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

Title: Li2S encapsulated by nitrogen-doped carbon for lithium sulfur batteries

Abstract

Using high-energy ball milling of the Li2S plus carbon black mixture followed by carbonization of pyrrole, we have established a facile approach to synthesize Li2S-plus-C composite particles of average size 400 nm, encapsulated by a nitrogen-doped carbon shell. Such an engineered core–shell structure exhibits an ultrahigh initial discharge specific capacity (1029 mAh/g), reaching 88% of the theoretical capacity (1,166 mAh/g of Li2S) and thus offering the highest utilization of Li2S in the cathode among all of the reported works for the encapsulated Li2S cathodes. This Li2S/C composite core with a nitrogen-doped carbon shell can still retain 652 mAh/g after prolonged 100 cycles. These superior properties are attributed to the nitrogen-doped carbon shell that can improve the conductivity to enhance the utilization of Li2S in the cathode. As a result, fine particle sizes and the presence of carbon black within the Li2S core may also play a role in high utilization of Li2S in the cathode.

Authors:
 [1];  [2];  [1];  [1];  [1]
  1. Wanger Institute for Sustainable Energy Research, Chicago, IL (United States); Illinois Institute of Technology, Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1237306
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 2; Journal Issue: 42; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Chen, Lin, Liu, Yuzi, Ashuri, Maziar, Liu, Caihong, and Shaw, Leon L. Li2S encapsulated by nitrogen-doped carbon for lithium sulfur batteries. United States: N. p., 2014. Web. doi:10.1039/C4TA04103H.
Chen, Lin, Liu, Yuzi, Ashuri, Maziar, Liu, Caihong, & Shaw, Leon L. Li2S encapsulated by nitrogen-doped carbon for lithium sulfur batteries. United States. https://doi.org/10.1039/C4TA04103H
Chen, Lin, Liu, Yuzi, Ashuri, Maziar, Liu, Caihong, and Shaw, Leon L. Fri . "Li2S encapsulated by nitrogen-doped carbon for lithium sulfur batteries". United States. https://doi.org/10.1039/C4TA04103H. https://www.osti.gov/servlets/purl/1237306.
@article{osti_1237306,
title = {Li2S encapsulated by nitrogen-doped carbon for lithium sulfur batteries},
author = {Chen, Lin and Liu, Yuzi and Ashuri, Maziar and Liu, Caihong and Shaw, Leon L.},
abstractNote = {Using high-energy ball milling of the Li2S plus carbon black mixture followed by carbonization of pyrrole, we have established a facile approach to synthesize Li2S-plus-C composite particles of average size 400 nm, encapsulated by a nitrogen-doped carbon shell. Such an engineered core–shell structure exhibits an ultrahigh initial discharge specific capacity (1029 mAh/g), reaching 88% of the theoretical capacity (1,166 mAh/g of Li2S) and thus offering the highest utilization of Li2S in the cathode among all of the reported works for the encapsulated Li2S cathodes. This Li2S/C composite core with a nitrogen-doped carbon shell can still retain 652 mAh/g after prolonged 100 cycles. These superior properties are attributed to the nitrogen-doped carbon shell that can improve the conductivity to enhance the utilization of Li2S in the cathode. As a result, fine particle sizes and the presence of carbon black within the Li2S core may also play a role in high utilization of Li2S in the cathode.},
doi = {10.1039/C4TA04103H},
journal = {Journal of Materials Chemistry. A},
number = 42,
volume = 2,
place = {United States},
year = {Fri Sep 26 00:00:00 EDT 2014},
month = {Fri Sep 26 00:00:00 EDT 2014}
}

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

Citation Metrics:
Cited by: 84 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

3D Hyperbranched Hollow Carbon Nanorod Architectures for High-Performance Lithium-Sulfur Batteries
journal, January 2014

  • Chen, Shuangqiang; Huang, Xiaodan; Liu, Hao
  • Advanced Energy Materials, Vol. 4, Issue 8
  • DOI: 10.1002/aenm.201301761

