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Title: Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes

Abstract

The lithium-sulfur (Li-S) battery is a very promising candidate for the next generation of energy storage systems required for electrical vehicles and grid energy storage applications due to its very high theoretical specific energy (2500 W h kg -1). However, low Coulombic efficiency (CE) during repeated Li metal plating/stripping has severely limited the practical application of rechargeable Li-S batteries. In this work, a new electrolyte system based on a high concentration of LiNO 3 in diglyme (G2) solvent is developed which enables an exceptionally high CE for Li metal plating/stripping and thus high stability of the Li anode in the sulfur-containing electrolyte. The tailoring of electrolyte properties for the Li anode has proven to be a highly successful strategy for improving the capacity retention and cycle life of Li-S batteries. This electrolyte provides a CE of greater than 99% for over 200 cycles of Li plating/stripping. In contrast, the Li anode cycles for less than 35 cycles (with a high CE) in the state-of-the-art 1 M LiTFSI + 0.3 M LiNO 3 in 1,3-dioxolane:1,2-dimethoxyethane (DOL:DME) electrolyte under the same conditions. Lastly, the stable Li anode enabled by the new electrolyte may accelerate the applications of high energy density Li-S batteriesmore » in both electrical vehicles and large-scale grid energy storage markets.« less

Authors:
 [1];  [2];  [2];  [3];  [1];  [1];  [4];  [4];  [3];  [4];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research (JCESR); Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR); Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research (JCESR); Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical & Computer Sciences Directorate
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1395291
Report Number(s):
PNNL-SA-124786
Journal ID: ISSN 2211-2855; PII: S2211285517305530
Grant/Contract Number:
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 40; Journal Issue: C; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; Li-S battery; Lithium nitrate; Coulombic efficiency; Cycling stability; Lithium metal

Citation Formats

Adams, Brian D., Carino, Emily V., Connell, Justin G., Han, Kee Sung, Cao, Ruiguo, Chen, Junzheng, Zheng, Jianming, Li, Qiuyan, Mueller, Karl T., Henderson, Wesley A., and Zhang, Ji-Guang. Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes. United States: N. p., 2017. Web. doi:10.1016/J.NANOEN.2017.09.015.
Adams, Brian D., Carino, Emily V., Connell, Justin G., Han, Kee Sung, Cao, Ruiguo, Chen, Junzheng, Zheng, Jianming, Li, Qiuyan, Mueller, Karl T., Henderson, Wesley A., & Zhang, Ji-Guang. Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes. United States. doi:10.1016/J.NANOEN.2017.09.015.
Adams, Brian D., Carino, Emily V., Connell, Justin G., Han, Kee Sung, Cao, Ruiguo, Chen, Junzheng, Zheng, Jianming, Li, Qiuyan, Mueller, Karl T., Henderson, Wesley A., and Zhang, Ji-Guang. 2017. "Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes". United States. doi:10.1016/J.NANOEN.2017.09.015.
@article{osti_1395291,
title = {Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes},
author = {Adams, Brian D. and Carino, Emily V. and Connell, Justin G. and Han, Kee Sung and Cao, Ruiguo and Chen, Junzheng and Zheng, Jianming and Li, Qiuyan and Mueller, Karl T. and Henderson, Wesley A. and Zhang, Ji-Guang},
abstractNote = {The lithium-sulfur (Li-S) battery is a very promising candidate for the next generation of energy storage systems required for electrical vehicles and grid energy storage applications due to its very high theoretical specific energy (2500 W h kg-1). However, low Coulombic efficiency (CE) during repeated Li metal plating/stripping has severely limited the practical application of rechargeable Li-S batteries. In this work, a new electrolyte system based on a high concentration of LiNO3 in diglyme (G2) solvent is developed which enables an exceptionally high CE for Li metal plating/stripping and thus high stability of the Li anode in the sulfur-containing electrolyte. The tailoring of electrolyte properties for the Li anode has proven to be a highly successful strategy for improving the capacity retention and cycle life of Li-S batteries. This electrolyte provides a CE of greater than 99% for over 200 cycles of Li plating/stripping. In contrast, the Li anode cycles for less than 35 cycles (with a high CE) in the state-of-the-art 1 M LiTFSI + 0.3 M LiNO3 in 1,3-dioxolane:1,2-dimethoxyethane (DOL:DME) electrolyte under the same conditions. Lastly, the stable Li anode enabled by the new electrolyte may accelerate the applications of high energy density Li-S batteries in both electrical vehicles and large-scale grid energy storage markets.},
doi = {10.1016/J.NANOEN.2017.09.015},
journal = {Nano Energy},
number = C,
volume = 40,
place = {United States},
year = 2017,
month = 9
}

