DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Toward Environmentally Friendly Lithium Sulfur Batteries: Probing the Role of Electrode Design in MoS2-Containing Li–S Batteries with a Green Electrolyte

Abstract

While lithium sulfur batteries (Li-S) hold promise as future high energy density low cost energy storage systems, barriers to implementation include low sulfur loading, limited cycle life, and the use of toxic electrolyte solvents. A comprehensive study of Li-S cells in the environmentally benign di(propylene glycol) dimethyl ether (DPGDME)-based electrolyte, using as-prepared MoS2 nanosheets derived from a facile aqueous microwave synthesis as polysulfide trapping agents, is reported herein for the first time. Conventional coated foil electrodes and binder-free electrodes (BFEs) with various structures are systematically generated and tested to correlate electrode design with the resulting electrochemical behavior. Significantly improved Li-S electrochemistry is demonstrated through the synergy of MoS2 chemistry and binder-free electrode engineering. In the coating configuration, the MoS2-containing cell evinced better rate performance and more stable cyclability than cell without MoS2. In comparison with the coating counterparts, the BFE cells exhibited excellent cycle stability and superior rate capability (10- fold capacties and energy density per electrode weight with 20% higher retention rate) despite 2X higher areal sulfur loading. The BFE cell improvement can be attributed to the synergistic effect of the i) interconnected macroporous structure of CNT interlayers, providing a conductive framework; and ii) the efficient polysulfide trapping bymore » the MoS2 nanosheets.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]
  1. State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
  2. State Univ. of New York at Stony Brook, Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1496231
Alternate Identifier(s):
OSTI ID: 1503512
Report Number(s):
BNL-211467-2019-JAAM
Journal ID: ISSN 2168-0485
Grant/Contract Number:  
EE0008208; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 7; Journal Issue: 5; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Electrode design; Green electrolyte; Li−S battery; MoS2 nanosheet; Polysulfide; Sulfur

Citation Formats

Wang, Lei, Abraham, Alyson, Lutz, Diana M., Quilty, Calvin D., Takeuchi, Esther S., Takeuchi, Kenneth J., and Marschilok, Amy C. Toward Environmentally Friendly Lithium Sulfur Batteries: Probing the Role of Electrode Design in MoS2-Containing Li–S Batteries with a Green Electrolyte. United States: N. p., 2019. Web. doi:10.1021/acssuschemeng.8b06141.
Wang, Lei, Abraham, Alyson, Lutz, Diana M., Quilty, Calvin D., Takeuchi, Esther S., Takeuchi, Kenneth J., & Marschilok, Amy C. Toward Environmentally Friendly Lithium Sulfur Batteries: Probing the Role of Electrode Design in MoS2-Containing Li–S Batteries with a Green Electrolyte. United States. https://doi.org/10.1021/acssuschemeng.8b06141
Wang, Lei, Abraham, Alyson, Lutz, Diana M., Quilty, Calvin D., Takeuchi, Esther S., Takeuchi, Kenneth J., and Marschilok, Amy C. Mon . "Toward Environmentally Friendly Lithium Sulfur Batteries: Probing the Role of Electrode Design in MoS2-Containing Li–S Batteries with a Green Electrolyte". United States. https://doi.org/10.1021/acssuschemeng.8b06141. https://www.osti.gov/servlets/purl/1496231.
@article{osti_1496231,
title = {Toward Environmentally Friendly Lithium Sulfur Batteries: Probing the Role of Electrode Design in MoS2-Containing Li–S Batteries with a Green Electrolyte},
author = {Wang, Lei and Abraham, Alyson and Lutz, Diana M. and Quilty, Calvin D. and Takeuchi, Esther S. and Takeuchi, Kenneth J. and Marschilok, Amy C.},
abstractNote = {While lithium sulfur batteries (Li-S) hold promise as future high energy density low cost energy storage systems, barriers to implementation include low sulfur loading, limited cycle life, and the use of toxic electrolyte solvents. A comprehensive study of Li-S cells in the environmentally benign di(propylene glycol) dimethyl ether (DPGDME)-based electrolyte, using as-prepared MoS2 nanosheets derived from a facile aqueous microwave synthesis as polysulfide trapping agents, is reported herein for the first time. Conventional coated foil electrodes and binder-free electrodes (BFEs) with various structures are systematically generated and tested to correlate electrode design with the resulting electrochemical behavior. Significantly improved Li-S electrochemistry is demonstrated through the synergy of MoS2 chemistry and binder-free electrode engineering. In the coating configuration, the MoS2-containing cell evinced better rate performance and more stable cyclability than cell without MoS2. In comparison with the coating counterparts, the BFE cells exhibited excellent cycle stability and superior rate capability (10- fold capacties and energy density per electrode weight with 20% higher retention rate) despite 2X higher areal sulfur loading. The BFE cell improvement can be attributed to the synergistic effect of the i) interconnected macroporous structure of CNT interlayers, providing a conductive framework; and ii) the efficient polysulfide trapping by the MoS2 nanosheets.},
doi = {10.1021/acssuschemeng.8b06141},
journal = {ACS Sustainable Chemistry & Engineering},
number = 5,
volume = 7,
place = {United States},
year = {Mon Feb 04 00:00:00 EST 2019},
month = {Mon Feb 04 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Advances in Li–S batteries
journal, January 2010

