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 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 electricalmore »
- Authors:
-
- 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
- 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
- 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
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1395291
- Alternate Identifier(s):
- OSTI ID: 1549956
- Report Number(s):
- PNNL-SA-124786
Journal ID: ISSN 2211-2855; PII: S2211285517305530
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- 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. https://doi.org/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. Fri .
"Long term stability of Li-S batteries using high concentration lithium nitrate electrolytes". United States. https://doi.org/10.1016/J.NANOEN.2017.09.015. https://www.osti.gov/servlets/purl/1395291.
@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 = {Fri Sep 08 00:00:00 EDT 2017},
month = {Fri Sep 08 00:00:00 EDT 2017}
}
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Works referenced in this record:
Towards Stable Lithium-Sulfur Batteries with a Low Self-Discharge Rate: Ion Diffusion Modulation and Anode Protection
journal, June 2015
- Xu, Wen-Tao; Peng, Hong-Jie; Huang, Jia-Qi
- ChemSusChem, Vol. 8, Issue 17
Direct Measurement of Polysulfide Shuttle Current: A Window into Understanding the Performance of Lithium-Sulfur Cells
journal, November 2014
- Moy, Derek; Manivannan, A.; Narayanan, S. R.
- Journal of The Electrochemical Society, Vol. 162, Issue 1
Sparingly Solvating Electrolytes for High Energy Density Lithium–Sulfur Batteries
journal, August 2016
- Cheng, Lei; Curtiss, Larry A.; Zavadil, Kevin R.
- ACS Energy Letters, Vol. 1, Issue 3
The Effect of Interactions and Reduction Products of LiNO 3 , the Anti-Shuttle Agent, in Li-S Battery Systems
journal, December 2014
- Rosenman, Ariel; Elazari, Ran; Salitra, Gregory
- Journal of The Electrochemical Society, Vol. 162, Issue 3
Following the Transient Reactions in Lithium–Sulfur Batteries Using an In Situ Nuclear Magnetic Resonance Technique
journal, April 2015
- Xiao, Jie; Hu, Jian Zhi; Chen, Honghao
- Nano Letters, Vol. 15, Issue 5
Building better lithium-sulfur batteries: from LiNO3 to solid oxide catalyst
journal, September 2016
- Ding, Ning; Zhou, Lan; Zhou, Changwei
- Scientific Reports, Vol. 6, Issue 1
Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries
journal, August 2014
- Pang, Quan; Kundu, Dipan; Cuisinier, Marine
- Nature Communications, Vol. 5, Issue 1
Effect of the Anion Activity on the Stability of Li Metal Anodes in Lithium-Sulfur Batteries
journal, March 2016
- Cao, Ruiguo; Chen, Junzheng; Han, Kee Sung
- Advanced Functional Materials, Vol. 26, Issue 18
Low Temperature Performance of Li/S Batteries
journal, January 2003
- Mikhaylik, Yuriy V.; Akridge, James R.
- Journal of The Electrochemical Society, Vol. 150, Issue 3
Improved cycling performances of lithium sulfur batteries with LiNO3-modified electrolyte
journal, November 2011
- Liang, Xiao; Wen, Zhaoyin; Liu, Yu
- Journal of Power Sources, Vol. 196, Issue 22
The critical role of lithium nitrate in the gas evolution of lithium–sulfur batteries
journal, January 2016
- Jozwiuk, Anna; Berkes, Balázs B.; Weiß, Thomas
- Energy & Environmental Science, Vol. 9, Issue 8
Role of LiNO3 in rechargeable lithium/sulfur battery
journal, May 2012
- Zhang, Sheng S.
- Electrochimica Acta, Vol. 70
Properties of surface film on lithium anode with LiNO3 as lithium salt in electrolyte solution for lithium–sulfur batteries
journal, November 2012
- Xiong, Shizhao; Xie, Kai; Diao, Yan
- Electrochimica Acta, Vol. 83
A new finding on the role of LiNO3 in lithium-sulfur battery
journal, August 2016
- Zhang, Sheng S.
