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Mechanism for the Stable Performance of Sulfur-Copolymer Cathode in Lithium–Sulfur Battery Studied by Solid-State NMR Spectroscopy

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    Mechanism for the Stable Performance of Sulfur-Copolymer Cathode in Lithium–Sulfur Battery Studied by Solid-State NMR Spectroscopy
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    • Alexander Hoefling
      Alexander Hoefling
      Department of Chemistry, Institute for Technical and Macromolecular Chemistry, University of Hamburg, Bundesstrasse 45, 20146 Hamburg, Germany
      More by Alexander Hoefling
    • Dan Thien Nguyen
      Dan Thien Nguyen
      Department of Chemical Engineering and Applied Chemistry, Chungnam National University, Daejeon 34134, Republic of Korea
      More by Dan Thien Nguyen
    • Pouya Partovi-Azar
      Pouya Partovi-Azar
      Institute of Chemistry, Martin-Luther-University Halle-Wittenberg, Von-Danckelmann-Platz 4, 06120 Halle (Saale), Germany
      More by Pouya Partovi-Azar
    • Daniel Sebastiani
      Daniel Sebastiani
      Institute of Chemistry, Martin-Luther-University Halle-Wittenberg, Von-Danckelmann-Platz 4, 06120 Halle (Saale), Germany
      More by Daniel Sebastiani
      Orcidhttp://orcid.org/0000-0003-2240-3938
    • Patrick Theato
      Patrick Theato
      Department of Chemistry, Institute for Technical and Macromolecular Chemistry, University of Hamburg, Bundesstrasse 45, 20146 Hamburg, Germany
      More by Patrick Theato
      Orcidhttp://orcid.org/0000-0002-4562-9254
    • Seung-Wan Song*
      Seung-Wan Song
      Department of Chemical Engineering and Applied Chemistry, Chungnam National University, Daejeon 34134, Republic of Korea
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0003-4208-206X
    • Young Joo Lee*
      Young Joo Lee
      Department of Chemistry, Institute of Inorganic and Applied Chemistry, University of Hamburg, Martin-Luther-King-Platz 6, 20146 Hamburg, Germany
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0002-5782-6431
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    Chemistry of Materials

    Cite this: Chem. Mater. 2018, 30, 9, 2915–2923
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    https://doi.org/10.1021/acs.chemmater.7b05105
    Published April 12, 2018
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    Abstract

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    Rechargeable lithium–sulfur (Li–S) batteries have drawn significant attention as next-generation energy storage systems. Sulfur-copolymers are promising alternative cathode materials to elemental sulfur in Li–S batteries as they provide high reversible capacity. However, the redox mechanisms of these materials are not well understood owing to the difficulty in characterizing amorphous structures and identifying individual ionic species. Here, we use solid-state NMR techniques together with electrochemistry experiments and quantum calculations to investigate the structural evolution of the prototype S-copolymer cathodes, sulfur–diisopropenylbenzene copolymers (poly(S-co-DIB)), during cycling. We demonstrate that polysulfides with different chain lengths can be distinguished by 13C and 7Li NMR spectroscopy, revealing that the structure of the copolymers can be tuned in terms of polysulfide chain lengths and resulting reaction pathways during electrochemical cycling. Our results show that the improved cyclability of these cathodes originates from the role of organic moieties acting as anchors that fixate polysulfides to the polymeric network during cycling, thus preventing their diffusion into the electrolyte. We provide a new methodological concept for the mechanistic studies to track the intermediate species and phase transition in Li–S batteries.

    Copyright © 2018 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.7b05105.

    • Deconvolution of 13C{1H} CP MAS NMR spectra of poly(S-co-DIB) copolymers, T1(13C) relaxation time, first-principles calculations of the systems bound to two polysulfide chains, solubility test, battery optimization procedure, deconvolution of 13C{1H} CP MAS NMR spectra of S-DIB-50 and S-DIB-10 cathodes at various SOD, 13C{1H} CP MAS NMR spectra of the electrodes after the washing step, and ex situ X-ray photoelectron spectroscopy (XPS) (PDF)

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    Cited By

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    This article is cited by 63 publications.

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    Cite this: Chem. Mater. 2018, 30, 9, 2915–2923
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.7b05105
    Published April 12, 2018
    Copyright © 2018 American Chemical Society
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