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Title: Probing battery chemistry with liquid cell electron energy loss spectroscopy

Abstract

Electron energy loss spectroscopy (EELS) was used to determine the chemistry and oxidation state of LiMn2O4 and Li4Ti5O12 thin film battery electrodes in liquid cells for in situ scanning/transmission electron microscopy (S/TEM). Using the L2,3 white line intensity ratio method we determine the oxidation state of Mn and Ti in a liquid electrolyte solvent and discuss experimental parameters that influence measurement sensitivity.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1237629
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ChemComm
Additional Journal Information:
Journal Volume: 51; Journal Issue: 91; Journal ID: ISSN 1359-7345
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Unocic, Raymond R., Baggetto, Loic, Veith, Gabriel M., Unocic, Kinga A., Sacci, Robert L., Dudney, Nancy J., More, Karren Leslie, and Aguiar, Jeffery A. Probing battery chemistry with liquid cell electron energy loss spectroscopy. United States: N. p., 2015. Web. doi:10.1039/C5CC07180A.
Unocic, Raymond R., Baggetto, Loic, Veith, Gabriel M., Unocic, Kinga A., Sacci, Robert L., Dudney, Nancy J., More, Karren Leslie, & Aguiar, Jeffery A. Probing battery chemistry with liquid cell electron energy loss spectroscopy. United States. https://doi.org/10.1039/C5CC07180A
Unocic, Raymond R., Baggetto, Loic, Veith, Gabriel M., Unocic, Kinga A., Sacci, Robert L., Dudney, Nancy J., More, Karren Leslie, and Aguiar, Jeffery A. Tue . "Probing battery chemistry with liquid cell electron energy loss spectroscopy". United States. https://doi.org/10.1039/C5CC07180A. https://www.osti.gov/servlets/purl/1237629.
@article{osti_1237629,
title = {Probing battery chemistry with liquid cell electron energy loss spectroscopy},
author = {Unocic, Raymond R. and Baggetto, Loic and Veith, Gabriel M. and Unocic, Kinga A. and Sacci, Robert L. and Dudney, Nancy J. and More, Karren Leslie and Aguiar, Jeffery A.},
abstractNote = {Electron energy loss spectroscopy (EELS) was used to determine the chemistry and oxidation state of LiMn2O4 and Li4Ti5O12 thin film battery electrodes in liquid cells for in situ scanning/transmission electron microscopy (S/TEM). Using the L2,3 white line intensity ratio method we determine the oxidation state of Mn and Ti in a liquid electrolyte solvent and discuss experimental parameters that influence measurement sensitivity.},
doi = {10.1039/C5CC07180A},
journal = {ChemComm},
number = 91,
volume = 51,
place = {United States},
year = {Tue Sep 15 00:00:00 EDT 2015},
month = {Tue Sep 15 00:00:00 EDT 2015}
}

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Cited by: 18 works
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Works referenced in this record:

Surface chemistry of metal oxide coated lithium manganese nickel oxide thin film cathodes studied by XPS
journal, February 2013


Electron microscopy of specimens in liquid
journal, October 2011

  • de Jonge, Niels; Ross, Frances M.
  • Nature Nanotechnology, Vol. 6, Issue 11, p. 695-704
  • DOI: 10.1038/nnano.2011.161

Probing the Degradation Mechanisms in Electrolyte Solutions for Li-Ion Batteries by in Situ Transmission Electron Microscopy
journal, February 2014

  • Abellan, Patricia; Mehdi, B. Layla; Parent, Lucas R.
  • Nano Letters, Vol. 14, Issue 3
  • DOI: 10.1021/nl404271k

Charged Nanoparticle Dynamics in Water Induced by Scanning Transmission Electron Microscopy
journal, February 2012

  • White, E. R.; Mecklenburg, Matthew; Shevitski, Brian
  • Langmuir, Vol. 28, Issue 8
  • DOI: 10.1021/la2048486

Extraction of EELS white-line intensities of manganese compounds: Methods, accuracy, and valence sensitivity
journal, March 2006


