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Title: Insights into the Interconnection of the Electrodes and Electrolyte Species in Lithium–Sulfur Batteries Using Spatially Resolved Operando X-ray Absorption Spectroscopy and X-ray Fluorescence Mapping

Abstract

The lithium–sulfur (Li–S) battery chemistry has attracted great interest in the last decade because of its outstanding theoretical gravimetric energy density compared to the state-of-the-art lithium-ion battery technology. However, practically achieved energy density is still far below the theoretical value, even in small laboratory-scale batteries. The problems seen in laboratory-scale batteries will inevitably increase during scale-up to large application-format cells, as the electrolyte to active material (AM) ratio will need to be reduced in these cells to achieve high gravimetric energy density on cell-level basis. Our paper shows the unique possibility of X-ray fluorescence (XRF) mapping to visualize the spatial distribution of the AM inside operating Li–S batteries in all cell components [working electrode (WE), separator, and counter electrode (CE)]. Through a combination of operando XRF mapping and X-ray absorption spectroscopy, we show that unless self-discharge is efficiently prevented, the AM can completely dissolve and distribute throughout the cell stack within a time frame of 2 h, causing poor capacity retention. Finally, using a polysulfide diffusion barrier between the WE and the CE, we successfully suppress these processes and thereby establish a tool for examining the sealed cathode electrode compartment, enabling sophisticated studies for future optimization of the WE processes.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [1];  [3]; ORCiD logo [1]
  1. Technical Univ. of Munich, Garching (Germany). Chair of Technical Electrochemistry. Dept. of Chemistry. Catalysis Research Center
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
  3. Univ. of Amsterdam (Netherlands). Sustainable Materials Characterization. Van’t Hoff Inst. for Molecular Sciences
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Technical Univ. of Munich, Garching (Germany); Univ. of Amsterdam (Netherlands)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Federal Ministry for Economic Affairs and Energy (BMWi) (Germany); Netherlands Organisation for Scientific Research (NWO)
OSTI Identifier:
1471518
Grant/Contract Number:  
AC02-76SF00515; 03ET6045D; VIDI 723.014.010
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 10; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Freiberg, Anna T. S., Siebel, Armin, Berger, Anne, Webb, Samuel M., Gorlin, Yelena, Tromp, Moniek, and Gasteiger, Hubert A. Insights into the Interconnection of the Electrodes and Electrolyte Species in Lithium–Sulfur Batteries Using Spatially Resolved Operando X-ray Absorption Spectroscopy and X-ray Fluorescence Mapping. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.7b12799.
Freiberg, Anna T. S., Siebel, Armin, Berger, Anne, Webb, Samuel M., Gorlin, Yelena, Tromp, Moniek, & Gasteiger, Hubert A. Insights into the Interconnection of the Electrodes and Electrolyte Species in Lithium–Sulfur Batteries Using Spatially Resolved Operando X-ray Absorption Spectroscopy and X-ray Fluorescence Mapping. United States. doi:10.1021/acs.jpcc.7b12799.
Freiberg, Anna T. S., Siebel, Armin, Berger, Anne, Webb, Samuel M., Gorlin, Yelena, Tromp, Moniek, and Gasteiger, Hubert A. Thu . "Insights into the Interconnection of the Electrodes and Electrolyte Species in Lithium–Sulfur Batteries Using Spatially Resolved Operando X-ray Absorption Spectroscopy and X-ray Fluorescence Mapping". United States. doi:10.1021/acs.jpcc.7b12799. https://www.osti.gov/servlets/purl/1471518.
@article{osti_1471518,
title = {Insights into the Interconnection of the Electrodes and Electrolyte Species in Lithium–Sulfur Batteries Using Spatially Resolved Operando X-ray Absorption Spectroscopy and X-ray Fluorescence Mapping},
author = {Freiberg, Anna T. S. and Siebel, Armin and Berger, Anne and Webb, Samuel M. and Gorlin, Yelena and Tromp, Moniek and Gasteiger, Hubert A.},
abstractNote = {The lithium–sulfur (Li–S) battery chemistry has attracted great interest in the last decade because of its outstanding theoretical gravimetric energy density compared to the state-of-the-art lithium-ion battery technology. However, practically achieved energy density is still far below the theoretical value, even in small laboratory-scale batteries. The problems seen in laboratory-scale batteries will inevitably increase during scale-up to large application-format cells, as the electrolyte to active material (AM) ratio will need to be reduced in these cells to achieve high gravimetric energy density on cell-level basis. Our paper shows the unique possibility of X-ray fluorescence (XRF) mapping to visualize the spatial distribution of the AM inside operating Li–S batteries in all cell components [working electrode (WE), separator, and counter electrode (CE)]. Through a combination of operando XRF mapping and X-ray absorption spectroscopy, we show that unless self-discharge is efficiently prevented, the AM can completely dissolve and distribute throughout the cell stack within a time frame of 2 h, causing poor capacity retention. Finally, using a polysulfide diffusion barrier between the WE and the CE, we successfully suppress these processes and thereby establish a tool for examining the sealed cathode electrode compartment, enabling sophisticated studies for future optimization of the WE processes.},
doi = {10.1021/acs.jpcc.7b12799},
journal = {Journal of Physical Chemistry. C},
number = 10,
volume = 122,
place = {United States},
year = {2018},
month = {2}
}

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