  • Ji, Xiulei; Nazar, Linda F.
  • Journal of Materials Chemistry, Vol. 20, Issue 44, p. 9821-9826
  • DOI: 10.1039/b925751a

Understanding Conversion-Type Electrodes for Lithium Rechargeable Batteries
journal, January 2018


Recent development of metal compound applications in lithium–sulphur batteries
journal, July 2017


Polysulfide Shuttle Study in the Li/S Battery System
journal, January 2004

  • Mikhaylik, Yuriy V.; Akridge, James R.
  • Journal of The Electrochemical Society, Vol. 151, Issue 11, p. A1969-A1976
  • DOI: 10.1149/1.1806394

New Approaches for High Energy Density Lithium–Sulfur Battery Cathodes
journal, June 2012

  • Evers, Scott; Nazar, Linda F.
  • Accounts of Chemical Research, Vol. 46, Issue 5
  • DOI: 10.1021/ar3001348

Transport Properties of Polysulfide Species in Lithium–Sulfur Battery Electrolytes: Coupling of Experiment and Theory
journal, July 2016


“Shuttle” in Polysulfide Shuttle: Friend or Foe?
journal, September 2018

  • Mistry, Aashutosh N.; Mukherjee, Partha P.
  • The Journal of Physical Chemistry C, Vol. 122, Issue 42
  • DOI: 10.1021/acs.jpcc.8b06077

A conductive interwoven bamboo carbon fiber membrane for Li–S batteries
journal, January 2015

  • Gu, Xingxing; Lai, Chao; Liu, Fei
  • Journal of Materials Chemistry A, Vol. 3, Issue 18
  • DOI: 10.1039/C5TA00681C

A simple approach for making a viable, safe, and high-performances lithium-sulfur battery
journal, February 2018


Fabricating multifunctional nanoparticle membranes by a fast layer-by-layer Langmuir–Blodgett process: application in lithium–sulfur batteries
journal, January 2016

  • Kim, M. S.; Ma, L.; Choudhury, S.
  • Journal of Materials Chemistry A, Vol. 4, Issue 38
  • DOI: 10.1039/C6TA06018H

Biomimetic Ant-Nest Electrode Structures for High Sulfur Ratio Lithium–Sulfur Batteries
journal, August 2016


Nanostructured Host Materials for Trapping Sulfur in Rechargeable Li-S Batteries: Structure Design and Interfacial Chemistry
journal, November 2017


Two-Dimensional Materials for Beyond-Lithium-Ion Batteries
journal, March 2016


High Energy Density Lithium-Sulfur Batteries: Challenges of Thick Sulfur Cathodes
journal, March 2015

  • Lv, Dongping; Zheng, Jianming; Li, Qiuyan
  • Advanced Energy Materials, Vol. 5, Issue 16, Article No. 1402290
  • DOI: 10.1002/aenm.201402290

Tailoring Porosity in Carbon Nanospheres for Lithium–Sulfur Battery Cathodes
journal, November 2013

  • He, Guang; Evers, Scott; Liang, Xiao
  • ACS Nano, Vol. 7, Issue 12
  • DOI: 10.1021/nn404439r

Enabling High-Energy-Density Cathode for Lithium–Sulfur Batteries
journal, June 2018

