skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Rational Design of Statically and Dynamically Stable Lithium-Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio

Abstract

Here, the primary challenge with lithium–sulfur battery research is the design of sulfur cathodes that exhibit high electrochemical efficiency and stability while keeping the sulfur content and loading high and the electrolyte/sulfur ratio low. With a systematic investigation, a novel graphene/cotton–carbon cathode is presented here that enables sulfur loading and content as high as 46 mg cm–2 and 70 wt% with an electrolyte/sulfur ratio of as low as only 5. The graphene/cotton–carbon cathodes deliver peak capacities of 926 and 765 mA h g–1, respectively, at C/10 and C/5 rates, which translate into high areal, gravimetric, and volumetric capacities of, respectively, 43 and 35 mA h cm–2, 648 and 536 mA h g–1, and 1067 and 881 mA h cm–3 with a stable cyclability. They also exhibit superior cell–storage capability with 95% capacity–retention, a low self–discharge constant of just 0.0012 per day, and stable poststorage cyclability after storing over a long period of six months. Here, this work demonstrates a viable approach to develop lithium–sulfur batteries with practical energy densities exceeding that of lithium–ion batteries.

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Texas at Austin, Austin, TX (United States)
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1488238
Alternate Identifier(s):
OSTI ID: 1414806
Grant/Contract Number:  
EE0007218; DE‐EE0007218
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 6; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; cyclability; high loading; lithium–sulfur batteries; low electrolyte batteries; low self‐discharge

Citation Formats

Chung, Sheng -Heng, and Manthiram, Arumugam. Rational Design of Statically and Dynamically Stable Lithium-Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio. United States: N. p., 2017. Web. https://doi.org/10.1002/adma.201705951.
Chung, Sheng -Heng, & Manthiram, Arumugam. Rational Design of Statically and Dynamically Stable Lithium-Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio. United States. https://doi.org/10.1002/adma.201705951
Chung, Sheng -Heng, and Manthiram, Arumugam. Fri . "Rational Design of Statically and Dynamically Stable Lithium-Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio". United States. https://doi.org/10.1002/adma.201705951. https://www.osti.gov/servlets/purl/1488238.
@article{osti_1488238,
title = {Rational Design of Statically and Dynamically Stable Lithium-Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio},
author = {Chung, Sheng -Heng and Manthiram, Arumugam},
abstractNote = {Here, the primary challenge with lithium–sulfur battery research is the design of sulfur cathodes that exhibit high electrochemical efficiency and stability while keeping the sulfur content and loading high and the electrolyte/sulfur ratio low. With a systematic investigation, a novel graphene/cotton–carbon cathode is presented here that enables sulfur loading and content as high as 46 mg cm–2 and 70 wt% with an electrolyte/sulfur ratio of as low as only 5. The graphene/cotton–carbon cathodes deliver peak capacities of 926 and 765 mA h g–1, respectively, at C/10 and C/5 rates, which translate into high areal, gravimetric, and volumetric capacities of, respectively, 43 and 35 mA h cm–2, 648 and 536 mA h g–1, and 1067 and 881 mA h cm–3 with a stable cyclability. They also exhibit superior cell–storage capability with 95% capacity–retention, a low self–discharge constant of just 0.0012 per day, and stable poststorage cyclability after storing over a long period of six months. Here, this work demonstrates a viable approach to develop lithium–sulfur batteries with practical energy densities exceeding that of lithium–ion batteries.},
doi = {10.1002/adma.201705951},
journal = {Advanced Materials},
number = 6,
volume = 30,
place = {United States},
year = {2017},
month = {12}
}

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

Citation Metrics:
Cited by: 22 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Highly Reversible Lithium/Dissolved Polysulfide Batteries with Carbon Nanotube Electrodes
journal, May 2013

  • Fu, Yongzhu; Su, Yu-Sheng; Manthiram, Arumugam
  • Angewandte Chemie International Edition, Vol. 52, Issue 27
  • DOI: 10.1002/anie.201301250

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
  • DOI: 10.1002/anie.201304762

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

Critical Link between Materials Chemistry and Cell-Level Design for High Energy Density and Low Cost Lithium-Sulfur Transportation Battery
journal, January 2015