Atomic-Scale Imaging and Spectroscopy for In Situ Liquid Scanning Transmission Electron Microscopy
journal, May 2012

  • Jungjohann, Katherine L.; Evans, James E.; Aguiar, Jeffery A.
  • Microscopy and Microanalysis, Vol. 18, Issue 3
  • DOI: 10.1017/S1431927612000104

Bubble and Pattern Formation in Liquid Induced by an Electron Beam
journal, December 2013

  • Grogan, Joseph M.; Schneider, Nicholas M.; Ross, Frances M.
  • Nano Letters, Vol. 14, Issue 1
  • DOI: 10.1021/nl404169a

Nanoscale Imaging of Lithium Ion Distribution During In Situ Operation of Battery Electrode and Electrolyte
journal, February 2014

  • Holtz, Megan E.; Yu, Yingchao; Gunceler, Deniz
  • Nano Letters, Vol. 14, Issue 3
  • DOI: 10.1021/nl404577c

Excess lithium storage and charge compensation in nanoscale Li 4+ x Ti 5 O 12
journal, September 2013


Core-level satellites and outer core-level multiplet splitting in Mn model compounds
journal, July 2000

  • Nelson, A. J.; Reynolds, John G.; Roos, Joseph W.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 18, Issue 4
  • DOI: 10.1116/1.582302

Direct Observation of Aggregative Nanoparticle Growth: Kinetic Modeling of the Size Distribution and Growth Rate
journal, December 2013

  • Woehl, Taylor J.; Park, Chiwoo; Evans, James E.
  • Nano Letters, Vol. 14, Issue 1
  • DOI: 10.1021/nl4043328

Thickness measurements with electron energy loss spectroscopy
journal, August 2008

  • Iakoubovskii, K.; Mitsuishi, K.; Nakayama, Y.
  • Microscopy Research and Technique, Vol. 71, Issue 8
  • DOI: 10.1002/jemt.20597

Correlation Between Oxygen Vacancy, Microstrain, and Cation Distribution in Lithium-Excess Layered Oxides During the First Electrochemical Cycle
journal, April 2013

  • Fell, Christopher R.; Qian, Danna; Carroll, Kyler J.
  • Chemistry of Materials, Vol. 25, Issue 9
  • DOI: 10.1021/cm4000119

Direct visualization of initial SEI morphology and growth kinetics during lithium deposition by in situ electrochemical transmission electron microscopy
journal, January 2014

  • Sacci, Robert L.; Dudney, Nancy J.; More, Karren L.
  • Chemical Communications, Vol. 50, Issue 17
  • DOI: 10.1039/c3cc49029g

In Situ Electron Energy-Loss Spectroscopy in Liquids
journal, May 2013


Electron microscopy of whole cells in liquid with nanometer resolution
journal, January 2009

  • Jonge, N. d.; Peckys, D. B.; Kremers, G. J.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 7
  • DOI: 10.1073/pnas.0809567106

Morphological changes in and around Sn electrodes during Li ion cycling characterized by in situ environmental TEM
journal, November 2013


Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters
journal, February 2015

  • Sacci, Robert L.; Black, Jennifer M.; Balke, Nina
  • Nano Letters, Vol. 15, Issue 3
  • DOI: 10.1021/nl5048626

XPS investigation of Mn valence in lanthanum manganite thin films under variation of oxygen content
journal, April 2006


Direct in Situ Determination of the Mechanisms Controlling Nanoparticle Nucleation and Growth
journal, September 2012

  • Woehl, Taylor J.; Evans, James E.; Arslan, Ilke
  • ACS Nano, Vol. 6, Issue 10
  • DOI: 10.1021/nn303371y

Direct Visualization of Solid Electrolyte Interphase Formation in Lithium-Ion Batteries with In Situ Electrochemical Transmission Electron Microscopy
journal, July 2014

  • Unocic, Raymond R.; Sun, Xiao-Guang; Sacci, Robert L.
  • Microscopy and Microanalysis, Vol. 20, Issue 4
  • DOI: 10.1017/S1431927614012744

