In Situ NMR Observation of the Temporal Speciation of Lithium Sulfur Batteries during Electrochemical Cycling
Abstract
The understanding of the reaction mechanism and temporal speciation of the lithium sulfur batteries is challenged by complex polysulfide disproportionation chemistry coupled with the precipitation and dissolution of species. In this report, for the first time, we present a comprehensive method to investigate lithium sulfur electrochemistry using in situ 7Li NMR spectroscopy, a technique that is capable of quantitatively capturing the evolution of the soluble and precipitated lithium (poly)sulfides during electrochemical cycling. Furthermore, through deconvolution and quantification, every lithium-bearing species was closely tracked and four-step soluble lithium polysulfide-mediated lithium sulfur electrochemistry was demonstrated in never before seen detail. Significant irreversible accumulation of Li2S is observed on the Li metal anode after four cycles because of sulfur shuttling. We present the application of the method in order to study electrolyte/additive development and lithium protection research can be readily envisaged.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research, Chemical Sciences and Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research; Univ. of Waterloo, ON (Canada). Dept. of Chemistry
- Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research, X-ray Science Division
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1392950
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 11; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE
Citation Formats
Wang, Hao, Sa, Niya, He, Meinan, Liang, Xiao, Nazar, Linda F., Balasubramanian, Mahalingam, Gallagher, Kevin G., and Key, Baris. In Situ NMR Observation of the Temporal Speciation of Lithium Sulfur Batteries during Electrochemical Cycling. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b01922.
Wang, Hao, Sa, Niya, He, Meinan, Liang, Xiao, Nazar, Linda F., Balasubramanian, Mahalingam, Gallagher, Kevin G., & Key, Baris. In Situ NMR Observation of the Temporal Speciation of Lithium Sulfur Batteries during Electrochemical Cycling. United States. https://doi.org/10.1021/acs.jpcc.7b01922
Wang, Hao, Sa, Niya, He, Meinan, Liang, Xiao, Nazar, Linda F., Balasubramanian, Mahalingam, Gallagher, Kevin G., and Key, Baris. Fri .
"In Situ NMR Observation of the Temporal Speciation of Lithium Sulfur Batteries during Electrochemical Cycling". United States. https://doi.org/10.1021/acs.jpcc.7b01922. https://www.osti.gov/servlets/purl/1392950.
@article{osti_1392950,
title = {In Situ NMR Observation of the Temporal Speciation of Lithium Sulfur Batteries during Electrochemical Cycling},
author = {Wang, Hao and Sa, Niya and He, Meinan and Liang, Xiao and Nazar, Linda F. and Balasubramanian, Mahalingam and Gallagher, Kevin G. and Key, Baris},
abstractNote = {The understanding of the reaction mechanism and temporal speciation of the lithium sulfur batteries is challenged by complex polysulfide disproportionation chemistry coupled with the precipitation and dissolution of species. In this report, for the first time, we present a comprehensive method to investigate lithium sulfur electrochemistry using in situ 7Li NMR spectroscopy, a technique that is capable of quantitatively capturing the evolution of the soluble and precipitated lithium (poly)sulfides during electrochemical cycling. Furthermore, through deconvolution and quantification, every lithium-bearing species was closely tracked and four-step soluble lithium polysulfide-mediated lithium sulfur electrochemistry was demonstrated in never before seen detail. Significant irreversible accumulation of Li2S is observed on the Li metal anode after four cycles because of sulfur shuttling. We present the application of the method in order to study electrolyte/additive development and lithium protection research can be readily envisaged.},
doi = {10.1021/acs.jpcc.7b01922},
journal = {Journal of Physical Chemistry. C},
number = 11,
volume = 121,
place = {United States},
year = {Fri Mar 03 00:00:00 EST 2017},
month = {Fri Mar 03 00:00:00 EST 2017}
}
Web of Science
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