. Doan-Nguyen, Kota S. Subrahmanyam, Megan M. Butala, Jeffrey A. Gerbec, Saiful M. Islam, Katherine N. Kanipe, Catrina E. Wilson, Mahalingam Balasubramanian, Kamila M. Wiaderek, Olaf J. Borkiewicz, Karena W. Chapman, Peter J. Chupas, Martin Moskovits, Bruce S. Dunn, Mercouri G. Kanatzidis, Ram Seshadri

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35 Citations (Scopus)

Abstract

Sulfur cathodes in conversion reaction batteries offer high gravimetric capacity but suffer from parasitic polysulfide shuttling. We demonstrate here that transition metal chalcogels of approximate formula MoS3.4 achieve a high gravimetric capacity close to 600 mAh g-1 (close to 1000 mAh g-1 on a sulfur basis) as electrode materials for lithium-ion batteries. Transition metal chalcogels are amorphous and comprise polysulfide chains connected by inorganic linkers. The linkers appear to act as a "glue" in the electrode to prevent polysulfide shuttling. The Mo chalcogels function as electrodes in carbonate- and ether-based electrolytes, which further provides evidence of polysulfide solubility not being a limiting issue. We employ X-ray spectroscopy and operando pair distribution function techniques to elucidate the structural evolution of the electrode. Raman and X-ray photoelectron spectroscopy track the chemical moieties that arise during the anion-redox-driven processes. We find the redox state of Mo remains unchanged across the electrochemical cycling and, correspondingly, the redox is anion-driven.

Original languageEnglish
Pages (from-to)8357-8365
Number of pages9
JournalChemistry of Materials
Volume28
Issue number22
DOIs
Publication statusPublished - Nov 22 2016

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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    Doan-Nguyen, V. V. T., Subrahmanyam, K. S., Butala, M. M., Gerbec, J. A., Islam, S. M., Kanipe, K. N., Wilson, C. E., Balasubramanian, M., Wiaderek, K. M., Borkiewicz, O. J., Chapman, K. W., Chupas, P. J., Moskovits, M., Dunn, B. S., Kanatzidis, M. G., & Seshadri, R. (2016). Molybdenum polysulfide chalcogels as high-capacity, anion-redox-driven electrode materials for Li-ion batteries. Chemistry of Materials, 28(22), 8357-8365. https://doi.org/10.1021/acs.chemmater.6b03656