Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode
Abstract
The insulating nature of sulfur, polysulfide shuttle effect, and lithium metal deterioration cause a decrease in practical energy density and fast capacity fade in lithium-sulfur batteries. Here, we present an integrated strategy for the development of hybrid Li-S batteries based on a gel sulfur cathode, a solid electrolyte, and a protective anolyte composed of highly-concentrated salt electrolyte containing mixed additives. The dense solid electrolyte completely blocks polysulfide diffusion, and also makes it possible to investigate the cathode and anode independently. This gel cathode effectively traps the polysulfide active material while maintaining a low electrolyte to sulfur ratio (E/S) of 5.2 mL/g. The anolyte effectively protects the Li metal and suppresses the consumption of liquid electrolyte, enabling stable long-term cycling for over 700 hours in Li symmetric cells. This advanced design can simultaneously suppress the polysulfide shuttle, protect Li metal, and reduce the liquid electrolyte usage. The assembled hybrid batteries exhibit remarkably stable cycling performance over 300 cycles with high capacity. Finally, surface-sensitive techniques were carried out to directly visualize and to probe the interphase formed on the surface of the LAGP pellet, which may help stabilize the solid-liquid interface.
- Authors:
-
[1]
- Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program and Texas Materials Institute
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1598233
- Alternate Identifier(s):
- OSTI ID: 1464429
- Grant/Contract Number:
- SC0005397
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 23; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 25 ENERGY STORAGE; gel cathodes; lithium protection; lithium‐sulfur batteries; polysulfide trapping
Citation Formats
Xu, Henghui, Wang, Shaofei, and Manthiram, Arumugam. Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode. United States: N. p., 2018.
Web. doi:10.1002/aenm.201800813.
Xu, Henghui, Wang, Shaofei, & Manthiram, Arumugam. Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode. United States. https://doi.org/10.1002/aenm.201800813
Xu, Henghui, Wang, Shaofei, and Manthiram, Arumugam. Mon .
"Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode". United States. https://doi.org/10.1002/aenm.201800813. https://www.osti.gov/servlets/purl/1598233.
@article{osti_1598233,
title = {Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode},
author = {Xu, Henghui and Wang, Shaofei and Manthiram, Arumugam},
abstractNote = {The insulating nature of sulfur, polysulfide shuttle effect, and lithium metal deterioration cause a decrease in practical energy density and fast capacity fade in lithium-sulfur batteries. Here, we present an integrated strategy for the development of hybrid Li-S batteries based on a gel sulfur cathode, a solid electrolyte, and a protective anolyte composed of highly-concentrated salt electrolyte containing mixed additives. The dense solid electrolyte completely blocks polysulfide diffusion, and also makes it possible to investigate the cathode and anode independently. This gel cathode effectively traps the polysulfide active material while maintaining a low electrolyte to sulfur ratio (E/S) of 5.2 mL/g. The anolyte effectively protects the Li metal and suppresses the consumption of liquid electrolyte, enabling stable long-term cycling for over 700 hours in Li symmetric cells. This advanced design can simultaneously suppress the polysulfide shuttle, protect Li metal, and reduce the liquid electrolyte usage. The assembled hybrid batteries exhibit remarkably stable cycling performance over 300 cycles with high capacity. Finally, surface-sensitive techniques were carried out to directly visualize and to probe the interphase formed on the surface of the LAGP pellet, which may help stabilize the solid-liquid interface.},
doi = {10.1002/aenm.201800813},
journal = {Advanced Energy Materials},
number = 23,
volume = 8,
place = {United States},