A High-Performance Polymer Tin Sulfur Lithium Ion Battery
journal, February 2010

  • Hassoun, Jusef; Scrosati, Bruno
  • Angewandte Chemie International Edition, Vol. 49, Issue 13, p. 2371-2374
  • DOI: 10.1002/anie.200907324

Preparation of carbon-coated MgFe2O4 with excellent cycling and rate performance
journal, February 2013


Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium–Sulfur Battery Cathode Material with High Capacity and Cycling Stability
journal, July 2011

  • Wang, Hailiang; Yang, Yuan; Liang, Yongye
  • Nano Letters, Vol. 11, Issue 7, p. 2644-2647
  • DOI: 10.1021/nl200658a

Stabilizing lithium–sulphur cathodes using polysulphide reservoirs
journal, May 2011

  • Ji, Xiulei; Evers, Scott; Black, Robert
  • Nature Communications, Vol. 2, Article No. 325
  • DOI: 10.1038/ncomms1293

Nanostructured Materials for Electrochemical Energy Conversion and Storage Devices
journal, August 2008


Enhancement of long stability of sulfur cathode by encapsulating sulfur into micropores of carbon spheres
journal, January 2010

  • Zhang, B.; Qin, X.; Li, G. R.
  • Energy & Environmental Science, Vol. 3, Issue 10
  • DOI: 10.1039/c002639e

Polyacrylonitrile/graphene composite as a precursor to a sulfur-based cathode material for high-rate rechargeable Li–S batteries
journal, January 2012

  • Yin, Lichao; Wang, Jiulin; Lin, Fengjiao
  • Energy & Environmental Science, Vol. 5, Issue 5
  • DOI: 10.1039/c2ee03495f

CNT enhanced sulfur composite cathode material for high rate lithium battery
journal, May 2011


Lithium Superionic Sulfide Cathode for All-Solid Lithium–Sulfur Batteries
journal, March 2013

  • Lin, Zhan; Liu, Zengcai; Dudney, Nancy J.
  • ACS Nano, Vol. 7, Issue 3, p. 2829-2833
  • DOI: 10.1021/nn400391h

Nitrogen-Doped Porous Carbon Nanofiber Webs as Anodes for Lithium Ion Batteries with a Superhigh Capacity and Rate Capability
journal, March 2012


In Situ Formed Lithium Sulfide/Microporous Carbon Cathodes for Lithium-Ion Batteries
journal, November 2013

  • Zheng, Shiyou; Chen, Yvonne; Xu, Yunhua
  • ACS Nano, Vol. 7, Issue 12
  • DOI: 10.1021/nn404601h

Porous Li4Ti5O12 Coated with N-Doped Carbon from Ionic Liquids for Li-Ion Batteries
journal, February 2011

  • Zhao, Liang; Hu, Yong-Sheng; Li, Hong
  • Advanced Materials, Vol. 23, Issue 11, p. 1385-1388
  • DOI: 10.1002/adma.201003294

Amphiphilic Surface Modification of Hollow Carbon Nanofibers for Improved Cycle Life of Lithium Sulfur Batteries
journal, February 2013

  • Zheng, Guangyuan; Zhang, Qianfan; Cha, Judy J.
  • Nano Letters, Vol. 13, Issue 3, p. 1265-1270
  • DOI: 10.1021/nl304795g

A Soft Approach to Encapsulate Sulfur: Polyaniline Nanotubes for Lithium-Sulfur Batteries with Long Cycle Life
journal, January 2012

  • Xiao, Lifen; Cao, Yuliang; Xiao, Jie
  • Advanced Materials, Vol. 24, Issue 9, p. 1176-1181
  • DOI: 10.1002/adma.201103392

Nanostructured Li 2 S–C Composites as Cathode Material for High-Energy Lithium/Sulfur Batteries
journal, February 2012

  • Cai, Kunpeng; Song, Min-Kyu; Cairns, Elton J.
  • Nano Letters, Vol. 12, Issue 12
  • DOI: 10.1021/nl303965a

