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Title: Effect of Electrolyte on High Sulfur Loading Li-S Batteries

Abstract

Practical lithium-sulfur batteries require high sulfur electrode loading and lean electrolyte designs, which entail more research efforts on the two cell-design parameters - sulfur loading and electrolyte/sulfur loading ratio (E/S). In this work, a systematic investigation is performed to understand the impact of these two variables over key Li-S cell performance parameters. It is demonstrated that Li-S cells’ power performance strongly depends on the E/S ratio, while both E/S ratio and sulfur loading significantly influence the cycle life of Li-S cells. Low E/S ratio and high sulfur loading both give rise to fast lithium anode corrosion, which induces fast capacity fade and Coulombic efficiency decay. Pre-passivation of the lithium anode with an ionic conductor Li3PO4 protection layer only improves the Coulombic efficiency retention at sulfur loading levels much lower than the practical threshold. Meanwhile, increasing the concentration of LiNO3 additive in the electrolyte is found effective in sustaining the cycling capacity and the Coulombic efficiency over a reasonable usage window (~200 cycles). In conclusion, the role of LiNO3 is the protection of lithium anode during cycling.

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [4];  [5]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Univ. of Florida, Gainesville, FL (United States)
  3. Columbia Univ., New York, NY (United States)
  4. Stony Brook Univ., Stony Brook, NY (United States)
  5. Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1460834
Report Number(s):
BNL-207854-2018-JAAM
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 165; Journal Issue: 2; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Sun, Ke, Matarasso, Avi K., Epler, Ruby M., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Gan, Hong. Effect of Electrolyte on High Sulfur Loading Li-S Batteries. United States: N. p., 2018. Web. doi:10.1149/2.0071803jes.
Sun, Ke, Matarasso, Avi K., Epler, Ruby M., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., & Gan, Hong. Effect of Electrolyte on High Sulfur Loading Li-S Batteries. United States. doi:10.1149/2.0071803jes.
Sun, Ke, Matarasso, Avi K., Epler, Ruby M., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Gan, Hong. Tue . "Effect of Electrolyte on High Sulfur Loading Li-S Batteries". United States. doi:10.1149/2.0071803jes. https://www.osti.gov/servlets/purl/1460834.
@article{osti_1460834,
title = {Effect of Electrolyte on High Sulfur Loading Li-S Batteries},
author = {Sun, Ke and Matarasso, Avi K. and Epler, Ruby M. and Tong, Xiao and Su, Dong and Marschilok, Amy C. and Takeuchi, Kenneth J. and Takeuchi, Esther S. and Gan, Hong},
abstractNote = {Practical lithium-sulfur batteries require high sulfur electrode loading and lean electrolyte designs, which entail more research efforts on the two cell-design parameters - sulfur loading and electrolyte/sulfur loading ratio (E/S). In this work, a systematic investigation is performed to understand the impact of these two variables over key Li-S cell performance parameters. It is demonstrated that Li-S cells’ power performance strongly depends on the E/S ratio, while both E/S ratio and sulfur loading significantly influence the cycle life of Li-S cells. Low E/S ratio and high sulfur loading both give rise to fast lithium anode corrosion, which induces fast capacity fade and Coulombic efficiency decay. Pre-passivation of the lithium anode with an ionic conductor Li3PO4 protection layer only improves the Coulombic efficiency retention at sulfur loading levels much lower than the practical threshold. Meanwhile, increasing the concentration of LiNO3 additive in the electrolyte is found effective in sustaining the cycling capacity and the Coulombic efficiency over a reasonable usage window (~200 cycles). In conclusion, the role of LiNO3 is the protection of lithium anode during cycling.},
doi = {10.1149/2.0071803jes},
journal = {Journal of the Electrochemical Society},
number = 2,
volume = 165,
place = {United States},
year = {2018},
month = {2}
}

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Works referenced in this record:

A graphene foam electrode with high sulfur loading for flexible and high energy Li-S batteries
journal, January 2015


Critical Link between Materials Chemistry and Cell-Level Design for High Energy Density and Low Cost Lithium-Sulfur Transportation Battery
journal, January 2015

  • Eroglu, Damla; Zavadil, Kevin R.; Gallagher, Kevin G.
  • Journal of The Electrochemical Society, Vol. 162, Issue 6
  • DOI: 10.1149/2.0611506jes

Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium–Sulfur Battery Cathode Material with High Capacity and Cycling Stability
journal, July 2011

  • Wang, Hailiang; Yang, Yuan; Liang, Yongye
  • Nano Letters, Vol. 11, Issue 7, p. 2644-2647
  • DOI: 10.1021/nl200658a

A potential pyrrhotite (Fe 7 S 8 ) anode material for lithium storage
journal, January 2015

  • Zhang, Kailong; Zhang, Tingwei; Liang, Jianwen
  • RSC Advances, Vol. 5, Issue 19
  • DOI: 10.1039/C4RA14819C

Interaction of TiS 2 and Sulfur in Li-S Battery System
journal, January 2017

  • Sun, Ke; Zhang, Qing; Bock, David C.
  • Journal of The Electrochemical Society, Vol. 164, Issue 6
  • DOI: 10.1149/2.1631706jes

Li metal coated with amorphous Li3PO4 via magnetron sputtering for stable and long-cycle life lithium metal batteries
journal, February 2017


Liquid electrolyte lithium/sulfur battery: Fundamental chemistry, problems, and solutions
journal, June 2013


Rechargeable Lithium–Sulfur Batteries
journal, July 2014

  • Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
  • Chemical Reviews, Vol. 114, Issue 23
  • DOI: 10.1021/cr500062v

Role of LiNO3 in rechargeable lithium/sulfur battery
journal, May 2012


Lithium-Sulfur Cells: The Gap between the State-of-the-Art and the Requirements for High Energy Battery Cells
journal, April 2015

  • Hagen, Markus; Hanselmann, Dominik; Ahlbrecht, Katharina
  • Advanced Energy Materials, Vol. 5, Issue 16, 1401986
  • DOI: 10.1002/aenm.201401986

Sulfur-Impregnated Activated Carbon Fiber Cloth as a Binder-Free Cathode for Rechargeable Li-S Batteries
journal, November 2011

  • Elazari, Ran; Salitra, Gregory; Garsuch, Arnd
  • Advanced Materials, Vol. 23, Issue 47, p. 5641-5644
  • DOI: 10.1002/adma.201103274

Improving Lithium–Sulfur Battery Performance under Lean Electrolyte through Nanoscale Confinement in Soft Swellable Gels
journal, April 2017


Strategies of constructing stable and high sulfur loading cathodes based on the blade-casting technique
journal, January 2017

  • Zeng, Fanglei; Wang, Anbang; Wang, Weikun
  • Journal of Materials Chemistry A, Vol. 5, Issue 25
  • DOI: 10.1039/C7TA01675A

Li–O2 and Li–S batteries with high energy storage
journal, January 2012

  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191

Effect of Carbon and Binder on High Sulfur Loading Electrode for Li-S Battery Technology
journal, May 2017


High-Energy-Density Lithium–Sulfur Batteries Based on Blade-Cast Pure Sulfur Electrodes
journal, April 2016


Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes
journal, September 2016


Cell energy density and electrolyte/sulfur ratio in Li–S cells
journal, October 2014


How to Obtain Reproducible Results for Lithium Sulfur Batteries?
journal, January 2013

  • Zheng, Jianming; Lv, Dongping; Gu, Meng
  • Journal of The Electrochemical Society, Vol. 160, Issue 11
  • DOI: 10.1149/2.106311jes

Sulfur-Impregnated Disordered Carbon Nanotubes Cathode for Lithium–Sulfur Batteries
journal, October 2011

  • Guo, Juchen; Xu, Yunhua; Wang, Chunsheng
  • Nano Letters, Vol. 11, Issue 10, p. 4288-4294
  • DOI: 10.1021/nl202297p

High Energy Density Lithium-Sulfur Batteries: Challenges of Thick Sulfur Cathodes
journal, March 2015

  • Lv, Dongping; Zheng, Jianming; Li, Qiuyan
  • Advanced Energy Materials, Vol. 5, Issue 16, Article No. 1402290
  • DOI: 10.1002/aenm.201402290

Rational Design of Si/SiO 2 @Hierarchical Porous Carbon Spheres as Efficient Polysulfide Reservoirs for High-Performance Li-S Battery
journal, February 2016

  • Rehman, Sarish; Guo, Shaojun; Hou, Yanglong
  • Advanced Materials, Vol. 28, Issue 16
  • DOI: 10.1002/adma.201506111