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Title: Interfacial reaction dependent performance of hollow carbon nanosphere - sulfur composite as a cathode for Li-S battery

Abstract

Lithium-sulfur (Li-S) battery is a promising energy storage system due to its high energy density, cost effectiveness and environmental friendliness of sulfur. However, there are still a number of challenges, such as low Coulombic efficiency and poor long-term cycling stability, impeding the commercialization of Li-S battery. The electrochemical performance of Li-S battery is closely related with the interfacial reactions occurring between hosting substrate and active sulfur species which are poorly conducting at fully oxidized and reduced states. Here, we correlate the relationship between the performance and interfacial reactions in the Li-S battery system, using a hollow carbon nanosphere (HCNS) with highly graphitic character as hosting substrate for sulfur. With an appropriate amount of sulfur loading, HCNS/S composite exhibits excellent electrochemical performance because of the fast interfacial reactions between HCNS and the polysulfides. However, further increase of sulfur loading leads to increased formation of highly resistive insoluble reaction products (Li2S2/Li2S) which limits the reversibility of the interfacial reactions and results in poor electrochemical performance. In conclusion, these findings demonstrate the importance of the interfacial reaction reversibility in the whole electrode system on achieving high capacity and long cycle life of sulfur cathode for Li-S batteries.

Authors:
 [1];  [1];  [1];  [2];  [2];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. George Washington Univ., Washington, DC (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1221498
Report Number(s):
PNNL-SA-107585
Journal ID: ISSN 2296-598X; 48146; VT1201000
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Frontiers in Energy Research
Additional Journal Information:
Journal Volume: 3; Journal ID: ISSN 2296-598X
Publisher:
Frontiers Research Foundation
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 77 NANOSCIENCE AND NANOTECHNOLOGY; Environmental Molecular Sciences Laboratory; sulfur composite; interfacial reaction; sulfur utilization; cycling stability; rate capability; Li-S battery

Citation Formats

Zheng, Jianming, Yan, Pengfei, Gu, Meng, Wagner, Michael J., Hays, Kevin A., Chen, Junzheng, Li, Xiaohong S., Wang, Chong M., Zhang, Ji -Guang, Liu, Jun, and Xiao, Jie. Interfacial reaction dependent performance of hollow carbon nanosphere - sulfur composite as a cathode for Li-S battery. United States: N. p., 2015. Web. doi:10.3389/fenrg.2015.00025.
Zheng, Jianming, Yan, Pengfei, Gu, Meng, Wagner, Michael J., Hays, Kevin A., Chen, Junzheng, Li, Xiaohong S., Wang, Chong M., Zhang, Ji -Guang, Liu, Jun, & Xiao, Jie. Interfacial reaction dependent performance of hollow carbon nanosphere - sulfur composite as a cathode for Li-S battery. United States. https://doi.org/10.3389/fenrg.2015.00025
Zheng, Jianming, Yan, Pengfei, Gu, Meng, Wagner, Michael J., Hays, Kevin A., Chen, Junzheng, Li, Xiaohong S., Wang, Chong M., Zhang, Ji -Guang, Liu, Jun, and Xiao, Jie. Tue . "Interfacial reaction dependent performance of hollow carbon nanosphere - sulfur composite as a cathode for Li-S battery". United States. https://doi.org/10.3389/fenrg.2015.00025. https://www.osti.gov/servlets/purl/1221498.
@article{osti_1221498,
title = {Interfacial reaction dependent performance of hollow carbon nanosphere - sulfur composite as a cathode for Li-S battery},
author = {Zheng, Jianming and Yan, Pengfei and Gu, Meng and Wagner, Michael J. and Hays, Kevin A. and Chen, Junzheng and Li, Xiaohong S. and Wang, Chong M. and Zhang, Ji -Guang and Liu, Jun and Xiao, Jie},
abstractNote = {Lithium-sulfur (Li-S) battery is a promising energy storage system due to its high energy density, cost effectiveness and environmental friendliness of sulfur. However, there are still a number of challenges, such as low Coulombic efficiency and poor long-term cycling stability, impeding the commercialization of Li-S battery. The electrochemical performance of Li-S battery is closely related with the interfacial reactions occurring between hosting substrate and active sulfur species which are poorly conducting at fully oxidized and reduced states. Here, we correlate the relationship between the performance and interfacial reactions in the Li-S battery system, using a hollow carbon nanosphere (HCNS) with highly graphitic character as hosting substrate for sulfur. With an appropriate amount of sulfur loading, HCNS/S composite exhibits excellent electrochemical performance because of the fast interfacial reactions between HCNS and the polysulfides. However, further increase of sulfur loading leads to increased formation of highly resistive insoluble reaction products (Li2S2/Li2S) which limits the reversibility of the interfacial reactions and results in poor electrochemical performance. In conclusion, these findings demonstrate the importance of the interfacial reaction reversibility in the whole electrode system on achieving high capacity and long cycle life of sulfur cathode for Li-S batteries.},
doi = {10.3389/fenrg.2015.00025},
journal = {Frontiers in Energy Research},
number = ,
volume = 3,
place = {United States},
year = {Tue May 26 00:00:00 EDT 2015},
month = {Tue May 26 00:00:00 EDT 2015}
}

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In Situ Synthesis of Bipyramidal Sulfur with 3D Carbon Nanotube Framework for Lithium-Sulfur Batteries
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  • DOI: 10.1002/adfm.201302915