year = {Mon May 28 00:00:00 EDT 2018},
month = {Mon May 28 00:00:00 EDT 2018}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 47 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Rechargeable Lithium–Sulfur Batteries
journal, July 2014
- Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
- Chemical Reviews, Vol. 114, Issue 23
Lithium-Sulfur Batteries: Electrochemistry, Materials, and Prospects
journal, November 2013
- Yin, Ya-Xia; Xin, Sen; Guo, Yu-Guo
- Angewandte Chemie International Edition, Vol. 52, Issue 50
A facile synthesis of three dimensional graphene sponge composited with sulfur nanoparticles for flexible Li–S cathodes
journal, January 2016
- Lin, Chao; Niu, Chaojiang; Xu, Xu
- Physical Chemistry Chemical Physics, Vol. 18, Issue 32
Review on High-Loading and High-Energy Lithium-Sulfur Batteries
journal, May 2017
- Peng, Hong-Jie; Huang, Jia-Qi; Cheng, Xin-Bing
- Advanced Energy Materials, Vol. 7, Issue 24
Hollow cobalt sulfide polyhedra-enabled long-life, high areal-capacity lithium-sulfur batteries
journal, March 2017
- Xu, Henghui; Manthiram, Arumugam
- Nano Energy, Vol. 33
An integrally-designed, flexible polysulfide host for high-performance lithium-sulfur batteries with stabilized lithium-metal anode
journal, August 2016
- Xu, Henghui; Qie, Long; Manthiram, Arumugam
- Nano Energy, Vol. 26
Yolk-Shelled C@Fe 3 O 4 Nanoboxes as Efficient Sulfur Hosts for High-Performance Lithium-Sulfur Batteries
journal, July 2017
- He, Jiarui; Luo, Liu; Chen, Yuanfu
- Advanced Materials, Vol. 29, Issue 34
A 3D Hybrid of Chemically Coupled Nickel Sulfide and Hollow Carbon Spheres for High Performance Lithium-Sulfur Batteries
journal, July 2017
- Ye, Chao; Zhang, Lei; Guo, Chunxian
- Advanced Functional Materials, Vol. 27, Issue 33
A facile soft-template synthesis of mesoporous polymeric and carbonaceous nanospheres
journal, December 2013
- Liu, Jian; Yang, Tianyu; Wang, Da-Wei
- Nature Communications, Vol. 4, Issue 1
Free-standing sulfur host based on titanium-dioxide-modified porous-carbon nanofibers for lithium-sulfur batteries
journal, July 2017
- Song, Xiong; Gao, Tuo; Wang, Suqing
- Journal of Power Sources, Vol. 356
A high strength, free-standing cathode constructed by regulating graphitization and the pore structure in nitrogen-doped carbon nanofibers for flexible lithium–sulfur batteries
journal, January 2017
- Song, Xiong; Wang, Suqing; Bao, Yue
- Journal of Materials Chemistry A, Vol. 5, Issue 15
High-Performance All-Solid-State Lithium–Sulfur Battery Enabled by a Mixed-Conductive Li 2 S Nanocomposite
journal, June 2016
- Han, Fudong; Yue, Jie; Fan, Xiulin
- Nano Letters, Vol. 16, Issue 7
Three-dimensional bilayer garnet solid electrolyte based high energy density lithium metal–sulfur batteries
journal, January 2017
- Fu, Kun (Kelvin); Gong, Yunhui; Hitz, Gregory T.
- Energy & Environmental Science, Vol. 10, Issue 7
A gel-ceramic multi-layer electrolyte for long-life lithium sulfur batteries
journal, January 2016
- Wang, Qingsong; Wen, Zhaoyin; Jin, Jun
- Chemical Communications, Vol. 52, Issue 8
Polysulfide-Shuttle Control in Lithium-Sulfur Batteries with a Chemically/Electrochemically Compatible NaSICON-Type Solid Electrolyte
journal, August 2016
- Yu, Xingwen; Bi, Zhonghe; Zhao, Feng
- Advanced Energy Materials, Vol. 6, Issue 24
Durability of the Li 1+ x Ti 2– x Al x (PO 4 ) 3 Solid Electrolyte in Lithium–Sulfur Batteries
journal, November 2016
- Wang, Shaofei; Ding, Yu; Zhou, Guangmin
- ACS Energy Letters, Vol. 1, Issue 6
A high performance lithium-ion sulfur battery based on a Li 2 S cathode using a dual-phase electrolyte
journal, January 2015
- Wang, Lina; Wang, Yonggang; Xia, Yongyao
- Energy & Environmental Science, Vol. 8, Issue 5
Lithium–sulfur batteries: Influence of C-rate, amount of electrolyte and sulfur loading on cycle performance
journal, December 2014
- Brückner, Jan; Thieme, Sören; Grossmann, Hannah Tamara
- Journal of Power Sources, Vol. 268
Cell energy density and electrolyte/sulfur ratio in Li–S cells
journal, October 2014
- Hagen, M.; Fanz, P.; Tübke, J.
