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Title: Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries

Abstract

Despite the outstanding gravimetric performance of lithium-sulfur (Li-S) batteries, their practical volumetric energy density is normally lower than that of lithium-ion batteries, mainly due to the low density of nanostructured sulfur as well as the porous carbon hosts. Here, a novel approach is developed to fabricate high-density graphene bulk materials with ink-bottle-like mesopores by phosphoric acid (H 3PO 4) activation. These pores can effectively confine the polysulfides due to their unique structure with a wide body and narrow neck, which shows only a 0.05% capacity fade per cycle for 500 cycles (75% capacity retention) for accommodating polysulfides. With a density of 1.16 g cm -3, a hybrid cathode containing 54 wt% sulfur delivers a high volumetric capacity of 653 mA h cm -3. As a result, a device-level volumetric energy density as high as 408 W h L -1 is achieved with a cathode thickness of 100 mu m. This is a periodic yet practical advance to improve the volumetric performance of Li-S batteries from a device perspective. Furthermore, this work suggests a design principle for the real use Li-S batteries although there is a long way ahead to bridge the gap between Li-S batteries and Li-ion batteries in volumetricmore » performance.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [1];  [1];  [1];  [3];  [2]; ORCiD logo [4];  [5]
+ Show Author Affiliations
  1. Tianjin Univ., Tianjin (China)
  2. Tsinghua Univ., Shenzhen (China)
  3. UNSW Australia (The Univ. of New South Wales), Sydney, NSW (Australia)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Tianjin Univ., Tianjin (China); Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1466311
Alternate Identifier(s):
OSTI ID: 1425506
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 18; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; graphene monolith; ink-bottle-like pores; lithium-polysulfide batteries; polysulfides; volumetric performance

Citation Formats

Li, Huan, Tao, Ying, Zhang, Chen, Liu, Donghai, Luo, Jiayan, Fan, Weichao, Xu, Yue, Li, Youzhi, You, Conghui, Pan, Zheng -Ze, Ye, Mingchun, Chen, Zhengyu, Dong, Zhang, Wang, Da -Wei, Kang, Feiyu, Lu, Jun, and Yang, Quan -Hong. Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries. United States: N. p., 2018. Web. doi:10.1002/aenm.201703438.
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Li, Huan, Tao, Ying, Zhang, Chen, Liu, Donghai, Luo, Jiayan, Fan, Weichao, Xu, Yue, Li, Youzhi, You, Conghui, Pan, Zheng -Ze, Ye, Mingchun, Chen, Zhengyu, Dong, Zhang, Wang, Da -Wei, Kang, Feiyu, Lu, Jun, & Yang, Quan -Hong. Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries. United States. doi:10.1002/aenm.201703438.
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Li, Huan, Tao, Ying, Zhang, Chen, Liu, Donghai, Luo, Jiayan, Fan, Weichao, Xu, Yue, Li, Youzhi, You, Conghui, Pan, Zheng -Ze, Ye, Mingchun, Chen, Zhengyu, Dong, Zhang, Wang, Da -Wei, Kang, Feiyu, Lu, Jun, and Yang, Quan -Hong. Mon . "Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries". United States. doi:10.1002/aenm.201703438. https://www.osti.gov/servlets/purl/1466311.
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@article{osti_1466311,
title = {Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries},
author = {Li, Huan and Tao, Ying and Zhang, Chen and Liu, Donghai and Luo, Jiayan and Fan, Weichao and Xu, Yue and Li, Youzhi and You, Conghui and Pan, Zheng -Ze and Ye, Mingchun and Chen, Zhengyu and Dong, Zhang and Wang, Da -Wei and Kang, Feiyu and Lu, Jun and Yang, Quan -Hong},
abstractNote = {Despite the outstanding gravimetric performance of lithium-sulfur (Li-S) batteries, their practical volumetric energy density is normally lower than that of lithium-ion batteries, mainly due to the low density of nanostructured sulfur as well as the porous carbon hosts. Here, a novel approach is developed to fabricate high-density graphene bulk materials with ink-bottle-like mesopores by phosphoric acid (H3PO4) activation. These pores can effectively confine the polysulfides due to their unique structure with a wide body and narrow neck, which shows only a 0.05% capacity fade per cycle for 500 cycles (75% capacity retention) for accommodating polysulfides. With a density of 1.16 g cm-3, a hybrid cathode containing 54 wt% sulfur delivers a high volumetric capacity of 653 mA h cm-3. As a result, a device-level volumetric energy density as high as 408 W h L-1 is achieved with a cathode thickness of 100 mu m. This is a periodic yet practical advance to improve the volumetric performance of Li-S batteries from a device perspective. Furthermore, this work suggests a design principle for the real use Li-S batteries although there is a long way ahead to bridge the gap between Li-S batteries and Li-ion batteries in volumetric performance.},
doi = {10.1002/aenm.201703438},
journal = {Advanced Energy Materials},
number = 18,
volume = 8,
place = {United States},
year = {2018},
month = {3}
}
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Journal Article:
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DOI:  10.1002/aenm.201703438
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Cited by: 20 works
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Figures / Tables:

Fig. 1 Fig. 1 : Starting from a 3D graphene hydrogel, a commonly freeze-drying method results in a graphene monolith (GM) with hierarchical pores with low density (a); However, by H3PO4 activation and CEID method, a high density graphene monolith with large amounts of inkbottle-like pores (69%) was prepared (b); N2 adsorption-desorptionmore » isotherm (77K) of a typical (c) GM and (d) IBGM, where IBGM is prepared by controlling the H3PO4/GM mass ratio at 3 and is heat treated at 600 oC after washing; High-resolution TEM images of GM (e) and IBGM (f); (g) Pore size distributions determined by accumulative pore volume of IBGM; (h) FTIR spectra of GM and IBGM; (i) The cycling performance of IBGM and GM as the carbon host for confining the polysulfides at 0.5 C.« less
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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

Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report)
journal, October 2015

  • Thommes, Matthias; Kaneko, Katsumi; Neimark, Alexander V.
  • Pure and Applied Chemistry, Vol. 87, Issue 9-10
  • DOI: 10.1515/pac-2014-1117

Towards ultrahigh volumetric capacitance: graphene derived highly dense but porous carbons for supercapacitors
journal, October 2013

  • Tao, Ying; Xie, Xiaoying; Lv, Wei
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02975

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

Porosity in granular carbons activated with phosphoric acid
journal, January 1995

True Performance Metrics in Electrochemical Energy Storage
journal, November 2011

Liquid-Type Cathode Enabled by 3D Sponge-Like Carbon Nanotubes for High Energy Density and Long Cycling Life of Li-S Batteries
journal, October 2014

High Sulfur Loading in Hierarchical Porous Carbon Rods Constructed by Vertically Oriented Porous Graphene-Like Nanosheets for Li-S Batteries
journal, July 2016

  • Zheng, Zongmin; Guo, Hongchen; Pei, Fei
  • Advanced Functional Materials, Vol. 26, Issue 48
  • DOI: 10.1002/adfm.201601897

Compressed porous graphene particles for use as supercapacitor electrodes with excellent volumetric performance
journal, January 2015

Activated carbons from yellow poplar and white oak by H3PO4 activation
journal, January 1998

Towards superior volumetric performance: design and preparation of novel carbon materials for energy storage
journal, January 2015

  • Zhang, Chen; Lv, Wei; Tao, Ying
  • Energy & Environmental Science, Vol. 8, Issue 5
  • DOI: 10.1039/C5EE00389J

Self-Assembly of Graphene Oxide at Interfaces
journal, May 2014

A high-density graphene–sulfur assembly: a promising cathode for compact Li–S batteries
journal, January 2015

Adsorption hysteresis in ink-bottle pore
journal, July 2003

  • Morishige, Kunimitsu; Tateishi, Noriko
  • The Journal of Chemical Physics, Vol. 119, Issue 4
  • DOI: 10.1063/1.1585014

Aligned carbon nanotube/sulfur composite cathodes with high sulfur content for lithium–sulfur batteries
journal, March 2014

Porosity development in activated carbons obtained from date pits under chemical activation with phosphoric acid
journal, April 2002

Recent advances in the textural characterization of hierarchically structured nanoporous materials
journal, January 2017

  • Cychosz, Katie A.; Guillet-Nicolas, Rémy; García-Martínez, Javier
  • Chemical Society Reviews, Vol. 46, Issue 2
  • DOI: 10.1039/C6CS00391E

Graphene materials for lithium–sulfur batteries
journal, November 2015

Long-life Li/polysulphide batteries with high sulphur loading enabled by lightweight three-dimensional nitrogen/sulphur-codoped graphene sponge
journal, July 2015

  • Zhou, Guangmin; Paek, Eunsu; Hwang, Gyeong S.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8760

