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Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries

Author

Listed:
  • Quan Pang

    (University of Waterloo
    Joint Center for Energy Storage Research (JCESR))

  • Abhinandan Shyamsunder

    (University of Waterloo
    Joint Center for Energy Storage Research (JCESR))

  • Badri Narayanan

    (Joint Center for Energy Storage Research (JCESR)
    Argonne National Laboratory)

  • Chun Yuen Kwok

    (University of Waterloo
    Joint Center for Energy Storage Research (JCESR))

  • Larry A. Curtiss

    (Joint Center for Energy Storage Research (JCESR)
    Argonne National Laboratory)

  • Linda F. Nazar

    (University of Waterloo
    Joint Center for Energy Storage Research (JCESR))

Abstract

The lithium–sulfur battery is promising as an alternative to conventional lithium-ion technology due to the high energy density of both sulfur and lithium metal electrodes. An extended lifetime has been demonstrated, but two notable challenges still exist to realize its full potential: to overcome the undesired high electrolyte/sulfur ratio required for the catholyte-type mechanism that governs most cell configurations, and to inhibit Li dendrite growth and its parasitic reaction with the electrolyte that results in cell degradation. Here, we demonstrate that by tuning the electrolyte structure, the challenges at both electrodes can be tackled simultaneously. Specifically, the sulfur speciation pathway transforms from a dissolution–precipitation route to a quasi-solid state conversion in the presence of a lowered solvent activity and an extended electrolyte network, curtailing the need for high electrolyte volumes. Ab initio calculations reveal the nature of the network structure. With such an optimized structure, the electrolyte allows dendrite-free Li plating and shows a 20-fold reduction in parasitic reactions with Li, which avoids electrolyte consumption and greatly extends the life time of a low electrolyte/sulfur (5 µl mg–1) sulfur cell.

Suggested Citation

  • Quan Pang & Abhinandan Shyamsunder & Badri Narayanan & Chun Yuen Kwok & Larry A. Curtiss & Linda F. Nazar, 2018. "Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries," Nature Energy, Nature, vol. 3(9), pages 783-791, September.
  • Handle: RePEc:nat:natene:v:3:y:2018:i:9:d:10.1038_s41560-018-0214-0
    DOI: 10.1038/s41560-018-0214-0
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    Cited by:

    1. Ziyang Lu & Huijun Yang & Jianming Sun & Jun Okagaki & Yoongkee Choe & Eunjoo Yoo, 2024. "Conformational isomerism breaks the electrolyte solubility limit and stabilizes 4.9 V Ni-rich layered cathodes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Zheng Li & Harsha Rao & Rasha Atwi & Bhuvaneswari M. Sivakumar & Bharat Gwalani & Scott Gray & Kee Sung Han & Thomas A. Everett & Tanvi A. Ajantiwalay & Vijayakumar Murugesan & Nav Nidhi Rajput & Vila, 2023. "Non-polar ether-based electrolyte solutions for stable high-voltage non-aqueous lithium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    3. Chao Ye & Huan Li & Yujie Chen & Junnan Hao & Jiahao Liu & Jieqiong Shan & Shi-Zhang Qiao, 2024. "The role of electrocatalytic materials for developing post-lithium metal||sulfur batteries," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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