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A lithium-sulfur battery with a solution-mediated pathway operating under lean electrolyte conditions

Journal Article · · Nano Energy
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  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research (JCESR); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  5. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Joint Center for Energy Storage Research (JCESR)
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Lithium-sulfur (Li–S) battery is one of the most promising candidates for the next generation energy storage systems. However, several barriers, including polysulfide shuttle effect, the slow solid-solid surface reaction pathway in the lower discharge plateau, and corrosion of Li anode still limit its practical applications, especially under the lean electrolyte condition required for high energy density. In this paper, we propose a solution-mediated sulfur reduction pathway to improve the capacity and reversibility of the sulfur cathode. With this method, a high coulombic efficiency (99%) and stable cycle life over 100 cycles were achieved under application-relevant conditions (S loading: 6.2 mg cm-2; electrolyte to sulfur ratio: 3 mLE gs-1; sulfur weight ratio: 72 wt%). This result is enabled by a specially designed Li2S4-rich electrolyte, in which Li2S is formed through a chemical disproportionation reaction instead of electrochemical routes. A single diglyme solvent was used to obtain electrolytes with the optimum range of Li2S4 concentration. Operando X-ray absorption spectroscopy confirms the solution pathway in a practical Li–S cell. This solution pathway not only introduces a new electrolyte regime for practical Li–S batteries, but also provides a new perspective for bypassing the inefficient surface pathway for other electrochemical processes.

Research Organization:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC04-94AL85000
OSTI ID:
1639079
Alternate ID(s):
OSTI ID: 1809799
OSTI ID: 1834347
OSTI ID: 1647576
OSTI ID: 1780749
Report Number(s):
SAND--2020-6645J; 687016
Journal Information:
Nano Energy, Journal Name: Nano Energy Vol. 76; ISSN 2211-2855
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Li-S batteries
Li2S4-rich electrolyte
high ionic-associations strength anions
lean electrolyte conditions
solution-based pathway