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

Here, 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. Extended life time has been demonstrated, but two notable challenges still exist in battery applications: overcoming the undesired high electrolyte/sulfur ratio, and inhibiting Li dendrite growth and its parasitic reaction with the electrolyte. Here we demonstrate that by tuning the electrolyte structure, the challenges at both electrodes can be tackled simultaneously. The sulfur speciation pathway transforms from a dissolution-precipitation route to a quasi-solid-state conversion in the presence of lowered solvent activity and an extended electrolyte network structure as revealed by ab initio calculations, curtailing the need for high electrolyte volumes. With such an optimized structure, the Li plates dendrite-free and shows 20-fold reduction in parasitic reactions with Li, avoiding electrolyte consumption and greatly extending the life time of a low E/S (5 µl/mg -1) sulfur cell.
Authors:
ORCiD logo [1] ;  [1] ;  [2] ; ORCiD logo [1] ;  [2] ; ORCiD logo [1]
  1. Univ. of Waterloo, Waterloo, ON (Canada); Joint Center for Energy Storage Research (JCESR), Argonne, IL (United States)
  2. Joint Center for Energy Storage Research (JCESR), Argonne, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Joint Center for Energy Storage Research (JCESR); Natural Sciences and Engineering Research Council of Canada (NSERC)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1472132

Pang, Quan, Shyamsunder, Abhinandan, Narayanan, Badri, Kwok, Chun Yuen, Curtiss, Larry A., and Nazar, Linda F.. Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries. United States: N. p., Web. doi:10.1038/s41560-018-0214-0.
Pang, Quan, Shyamsunder, Abhinandan, Narayanan, Badri, Kwok, Chun Yuen, Curtiss, Larry A., & Nazar, Linda F.. Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries. United States. doi:10.1038/s41560-018-0214-0.
Pang, Quan, Shyamsunder, Abhinandan, Narayanan, Badri, Kwok, Chun Yuen, Curtiss, Larry A., and Nazar, Linda F.. 2018. "Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries". United States. doi:10.1038/s41560-018-0214-0.
@article{osti_1472132,
title = {Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries},
author = {Pang, Quan and Shyamsunder, Abhinandan and Narayanan, Badri and Kwok, Chun Yuen and Curtiss, Larry A. and Nazar, Linda F.},
abstractNote = {Here, 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. Extended life time has been demonstrated, but two notable challenges still exist in battery applications: overcoming the undesired high electrolyte/sulfur ratio, and inhibiting Li dendrite growth and its parasitic reaction with the electrolyte. Here we demonstrate that by tuning the electrolyte structure, the challenges at both electrodes can be tackled simultaneously. The sulfur speciation pathway transforms from a dissolution-precipitation route to a quasi-solid-state conversion in the presence of lowered solvent activity and an extended electrolyte network structure as revealed by ab initio calculations, curtailing the need for high electrolyte volumes. With such an optimized structure, the Li plates dendrite-free and shows 20-fold reduction in parasitic reactions with Li, avoiding electrolyte consumption and greatly extending the life time of a low E/S (5 µl/mg-1) sulfur cell.},
doi = {10.1038/s41560-018-0214-0},
journal = {Nature Energy},
number = 9,
volume = 3,
place = {United States},
year = {2018},
month = {8}
}

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