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

Title: Design Principles for Optimum Performance of Porous Carbons in Lithium-Sulfur Batteries

Abstract

Here, a series of experiments is presented that establishes for the first time the role of some of the key design parameters of porous carbons including surface area, pore volume, and pore size on battery performance. A series of hierarchical porous carbons is used as a model system with an open, 3D, interconnected porous framework and highly controlled porosity. Specifically, carbons with surface areas ranging from ≈500–2800 m 2 g -1, pore volume from ≈0.6–5 cm 3 g -1, and pore size from micropores (≈1 nm) to large mesopores (≈30 nm) are synthesized and tested. At high sulfur loadings (≈80 wt% S), pore volume is more important than surface area with respect to sulfur utilization. Mesopore size, in the range tested, does not affect the sulfur utilization. No relationship between porosity and long-term cycle life is observed. All systems fail after 200–300 cycles, which is likely due to the consumption of the LiNO 3 additive over cycling. Moreover, cryo-scanning transmission electron microscopy imaging of these carbon–sulfur composites combined with X-ray diffraction (XRD) provides further insights into the effect of initial sulfur distribution on sulfur utilization while also revealing the inadequacy of the indirect characterization techniques alone in reliably predicting distributionmore » of sulfur within porous carbon matrices.« less

Authors:
 [1];  [2];  [1];  [2];  [3];  [1]
  1. Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering
  2. Cornell Univ., Ithaca, NY (United States). School of Applied and Engineering Physics; Kavli Inst. at Cornell for Nanoscale Science, Ithaca NY (United States)
  3. Cornell Univ., Ithaca, NY (United States). Dept. of Chemistry and Chemical Biology
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Materials Center at Cornell (EMC2)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1370416
Grant/Contract Number:  
SC0001086
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 14; Related Information: Emc2 partners with Cornell University (lead); Lawrence Berkeley National Laboratory; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
cryo‐scanning TEM; hierarchical porous carbons; high sulfur loading; lithium–sulfur batteries; porosity dependence

Citation Formats

Sahore, Ritu, Levin, Barnaby D. A., Pan, Mian, Muller, David A., DiSalvo, Francis J., and Giannelis, Emmanuel P. Design Principles for Optimum Performance of Porous Carbons in Lithium-Sulfur Batteries. United States: N. p., 2016. Web. doi:10.1002/aenm.201600134.
Sahore, Ritu, Levin, Barnaby D. A., Pan, Mian, Muller, David A., DiSalvo, Francis J., & Giannelis, Emmanuel P. Design Principles for Optimum Performance of Porous Carbons in Lithium-Sulfur Batteries. United States. doi:10.1002/aenm.201600134.
Sahore, Ritu, Levin, Barnaby D. A., Pan, Mian, Muller, David A., DiSalvo, Francis J., and Giannelis, Emmanuel P. Mon . "Design Principles for Optimum Performance of Porous Carbons in Lithium-Sulfur Batteries". United States. doi:10.1002/aenm.201600134. https://www.osti.gov/servlets/purl/1370416.
@article{osti_1370416,
title = {Design Principles for Optimum Performance of Porous Carbons in Lithium-Sulfur Batteries},
author = {Sahore, Ritu and Levin, Barnaby D. A. and Pan, Mian and Muller, David A. and DiSalvo, Francis J. and Giannelis, Emmanuel P.},
abstractNote = {Here, a series of experiments is presented that establishes for the first time the role of some of the key design parameters of porous carbons including surface area, pore volume, and pore size on battery performance. A series of hierarchical porous carbons is used as a model system with an open, 3D, interconnected porous framework and highly controlled porosity. Specifically, carbons with surface areas ranging from ≈500–2800 m2 g-1, pore volume from ≈0.6–5 cm3 g-1, and pore size from micropores (≈1 nm) to large mesopores (≈30 nm) are synthesized and tested. At high sulfur loadings (≈80 wt% S), pore volume is more important than surface area with respect to sulfur utilization. Mesopore size, in the range tested, does not affect the sulfur utilization. No relationship between porosity and long-term cycle life is observed. All systems fail after 200–300 cycles, which is likely due to the consumption of the LiNO3 additive over cycling. Moreover, cryo-scanning transmission electron microscopy imaging of these carbon–sulfur composites combined with X-ray diffraction (XRD) provides further insights into the effect of initial sulfur distribution on sulfur utilization while also revealing the inadequacy of the indirect characterization techniques alone in reliably predicting distribution of sulfur within porous carbon matrices.},
doi = {10.1002/aenm.201600134},
journal = {Advanced Energy Materials},
number = 14,
volume = 6,
place = {United States},
year = {2016},
month = {5}
}

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

Citation Metrics:
Cited by: 51 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Lithium–sulfur batteries: Influence of C-rate, amount of electrolyte and sulfur loading on cycle performance
journal, December 2014