  • Lu, Dongping; Li, Qiuyan; Liu, Jian
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 27
  • DOI: 10.1021/acsami.8b05166

Eggshell Membrane-Derived Polysulfide Absorbents for Highly Stable and Reversible Lithium–Sulfur Cells
journal, September 2014

  • Chung, Sheng-Heng; Manthiram, Arumugam
  • ACS Sustainable Chemistry & Engineering, Vol. 2, Issue 10
  • DOI: 10.1021/sc500452j

Enhancement of electrochemical properties by polysulfide trapping in a graphene-coated sulfur cathode on patterned current collector
journal, January 2016

  • Yu, Seung-Ho; Lee, Bora; Choi, Sinho
  • Chemical Communications, Vol. 52, Issue 15
  • DOI: 10.1039/C5CC09694D

Highly flexible, freestanding tandem sulfur cathodes for foldable Li–S batteries with a high areal capacity
journal, January 2017

  • Chang, Chi-Hao; Chung, Sheng-Heng; Manthiram, Arumugam
  • Materials Horizons, Vol. 4, Issue 2
  • DOI: 10.1039/C6MH00426A

Designing Lithium-Sulfur Cells with Practically Necessary Parameters
journal, April 2018


High performance lithium sulfur batteries with a cassava-derived carbon sheet as a polysulfides inhibitor
journal, January 2014

  • Qin, Furong; Zhang, Kai; Fang, Jing
  • New J. Chem., Vol. 38, Issue 9
  • DOI: 10.1039/C4NJ00701H

Low Cost Metal Carbide Nanocrystals as Binding and Electrocatalytic Sites for High Performance Li–S Batteries
journal, January 2018


Interwoven MXene Nanosheet/Carbon-Nanotube Composites as Li-S Cathode Hosts
journal, November 2016

  • Liang, Xiao; Rangom, Yverick; Kwok, Chun Yuen
  • Advanced Materials, Vol. 29, Issue 3
  • DOI: 10.1002/adma.201603040

Tungsten Disulfide Catalysts Supported on a Carbon Cloth Interlayer for High Performance Li-S Battery
journal, January 2017

  • Park, Jungjin; Yu, Byeong-Chul; Park, Joong Sun
  • Advanced Energy Materials, Vol. 7, Issue 11
  • DOI: 10.1002/aenm.201602567

Catalytic oxidation of Li 2 S on the surface of metal sulfides for Li−S batteries
journal, January 2017

  • Zhou, Guangmin; Tian, Hongzhen; Jin, Yang
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 5
  • DOI: 10.1073/pnas.1615837114

Sulfur film sandwiched between few-layered MoS 2 electrocatalysts and conductive reduced graphene oxide as a robust cathode for advanced lithium–sulfur batteries
journal, January 2018

  • Wei, Yanju; Kong, Zhenkai; Pan, Yankai
  • Journal of Materials Chemistry A, Vol. 6, Issue 14
  • DOI: 10.1039/C8TA00222C

Rational design of a multidimensional N-doped porous carbon/MoS 2 /CNT nano-architecture hybrid for high performance lithium–sulfur batteries
journal, January 2018

  • Ren, Juan; Zhou, Yibei; Xia, Li
  • Journal of Materials Chemistry A, Vol. 6, Issue 28
  • DOI: 10.1039/C8TA04675A

Interaction of FeS 2 and Sulfur in Li-S Battery System
journal, September 2016

  • Sun, Ke; Cama, Christina A.; DeMayo, Rachel A.
  • Journal of The Electrochemical Society, Vol. 164, Issue 1
  • DOI: 10.1149/2.0041701jes

Properties of graphene-metal contacts probed by Raman spectroscopy
journal, February 2018


Rational design of exfoliated 1T MoS 2 @CNT-based bifunctional separators for lithium sulfur batteries
journal, January 2017

  • Jeong, Y. C.; Kim, J. H.; Kwon, S. H.
  • Journal of Materials Chemistry A, Vol. 5, Issue 45
  • DOI: 10.1039/C7TA08153G

A highly efficient double-hierarchical sulfur host for advanced lithium–sulfur batteries
journal, January 2018

  • Hu, Linyu; Dai, Chunlong; Lim, Jin-Myoung
  • Chemical Science, Vol. 9, Issue 3
  • DOI: 10.1039/C7SC03960C