- Journal of Power Sources, Vol. 322
On the Surface Chemical Aspects of Very High Energy Density, Rechargeable Li–Sulfur Batteries
journal, January 2009
- Aurbach, Doron; Pollak, Elad; Elazari, Ran
- Journal of The Electrochemical Society, Vol. 156, Issue 8, p. A694-A702
A Review of Solid Electrolyte Interphases on Lithium Metal Anode
journal, November 2015
- Cheng, Xin-Bing; Zhang, Rui; Zhao, Chen-Zi
- Advanced Science, Vol. 3, Issue 3
Recent Developments of the Lithium Metal Anode for Rechargeable Non-Aqueous Batteries
journal, July 2016
- Zhang, Kai; Lee, Gi-Hyeok; Park, Mihui
- Advanced Energy Materials, Vol. 6, Issue 20
An Artificial Solid Electrolyte Interphase Layer for Stable Lithium Metal Anodes
journal, December 2015
- Li, Nian-Wu; Yin, Ya-Xia; Yang, Chun-Peng
- Advanced Materials, Vol. 28, Issue 9
A lithium anode protection guided highly-stable lithium–sulfur battery
journal, January 2014
- Ma, Guoqiang; Wen, Zhaoyin; Wu, Meifen
- Chem. Commun., Vol. 50, Issue 91
Protected lithium anode with porous Al 2 O 3 layer for lithium–sulfur battery
journal, January 2015
- Jing, Hang-Kun; Kong, Ling-Long; Liu, Sheng
- Journal of Materials Chemistry A, Vol. 3, Issue 23
Dendrite-free Li deposition using trace-amounts of water as an electrolyte additive
journal, July 2015
- Qian, Jiangfeng; Xu, Wu; Bhattacharya, Priyanka
- Nano Energy, Vol. 15
Nitrogen-doped diamond-like carbon as optically transparent electrode for infrared attenuated total reflection spectroelectrochemistry
journal, January 2011
- Menegazzo, Nicola; Kahn, Markus; Berghauser, Roswitha
- The Analyst, Vol. 136, Issue 9
The synergetic effect of lithium polysulfide and lithium nitrate to prevent lithium dendrite growth
journal, June 2015
- Li, Weiyang; Yao, Hongbin; Yan, Kai
- Nature Communications, Vol. 6, Issue 1
Glyme−Lithium Salt Phase Behavior
journal, July 2006
- Henderson, Wesley A.
- The Journal of Physical Chemistry B, Vol. 110, Issue 26
Lithium metal protection through in-situ formed solid electrolyte interphase in lithium-sulfur batteries: The role of polysulfides on lithium anode
journal, September 2016
- Yan, Chong; Cheng, Xin-Bing; Zhao, Chen-Zi
- Journal of Power Sources, Vol. 327
High rate and stable cycling of lithium metal anode
journal, February 2015
- Qian, Jiangfeng; Henderson, Wesley A.; Xu, Wu
- Nature Communications, Vol. 6, Issue 1
Anode-Free Rechargeable Lithium Metal Batteries
journal, August 2016
- Qian, Jiangfeng; Adams, Brian D.; Zheng, Jianming
- Advanced Functional Materials, Vol. 26, Issue 39
Failure Mechanism for Fast-Charged Lithium Metal Batteries with Liquid Electrolytes
journal, September 2014
- Lu, Dongping; Shao, Yuyan; Lozano, Terence
- Advanced Energy Materials, Vol. 5, Issue 3
High Field Multinuclear NMR Investigation of the SEI Layer in Lithium Rechargeable Batteries
journal, January 2005
- Meyer, Benjamin M.; Leifer, Nicole; Sakamoto, Sarah
- Electrochemical and Solid-State Letters, Vol. 8, Issue 3
NMR Chemical Shifts of Trace Impurities: Common Laboratory Solvents, Organics, and Gases in Deuterated Solvents Relevant to the Organometallic Chemist
journal, May 2010
- Fulmer, Gregory R.; Miller, Alexander J. M.; Sherden, Nathaniel H.
