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

Title: X-ray Absorption Spectroscopy Characterization of a Li/S Cell

Abstract

© 2016 by the authors; licensee MDPI, Basel, Switzerland. The X-ray absorption spectroscopy technique has been applied to study different stages of the lithium/sulfur (Li/S) cell life cycle. We have investigated how speciation of S in Li/S cathodes changes upon the introduction of CTAB (cetyltrimethylammonium bromide, CH 3 (CH 2 )i 5 N+(CH 3 ) 3 Br~) and with charge/discharge cycling. The introduction of CTAB changes the synthesis reaction pathway dramatically due to the interaction of CTAB with the terminal S atoms of the polysulfide ions in the Na2S x solution. For the cycled Li/S cell, the loss of electrochemically active sulfur and the accumulation of a compact blocking insulating layer of unexpected sulfur reaction products on the cathode surface during the charge/discharge processes make the capacity decay. A modified coin cell and a vacuum-compatible three-electrode electro-chemical cell have been introduced for further in-situ/in-operando studies.

Authors:
 [1];  [2];  [3];  [4];  [5];  [5];  [5];  [2];  [6];  [7]
  1. Univ. of Science and Technology of China, Hefei (China); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Environmental Energy Technologies Division; Univ. of California, Berkeley, CA (United States)
  3. Washington State Univ., Pullman, WA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Harbin Inst. of Technology (China)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Santa Cruz, CA (United States)
  7. Univ. of Science and Technology of China, Hefei (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1254009
Alternate Identifier(s):
OSTI ID: 1379029
Grant/Contract Number:  
AC02-05CH11231; 2013CB834605; U1232102; 21173200; 21473178; (2015SRG-HSC031; 2015HSC-UP022
Resource Type:
Accepted Manuscript
Journal Name:
Nanomaterials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2079-4991
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
62 RADIOLOGY AND NUCLEAR MEDICINE; lithium/sulfur cell; X-ray absorption spectroscopy; cetyltrimethylammonium bromide; synthesis; capacity decay; cycled cathode materials; insulating layer; in-situ/in-operando

Citation Formats

Ye, Yifan, Kawase, Ayako, Song, Min-Kyu, Feng, Bingmei, Liu, Yi-Sheng, Marcus, Matthew A., Feng, Jun, Cairns, Elton J., Guo, Jinghua, and Zhu, Junfa. X-ray Absorption Spectroscopy Characterization of a Li/S Cell. United States: N. p., 2016. Web. doi:10.3390/nano6010014.
Ye, Yifan, Kawase, Ayako, Song, Min-Kyu, Feng, Bingmei, Liu, Yi-Sheng, Marcus, Matthew A., Feng, Jun, Cairns, Elton J., Guo, Jinghua, & Zhu, Junfa. X-ray Absorption Spectroscopy Characterization of a Li/S Cell. United States. https://doi.org/10.3390/nano6010014
Ye, Yifan, Kawase, Ayako, Song, Min-Kyu, Feng, Bingmei, Liu, Yi-Sheng, Marcus, Matthew A., Feng, Jun, Cairns, Elton J., Guo, Jinghua, and Zhu, Junfa. Mon . "X-ray Absorption Spectroscopy Characterization of a Li/S Cell". United States. https://doi.org/10.3390/nano6010014. https://www.osti.gov/servlets/purl/1254009.
@article{osti_1254009,
title = {X-ray Absorption Spectroscopy Characterization of a Li/S Cell},
author = {Ye, Yifan and Kawase, Ayako and Song, Min-Kyu and Feng, Bingmei and Liu, Yi-Sheng and Marcus, Matthew A. and Feng, Jun and Cairns, Elton J. and Guo, Jinghua and Zhu, Junfa},
abstractNote = {© 2016 by the authors; licensee MDPI, Basel, Switzerland. The X-ray absorption spectroscopy technique has been applied to study different stages of the lithium/sulfur (Li/S) cell life cycle. We have investigated how speciation of S in Li/S cathodes changes upon the introduction of CTAB (cetyltrimethylammonium bromide, CH 3 (CH 2 )i 5 N+(CH 3 ) 3 Br~) and with charge/discharge cycling. The introduction of CTAB changes the synthesis reaction pathway dramatically due to the interaction of CTAB with the terminal S atoms of the polysulfide ions in the Na2S x solution. For the cycled Li/S cell, the loss of electrochemically active sulfur and the accumulation of a compact blocking insulating layer of unexpected sulfur reaction products on the cathode surface during the charge/discharge processes make the capacity decay. A modified coin cell and a vacuum-compatible three-electrode electro-chemical cell have been introduced for further in-situ/in-operando studies.},
doi = {10.3390/nano6010014},
journal = {Nanomaterials},
number = 1,
volume = 6,
place = {United States},
year = {2016},
month = {1}
}