Understanding the Anchoring Effect of Two-Dimensional Layered Materials for Lithium–Sulfur Batteries
journal, May 2015


High Electrochemical Selectivity of Edge versus Terrace Sites in Two-Dimensional Layered MoS 2 Materials
journal, November 2014

  • Wang, Haotian; Zhang, Qianfan; Yao, Hongbin
  • Nano Letters, Vol. 14, Issue 12
  • DOI: 10.1021/nl503730c

Highly conductive carbon black supported amorphous molybdenum disulfide for efficient hydrogen evolution reaction
journal, April 2017


Vertically Aligned Interlayer Expanded MoS 2 Nanosheets on a Carbon Support for Hydrogen Evolution Electrocatalysis
journal, March 2017


Preparation, characterization and properties of MoS2 nanosheets via a microwave-assisted wet-chemical route
journal, April 2018


Effects of Liquid Electrolytes on the Charge–Discharge Performance of Rechargeable Lithium/Sulfur Batteries: Electrochemical and in-Situ X-ray Absorption Spectroscopic Studies
journal, October 2011

  • Gao, Jie; Lowe, Michael A.; Kiya, Yasuyuki
  • The Journal of Physical Chemistry C, Vol. 115, Issue 50, p. 25132-25137
  • DOI: 10.1021/jp207714c

Lithium–sulfur batteries—the solution is in the electrolyte, but is the electrolyte a solution?
journal, January 2014

  • Barghamadi, Marzieh; Best, Adam S.; Bhatt, Anand I.
  • Energy Environ. Sci., Vol. 7, Issue 12
  • DOI: 10.1039/C4EE02192D

Probing Titanium Disulfide-Sulfur Composite Materials for Li-S Batteries via In Situ X-ray Diffraction (XRD)
journal, January 2017

  • Zhang, Qing; Bock, David C.; Takeuchi, Kenneth J.
  • Journal of The Electrochemical Society, Vol. 164, Issue 4
  • DOI: 10.1149/2.1661704jes

Glymes as versatile solvents for chemical reactions and processes: from the laboratory to industry
journal, January 2014


Oxidative-Stability Enhancement and Charge Transport Mechanism in Glyme–Lithium Salt Equimolar Complexes
journal, August 2011

  • Yoshida, Kazuki; Nakamura, Megumi; Kazue, Yuichi
  • Journal of the American Chemical Society, Vol. 133, Issue 33, p. 13121-13129
  • DOI: 10.1021/ja203983r

New toxicity data for the propylene glycol ethers – a commitment to public health and safety
journal, March 2005


Synthesis and Characterization of CuFe 2 O 4 Nano/Submicron Wire–Carbon Nanotube Composites as Binder-free Anodes for Li-Ion Batteries
journal, February 2018

  • Wang, Lei; Bock, David C.; Li, Jing
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 10
  • DOI: 10.1021/acsami.8b00244

Potassium-Based α-Manganese Dioxide Nanofiber Binder-Free Self-Supporting Electrodes: A Design Strategy for High Energy Density Batteries
journal, May 2016

  • Poyraz, Altug S.; Huang, Jianping; Wu, Lijun
  • Energy Technology, Vol. 4, Issue 11
  • DOI: 10.1002/ente.201600128

A binder-free sulfur/carbon composite electrode prepared by a sulfur sublimation method for Li–S batteries
journal, January 2016


A Binder Free and High Sulfur Loaded Three-Dimensional Carbon Nanotubes Electrode for High Performance Li-S Batteries
journal, July 2017

  • Patel, Mumukshu D.; Cha, Eunho; Choi, Wonbong
  • ECS Transactions, Vol. 77, Issue 11
  • DOI: 10.1149/07711.0437ecst

Stabilizing polysulfide-shuttle in a Li–S battery using transition metal carbide nanostructures
journal, January 2016

  • Al Salem, Hesham; Chitturi, Venkateswara Rao; Babu, Ganguli
  • RSC Advances, Vol. 6, Issue 111
  • DOI: 10.1039/C6RA22434B

Ligand-induced dependence of charge transfer in nanotube–quantum dot heterostructures
journal, January 2016

  • Wang, Lei; Han, Jinkyu; Sundahl, Bryan
  • Nanoscale, Vol. 8, Issue 34
  • DOI: 10.1039/C6NR03091B