- Organometallics, Vol. 29, Issue 9
Effects of Electrolyte Salts on the Performance of Li–O 2 Batteries
journal, February 2013
- Nasybulin, Eduard; Xu, Wu; Engelhard, Mark H.
- The Journal of Physical Chemistry C, Vol. 117, Issue 6
Ionic Liquid Electrolytes for Li–Air Batteries: Lithium Metal Cycling
journal, May 2014
- Grande, Lorenzo; Paillard, Elie; Kim, Guk-Tae
- International Journal of Molecular Sciences, Vol. 15, Issue 5
Effect of Discharge Cutoff Voltage on Reversibility of Lithium/Sulfur Batteries with LiNO 3 -Contained Electrolyte
journal, January 2012
- Zhang, Sheng S.
- Journal of The Electrochemical Society, Vol. 159, Issue 7
Catalytic Behavior of Lithium Nitrate in Li-O 2 Cells
journal, July 2015
- Sharon, Daniel; Hirsberg, Daniel; Afri, Michal
- ACS Applied Materials & Interfaces, Vol. 7, Issue 30
The Application of In Situ FTIR Spectroscopy to the Study of Surface Films Formed on Lithium and Noble Metals at Low Potentials in Li Battery Electrolytes
journal, January 1991
- Goren, Elisha
- Journal of The Electrochemical Society, Vol. 138, Issue 5
Synergistic Effect of Oxygen and LiNO 3 on the Interfacial Stability of Lithium Metal in a Li/O 2 Battery
journal, January 2013
- Giordani, Vincent; Walker, Wesley; Bryantsev, Vyacheslav S.
- Journal of The Electrochemical Society, Vol. 160, Issue 9
Enhanced cycling performance of a Li metal anode in a dimethylsulfoxide-based electrolyte using highly concentrated lithium salt for a lithium−oxygen battery
journal, March 2016
- Togasaki, Norihiro; Momma, Toshiyuki; Osaka, Tetsuya
- Journal of Power Sources, Vol. 307
On the Way Toward Understanding Solution Chemistry of Lithium Polysulfides for High Energy Li-S Redox Flow Batteries
journal, April 2015
- Pan, Huilin; Wei, Xiaoliang; Henderson, Wesley A.
- Advanced Energy Materials, Vol. 5, Issue 16
Enhanced Cyclability of Li/Polysulfide Batteries by a Polymer-Modified Carbon Paper Current Collector
journal, August 2015
- Cui, Yi; Fu, Yongzhu
- ACS Applied Materials & Interfaces, Vol. 7, Issue 36
A membrane-free lithium/polysulfide semi-liquid battery for large-scale energy storage
journal, January 2013
- Yang, Yuan; Zheng, Guangyuan; Cui, Yi
- Energy & Environmental Science, Vol. 6, Issue 5
A proof-of-concept lithium/sulfur liquid battery with exceptionally high capacity density
journal, August 2012
- Zhang, Sheng S.; Tran, Dat T.
- Journal of Power Sources, Vol. 211
Works referencing / citing this record:
Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries
journal, August 2018
- Pang, Quan; Shyamsunder, Abhinandan; Narayanan, Badri
- Nature Energy, Vol. 3, Issue 9
Insight into the effect of additives widely used in lithium–sulfur batteries
journal, January 2019
- Duangdangchote, Salatan; Krittayavathananon, Atiweena; Phattharasupakun, Nutthaphon
- Chemical Communications, Vol. 55, Issue 93
Stabilizing polymer electrolytes in high-voltage lithium batteries
journal, July 2019
- Choudhury, Snehashis; Tu, Zhengyuan; Nijamudheen, A.
