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Title: Interaction of FeS 2 and Sulfur in Li-S Battery System

Abstract

Many transition metal sulfides are electronically conductive, electrochemically active and reversible in reactions with lithium. However, the application of transition metal sulfides as sulfur cathode additives in lithium-sulfur (Li-S) batteries has not been fully explored. In this study, Pyrite (FeS 2) is studied as a capacity contributing conductive additive in sulfur cathode for Li-S batteries. Electrochemically discharging the S-FeS 2 composite electrodes to 1.0 V activates the FeS 2 component, contributing to the improved Li-S cell discharge energy density. However, direct activation of the FeS 2 component in a fresh S-FeS 2 cell results in a significant shuttling effect in the subsequent charging process, preventing further cell cycling. The slight FeS 2 solubility in electrolyte and its activation alone in S-FeS 2 cells are not the root causes of the severe shuttling effect. The observed severe shuttling effect is strongly correlated to the 1st charging of the activated S-FeS 2 electrode that promotes iron dissolution in electrolyte and the deposition of electronically conductive FeS on the anode SEI. Pre-cycling of the S-FeS 2 cell prior to the FeS 2 activation or the use of LiNO 3 electrolyte additive help to prevent the severe shuttling effect and allow the cell tomore » cycle between 2.6 V to 1.0 V with an extra capacity contribution from the FeS2 components. However, a more effective method of anode pre-passivation is still needed to fully protect the lithium surface from FeS deposition and allow the S-FeS 2 electrode to maintain high energy density over extended cycles. A mechanism explaining the observed phenomena based on the experimental data is proposed and discussed« less

Authors:
 [1];  [2];  [2];  [1];  [1];  [1];  [2];  [2];  [3];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Stony Brook Univ., NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1389218
Report Number(s):
BNL-114124-2017-JA
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 1; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Sun, Ke, Cama, Christina A., DeMayo, Rachel A., Bock, David C., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Gan, Hong. Interaction of FeS 2 and Sulfur in Li-S Battery System. United States: N. p., 2016. Web. doi:10.1149/2.0041701jes.
Sun, Ke, Cama, Christina A., DeMayo, Rachel A., Bock, David C., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., & Gan, Hong. Interaction of FeS 2 and Sulfur in Li-S Battery System. United States. doi:10.1149/2.0041701jes.
Sun, Ke, Cama, Christina A., DeMayo, Rachel A., Bock, David C., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Gan, Hong. Fri . "Interaction of FeS 2 and Sulfur in Li-S Battery System". United States. doi:10.1149/2.0041701jes. https://www.osti.gov/servlets/purl/1389218.
@article{osti_1389218,
title = {Interaction of FeS 2 and Sulfur in Li-S Battery System},
author = {Sun, Ke and Cama, Christina A. and DeMayo, Rachel A. and Bock, David C. and Tong, Xiao and Su, Dong and Marschilok, Amy C. and Takeuchi, Kenneth J. and Takeuchi, Esther S. and Gan, Hong},
abstractNote = {Many transition metal sulfides are electronically conductive, electrochemically active and reversible in reactions with lithium. However, the application of transition metal sulfides as sulfur cathode additives in lithium-sulfur (Li-S) batteries has not been fully explored. In this study, Pyrite (FeS2) is studied as a capacity contributing conductive additive in sulfur cathode for Li-S batteries. Electrochemically discharging the S-FeS2 composite electrodes to 1.0 V activates the FeS2 component, contributing to the improved Li-S cell discharge energy density. However, direct activation of the FeS2 component in a fresh S-FeS2 cell results in a significant shuttling effect in the subsequent charging process, preventing further cell cycling. The slight FeS2 solubility in electrolyte and its activation alone in S-FeS2 cells are not the root causes of the severe shuttling effect. The observed severe shuttling effect is strongly correlated to the 1st charging of the activated S-FeS2 electrode that promotes iron dissolution in electrolyte and the deposition of electronically conductive FeS on the anode SEI. Pre-cycling of the S-FeS2 cell prior to the FeS2 activation or the use of LiNO3 electrolyte additive help to prevent the severe shuttling effect and allow the cell to cycle between 2.6 V to 1.0 V with an extra capacity contribution from the FeS2 components. However, a more effective method of anode pre-passivation is still needed to fully protect the lithium surface from FeS deposition and allow the S-FeS2 electrode to maintain high energy density over extended cycles. A mechanism explaining the observed phenomena based on the experimental data is proposed and discussed},
doi = {10.1149/2.0041701jes},
journal = {Journal of the Electrochemical Society},
number = 1,
volume = 164,
place = {United States},
year = {Fri Sep 09 00:00:00 EDT 2016},
month = {Fri Sep 09 00:00:00 EDT 2016}
}

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Works referenced in this record:

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