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

Citation Metrics:
Cited by: 30 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Solution-Based Processing of Graphene-Li 2 S Composite Cathodes for Lithium-Ion and Lithium-Sulfur Batteries
journal, February 2014

  • Wu, Feixiang; Lee, Jung Tae; Magasinski, Alexandre
  • Particle & Particle Systems Characterization, Vol. 31, Issue 6
  • DOI: 10.1002/ppsc.201300358

Mg deposition observed by in situ electrochemical Mg K-edge X-ray absorption spectroscopy
journal, October 2012


Copper-Stabilized Sulfur-Microporous Carbon Cathodes for Li-S Batteries
journal, March 2014

  • Zheng, Shiyou; Yi, Feng; Li, Zhipeng
  • Advanced Functional Materials, Vol. 24, Issue 26
  • DOI: 10.1002/adfm.201304156

Understanding the Nature of Absorption/Adsorption in Nanoporous Polysulfide Sorbents for the Li–S Battery
journal, September 2012

  • Evers, Scott; Yim, Taeeun; Nazar, Linda F.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 37
  • DOI: 10.1021/jp304380j

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

A Review on the Structural Studies of Batteries and Host Materials by X-Ray Absorption Spectroscopy
journal, January 2013


Sulfur Speciation in Li–S Batteries Determined by Operando X-ray Absorption Spectroscopy
journal, September 2013

  • Cuisinier, Marine; Cabelguen, Pierre-Etienne; Evers, Scott
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 19
  • DOI: 10.1021/jz401763d

Progress and prospective of solid-state lithium batteries
journal, February 2013


A Long-Life, High-Rate Lithium/Sulfur Cell: A Multifaceted Approach to Enhancing Cell Performance
journal, November 2013

  • Song, Min-Kyu; Zhang, Yuegang; Cairns, Elton J.
  • Nano Letters, Vol. 13, Issue 12
  • DOI: 10.1021/nl402793z

High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene
journal, July 2014

  • Qiu, Yongcai; Li, Wanfei; Zhao, Wen
  • Nano Letters, Vol. 14, Issue 8
  • DOI: 10.1021/nl5020475

Challenges and Prospects of Lithium–Sulfur Batteries
journal, June 2012

  • Manthiram, Arumugam; Fu, Yongzhu; Su, Yu-Sheng
  • Accounts of Chemical Research, Vol. 46, Issue 5
  • DOI: 10.1021/ar300179v

Using X-ray absorption to probe sulfur oxidation states in complex molecules
journal, October 1998


Advances in Li–S batteries
journal, January 2010

  • Ji, Xiulei; Nazar, Linda F.
  • Journal of Materials Chemistry, Vol. 20, Issue 44, p. 9821-9826
  • DOI: 10.1039/b925751a

Diamond xenolith and matrix organic matter in the Sutter's Mill meteorite measured by C-XANES
journal, October 2014

  • Kebukawa, Yoko; Zolensky, Michael E.; Kilcoyne, A. L. David
  • Meteoritics & Planetary Science, Vol. 49, Issue 11
  • DOI: 10.1111/maps.12312

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

Electronic structure and chemical bonding of a graphene oxide–sulfur nanocomposite for use in superior performance lithium–sulfur cells
journal, January 2012

  • Zhang, Liang; Ji, Liwen; Glans, Per-Anders
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 39
  • DOI: 10.1039/c2cp42866k