  • Eroglu, Damla; Zavadil, Kevin R.; Gallagher, Kevin G.
  • Journal of The Electrochemical Society, Vol. 162, Issue 6
  • DOI: 10.1149/2.0611506jes

Micro- and Mesoporous Carbide-Derived Carbon-Selenium Cathodes for High-Performance Lithium Selenium Batteries
journal, August 2014

  • Lee, Jung Tae; Kim, Hyea; Oschatz, Martin
  • Advanced Energy Materials, Vol. 5, Issue 1
  • DOI: 10.1002/aenm.201400981

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

A Lithium/Dissolved Sulfur Battery with an Organic Electrolyte
journal, January 1979

  • Rauh, R. D.
  • Journal of The Electrochemical Society, Vol. 126, Issue 4
  • DOI: 10.1149/1.2129079

A Strategy for Configuration of an Integrated Flexible Sulfur Cathode for High-Performance Lithium-Sulfur Batteries
journal, February 2016

  • Wang, Hongqiang; Zhang, Wenchao; Liu, Huakun
  • Angewandte Chemie International Edition, Vol. 55, Issue 12
  • DOI: 10.1002/anie.201511673

Development and costs calculation of lithium–sulfur cells with high sulfur load and binder free electrodes
journal, February 2013


Graphene-based electrodes for electrochemical energy storage
journal, January 2013

  • Xu, Chaohe; Xu, Binghui; Gu, Yi
  • Energy & Environmental Science, Vol. 6, Issue 5
  • DOI: 10.1039/c3ee23870a

A sulfur host based on titanium monoxide@carbon hollow spheres for advanced lithium–sulfur batteries
journal, October 2016

  • Li, Zhen; Zhang, Jintao; Guan, Buyuan
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13065

Self-discharge of lithium–sulfur cells using stainless-steel current-collectors
journal, February 2005


Lithium-Sulfur Batteries: Progress and Prospects
journal, February 2015

  • Manthiram, Arumugam; Chung, Sheng-Heng; Zu, Chenxi
  • Advanced Materials, Vol. 27, Issue 12
  • DOI: 10.1002/adma.201405115

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

Improving Lithium–Sulfur Battery Performance under Lean Electrolyte through Nanoscale Confinement in Soft Swellable Gels
journal, April 2017


Understanding the Lithium Sulfur Battery System at Relevant Scales
journal, August 2015


Nanostructured energy materials for electrochemical energy conversion and storage: A review
journal, November 2016


Li–S batteries: simple approaches for superior performance
journal, January 2012

  • Demir-Cakan, Rezan; Morcrette, Mathieu
  • Energy & Environmental Science, Vol. 6, Issue 1
  • DOI: 10.1039/c2ee23411d

Recent progress and remaining challenges in sulfur-based lithium secondary batteries – a review
journal, January 2013

  • Bresser, Dominic; Passerini, Stefano; Scrosati, Bruno
  • Chemical Communications, Vol. 49, Issue 90
  • DOI: 10.1039/c3cc46131a

Progress Towards Commercially Viable Li-S Battery Cells
journal, April 2015

  • Urbonaite, Sigita; Poux, Tiphaine; Novák, Petr
  • Advanced Energy Materials, Vol. 5, Issue 16
  • DOI: 10.1002/aenm.201500118

Challenges in the development of advanced Li-ion batteries: a review
journal, January 2011

  • Etacheri, Vinodkumar; Marom, Rotem; Elazari, Ran
  • Energy & Environmental Science, Vol. 4, Issue 9
  • DOI: 10.1039/c1ee01598b

Lithium sulfur batteries, a mechanistic review
journal, January 2015

  • Wild, M.; O'Neill, L.; Zhang, T.
  • Energy & Environmental Science, Vol. 8, Issue 12
  • DOI: 10.1039/C5EE01388G

Carbon–sulfur composites for Li–S batteries: status and prospects
journal, January 2013

  • Wang, Da-Wei; Zeng, Qingcong; Zhou, Guangmin
  • Journal of Materials Chemistry A, Vol. 1, Issue 33
  • DOI: 10.1039/c3ta11045a

Bifunctional Separator with a Light-Weight Carbon-Coating for Dynamically and Statically Stable Lithium-Sulfur Batteries
journal, June 2014