Li 2 S-Carbon Sandwiched Electrodes with Superior Performance for Lithium-Sulfur Batteries
journal, August 2013

  • Fu, Yongzhu; Su, Yu-Sheng; Manthiram, Arumugam
  • Advanced Energy Materials, Vol. 4, Issue 1
  • DOI: 10.1002/aenm.201300655

Evolution of Microstructures and Nitrogen Sorption during High-Energy Milling of Silicon in Ammonia
journal, August 2000


Power sources for portable electronics and hybrid cars: lithium batteries and fuel cells
journal, January 2005


Recent advances in rechargeable battery materials: a chemist’s perspective
journal, January 2009

  • Palacín, M. Rosa
  • Chemical Society Reviews, Vol. 38, Issue 9
  • DOI: 10.1039/b820555h

Polymorphic transformation and powder characteristics of TiO2 during high energy milling
journal, December 2000

  • Ren, Ruiming; Yang, Zhenguo; Shaw, L. L.
  • Journal of Materials Science, Vol. 35, Issue 23, p. 6015-6026
  • DOI: 10.1023/a:1026751017284

Low-cost, porous carbon current collector with high sulfur loading for lithium–sulfur batteries
journal, January 2014


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

High capacity cathode materials for Li–S batteries
journal, January 2013

  • Ryu, Ho Suk; Park, Jin Woo; Park, Jinsoo
  • J. Mater. Chem. A, Vol. 1, Issue 5
  • DOI: 10.1039/c2ta00056c

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

Recent advances in lithium–sulfur batteries
journal, December 2014


Li2S-reduced graphene oxide nanocomposites as cathode material for lithium sulfur batteries
journal, April 2014


Facile synthesis of Li2S–polypyrrole composite structures for high-performance Li2S cathodes
journal, January 2014

  • Seh, Zhi Wei; Wang, Haotian; Hsu, Po-Chun
  • Energy & Environmental Science, Vol. 7, Issue 2
  • DOI: 10.1039/c3ee43395a

High-Capacity Micrometer-Sized Li2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries
journal, September 2012

  • Yang, Yuan; Zheng, Guangyuan; Misra, Sumohan
  • Journal of the American Chemical Society, Vol. 134, Issue 37, p. 15387-15394
  • DOI: 10.1021/ja3052206

Nitrogen-doped graphene and its electrochemical applications
journal, January 2010

  • Shao, Yuyan; Zhang, Sheng; Engelhard, Mark H.
  • Journal of Materials Chemistry, Vol. 20, Issue 35
  • DOI: 10.1039/c0jm00782j

Effects of process-control agents on mechanical alloying of nanostructured aluminum alloys
journal, January 2003

  • Shaw, L.; Villegas, J.; Luo, H.
  • Metallurgical and Materials Transactions A, Vol. 34, Issue 1
  • DOI: 10.1007/s11661-003-0217-7

Lithium-sulfur batteries
journal, May 2014

  • Nazar, Linda F.; Cuisinier, Marine; Pang, Quan
  • MRS Bulletin, Vol. 39, Issue 5
  • DOI: 10.1557/mrs.2014.86

Li–O2 and Li–S batteries with high energy storage
journal, January 2012

  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191

A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries
journal, May 2009

  • Ji, Xiulei; Lee, Kyu Tae; Nazar, Linda F.
  • Nature Materials, Vol. 8, Issue 6, p. 500-506
  • DOI: 10.1038/nmat2460

Durable Carbon-Coated Li 2 S Core–Shell Spheres for High Performance Lithium/Sulfur Cells
journal, March 2014

  • Nan, Caiyun; Lin, Zhan; Liao, Honggang
  • Journal of the American Chemical Society, Vol. 136, Issue 12
  • DOI: 10.1021/ja412943h

Synthesis of Nanostructured Silicon Carbide through an Integrated Mechanical and Thermal Activation Process
journal, April 2002


