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Title: A Shell-Shaped Carbon Architecture with High-Loading Capability for Lithium Sulfide Cathodes

Abstract

We present that lithium sulfide (Li 2S) is considered a highly attractive cathode for establishing high-energy-density rechargeable batteries, especially due to its high charge-storage capacity and compatibility with lithium-metal-free anodes. Although various approaches have recently been pursued with Li 2S to obtain high performance, formidable challenges still remain with cell design (e.g., low Li 2S loading, insufficient Li 2S content, and an excess electrolyte) to realize high areal, gravimetric, and volumetric capacities. This study demonstrates a shell-shaped carbon architecture for holding pure Li 2S, offering innovation in cell-design parameters and gains in electrochemical characteristics. The Li 2S core–carbon shell electrode encapsulates the redox products within the conductive shell so as to facilitate facile accessibility to electrons and ions. The fast redox-reaction kinetics enables the cells to attain the highest Li 2S loading of 8 mg cm -2 and the lowest electrolyte/Li 2S ratio of 9/1, which is the best cell-design specifications ever reported with Li 2S cathodes so far. Lastly, benefiting from the excellent cell-design criterion, the core–shell cathodes exhibit stable cyclability from slow to fast cycle rates and, for the first time, simultaneously achieve superior performance metrics with areal, gravimetric, and volumetric capacities.

Authors:
 [1];  [1];  [1];  [1]
  1. Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program, Texas Materials Institute
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States); Univ. of Texas at Austin, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1430177
Alternate Identifier(s):
OSTI ID: 1378808; OSTI ID: 1487393
Grant/Contract Number:  
EE0007218
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 7; Journal Issue: 17; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE

Citation Formats

Chung, Sheng-Heng, Han, Pauline, Chang, Chi-Hao, and Manthiram, Arumugam. A Shell-Shaped Carbon Architecture with High-Loading Capability for Lithium Sulfide Cathodes. United States: N. p., 2017. Web. doi:10.1002/aenm.201700537.
Chung, Sheng-Heng, Han, Pauline, Chang, Chi-Hao, & Manthiram, Arumugam. A Shell-Shaped Carbon Architecture with High-Loading Capability for Lithium Sulfide Cathodes. United States. doi:10.1002/aenm.201700537.
Chung, Sheng-Heng, Han, Pauline, Chang, Chi-Hao, and Manthiram, Arumugam. Thu . "A Shell-Shaped Carbon Architecture with High-Loading Capability for Lithium Sulfide Cathodes". United States. doi:10.1002/aenm.201700537. https://www.osti.gov/servlets/purl/1430177.
@article{osti_1430177,
title = {A Shell-Shaped Carbon Architecture with High-Loading Capability for Lithium Sulfide Cathodes},
author = {Chung, Sheng-Heng and Han, Pauline and Chang, Chi-Hao and Manthiram, Arumugam},
abstractNote = {We present that lithium sulfide (Li2S) is considered a highly attractive cathode for establishing high-energy-density rechargeable batteries, especially due to its high charge-storage capacity and compatibility with lithium-metal-free anodes. Although various approaches have recently been pursued with Li2S to obtain high performance, formidable challenges still remain with cell design (e.g., low Li2S loading, insufficient Li2S content, and an excess electrolyte) to realize high areal, gravimetric, and volumetric capacities. This study demonstrates a shell-shaped carbon architecture for holding pure Li2S, offering innovation in cell-design parameters and gains in electrochemical characteristics. The Li2S core–carbon shell electrode encapsulates the redox products within the conductive shell so as to facilitate facile accessibility to electrons and ions. The fast redox-reaction kinetics enables the cells to attain the highest Li2S loading of 8 mg cm-2 and the lowest electrolyte/Li2S ratio of 9/1, which is the best cell-design specifications ever reported with Li2S cathodes so far. Lastly, benefiting from the excellent cell-design criterion, the core–shell cathodes exhibit stable cyclability from slow to fast cycle rates and, for the first time, simultaneously achieve superior performance metrics with areal, gravimetric, and volumetric capacities.},
doi = {10.1002/aenm.201700537},
journal = {Advanced Energy Materials},
number = 17,
volume = 7,
place = {United States},
year = {2017},
month = {5}
}

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Cited by: 19 works
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Figures / Tables:

Figure 1 Figure 1: (a) Schematic structure of a core-shell Li2S cathode. Optimization of the cell-design parameters: (b) E/L-ratio, (c) active-material-amount, (d) literature analysis based on references R1 – R55 (listed at the end of the supporting information) and this work. The calculation of parameters including everything in the cathode region andmore » the cathode material alone are marked, respectively, with and without *.« 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

High-capacity Li2S–nanocarbon composite electrode for all-solid-state rechargeable lithium batteries
journal, January 2012

  • Nagao, Motohiro; Hayashi, Akitoshi; Tatsumisago, Masahiro
  • Journal of Materials Chemistry, Vol. 22, Issue 19
  • DOI: 10.1039/c2jm16802b

A high performance lithium-ion sulfur battery based on a Li 2 S cathode using a dual-phase electrolyte
journal, January 2015