  • Chung, Sheng-Heng; Manthiram, Arumugam
  • Advanced Functional Materials, Vol. 24, Issue 33
  • DOI: 10.1002/adfm.201400845

Li-ion battery materials: present and future
journal, June 2015


Lithium-Sulfur Cells: The Gap between the State-of-the-Art and the Requirements for High Energy Battery Cells
journal, April 2015

  • Hagen, Markus; Hanselmann, Dominik; Ahlbrecht, Katharina
  • Advanced Energy Materials, Vol. 5, Issue 16, 1401986
  • DOI: 10.1002/aenm.201401986

A Comprehensive Approach toward Stable Lithium–Sulfur Batteries with High Volumetric Energy Density
journal, November 2016

  • Pang, Quan; Liang, Xiao; Kwok, Chun Yuen
  • Advanced Energy Materials, Vol. 7, Issue 6
  • DOI: 10.1002/aenm.201601630

Lithium–Sulfur Batteries with the Lowest Self-Discharge and the Longest Shelf life
journal, April 2017


A layer-by-layer supramolecular structure for a sulfur cathode
journal, January 2016

  • Bucur, Claudiu B.; Muldoon, John; Lita, Adrian
  • Energy & Environmental Science, Vol. 9, Issue 3
  • DOI: 10.1039/C5EE02367J

Self-discharge characteristics of lithium/sulfur batteries using TEGDME liquid electrolyte
journal, December 2006


Porous Carbon Mat as an Electrochemical Testing Platform for Investigating the Polysulfide Retention of Various Cathode Configurations in Li–S Cells
journal, May 2015

  • Chung, Sheng-Heng; Singhal, Richa; Kalra, Vibha
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 12
  • DOI: 10.1021/acs.jpclett.5b00927

A Shell-Shaped Carbon Architecture with High-Loading Capability for Lithium Sulfide Cathodes
journal, May 2017

  • Chung, Sheng-Heng; Han, Pauline; Chang, Chi-Hao
  • Advanced Energy Materials, Vol. 7, Issue 17
  • DOI: 10.1002/aenm.201700537

A core–shell electrode for dynamically and statically stable Li–S battery chemistry
journal, January 2016

  • Chung, Sheng-Heng; Chang, Chi-Hao; Manthiram, Arumugam
  • Energy & Environmental Science, Vol. 9, Issue 10
  • DOI: 10.1039/C6EE01280A

A review of electrolytes for lithium–sulphur batteries
journal, June 2014


Attainable Gravimetric and Volumetric Energy Density of Li–S and Li Ion Battery Cells with Solid Separator-Protected Li Metal Anodes
journal, October 2015


Nanoarchitectured Graphene/CNT@Porous Carbon with Extraordinary Electrical Conductivity and Interconnected Micro/Mesopores for Lithium-Sulfur Batteries
journal, January 2014

  • Peng, Hong-Jie; Huang, Jia-Qi; Zhao, Meng-Qiang
  • Advanced Functional Materials, Vol. 24, Issue 19
  • DOI: 10.1002/adfm.201303296

A Carbon-Cotton Cathode with Ultrahigh-Loading Capability for Statically and Dynamically Stable Lithium–Sulfur Batteries
journal, October 2016


Multi-functional separator/interlayer system for high-stable lithium-sulfur batteries: Progress and prospects
journal, November 2015


Self-adaptive strain-relaxation optimization for high-energy lithium storage material through crumpling of graphene
journal, August 2014

  • Zhao, Yunlong; Feng, Jiangang; Liu, Xue
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5565

Carbonized Eggshell Membrane as a Natural Polysulfide Reservoir for Highly Reversible Li-S Batteries
journal, November 2013


Structural Design of Cathodes for Li-S Batteries
journal, April 2015


Highly Reversible Lithium/Dissolved Polysulfide Batteries with Carbon Nanotube Electrodes
journal, May 2013

  • Fu, Yongzhu; Su, Yu-Sheng; Manthiram, Arumugam
  • Angewandte Chemie, Vol. 125, Issue 27, p. 7068-7073
  • DOI: 10.1002/ange.201301250

    Works referencing / citing this record:

    Conductive CoOOH as Carbon‐Free Sulfur Immobilizer to Fabricate Sulfur‐Based Composite for Lithium–Sulfur Battery
    journal, April 2019

    • Wang, Zhen‐Yu; Wang, Lu; Liu, Sheng
    • Advanced Functional Materials, Vol. 29, Issue 23
    • DOI: 10.1002/adfm.201901051

    A Facile, Low-Cost Hot-Pressing Process for Fabricating Lithium-Sulfur Cells with Stable Dynamic and Static Electrochemistry
    journal, October 2018

    • Chung, Sheng-Heng; Lai, Ke-Yu; Manthiram, Arumugam
    • Advanced Materials, Vol. 30, Issue 46
    • DOI: 10.1002/adma.201805571

    Current Status and Future Prospects of Metal–Sulfur Batteries
    journal, May 2019


    A Nacre-Like Carbon Nanotube Sheet for High Performance Li-Polysulfide Batteries with High Sulfur Loading
    journal, April 2018


    Porphyrin-Derived Graphene-Based Nanosheets Enabling Strong Polysulfide Chemisorption and Rapid Kinetics in Lithium-Sulfur Batteries
    journal, April 2018

    • Kong, Long; Li, Bo-Quan; Peng, Hong-Jie
    • Advanced Energy Materials, Vol. 8, Issue 20
    • DOI: 10.1002/aenm.201800849

    Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries
    journal, June 2018

    • Luo, Liu; Chung, Sheng-Heng; Manthiram, Arumugam
    • Advanced Energy Materials, Vol. 8, Issue 24
    • DOI: 10.1002/aenm.201801014

    A Lithium-Sulfur Cell Based on Reversible Lithium Deposition from a Li 2 S Cathode Host onto a Hostless-Anode Substrate
    journal, July 2018

    • Nanda, Sanjay; Gupta, Abhay; Manthiram, Arumugam
    • Advanced Energy Materials, Vol. 8, Issue 25
    • DOI: 10.1002/aenm.201801556

    MoN Supported on Graphene as a Bifunctional Interlayer for Advanced Li‐S Batteries
    journal, November 2019


    ZnS coating of cathode facilitates lean‐electrolyte Li‐S batteries
    journal, October 2019

    • Shin, Woochul; Lu, Jun; Ji, Xiulei
    • Carbon Energy, Vol. 1, Issue 2
    • DOI: 10.1002/cey2.10

    Group IV Monochalcogenides MX (M=Ge, Sn; X=S, Se) as Chemical Anchors of Polysulfides for Lithium-Sulfur Batteries
    journal, July 2018

    • Lv, Xingshuai; Wei, Wei; Yang, Hongchao
    • Chemistry - A European Journal, Vol. 24, Issue 43
    • DOI: 10.1002/chem.201801925

    A Perspective on Energy Densities of Rechargeable Li-S Batteries and Alternative Sulfur-Based Cathode Materials
    journal, March 2018

    • Guo, Wei; Fu, Yongzhu
    • Energy & Environmental Materials, Vol. 1, Issue 1
    • DOI: 10.1002/eem2.12003

    Nonuniform Redistribution of Sulfur and Lithium upon Cycling: Probing the Origin of Capacity Fading in Lithium–Sulfur Pouch Cells
    journal, April 2019


    Polysulfide Shuttle Suppression by Electrolytes with Low‐Density for High‐Energy Lithium–Sulfur Batteries
    journal, May 2019

    • Weller, Christine; Pampel, Jonas; Dörfler, Susanne
    • Energy Technology, Vol. 7, Issue 12
    • DOI: 10.1002/ente.201900625

    Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries
    journal, October 2019

    • Li, Bo‐Quan; Kong, Long; Zhao, Chang‐Xin
    • InfoMat, Vol. 1, Issue 4
    • DOI: 10.1002/inf2.12056

    Dual‐Function, Tunable, Nitrogen‐Doped Carbon for High‐Performance Li Metal–Sulfur Full Cell
    journal, January 2019


    Structural Design of Lithium–Sulfur Batteries: From Fundamental Research to Practical Application
    journal, June 2018


    Bridging the academic and industrial metrics for next-generation practical batteries
    journal, February 2019