Facile synthesis of ultrahigh-surface-area hollow carbon nanospheres for enhanced adsorption and energy storage
journal, June 2015

  • Xu, Fei; Tang, Zhiwei; Huang, Siqi
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8221

Nanostructured sulfur cathodes
journal, January 2013

  • Yang, Yuan; Zheng, Guangyuan; Cui, Yi
  • Chemical Society Reviews, Vol. 42, Issue 7, p. 3018-3032
  • DOI: 10.1039/c2cs35256g

Pie-like electrode design for high-energy density lithium–sulfur batteries
journal, November 2015

  • Li, Zhen; Zhang, Jin Tao; Chen, Yu Ming
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9850

High sulfur loading composite wrapped by 3D nitrogen-doped graphene as a cathode material for lithium–sulfur batteries
journal, January 2014

  • Wang, Chao; Su, Kai; Wan, Wang
  • J. Mater. Chem. A, Vol. 2, Issue 14
  • DOI: 10.1039/C3TA14921H

Evolution of the effect of sulfur confinement in graphene-based porous carbons for use in Li–S batteries
journal, January 2016

  • Jia, Xiangling; Zhang, Chen; Liu, Juanjuan
  • Nanoscale, Vol. 8, Issue 8
  • DOI: 10.1039/C5NR08839A

Dense integration of graphene and sulfur through the soft approach for compact lithium/sulfur battery cathode
journal, March 2015

Preparation of activated carbon from lignin by chemical activation
journal, January 2000

Monodispersed Sulfur Nanoparticles for Lithium–Sulfur Batteries with Theoretical Performance
journal, December 2014

  • Chen, Hongwei; Wang, Changhong; Dong, Weiling
  • Nano Letters, Vol. 15, Issue 1
  • DOI: 10.1021/nl504963e

Smaller Sulfur Molecules Promise Better Lithium–Sulfur Batteries
journal, October 2012

  • Xin, Sen; Gu, Lin; Zhao, Na-Hong
  • Journal of the American Chemical Society, Vol. 134, Issue 45
  • DOI: 10.1021/ja308170k

Designing high-energy lithium–sulfur batteries
journal, January 2016

  • Seh, Zhi Wei; Sun, Yongming; Zhang, Qianfan
  • Chemical Society Reviews, Vol. 45, Issue 20
  • DOI: 10.1039/C5CS00410A

Synthetic carbons activated with phosphoric acid
journal, August 2002

Graphene-based materials for electrochemical energy storage devices: Opportunities and challenges
journal, January 2016

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

Nitrogen-doped mesoporous carbon of extraordinary capacitance for electrochemical energy storage
journal, December 2015

Partially unzipped carbon nanotubes for high-rate and stable lithium–sulfur batteries
journal, January 2016

  • Jeong, Y. C.; Lee, K.; Kim, T.
  • Journal of Materials Chemistry A, Vol. 4, Issue 3
  • DOI: 10.1039/C5TA07818K

A membrane-free lithium/polysulfide semi-liquid battery for large-scale energy storage
journal, January 2013

  • Yang, Yuan; Zheng, Guangyuan; Cui, Yi
  • Energy & Environmental Science, Vol. 6, Issue 5
  • DOI: 10.1039/c3ee00072a

A Metal-Free Supercapacitor Electrode Material with a Record High Volumetric Capacitance over 800 F cm −3
journal, November 2015

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

N/P-Codoped Thermally Reduced Graphene for High-Performance Supercapacitor Applications
journal, July 2013

  • Wang, Chunlei; Zhou, Ying; Sun, Li
  • The Journal of Physical Chemistry C, Vol. 117, Issue 29
  • DOI: 10.1021/jp4015959

3D Interconnected Electrode Materials with Ultrahigh Areal Sulfur Loading for Li-S Batteries
journal, March 2016

  • Fang, Ruopian; Zhao, Shiyong; Hou, Pengxiang
  • Advanced Materials, Vol. 28, Issue 17
  • DOI: 10.1002/adma.201506014

Stabilization of Insoluble Discharge Products by Facile Aniline Modification for High Performance Li-S Batteries
journal, May 2015

  • Kim, Jae Ho; Kim, Taehoon; Jeong, Yo Chan
  • Advanced Energy Materials, Vol. 5, Issue 14
  • DOI: 10.1002/aenm.201500268

HEMP-derived activated carbon fibers by chemical activation with phosphoric acid
journal, January 2009

Preparation of activated carbon from bituminous coal with phosphoric acid activation
journal, September 1998

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