Sulfur-Impregnated Activated Carbon Fiber Cloth as a Binder-Free Cathode for Rechargeable Li-S Batteries
journal, November 2011

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A Soft Approach to Encapsulate Sulfur: Polyaniline Nanotubes for Lithium-Sulfur Batteries with Long Cycle Life
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High-Performance LiNi 0.5 Mn 1.5 O 4 Spinel Controlled by Mn 3+ Concentration and Site Disorder
journal, March 2012


Ultrasound Assisted Design of Sulfur/Carbon Cathodes with Partially Fluorinated Ether Electrolytes for Highly Efficient Li/S Batteries
journal, January 2013


Porous Hollow Carbon@Sulfur Composites for High-Power Lithium-Sulfur Batteries
journal, May 2011

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  • DOI: 10.1002/anie.201100637

Ordered mesoporous carbon/sulfur nanocomposite of high performances as cathode for lithium–sulfur battery
journal, November 2011


Interface modifications by anion receptors for high energy lithium ion batteries
journal, March 2014


Following the Transient Reactions in Lithium–Sulfur Batteries Using an In Situ Nuclear Magnetic Resonance Technique
journal, April 2015


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

Structural and Chemical Evolution of Li- and Mn-Rich Layered Cathode Material
journal, February 2015

  • Zheng, Jianming; Xu, Pinghong; Gu, Meng
  • Chemistry of Materials, Vol. 27, Issue 4
  • DOI: 10.1021/cm5045978

Hierarchically Structured Sulfur/Carbon Nanocomposite Material for High-Energy Lithium Battery
journal, October 2009

  • Liang, Chengdu; Dudney, Nancy J.; Howe, Jane Y.
  • Chemistry of Materials, Vol. 21, Issue 19, p. 4724-4730
  • DOI: 10.1021/cm902050j

Graphene Oxide as a Sulfur Immobilizer in High Performance Lithium/Sulfur Cells
journal, November 2011

  • Ji, Liwen; Rao, Mumin; Zheng, Haimei
  • Journal of the American Chemical Society, Vol. 133, Issue 46, p. 18522-18525
  • DOI: 10.1021/ja206955k

Orthorhombic Bipyramidal Sulfur Coated with Polypyrrole Nanolayers As a Cathode Material for Lithium–Sulfur Batteries
journal, April 2012

  • Fu, Yongzhu; Manthiram, Arumugam
  • The Journal of Physical Chemistry C, Vol. 116, Issue 16
  • DOI: 10.1021/jp300950m

Hollow Carbon Nanofiber-Encapsulated Sulfur Cathodes for High Specific Capacity Rechargeable Lithium Batteries
journal, October 2011

  • Zheng, Guangyuan; Yang, Yuan; Cha, Judy J.
  • Nano Letters, Vol. 11, Issue 10, p. 4462-4467
  • DOI: 10.1021/nl2027684

Lewis Acid–Base Interactions between Polysulfides and Metal Organic Framework in Lithium Sulfur Batteries
journal, April 2014

  • Zheng, Jianming; Tian, Jian; Wu, Dangxin
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl404721h

Mitigating Voltage Fade in Cathode Materials by Improving the Atomic Level Uniformity of Elemental Distribution
journal, April 2014

  • Zheng, Jianming; Gu, Meng; Genc, Arda
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl500486y

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

Manipulating surface reactions in lithium–sulphur batteries using hybrid anode structures
journal, January 2014

  • Huang, Cheng; Xiao, Jie; Shao, Yuyan
  • Nature Communications, Vol. 5, Issue 1, Article No. 3015
  • DOI: 10.1038/ncomms4015

A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries
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Sulfur–Polythiophene Composite Cathode Materials for Rechargeable Lithium Batteries
journal, January 2010

  • Wu, Feng; Wu, Shengxian; Chen, Renjie
  • Electrochemical and Solid-State Letters, Vol. 13, Issue 4
  • DOI: 10.1149/1.3290668

Revisit Carbon/Sulfur Composite for Li-S Batteries
journal, January 2013

  • Zheng, Jianming; Gu, Meng; Wagner, Michael J.
  • Journal of The Electrochemical Society, Vol. 160, Issue 10
  • DOI: 10.1149/2.013310jes

Controlled Nucleation and Growth Process of Li2S2/Li2S in Lithium-Sulfur Batteries
journal, January 2013

  • Zheng, Jianming; Gu, Meng; Wang, Chongmin
  • Journal of The Electrochemical Society, Vol. 160, Issue 11, p. A1992-A1996
  • DOI: 10.1149/2.032311jes

Direct Observation of Sulfur Radicals as Reaction Media in Lithium Sulfur Batteries
journal, December 2014

  • Wang, Qiang; Zheng, Jianming; Walter, Eric
  • Journal of The Electrochemical Society, Vol. 162, Issue 3
  • DOI: 10.1149/2.0851503jes

Lattice Mn 3+ Behaviors in Li 4 Ti 5 O 12 /LiNi 0.5 Mn 1.5 O 4 Full Cells
journal, January 2013

  • Zheng, Jianming; Xiao, Jie; Nie, Zimin
  • Journal of The Electrochemical Society, Vol. 160, Issue 8
  • DOI: 10.1149/2.097308jes

Works referencing / citing this record:

One-step synthesis of carbon nanosheet-decorated carbon nanofibers as a 3D interconnected porous carbon scaffold for lithium–sulfur batteries
journal, January 2017

  • Feng, Shuo; Song, Junhua; Fu, Shaofang
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