Journal Article:
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  • Lithium-sulfur (Li-S) battery is a very promising candidate for the next generation of energy storage systems required for electrical vehicles and grid energy storage applications due to its very high theoretical specific energy (2500 W h kg-1). However, the low coulombic efficiency (CE) during repeated Li plating/stripping of these processes have limited practical application of rechargeable Li-S batteries. In this work, a new electrolyte system based on high concentration of LiNO3 in diglyme solvent is developed which enables high CE of Li metal plating/stripping and high stability of Li anode in the sulfur containing electrolyte. Tailoring of electrolyte properties formore » the Li negative electrode has proven to be a successful strategy for improving the capacity retention and cycle life of Li-S batteries. This electrolyte provides a CE for Li plating/stripping of greater than 99% for over 200 cycles. In contrast, Li metal cycles for only less than 35 cycles at high CE in the standard 1 M LiTFSI + 2wt% LiNO3 in DOL:DME electrolyte under the same conditions. The stable Li metal anode enabled by the new electrolyte may accelerate the applications of high energy density Li-S batteries in both electrical vehicles and large-scale grid energy storage markets.« less
  • The lithium-sulfur (Li-S) battery is a very promising candidate for the next generation of energy storage systems required for electrical vehicles and grid energy storage applications due to its very high theoretical specific energy (2500 W h kg(-1)). However, low Coulombic efficiency (CE) during repeated Li metal plating/stripping has severely limited the practical application of rechargeable Li-S batteries. In this work, a new electrolyte system based on a high concentration of LiNO3 in diglyme (G2) solvent is developed which enables an exceptionally high CE for Li metal plating/stripping and thus high stability of the Li anode in the sulfur-containing electrolyte.more » The tailoring of electrolyte properties for the Li anode has proven to be a highly successful strategy for improving the capacity retention and cycle life of Li-S batteries. This electrolyte provides a CE of greater than 99% for over 200 cycles of Li plating/stripping. In contrast, the Li anode cycles for less than 35 cycles (with a high CE) in the state-of-the-art 1 M LiTFSI + 0.3 M LiNO3 in 1,3-dioxolane: 1,2-dimethoxyethane (DOL:DME) electrolyte under the same conditions. The stable Li anode enabled by the new electrolyte may accelerate the applications of high energy density Li-S batteries in both electrical vehicles and large-scale grid energy storage markets.« less
  • The electrolyte stability against reactive reduced-oxygen species is crucial for the development of rechargeable Li-O2 batteries. In this work, we systematically investigated the effect of lithium salt concentration in 1,2-dimethoxyethane (DME)-based electrolytes on the cycling stability of Li-O2 batteries. Cells with high concentration electrolyte illustrate largely enhanced cycling stability under both the full discharge/charge (2.0-4.5 V vs. Li/Li+) and the capacity limited (at 1,000 mAh g-1) conditions. These cells also exhibit much less reaction-residual on the charged air electrode surface, and much less corrosion to the Li metal anode. The density functional theory calculations are conducted on the molecular orbitalmore » energies of the electrolyte components and the Gibbs activation barriers for superoxide radical anion to attack DME solvent and Li+-(DME)n solvates. In a highly concentrated electrolyte, all DME molecules have been coordinated with salt and the C-H bond scission of a DME molecule becomes more difficult. Therefore, the decomposition of highly concentrated electrolyte in a Li-O2 battery can be mitigated and both air-cathodes and Li-metal anodes exhibits much better reversibility. As a results, the cyclability of Li-O2 can be largely improved.« less
  • We report a design of high voltage magnesium-lithium (Mg-Li) hybrid batteries through rational controls of the electrolyte chemistry, electrode materials and cell architectures. Prototype devices with LiFePO4 and LiMn 2O 4 cathodes exhibit voltages higher than 2.5 V (vs. Mg) and a high specific energy density of 246 Wh/kg under conditions that are amenable for practical applications. The successful demonstrations reported here could be a significant step forward for practical hybrid batteries.