    Synchronous immobilization and conversion of polysulfides on a VO 2 –VN binary host targeting high sulfur load Li–S batteries
    journal, January 2018

    • Song, Yingze; Zhao, Wen; Kong, Long
    • Energy & Environmental Science, Vol. 11, Issue 9
    • DOI: 10.1039/c8ee01402g

    The fabrication of a 3D current collector with bitter melon-like TiO 2 –NCNFs for highly stable lithium–sulfur batteries
    journal, January 2019

    • Zhang, Xuzi; Chen, Zhihong; Shui, Lingling
    • Nanoscale Advances, Vol. 1, Issue 2
    • DOI: 10.1039/c8na00160j

    Graphene-based Fe-coordinated framework porphyrin as an interlayer for lithium–sulfur batteries
    journal, January 2019

    • Qin, Jin-Lei; Li, Bo-Quan; Huang, Jia-Qi
    • Materials Chemistry Frontiers, Vol. 3, Issue 4
    • DOI: 10.1039/c8qm00645h

    A lightweight and binder-free electrode enabled by lignin fibers@carbon-nanotubes and graphene for ultrastable lithium–sulfur batteries
    journal, January 2018

    • Liu, Tao; Sun, Shimei; Song, Wei
    • Journal of Materials Chemistry A, Vol. 6, Issue 46
    • DOI: 10.1039/c8ta08521h

    A core–shell cathode substrate for developing high-loading, high-performance lithium–sulfur batteries
    journal, January 2018

    • Yu, Ran; Chung, Sheng-Heng; Chen, Chun-Hua
    • Journal of Materials Chemistry A, Vol. 6, Issue 48
    • DOI: 10.1039/c8ta09059a

    Rational design of two-dimensional nanomaterials for lithium–sulfur batteries
    journal, January 2020

    • Jana, Milan; Xu, Rui; Cheng, Xin-Bing
    • Energy & Environmental Science, Vol. 13, Issue 4
    • DOI: 10.1039/c9ee02049g

    A sustainable sulfur–carbonaceous composite electrode toward high specific energy rechargeable cells
    journal, January 2020

    • Hwa, Yoon; Kim, Hyo Won; Shen, Hao
    • Materials Horizons, Vol. 7, Issue 2
    • DOI: 10.1039/c9mh01224a

    A Li–urine battery based on organic/aqueous hybrid electrolytes
    journal, January 2019

    • Lv, Yang; Shi, Shuai; Wang, Yahui
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 7
    • DOI: 10.1039/c9qi00291j

    Stabilization of Li–S batteries with a lean electrolyte via ion-exchange trapping of lithium polysulfides using a cationic, polybenzimidazolium binder
    journal, January 2020

    • Pham, Chuyen Van; Liu, Lili; Britton, Benjamin
    • Sustainable Energy & Fuels, Vol. 4, Issue 3
    • DOI: 10.1039/c9se01092k

    Akin solid–solid biphasic conversion of a Li–S battery achieved by coordinated carbonate electrolytes
    journal, January 2019

    • Huang, Feifei; Gao, Lujie; Zou, Yiping
    • Journal of Materials Chemistry A, Vol. 7, Issue 20
    • DOI: 10.1039/c9ta02877c

    Recent advances in polysulfide mediation of lithium-sulfur batteries via facile cathode and electrolyte modification
    journal, August 2019

    • Fang, Chen; Zhang, Guangzhao; Lau, Jonathan
    • APL Materials, Vol. 7, Issue 8
    • DOI: 10.1063/1.5110525

    Self-Discharge Behavior of Lithium-Sulfur Batteries at Different Electrolyte/Sulfur Ratios
    journal, January 2019

    • Shen, Chao; Xie, Jianxin; Zhang, Mei
    • Journal of The Electrochemical Society, Vol. 166, Issue 3
    • DOI: 10.1149/2.0461903jes

    Brush-structured sulfur–polyaniline–graphene composite as cathodes for lithium–sulfur batteries
    journal, November 2019

    • Liu, Heguang; Jing, Ruixuan; You, Caiyin
    • MRS Communications, Vol. 9, Issue 4
    • DOI: 10.1557/mrc.2019.149