X-ray Absorption Spectra of Dissolved Polysulfides in Lithium–Sulfur Batteries from First-Principles
journal, April 2014

  • Pascal, Tod A.; Wujcik, Kevin H.; Velasco-Velez, Juan
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 9
  • DOI: 10.1021/jz500260s

Mechanistic insights into operational lithium–sulfur batteries by in situ X-ray diffraction and absorption spectroscopy
journal, January 2014

  • Lowe, Michael A.; Gao, Jie; Abruña, Héctor D.
  • RSC Advances, Vol. 4, Issue 35
  • DOI: 10.1039/c4ra01388c

Rechargeable Lithium–Sulfur Batteries
journal, July 2014

  • Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
  • Chemical Reviews, Vol. 114, Issue 23
  • DOI: 10.1021/cr500062v

High-Resolution X-ray Emission and X-ray Absorption Spectroscopy
journal, June 2001


Perspectives of in situ/operando resonant inelastic X-ray scattering in catalytic energy materials science
journal, April 2015

  • Liu, Yi-Sheng; Glans, Per-Anders; Chuang, Cheng-Hao
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 200
  • DOI: 10.1016/j.elspec.2015.07.004

XANES spectra of a variety of widely used organic polymers at the C K-edge
journal, November 1996


The probing depth of total electron yield in the sub-keV range: TEY-XAS and X-PEEM
journal, July 2003


X-ray absorption near edge structure spectroscopic study of Hayabusa category 3 carbonaceous particles
journal, December 2014

  • Yabuta, Hikaru; Uesugi, Masayuki; Naraoka, Hiroshi
  • Earth, Planets and Space, Vol. 66, Issue 1
  • DOI: 10.1186/s40623-014-0156-0

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

Effects of Nanosized Adsorbing Material on Electrochemical Properties of Sulfur Cathodes for Li/S Secondary Batteries
journal, January 2004

  • Song, Min-Sang; Han, Sang-Cheol; Kim, Hyun-Seok
  • Journal of The Electrochemical Society, Vol. 151, Issue 6, p. A791-A795
  • DOI: 10.1149/1.1710895

High-performance lithium/sulfur cells with a bi-functionally immobilized sulfur cathode
journal, October 2014


X-ray Absorption Near-Edge Structure and Nuclear Magnetic Resonance Study of the Lithium-Sulfur Battery and its Components
journal, February 2014

  • Patel, Manu U. M.; Arčon, Iztok; Aquilanti, Giuliana
  • ChemPhysChem, Vol. 15, Issue 5
  • DOI: 10.1002/cphc.201300972

Distinct charge dynamics in battery electrodes revealed by in situ and operando soft X-ray spectroscopy
journal, October 2013

  • Liu, Xiaosong; Wang, Dongdong; Liu, Gao
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3568

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

  • Jayaprakash, N.; Shen, J.; Moganty, Surya S.
  • Angewandte Chemie, Vol. 123, Issue 26, p. 6026-6030
  • DOI: 10.1002/ange.201100637

Sulfur: Not a “Silent” Element Any More
journal, May 2007


Works referencing / citing this record:

In Situ Techniques for Developing Robust Li-S Batteries
journal, August 2018


The improvement of pitch activation by graphene for long-cycle Li–S batteries
journal, January 2018

  • Cheng, Miao; Zhao, Huifang; Zhao, Zheng
  • Green Chemistry, Vol. 20, Issue 20
  • DOI: 10.1039/c8gc01799a

A versatile liquid-jet/sessile droplet system for operando studies of reactions in liquid dispersions and solutions by X-ray absorption spectroscopy
journal, January 2019

  • Chang, S. -Y.; Kathyola, T. A.; Willneff, E. A.
  • Reaction Chemistry & Engineering, Vol. 4, Issue 4
  • DOI: 10.1039/c8re00207j

Method for Creation of Fine Sulfur Particles with Graphene Oxide for Lithium/Sulfur Cells
journal, January 2018

  • Kawase, Ayako; Cairns, Elton J.
  • Journal of The Electrochemical Society, Vol. 165, Issue 14
  • DOI: 10.1149/2.0181814jes