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

Abstract

With the ability to adsorb polysulfide, electronically conductive and electrochemically active TiS 2 is an effective multifunctional cathode additive to improve Li-S battery cycling performance. Furthermore, by using X-ray Photoelectron Spectroscopy (XPS), direct evidence is obtained to demonstrate the strong interaction between Li-polysulfide and TiS 2. The observation of Li signature on Li 2S 8 treated TiS 2 proves that the TiS 2 possesses the ability to adsorb Li-polysulfides species on its surface. An electron density transfer from Ti to Li and S is identified based on the positions of the peaks in the XPS spectrum before and after the interaction, which is consistent with the theoretically predicted polysulfide-TiS 2 interaction models in the literature. TiS 2 sample with 2.5x higher BET surface area is obtained by milling the raw TiS 2 particles and used as cathode additive in the sulfur electrode. Furthermore, in the presence of TiS 2 additive, long cycle life and improved sulfur utilization of Li-S cells under high rate discharge are demonstrated. In addition, we find that a uniform TiS 2 distribution in the sulfur-TiS 2 hybrid electrode is vital in determining its effectiveness in enhancing the performance of sulfur electrodes. Thus, by processing method andmore » condition should be very important considerations in future development of sulfur electrodes with TiS 2 additive.« less

Authors:
 [1];  [2];  [3];  [4];  [4];  [5];  [6];  [5];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
  2. Stony Brook Univ., NY (United States). Dept. of Materials Science and Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Energy Sciences Directorate
  4. Stony Brook Univ., NY (United States). Dept. of Chemistry
  5. Stony Brook Univ., NY (United States). Dept. of Materials Science and Engineering and Dept. of Chemistry
  6. Stony Brook Univ., NY (United States). Dept. of Materials Science and Engineering and Dept. of Chemistry; Brookhaven National Lab. (BNL), Upton, NY (United States). Energy Sciences Directorate
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:
1377018
Report Number(s):
BNL-114113-2017-JA
Journal ID: ISSN 0013-4651
Grant/Contract Number:
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 6; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Li-S battery; polysulfide-TiS2 interaction; process method; sulfur-TiS2 hybrid electrode; TiS2 additive; uniform distribution

Citation Formats

Sun, Ke, Zhang, Qing, Bock, David C., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Gan, Hong. Interaction of TiS 2 and Sulfur in Li-S Battery System. United States: N. p., 2017. Web. doi:10.1149/2.1631706jes.
Sun, Ke, Zhang, Qing, Bock, David C., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., & Gan, Hong. Interaction of TiS 2 and Sulfur in Li-S Battery System. United States. doi:10.1149/2.1631706jes.
Sun, Ke, Zhang, Qing, Bock, David C., Tong, Xiao, Su, Dong, Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and Gan, Hong. 2017. "Interaction of TiS 2 and Sulfur in Li-S Battery System". United States. doi:10.1149/2.1631706jes. https://www.osti.gov/servlets/purl/1377018.
@article{osti_1377018,
title = {Interaction of TiS 2 and Sulfur in Li-S Battery System},
author = {Sun, Ke and Zhang, Qing 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 = {With the ability to adsorb polysulfide, electronically conductive and electrochemically active TiS2 is an effective multifunctional cathode additive to improve Li-S battery cycling performance. Furthermore, by using X-ray Photoelectron Spectroscopy (XPS), direct evidence is obtained to demonstrate the strong interaction between Li-polysulfide and TiS2. The observation of Li signature on Li2S8 treated TiS2 proves that the TiS2 possesses the ability to adsorb Li-polysulfides species on its surface. An electron density transfer from Ti to Li and S is identified based on the positions of the peaks in the XPS spectrum before and after the interaction, which is consistent with the theoretically predicted polysulfide-TiS2 interaction models in the literature. TiS2 sample with 2.5x higher BET surface area is obtained by milling the raw TiS2 particles and used as cathode additive in the sulfur electrode. Furthermore, in the presence of TiS2 additive, long cycle life and improved sulfur utilization of Li-S cells under high rate discharge are demonstrated. In addition, we find that a uniform TiS2 distribution in the sulfur-TiS2 hybrid electrode is vital in determining its effectiveness in enhancing the performance of sulfur electrodes. Thus, by processing method and condition should be very important considerations in future development of sulfur electrodes with TiS2 additive.},
doi = {10.1149/2.1631706jes},
journal = {Journal of the Electrochemical Society},
number = 6,
volume = 164,
place = {United States},
year = 2017,
month = 4
}

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  • Lithium-Sulfur (Li-S) battery has been a subject of intensive research in recent years due to its potential to provide much higher energy density and lower cost than the current state of the art lithiumion battery technology. In this work, we have investigated Cupric Sulfide (CuS) as a capacitycontributing conductive additive to the sulfur electrode in a Li-S battery. Galvanostatic charge/discharge cycling has been used to compare the performance of both sulfur electrodes and S:CuS hybrid electrodes with various ratios. We found that the conductive CuS additive enhanced the utilization of the sulfur cathode under a 1C rate discharge. However, undermore » a C/10 discharge rate, S:CuS hybrid electrodes exhibited lower sulfur utilization in the first discharge and faster capacity decay in later cycles than a pure sulfur electrode due to the dissolution of CuS. The CuS dissolution is found to be the result of strong interaction between the soluble low order polysulfide Li 2S 3 and CuS. As a result, we identified the presence of conductive copper-containing sulfides at the cycled lithium anode surface, which may degrade the effectiveness of the passivation function of the solid-electrolyte-interphase (SEI) layer, accounting for the poor cycling performance of the S:CuS hybrid cells at low rate.« less
  • 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 inmore » 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 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-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
  • In this paper the construction and performance of a sodium sulfur battery system with dynamic sulfur electrodes are described. Three cells were first connected in parallel, then two such groups were connected in series. Each cell included a liquid sodium filled {beta}{double prime}-alumina tube and a system to feed liquid sulfur into the annular cathode. Low resistance graphite felt was tightly packed around the {beta}{double prime}-alumina tube. Sodium pentasulfide was removed from the sulfur electrode. The battery was operated automatically and stably changed and discharged in the two-phase region. The discharged energy was 4372 Wh (capacity 1170 Ah) during amore » continuous operation of 19.5 h. The discharge/charge energy efficiency of the battery was 82% at an averaged current density of 100 mA/cm{sup 2} and operating temperature of 350{degrees}C. The deviation of the cell current in a parallel chain was less than 7%, and this was induced by the difference in internal resistance. In the daily charge/discharge cycle, cell capacity with the dynamic sulfur electrode was 1.5 times higher than that with the static sulfur electrode using the same active surface of {beta}{double prime}-alumina, because the internal resistance of the former cell was constant regardless of cell capacity. This battery system with a dynamic sulfur electrode can be applied to energy storage systems, such as large scale load leveling systems, electric vehicle batteries, and solar energy systems.« less