Quantifying the chemical, electrochemical heterogeneity and spatial distribution of (poly) sulfide species using Operando SANS
Abstract
In-situ and operando measurements are done to gain a better understanding of the precipitation mechanisms during charge and discharge in lithium sulfur batteries. A carbon felt networked with microfibers consisting of pores, 2 nm and smaller, is used as a freestanding sulfur host. Three different methods of sulfur infiltration are explored in order to determine the best one to fill most of the pores. It was identified to be a melt infiltration method in a vacuum oven, where the pores including the ultra-micropores, are successfully filled. In-situ electrochemical impedance spectroscopy measurements show a solid product formation occurring at the sulfur cathode, both during the high voltage plateau and at the end of discharge. In a 3-electrode EIS measurement, a similar solid product formation on the Li counter electrode due to its reaction with polysulfides is also observed. Operando small angle neutron scattering measurements show the solid product formation, in the carbon, both near the beginning and at the end of discharge, confirming the precipitation data via contrast changes as a function of charge and discharge. It is shown that Li2S precipitates in the pores at the beginning and the end of discharge, whereas S8 precipitates on the surface of themore »
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[3];
[3]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Institut Max von Laue-Paul Langevin, Grenoble (France)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1817553
- Alternate Identifier(s):
- OSTI ID: 1817254
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy Storage Materials
- Additional Journal Information:
- Journal Volume: 40; Journal ID: ISSN 2405-8297
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; lithium sulfur batteries; small angle neutron scattering; Li2S formation; operando characterization; sulfur filling
Citation Formats
Jafta, Charl, Prevost, Sylvain, He, Lilin, Li, Mengya, Sun, Xiao-Guang, Yang, Guang, Belharouak, Ilias, and Nanda, Jagjit. Quantifying the chemical, electrochemical heterogeneity and spatial distribution of (poly) sulfide species using Operando SANS. United States: N. p., 2021.
Web. doi:10.1016/j.ensm.2021.05.016.
Jafta, Charl, Prevost, Sylvain, He, Lilin, Li, Mengya, Sun, Xiao-Guang, Yang, Guang, Belharouak, Ilias, & Nanda, Jagjit. Quantifying the chemical, electrochemical heterogeneity and spatial distribution of (poly) sulfide species using Operando SANS. United States. https://doi.org/10.1016/j.ensm.2021.05.016
Jafta, Charl, Prevost, Sylvain, He, Lilin, Li, Mengya, Sun, Xiao-Guang, Yang, Guang, Belharouak, Ilias, and Nanda, Jagjit. Sat .
"Quantifying the chemical, electrochemical heterogeneity and spatial distribution of (poly) sulfide species using Operando SANS". United States. https://doi.org/10.1016/j.ensm.2021.05.016. https://www.osti.gov/servlets/purl/1817553.
@article{osti_1817553,
title = {Quantifying the chemical, electrochemical heterogeneity and spatial distribution of (poly) sulfide species using Operando SANS},
author = {Jafta, Charl and Prevost, Sylvain and He, Lilin and Li, Mengya and Sun, Xiao-Guang and Yang, Guang and Belharouak, Ilias and Nanda, Jagjit},
abstractNote = {In-situ and operando measurements are done to gain a better understanding of the precipitation mechanisms during charge and discharge in lithium sulfur batteries. A carbon felt networked with microfibers consisting of pores, 2 nm and smaller, is used as a freestanding sulfur host. Three different methods of sulfur infiltration are explored in order to determine the best one to fill most of the pores. It was identified to be a melt infiltration method in a vacuum oven, where the pores including the ultra-micropores, are successfully filled. In-situ electrochemical impedance spectroscopy measurements show a solid product formation occurring at the sulfur cathode, both during the high voltage plateau and at the end of discharge. In a 3-electrode EIS measurement, a similar solid product formation on the Li counter electrode due to its reaction with polysulfides is also observed. Operando small angle neutron scattering measurements show the solid product formation, in the carbon, both near the beginning and at the end of discharge, confirming the precipitation data via contrast changes as a function of charge and discharge. It is shown that Li2S precipitates in the pores at the beginning and the end of discharge, whereas S8 precipitates on the surface of the carbon felt. Finally, this lithium sulfur system shows both the quasi-solid-state and the solid-liquid-solid reactions in a typical ethereal electrolyte solution with a two-plateau discharge profile.},
doi = {10.1016/j.ensm.2021.05.016},
journal = {Energy Storage Materials},
number = ,
volume = 40,
place = {United States},
year = {Sat May 15 00:00:00 EDT 2021},
month = {Sat May 15 00:00:00 EDT 2021}
}
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