A facile approach for the synthesis of monolithic hierarchical porous carbons – high performance materials for amine based CO2 capture and supercapacitor electrode
journal, January 2013

  • Estevez, Luis; Dua, Rubal; Bhandari, Nidhi
  • Energy & Environmental Science, Vol. 6, Issue 6
  • DOI: 10.1039/c3ee40549d

Tuning the porous structure of carbon hosts for loading sulfur toward long lifespan cathode materials for Li–S batteries
journal, January 2013

  • Ye, Huan; Yin, Ya-Xia; Xin, Sen
  • Journal of Materials Chemistry A, Vol. 1, Issue 22
  • DOI: 10.1039/c3ta10735c

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

  • Elazari, Ran; Salitra, Gregory; Garsuch, Arnd
  • Advanced Materials, Vol. 23, Issue 47, p. 5641-5644
  • DOI: 10.1002/adma.201103274

Spherical Ordered Mesoporous Carbon Nanoparticles with High Porosity for Lithium-Sulfur Batteries
journal, March 2012

  • Schuster, Jörg; He, Guang; Mandlmeier, Benjamin
  • Angewandte Chemie International Edition, Vol. 51, Issue 15, p. 3591-3595
  • DOI: 10.1002/anie.201107817

High “C” rate Li-S cathodes: sulfur imbibed bimodal porous carbons
journal, January 2011

  • He, Guang; Ji, Xiulei; Nazar, Linda
  • Energy & Environmental Science, Vol. 4, Issue 8
  • DOI: 10.1039/c1ee01219c

Optimization of mesoporous carbon structures for lithium–sulfur battery applications
journal, January 2011

  • Li, Xiaolin; Cao, Yuliang; Qi, Wen
  • Journal of Materials Chemistry, Vol. 21, Issue 41
  • DOI: 10.1039/c1jm12979a

Sulfur-Impregnated Disordered Carbon Nanotubes Cathode for Lithium–Sulfur Batteries
journal, October 2011

  • Guo, Juchen; Xu, Yunhua; Wang, Chunsheng
  • Nano Letters, Vol. 11, Issue 10, p. 4288-4294
  • DOI: 10.1021/nl202297p

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

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-rate lithium–sulfur batteries enabled by hierarchical porous carbons synthesized via ice templation
journal, November 2015


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

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

Pig bone derived hierarchical porous carbon and its enhanced cycling performance of lithium–sulfur batteries
journal, January 2011

  • Wei, Shaochen; Zhang, Hao; Huang, Yaqin
  • Energy & Environmental Science, Vol. 4, Issue 3
  • DOI: 10.1039/c0ee00505c

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

  • Jayaprakash, N.; Shen, J.; Moganty, Surya S.
  • Angewandte Chemie International Edition, Vol. 50, Issue 26, p. 5904-5908
  • DOI: 10.1002/anie.201100637

Layer Structured Sulfur/Expanded Graphite Composite as Cathode for Lithium Battery
journal, January 2011

  • Li, Sheng; Xie, Ming; Liu, JingBing
  • Electrochemical and Solid-State Letters, Vol. 14, Issue 7
  • DOI: 10.1149/1.3582793

A microporous–mesoporous carbon with graphitic structure for a high-rate stable sulfur cathode in carbonate solvent-based Li–S batteries
journal, January 2012

  • Wang, Da-Wei; Zhou, Guangmin; Li, Feng
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 24
  • DOI: 10.1039/c2cp40808b

Insight into the Electrode Mechanism in Lithium-Sulfur Batteries with Ordered Microporous Carbon Confined Sulfur as the Cathode
journal, November 2013


Characterizing Sulfur in TEM and STEM, with Applications to Lithium Sulfur Batteries
journal, August 2014

  • Levin, Barnaby D. A.; Zachman, Michael J.; Werner, Jörg G.
  • Microscopy and Microanalysis, Vol. 20, Issue S3
  • DOI: 10.1017/S143192761400395X

Rechargeable Lithium Sulfur Battery
journal, January 2003

  • Cheon, Sang-Eun; Ko, Ki-Seok; Cho, Ji-Hoon
  • Journal of The Electrochemical Society, Vol. 150, Issue 6
  • DOI: 10.1149/1.1571532

Effects of carbon surface area on performance of lithium sulfur battery cathodes
journal, November 2013

  • Dornbusch, Donald A.; Hilton, Ramsey; Gordon, Michael J.
  • Journal of Industrial and Engineering Chemistry, Vol. 19, Issue 6
  • DOI: 10.1016/j.jiec.2013.03.005

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

A lithium–sulfur full cell with ultralong cycle life: influence of cathode structure and polysulfide additive
journal, January 2015

  • Thieme, Sören; Brückner, Jan; Meier, Andreas
  • Journal of Materials Chemistry A, Vol. 3, Issue 7
  • DOI: 10.1039/C4TA06748G

Pitfalls in the characterization of sulfur/carbon nanocomposite materials for lithium–sulfur batteries
journal, November 2014