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

Journal Article · · Journal of the Electrochemical Society
DOI:https://doi.org/10.1149/2.0181501jes· OSTI ID:1185290
 [1];  [2];  [1]
  1. Univ. of Southern California, Los Angeles, CA (United States)
  2. National Energy Technology Lab. (NETL), Morgantown, WV (United States)

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.

Research Organization:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)
Sponsoring Organization:
USDOE
OSTI ID:
1185290
Report Number(s):
A-NETL-PUB-115
Journal Information:
Journal of the Electrochemical Society, Vol. 162, Issue 1; ISSN 0013-4651
Publisher:
The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 188 works
Citation information provided by
Web of Science

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A Comprehensive Understanding of Lithium–Sulfur Battery Technology journal June 2019
A Cooperative Interface for Highly Efficient Lithium-Sulfur Batteries journal September 2016
Atomic Interlamellar Ion Path in High Sulfur Content Lithium-Montmorillonite Host Enables High-Rate and Stable Lithium-Sulfur Battery journal August 2018
Sulfiphilic Few‐Layered MoSe 2 Nanoflakes Decorated rGO as a Highly Efficient Sulfur Host for Lithium‐Sulfur Batteries journal August 2019
High Sulfur Content Material with Stable Cycling in Lithium-Sulfur Batteries journal October 2017
Elektrolytadditive für Lithiummetallanoden und wiederaufladbare Lithiummetallbatterien: Fortschritte und Perspektiven journal October 2018
Electrolyte Additives for Lithium Metal Anodes and Rechargeable Lithium Metal Batteries: Progress and Perspectives journal October 2018
Uncovering the Shuttle Effect in Organic Batteries and Counter‐Strategies Thereof: A Case Study of the N , N′ ‐Dimethylphenazine Cathode journal January 2020
Electrochemical studies on composite gel polymer electrolytes for lithium sulfur-batteries journal November 2016
Understanding the Role of Nano-Aluminum Oxide in All-Solid-State Lithium-Sulfur Batteries journal November 2018
Trapping of Polysulfides with Sulfur‐Rich Poly Ionic Liquid Cathode Materials for Ultralong‐Life Lithium–Sulfur Batteries journal January 2020
Ionic Liquids and their Polymers in Lithium‐Sulfur Batteries journal January 2019
Bio-Waste Derived Carbon as Interlayer and Scaffold for Li-S Batteries journal August 2018
Greatly Improved Conductivity of Double-Chain Polymer Network Binder for High Sulfur Loading Lithium-Sulfur Batteries with a Low Electrolyte/Sulfur Ratio journal July 2018
A Toolbox for Lithium-Sulfur Battery Research: Methods and Protocols journal June 2017
Sulfur Hosts against the Shuttle Effect journal April 2018
Solvent-Engineered Scalable Production of Polysulfide-Blocking Shields to Enhance Practical Lithium-Sulfur Batteries journal May 2018
Fe3O4-seated rGO–sulfur complex as a potential cathode material for lithium–sulfur batteries journal January 2020
In situ wrapping of the cathode material in lithium-sulfur batteries journal September 2017
Electrochemically primed functional redox mediator generator from the decomposition of solid state electrolyte journal April 2019
The Li–S battery: an investigation of redox shuttle and self-discharge behaviour with LiNO 3 -containing electrolytes journal January 2016
Sisal-derived activated carbons for cost-effective lithium–sulfur batteries journal January 2016
Facile and scalable synthesis of nanosized core–shell Li 2 S@C composite for high-performance lithium–sulfur batteries journal January 2016
Inhibiting polysulfide shuttling using dual-functional nanowire/nanotube modified layers for highly stable lithium–sulfur batteries journal January 2019
Promoting polysulfide conversion by catalytic ternary Fe 3 O 4 /carbon/graphene composites with ordered microchannels for ultrahigh-rate lithium–sulfur batteries journal January 2019
A new cathode material synthesized by a thiol-modified metal–organic framework (MOF) covalently connecting sulfur for superior long-cycling stability in lithium–sulfur batteries journal January 2019
Enhancing the kinetics of lithium–sulfur batteries under solid-state conversion by using tellurium as a eutectic accelerator journal January 2020
Electric vehicle battery parameter identification and SOC observability analysis: NiMH and Li-S case studies journal September 2017
A Microstructurally Resolved Model for Li-S Batteries Assessing the Impact of the Cathode Design on the Discharge Performance journal January 2016
Reference Performance Test Methodology for Degradation Assessment of Lithium-Sulfur Batteries journal January 2018
Pitfalls in Li–S Rate-Capability Evaluation journal January 2016
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Electric Vehicle Battery Parameter Identification and SOC Observability Analysis: NiMH and Li-S Case Studies conference January 2016
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