  • Wang, Lina; Wang, Yonggang; Xia, Yongyao
  • Energy & Environmental Science, Vol. 8, Issue 5
  • DOI: 10.1039/C5EE00058K

All-Solid-State Lithium Secondary Battery with Li[sub 2]S–C Composite Positive Electrode Prepared by Spark-Plasma-Sintering Process
journal, January 2010

  • Takeuchi, Tomonari; Kageyama, Hiroyuki; Nakanishi, Koji
  • Journal of The Electrochemical Society, Vol. 157, Issue 11
  • DOI: 10.1149/1.3486083

A Cooperative Interface for Highly Efficient Lithium-Sulfur Batteries
journal, September 2016

  • Peng, Hong-Jie; Zhang, Ze-Wen; Huang, Jia-Qi
  • Advanced Materials, Vol. 28, Issue 43
  • DOI: 10.1002/adma.201603401

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

Role of LiNO3 in rechargeable lithium/sulfur battery
journal, May 2012


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


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

Strain Anisotropies and Self-Limiting Capacities in Single-Crystalline 3D Silicon Microstructures: Models for High Energy Density Lithium-Ion Battery Anodes
journal, April 2011

  • Goldman, Jason L.; Long, Brandon R.; Gewirth, Andrew A.
  • Advanced Functional Materials, Vol. 21, Issue 13, p. 2412-2422
  • DOI: 10.1002/adfm.201002487

Space matters: Li + conduction versus strain effect at FePO 4 /LiFePO 4 interface
journal, February 2016

  • Lv, Weiqiang; Niu, Yinghua; Jian, Xian
  • Applied Physics Letters, Vol. 108, Issue 8
  • DOI: 10.1063/1.4942849

Activated Li 2 S as a High-Performance Cathode for Rechargeable Lithium–Sulfur Batteries
journal, November 2014

  • Zu, Chenxi; Klein, Michael; Manthiram, Arumugam
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 22
  • DOI: 10.1021/jz5021108

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


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


Electrochemical performance of lithium–sulfur batteries based on a sulfur cathode obtained by H2S gas treatment of a lithium salt
journal, March 2016


Phosphorous Pentasulfide as a Novel Additive for High-Performance Lithium-Sulfur Batteries
journal, June 2012

  • Lin, Zhan; Liu, Zengcai; Fu, Wujun
  • Advanced Functional Materials, Vol. 23, Issue 8
  • DOI: 10.1002/adfm.201200696

Cell energy density and electrolyte/sulfur ratio in Li–S cells
journal, October 2014


A Lithium-Ion Sulfur Battery Based on a Carbon-Coated Lithium-Sulfide Cathode and an Electrodeposited Silicon-Based Anode
journal, February 2014

  • Agostini, Marco; Hassoun, Jusef; Liu, Jun
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 14
  • DOI: 10.1021/am4057166

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

All-solid-state rechargeable lithium batteries with Li2S as a positive electrode material
journal, August 2008


3D Carbonaceous Current Collectors: The Origin of Enhanced Cycling Stability for High-Sulfur-Loading Lithium-Sulfur Batteries
journal, June 2016

  • Peng, Hong-Jie; Xu, Wen-Tao; Zhu, Lin
  • Advanced Functional Materials, Vol. 26, Issue 35
  • DOI: 10.1002/adfm.201602071

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

Janus Separator of Polypropylene-Supported Cellular Graphene Framework for Sulfur Cathodes with High Utilization in Lithium-Sulfur Batteries
journal, October 2015


Review on Li-Sulfur Battery Systems: an Integral Perspective
journal, May 2015

  • Rosenman, Ariel; Markevich, Elena; Salitra, Gregory
  • Advanced Energy Materials, Vol. 5, Issue 16
  • DOI: 10.1002/aenm.201500212

Nanostructured lithium sulfide materials for lithium-sulfur batteries
journal, August 2016


Graphene–Li 2 S–Carbon Nanocomposite for Lithium–Sulfur Batteries
journal, December 2015


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

Understanding abnormal potential behaviors at the 1st charge in Li 2 S cathode material for rechargeable Li–S batteries
journal, January 2016

  • Jung, Yongjo; Kang, Byoungwoo
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 31
  • DOI: 10.1039/C6CP03146C

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

Reversibility of electrochemical reactions of sulfur supported on inverse opal carbon in glyme–Li salt molten complex electrolytes
journal, January 2011

  • Tachikawa, Naoki; Yamauchi, Kento; Takashima, Eriko
  • Chemical Communications, Vol. 47, Issue 28
  • DOI: 10.1039/c1cc12415c

Lithium/Sulfur Batteries Upon Cycling: Structural Modifications and Species Quantification by In Situ and Operando X-Ray Diffraction Spectroscopy
journal, May 2015

  • Waluś, Sylwia; Barchasz, Céline; Bouchet, Renaud
  • Advanced Energy Materials, Vol. 5, Issue 16
  • DOI: 10.1002/aenm.201500165

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 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

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


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


The Use of Redox Mediators for Enhancing Utilization of Li 2 S Cathodes for Advanced Li–S Battery Systems
journal, February 2014

  • Meini, Stefano; Elazari, Ran; Rosenman, Ariel
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 5
  • DOI: 10.1021/jz500222f