Identifying surface structural changes in layered Li-excess nickel manganese oxides in high voltage lithium ion batteries: A joint experimental and theoretical study
journal, January 2011

  • Xu, Bo; Fell, Christopher R.; Chi, Miaofang
  • Energy & Environmental Science, Vol. 4, Issue 6
  • DOI: 10.1039/c1ee01131f

Observation of growth of metal nanoparticles
journal, January 2013

  • Liao, Hong-Gang; Niu, Kaiyang; Zheng, Haimei
  • Chemical Communications, Vol. 49, Issue 100
  • DOI: 10.1039/c3cc47473a

Real-time imaging and local elemental analysis of nanostructures in liquids
journal, January 2014

  • Lewis, Edward A.; Haigh, Sarah J.; Slater, Thomas J. A.
  • Chem. Commun., Vol. 50, Issue 70
  • DOI: 10.1039/C4CC02743D

Atomic-resolution imaging of oxidation states in manganites
journal, February 2009


Electron–Water Interactions and Implications for Liquid Cell Electron Microscopy
journal, September 2014

  • Schneider, Nicholas M.; Norton, Michael M.; Mendel, Brian J.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 38
  • DOI: 10.1021/jp507400n

Video-frequency scanning transmission electron microscopy of moving gold nanoparticles in liquid
journal, November 2012


Dynamic microscopy of nanoscale cluster growth at the solid–liquid interface
journal, July 2003

  • Williamson, M. J.; Tromp, R. M.; Vereecken, P. M.
  • Nature Materials, Vol. 2, Issue 8
  • DOI: 10.1038/nmat944

The GIF Quantum, a next generation post-column imaging energy filter
journal, July 2010


In Situ Transmission Electron Microscopy of Lead Dendrites and Lead Ions in Aqueous Solution
journal, June 2012

  • White, Edward R.; Singer, Scott B.; Augustyn, Veronica
  • ACS Nano, Vol. 6, Issue 7
  • DOI: 10.1021/nn3017469

High-Resolution Electron Microscopy and Spectroscopy of Ferritin in Biocompatible Graphene Liquid Cells and Graphene Sandwiches
journal, February 2014

  • Wang, Canhui; Qiao, Qiao; Shokuhfar, Tolou
  • Advanced Materials, Vol. 26, Issue 21
  • DOI: 10.1002/adma.201306069

Visualization of Electrode–Electrolyte Interfaces in LiPF 6 /EC/DEC Electrolyte for Lithium Ion Batteries via in Situ TEM
journal, March 2014

  • Zeng, Zhiyuan; Liang, Wen-I; Liao, Hong-Gang
  • Nano Letters, Vol. 14, Issue 4
  • DOI: 10.1021/nl403922u

X-ray Energy-Dispersive Spectrometry During In Situ Liquid Cell Studies Using an Analytical Electron Microscope
journal, February 2014

  • Zaluzec, Nestor J.; Burke, M. Grace; Haigh, Sarah J.
  • Microscopy and Microanalysis, Vol. 20, Issue 2
  • DOI: 10.1017/S1431927614000154

In Situ Structural Changes upon Electrochemical Lithium Insertion in Nanosized Anatase TiO 2
journal, December 2009

  • Lafont, U.; Carta, D.; Mountjoy, G.
  • The Journal of Physical Chemistry C, Vol. 114, Issue 2
  • DOI: 10.1021/jp908786t

Works referencing / citing this record:

In Situ Transmission Electron Microscopy on Energy‐Related Catalysis
journal, December 2019


Understanding materials challenges for rechargeable ion batteries with in situ transmission electron microscopy
journal, August 2017

  • Yuan, Yifei; Amine, Khalil; Lu, Jun
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15806

An In Situ Transmission Electron Microscopy Study of Localized Corrosion on Aluminum
journal, January 2016

  • Pinkowitz, Ainsley; Chee, See Wee; Engler, Brent J.
  • MRS Advances, Vol. 1, Issue 25
  • DOI: 10.1557/adv.2016.334