- Nature Communications, Vol. 10, Issue 1
A Comprehensive Understanding of Lithium–Sulfur Battery Technology
journal, June 2019
- Li, Tao; Bai, Xue; Gulzar, Umair
- Advanced Functional Materials, Vol. 29, Issue 32
A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions
journal, January 2020
- Zhang, Xue‐Qiang; Li, Tao; Li, Bo‐Quan
- Angewandte Chemie, Vol. 132, Issue 8
Self‐Formed Protection Layer on a 3D Lithium Metal Anode for Ultrastable Lithium–Sulfur Batteries
journal, April 2019
- Yan, Xinxiu; Zhang, Huan; Huang, Meiling
- ChemSusChem, Vol. 12, Issue 10
Constructing Universal Ionic Sieves via Alignment of Two‐Dimensional Covalent Organic Frameworks (COFs)
journal, October 2018
- Jiang, Cheng; Tang, Mi; Zhu, Shaolong
- Angewandte Chemie, Vol. 130, Issue 49
Rational design of spontaneous reactions for protecting porous lithium electrodes in lithium–sulfur batteries
journal, July 2019
- Ren, Y. X.; Zeng, L.; Jiang, H. R.
- Nature Communications, Vol. 10, Issue 1
Constructing Universal Ionic Sieves via Alignment of Two‐Dimensional Covalent Organic Frameworks (COFs)
journal, December 2018
- Jiang, Cheng; Tang, Mi; Zhu, Shaolong
- Angewandte Chemie International Edition, Vol. 57, Issue 49
A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions
journal, February 2020
- Zhang, Xue‐Qiang; Li, Tao; Li, Bo‐Quan
- Angewandte Chemie International Edition, Vol. 59, Issue 8
Electrolyte Concentration Effect on Sulfur Utilization of Li-S Batteries
journal, January 2019
- Sun, Ke; Li, Na; Su, Dong
- Journal of The Electrochemical Society, Vol. 166, Issue 2
Development and Challenges of Functional Electrolytes for High-Performance Lithium-Sulfur Batteries
journal, July 2018
- Wang, Lili; Ye, Yusheng; Chen, Nan
- Advanced Functional Materials, Vol. 28, Issue 38
How Far Away Are Lithium-Sulfur Batteries From Commercialization?
journal, November 2019
- Zhu, Kunlei; Wang, Chao; Chi, Zixiang
- Frontiers in Energy Research, Vol. 7
Formulierung von Elektrolyten mit gemischten Lithiumsalzen für Lithium‐Batterien
journal, December 2019
- Xu, Gaojie; Shangguan, Xuehui; Dong, Shanmu
- Angewandte Chemie, Vol. 132, Issue 9
Formulation of Blended‐Lithium‐Salt Electrolytes for Lithium Batteries
journal, December 2019
- Xu, Gaojie; Shangguan, Xuehui; Dong, Shanmu
- Angewandte Chemie International Edition, Vol. 59, Issue 9
A Ceramic-PVDF Composite Membrane with Modified Interfaces as an Ion-Conducting Electrolyte for Solid-State Lithium-Ion Batteries Operating at Room Temperature
journal, July 2018
- Yu, Jing; Kwok, Stephen C. T.; Lu, Ziheng
- ChemElectroChem, Vol. 5, Issue 19
A Concentrated Ternary‐Salts Electrolyte for High Reversible Li Metal Battery with Slight Excess Li
journal, December 2018
- Qiu, Feilong; Li, Xiang; Deng, Han
- Advanced Energy Materials, Vol. 9, Issue 6
Tailored Reaction Route by Micropore Confinement for Li-S Batteries Operating under Lean Electrolyte Conditions
journal, May 2018
- Wang, Hui; Adams, Brian D.; Pan, Huilin
- Advanced Energy Materials, Vol. 8, Issue 21
Carbon-Metal Oxide Nanocomposites as Lithium-Sulfur Battery Cathodes
book, February 2021
- Zhu, Sheng; Li, Yan
- Functional Materials for Next-Generation Rechargeable Batteries
Innenrücktitelbild: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. 8/2020)
journal, January 2020
- Zhang, Xue‐Qiang; Li, Tao; Li, Bo‐Quan
- Angewandte Chemie, Vol. 132, Issue 8
Inside Back Cover: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. Int. Ed. 8/2020)
journal, February 2020
- Zhang, Xue‐Qiang; Li, Tao; Li, Bo‐Quan
- Angewandte Chemie International Edition, Vol. 59, Issue 8