Carbon coated lithium sulfide particles for lithium battery cathodes
journal, August 2013


A High-Performance Polymer Tin Sulfur Lithium Ion Battery
journal, February 2010


Nanostructured Materials for Electrochemical Energy Conversion and Storage Devices
journal, December 2008


Works referencing / citing this record:

Solution-Based Chemical Process for Synthesis of Highly Active Li 2 S/Carbon Nanocomposite for Lithium-Sulfur Batteries
journal, April 2016


Cathode materials for lithium–sulfur batteries: a practical perspective
journal, January 2017

  • Eftekhari, Ali; Kim, Dong-Won
  • Journal of Materials Chemistry A, Vol. 5, Issue 34
  • DOI: 10.1039/c7ta00799j

Stabilizing the Performance of High-Capacity Sulfur Composite Electrodes by a New Gel Polymer Electrolyte Configuration
journal, August 2017


Progress in Mechanistic Understanding and Characterization Techniques of Li-S Batteries
journal, May 2015


A Hierarchical Particle-Shell Architecture for Long-Term Cycle Stability of Li 2 S Cathodes
journal, August 2015


Dodecylamine-Induced Synthesis of a Nitrogen-Doped Carbon Comb for Advanced Lithium-Sulfur Battery Cathodes
journal, February 2018

  • Lu, Qian; Zhong, Yijun; Zhou, Wei
  • Advanced Materials Interfaces, Vol. 5, Issue 9
  • DOI: 10.1002/admi.201701659

An Ultrahigh Capacity Graphite/Li 2 S Battery with Holey-Li 2 S Nanoarchitectures
journal, May 2018


Gyroidal Porous Carbon Activated with NH 3 or CO 2 as Lithium−Sulfur Battery Cathodes
journal, April 2018

  • Krüner, Benjamin; Dörr, Tobias S.; Shim, Hwirim
  • Batteries & Supercaps, Vol. 1, Issue 2
  • DOI: 10.1002/batt.201800013

Li 3 BN 2 as a Transition Metal Free, High Capacity Cathode for Li-ion Batteries
journal, November 2018

  • Emani, Satyanarayana; Liu, Caihong; Ashuri, Maziar
  • ChemElectroChem, Vol. 6, Issue 2
  • DOI: 10.1002/celc.201801415

Infiltrated Porous Polymer Sheets as Free-Standing Flexible Lithium-Sulfur Battery Electrodes
journal, May 2016


Highly Nitridated Graphene-Li 2 S Cathodes with Stable Modulated Cycles
journal, September 2015

  • Qiu, Yongcai; Rong, Genlan; Yang, Jie
  • Advanced Energy Materials, Vol. 5, Issue 23
  • DOI: 10.1002/aenm.201501369

Bifunctional MOF‐Derived Carbon Photonic Crystal Architectures for Advanced Zn–Air and Li–S Batteries: Highly Exposed Graphitic Nitrogen Matters
journal, July 2017

  • Yang, Meijia; Hu, Xuanhe; Fang, Zhengsong
  • Advanced Functional Materials, Vol. 27, Issue 36
  • DOI: 10.1002/adfm.201701971

Nitrogen-Doped Carbon for Red Phosphorous Based Anode Materials for Lithium Ion Batteries
journal, January 2018


Li 2 S-Based Solid Solutions as Positive Electrodes with Full Utilization and Superlong Cycle Life in All-Solid-State Li/S Batteries
journal, May 2017

  • Hakari, Takashi; Hayashi, Akitoshi; Tatsumisago, Masahiro
  • Advanced Sustainable Systems, Vol. 1, Issue 6
  • DOI: 10.1002/adsu.201700017

The adsorption effect of freestanding SiO x -decorated stabilized polyacrylonitrile interlayers in lithium–sulfur batteries
journal, January 2019

  • Cengiz, Elif Ceylan; Ansari Hamedani, Ali; Hayat Soytas, Serap
  • Dalton Transactions, Vol. 48, Issue 13
  • DOI: 10.1039/c8dt04674c