- Journal of Power Sources, Vol. 264
Improving Lithium–Sulfur Battery Performance under Lean Electrolyte through Nanoscale Confinement in Soft Swellable Gels
journal, April 2017
- Chen, Junzheng; Henderson, Wesley A.; Pan, Huilin
- Nano Letters, Vol. 17, Issue 5
Stabilization of Garnet/Liquid Electrolyte Interface Using Superbase Additives for Hybrid Li Batteries
journal, June 2017
- Xu, Biyi; Duan, Huanan; Liu, Hezhou
- ACS Applied Materials & Interfaces, Vol. 9, Issue 25
Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
journal, December 2016
- Li, Yutao; Xu, Biyi; Xu, Henghui
- Angewandte Chemie International Edition, Vol. 56, Issue 3
Mastering the interface for advanced all-solid-state lithium rechargeable batteries
journal, November 2016
- Li, Yutao; Zhou, Weidong; Chen, Xi
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 47
Dynamic formation of a solid-liquid electrolyte interphase and its consequences for hybrid-battery concepts
journal, March 2016
- Busche, Martin R.; Drossel, Thomas; Leichtweiss, Thomas
- Nature Chemistry, Vol. 8, Issue 5
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
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
Liquid-Phase Electrochemical Scanning Electron Microscopy for In Situ Investigation of Lithium Dendrite Growth and Dissolution
journal, January 2017
- Rong, Genlan; Zhang, Xinyi; Zhao, Wen
- Advanced Materials, Vol. 29, Issue 13
Li 2 S 5 -based ternary-salt electrolyte for robust lithium metal anode
journal, April 2016
- Zhao, Chen-Zi; Cheng, Xin-Bing; Zhang, Rui
- Energy Storage Materials, Vol. 3
Suppression of Lithium Dendrite Formation by Using LAGP-PEO (LiTFSI) Composite Solid Electrolyte and Lithium Metal Anode Modified by PEO (LiTFSI) in All-Solid-State Lithium Batteries
journal, April 2017
- Wang, Chunhua; Yang, Yifu; Liu, Xingjiang
- ACS Applied Materials & Interfaces, Vol. 9, Issue 15
All-solid-state lithium-oxygen battery with high safety in wide ambient temperature range
journal, August 2015
- Kitaura, Hirokazu; Zhou, Haoshen
- Scientific Reports, Vol. 5, Issue 1
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
Formation and Inhibition of Metallic Lithium Microstructures in Lithium Batteries Driven by Chemical Crossover
journal, May 2017
- Li, Wangda; Kim, Un-Hyuck; Dolocan, Andrei
- ACS Nano, Vol. 11, Issue 6
The Electrochemical Behavior of Alkali and Alkaline Earth Metals in Nonaqueous Battery Systems—The Solid Electrolyte Interphase Model
journal, January 1979
- Peled, E.
- Journal of The Electrochemical Society, Vol. 126, Issue 12
XPS Valence Characterization of Lithium Salts as a Tool to Study Electrode/Electrolyte Interfaces of Li-Ion Batteries
journal, July 2006
- Dedryvère, R.; Leroy, S.; Martinez, H.
- The Journal of Physical Chemistry B, Vol. 110, Issue 26
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
In-situ FTIR investigations on the reduction of vinylene electrolyte additives suitable for use in lithium-ion batteries
journal, May 2004
- Santner, H. J.; Korepp, C.; Winter, M.
- Analytical and Bioanalytical Chemistry, Vol. 379, Issue 2
The Carbon Electrode in Nonaqueous Li–O2 Cells
journal, December 2012
- Ottakam Thotiyl, Muhammed M.; Freunberger, Stefan A.; Peng, Zhangquan
- Journal of the American Chemical Society, Vol. 135, Issue 1, p. 494-500
How To Improve Capacity and Cycling Stability for Next Generation Li–O 2 Batteries: Approach with a Solid Electrolyte and Elevated Redox Mediator Concentrations
journal, March 2016
- Bergner, Benjamin J.; Busche, Martin R.; Pinedo, Ricardo
- ACS Applied Materials & Interfaces, Vol. 8, Issue 12
Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
journal, December 2016
- Li, Yutao; Xu, Biyi; Xu, Henghui
- Angewandte Chemie, Vol. 129, Issue 3
Works referencing / citing this record:
Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating
journal, November 2018
- Liu, Wei; Xia, Yuting; Wang, Wenwu
- Advanced Energy Materials, Vol. 9, Issue 3
Metal Sulfide‐Decorated Carbon Sponge as a Highly Efficient Electrocatalyst and Absorbant for Polysulfide in High‐Loading Li 2 S Batteries
journal, April 2019
- He, Jiarui; Chen, Yuanfu; Manthiram, Arumugam
- Advanced Energy Materials, Vol. 9, Issue 20
Defect Control in the Synthesis of 2 D MoS 2 Nanosheets: Polysulfide Trapping in Composite Sulfur Cathodes for Li–S Batteries
journal, March 2020
- Abraham, Alyson; Wang, Lei; Quilty, Calvin D.
- ChemSusChem, Vol. 13, Issue 6
High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)
journal, August 2019
- Xu, Henghui; Chien, Po-Hsiu; Shi, Jianjian
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 38
Graphitic Mesoporous Carbon/Mn 7 C 3 as Polysulfide Host for High Rate Li-S Batteries
journal, January 2019
- Liang, Xiaoqiang; Guo, Wenbin; Zhang, Panpan
- Journal of The Electrochemical Society, Vol. 166, Issue 10