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Title: Direct measurement of polysulfide shuttle current: A window into understanding the performance of lithium-sulfur cells

Abstract

The shuttling of polysulfide ions between the electrodes in a lithium-sulfur battery is a major technical issue limiting the self-discharge and cycle life of this high-energy rechargeable battery. Although there have been attempts to suppress the shuttling process, there has not been a direct measurement of the rate of shuttling. We report here a simple and direct measurement of the rate of the shuttling (that we term “shuttle current”), applicable to the study of any type of lithium-sulfur cell. We demonstrate the effectiveness of this measurement technique using cells with and without lithium nitrate (a widely-used shuttle suppressor additive). We present a phenomenological analysis of the shuttling process and simulate the shuttle currents as a function of the state-of-charge of a cell. We also demonstrate how the rate of decay of the shuttle current can be used to predict the capacity fade in a lithium-sulfur cell due to the shuttle process. As a result, we expect that this new ability to directly measure shuttle currents will provide greater insight into the performance differences observed with various additives and electrode modifications that are aimed at suppressing the rate of shuttling of polysulfide ions and increasing the cycle life of lithium-sulfur cells.

Authors:
 [1];  [2];  [1]
  1. Univ. of Southern California, Los Angeles, CA (United States)
  2. National Energy Technology Lab. (NETL), Morgantown, WV (United States)
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1185290
Report Number(s):
A-NETL-PUB-115
Journal ID: ISSN 0013-4651
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 162; Journal Issue: 1; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Moy, Derek, Manivannan, A., and Narayanan, S. R. Direct measurement of polysulfide shuttle current: A window into understanding the performance of lithium-sulfur cells. United States: N. p., 2014. Web. doi:10.1149/2.0181501jes.
Moy, Derek, Manivannan, A., & Narayanan, S. R. Direct measurement of polysulfide shuttle current: A window into understanding the performance of lithium-sulfur cells. United States. https://doi.org/10.1149/2.0181501jes
Moy, Derek, Manivannan, A., and Narayanan, S. R. 2014. "Direct measurement of polysulfide shuttle current: A window into understanding the performance of lithium-sulfur cells". United States. https://doi.org/10.1149/2.0181501jes. https://www.osti.gov/servlets/purl/1185290.
@article{osti_1185290,
title = {Direct measurement of polysulfide shuttle current: A window into understanding the performance of lithium-sulfur cells},
author = {Moy, Derek and Manivannan, A. and Narayanan, S. R.},
abstractNote = {The shuttling of polysulfide ions between the electrodes in a lithium-sulfur battery is a major technical issue limiting the self-discharge and cycle life of this high-energy rechargeable battery. Although there have been attempts to suppress the shuttling process, there has not been a direct measurement of the rate of shuttling. We report here a simple and direct measurement of the rate of the shuttling (that we term “shuttle current”), applicable to the study of any type of lithium-sulfur cell. We demonstrate the effectiveness of this measurement technique using cells with and without lithium nitrate (a widely-used shuttle suppressor additive). We present a phenomenological analysis of the shuttling process and simulate the shuttle currents as a function of the state-of-charge of a cell. We also demonstrate how the rate of decay of the shuttle current can be used to predict the capacity fade in a lithium-sulfur cell due to the shuttle process. As a result, we expect that this new ability to directly measure shuttle currents will provide greater insight into the performance differences observed with various additives and electrode modifications that are aimed at suppressing the rate of shuttling of polysulfide ions and increasing the cycle life of lithium-sulfur cells.},
doi = {10.1149/2.0181501jes},
url = {https://www.osti.gov/biblio/1185290}, journal = {Journal of the Electrochemical Society},
issn = {0013-4651},
number = 1,
volume = 162,
place = {United States},
year = {Tue Nov 04 00:00:00 EST 2014},
month = {Tue Nov 04 00:00:00 EST 2014}
}

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Works referenced in this record:

Positive Electrode Materials for Li-Ion and Li-Batteries
journal, February 2010


Lithium batteries: Status, prospects and future
journal, May 2010


Lithium/sulfur batteries with high specific energy: old challenges and new opportunities
journal, January 2013


A Review on Li-S Batteries as a High Efficiency Rechargeable Lithium Battery
journal, January 2013


Lithium-Sulfur Batteries: Electrochemistry, Materials, and Prospects
journal, November 2013


Lithium-sulfur batteries
journal, May 2014


High Energy Rechargeable Li-S Cells for EV Application: Status, Remaining Problems and Solutions
conference, January 2010


Binder Based on Polyelectrolyte for High Capacity Density Lithium/Sulfur Battery
journal, January 2012


Sulphur–TiO2 yolk–shell nanoarchitecture with internal void space for long-cycle lithium–sulphur batteries
journal, January 2013


Role of Polysulfides in Self-Healing Lithium-Sulfur Batteries
journal, February 2013


Graphene-Based Three-Dimensional Hierarchical Sandwich-type Architecture for High-Performance Li/S Batteries
journal, September 2013


Polysulfide Shuttle Study in the Li/S Battery System
journal, January 2004


Phosphorous Pentasulfide as a Novel Additive for High-Performance Lithium-Sulfur Batteries
journal, June 2012


High “C” rate Li-S cathodes: sulfur imbibed bimodal porous carbons
journal, January 2011


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


Influence of different electrode compositions and binder materials on the performance of lithium–sulfur batteries
journal, May 2012


High-rate lithium–sulfur batteries promoted by reduced graphene oxide coating
journal, January 2012


A sulfur–carbon composite for lithium/sulfur battery based on activated vapor-grown carbon fiber
journal, May 2013


Lithium–Sulfur Battery Cathode Enabled by Lithium–Nitrile Interaction
journal, December 2012


Porous carbon nanotubes improved sulfur composite cathode for lithium-sulfur battery
journal, February 2013


A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries
journal, February 2013


Challenges and Prospects of Lithium–Sulfur Batteries
journal, June 2012


A membrane-free lithium/polysulfide semi-liquid battery for large-scale energy storage
journal, January 2013


Exceptional electrochemical performance of rechargeable Li–S batteries with a polysulfide-containing electrolyte
journal, January 2013


Mechanistic modeling of polysulfide shuttle and capacity loss in lithium–sulfur batteries
journal, August 2014


Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer
journal, January 2012


Low Temperature Performance of Li/S Batteries
journal, January 2003


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


On the Surface Chemical Aspects of Very High Energy Density, Rechargeable Li–Sulfur Batteries
journal, January 2009


Lithium-sulfur batteries: Problems and solutions
journal, May 2008


A Mathematical Model for a Lithium–Sulfur Cell
journal, January 2008


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The Li–S battery: an investigation of redox shuttle and self-discharge behaviour with LiNO 3 -containing electrolytes
journal, January 2016


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journal, January 2016


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journal, January 2018


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journal, January 2016


The Effects of Lithium Sulfur Battery Ageing on Second-Life Possibilities and Environmental Life Cycle Assessment Studies
journal, June 2019


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journal, February 2019


In situ wrapping of the cathode material in lithium-sulfur batteries
journal, September 2017


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journal, April 2019


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