A Catalytic Etching-Wetting-Dewetting Mechanism in the Formation of Hollow Graphitic Carbon Fiber
journal, February 2017


In situ crystallization kinetics of two-dimensional MoS 2
journal, November 2017


Defect engineering of two-dimensional transition metal dichalcogenides
journal, April 2016


Anomalous Lattice Vibrations of Single- and Few-Layer MoS 2
journal, March 2010

  • Lee, Changgu; Yan, Hugen; Brus, Louis E.
  • ACS Nano, Vol. 4, Issue 5
  • DOI: 10.1021/nn1003937

Lignin-assisted exfoliation of molybdenum disulfide in aqueous media and its application in lithium ion batteries
journal, January 2015

  • Liu, Wanshuang; Zhao, Chenyang; Zhou, Rui
  • Nanoscale, Vol. 7, Issue 21
  • DOI: 10.1039/C5NR01891A

Lithium Polysulfide Radical Anions in Ether-Based Solvents
journal, August 2016

  • Wujcik, Kevin H.; Wang, Dunyang Rita; Raghunathan, Aditya
  • The Journal of Physical Chemistry C, Vol. 120, Issue 33
  • DOI: 10.1021/acs.jpcc.6b04264

Experimental and Theoretical Analysis of Products and Reaction Intermediates of Lithium–Sulfur Batteries
journal, May 2014

  • Cañas, Natalia A.; Fronczek, David N.; Wagner, Norbert
  • The Journal of Physical Chemistry C, Vol. 118, Issue 23
  • DOI: 10.1021/jp5013208

Confining Sulfur in N-Doped Porous Carbon Microspheres Derived from Microalgaes for Advanced Lithium–Sulfur Batteries
journal, July 2017

  • Xia, Yang; Fang, Ruyi; Xiao, Zhen
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 28
  • DOI: 10.1021/acsami.7b05798

Spherical Macroporous Carbon Nanotube Particles with Ultrahigh Sulfur Loading for Lithium–Sulfur Battery Cathodes
journal, January 2018


A Lithium-Ion Battery using a 3 D-Array Nanostructured Graphene-Sulfur Cathode and a Silicon Oxide-Based Anode
journal, April 2018

  • Benítez, Almudena; Di Lecce, Daniele; Elia, Giuseppe Antonio
  • ChemSusChem, Vol. 11, Issue 9
  • DOI: 10.1002/cssc.201800242

Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer
journal, January 2012

  • Su, Yu-Sheng; Manthiram, Arumugam
  • Nature Communications, Vol. 3, Article No. 1166
  • DOI: 10.1038/ncomms2163

Thin-Layered Molybdenum Disulfide Nanoparticles as an Effective Polysulfide Mediator in Lithium–Sulfur Batteries
journal, June 2018

  • Han, Pauline; Chung, Sheng-Heng; Manthiram, Arumugam
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 27
  • DOI: 10.1021/acsami.8b05397

Mitigation of Shuttle Effect in Li–S Battery Using a Self-Assembled Ultrathin Molybdenum Disulfide Interlayer
journal, December 2018

  • Yu, Xiaoyun; Zhou, Guangmin; Cui, Yi
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 3
  • DOI: 10.1021/acsami.8b19354

MoS 2 /Celgard Separator as Efficient Polysulfide Barrier for Long-Life Lithium-Sulfur Batteries
journal, March 2017

  • Ghazi, Zahid Ali; He, Xiao; Khattak, Abdul Muqsit
  • Advanced Materials, Vol. 29, Issue 21
  • DOI: 10.1002/adma.201606817

Single step transformation of sulphur to Li2S2/Li2S in Li-S batteries
journal, July 2015

  • Helen, M.; Reddy, M. Anji; Diemant, Thomas
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep12146

Works referencing / citing this record:

Defect Control in the Synthesis of 2 D MoS 2 Nanosheets: Polysulfide Trapping in Composite Sulfur Cathodes for Li–S Batteries
journal, March 2020


Encapsulation of Few-Layer MoS2 in the Pores of Mesoporous Carbon Hollow Spheres for Lithium-Sulfur Batteries
journal, September 2019

  • Zhao, Yunyan; Zhuang, Qianyu; Li, Wenda
  • Nanomaterials, Vol. 9, Issue 9
  • DOI: 10.3390/nano9091247