Investigating Li Microstructure Formation on Li Anodes for Lithium Batteries by in Situ <sup>6</sup>Li/<sup>7</sup>Li NMR and SEM

Hee Jung Chang, Nicole M. Trease, Andrew J. Ilott, Dongli Zeng, Lin Shu Du, Alexej Jerschow, Clare P. Grey

Research output: Contribution to journalArticle

Abstract

The growth of lithium microstructures during battery cycling has, to date, prohibited the use of Li metal anodes and raises serious safety concerns even in conventional lithium-ion rechargeable batteries, particularly if they are charged at high rates. The electrochemical conditions under which these Li microstructures grow have, therefore, been investigated by in situ nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), and susceptibility calculations. Lithium metal symmetric bag cells containing LiPF<inf>6</inf> in EC/DMC electrolytes were used. Distinct <sup>7</sup>Li NMR resonances were observed due to the Li metal bulk electrodes and microstructures, the changes in peak positions and intensities being monitored in situ during Li deposition. The changes in the NMR spectra, observed as a function of separator thickness and porosity (using Celgard and Whatmann glass microfiber membranes) and different applied pressures, were correlated with changes in the type of microstructure, by using SEM. Isotopically enriched <sup>6</sup>Li metal electrodes were used against natural abundance predominantly <sup>7</sup>Li metal counter electrodes to investigate radiofrequency (rf) field penetration into the Li anode and to confirm the assignment of the higher frequency peak to Li dendrites. The conclusions were supported by calculations performed to explore the effect of the different microstructures on peak position/broadening, the study showing that Li NMR spectroscopy can be used as a sensitive probe of both the amount and type of microstructure formation.

Original languageEnglish (US)
Pages (from-to)16443-16451
Number of pages9
JournalJournal of Physical Chemistry C
Volume119
Issue number29
DOIs
StatePublished - Jul 23 2015

Fingerprint

Lithium batteries
lithium batteries
Anodes
anodes
Nuclear magnetic resonance
Metals
nuclear magnetic resonance
microstructure
Microstructure
Scanning electron microscopy
scanning electron microscopy
Lithium
metals
lithium
Electrodes
electrodes
electric batteries
microfibers
Secondary batteries
magnetic resonance spectroscopy

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

Investigating Li Microstructure Formation on Li Anodes for Lithium Batteries by in Situ <sup>6</sup>Li/<sup>7</sup>Li NMR and SEM. / Chang, Hee Jung; Trease, Nicole M.; Ilott, Andrew J.; Zeng, Dongli; Du, Lin Shu; Jerschow, Alexej; Grey, Clare P.

In: Journal of Physical Chemistry C, Vol. 119, No. 29, 23.07.2015, p. 16443-16451.

Research output: Contribution to journalArticle

Chang, Hee Jung ; Trease, Nicole M. ; Ilott, Andrew J. ; Zeng, Dongli ; Du, Lin Shu ; Jerschow, Alexej ; Grey, Clare P. / Investigating Li Microstructure Formation on Li Anodes for Lithium Batteries by in Situ <sup>6</sup>Li/<sup>7</sup>Li NMR and SEM. In: Journal of Physical Chemistry C. 2015 ; Vol. 119, No. 29. pp. 16443-16451.
@article{d6e7ac21153245de821c26966b23320b,
title = "Investigating Li Microstructure Formation on Li Anodes for Lithium Batteries by in Situ 6Li/7Li NMR and SEM",
abstract = "The growth of lithium microstructures during battery cycling has, to date, prohibited the use of Li metal anodes and raises serious safety concerns even in conventional lithium-ion rechargeable batteries, particularly if they are charged at high rates. The electrochemical conditions under which these Li microstructures grow have, therefore, been investigated by in situ nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), and susceptibility calculations. Lithium metal symmetric bag cells containing LiPF6 in EC/DMC electrolytes were used. Distinct 7Li NMR resonances were observed due to the Li metal bulk electrodes and microstructures, the changes in peak positions and intensities being monitored in situ during Li deposition. The changes in the NMR spectra, observed as a function of separator thickness and porosity (using Celgard and Whatmann glass microfiber membranes) and different applied pressures, were correlated with changes in the type of microstructure, by using SEM. Isotopically enriched 6Li metal electrodes were used against natural abundance predominantly 7Li metal counter electrodes to investigate radiofrequency (rf) field penetration into the Li anode and to confirm the assignment of the higher frequency peak to Li dendrites. The conclusions were supported by calculations performed to explore the effect of the different microstructures on peak position/broadening, the study showing that Li NMR spectroscopy can be used as a sensitive probe of both the amount and type of microstructure formation.",
author = "Chang, {Hee Jung} and Trease, {Nicole M.} and Ilott, {Andrew J.} and Dongli Zeng and Du, {Lin Shu} and Alexej Jerschow and Grey, {Clare P.}",
year = "2015",
month = "7",
day = "23",
doi = "10.1021/acs.jpcc.5b03396",
language = "English (US)",
volume = "119",
pages = "16443--16451",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "29",

}

TY - JOUR

T1 - Investigating Li Microstructure Formation on Li Anodes for Lithium Batteries by in Situ 6Li/7Li NMR and SEM

AU - Chang, Hee Jung

AU - Trease, Nicole M.

AU - Ilott, Andrew J.

AU - Zeng, Dongli

AU - Du, Lin Shu

AU - Jerschow, Alexej

AU - Grey, Clare P.

PY - 2015/7/23

Y1 - 2015/7/23

N2 - The growth of lithium microstructures during battery cycling has, to date, prohibited the use of Li metal anodes and raises serious safety concerns even in conventional lithium-ion rechargeable batteries, particularly if they are charged at high rates. The electrochemical conditions under which these Li microstructures grow have, therefore, been investigated by in situ nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), and susceptibility calculations. Lithium metal symmetric bag cells containing LiPF6 in EC/DMC electrolytes were used. Distinct 7Li NMR resonances were observed due to the Li metal bulk electrodes and microstructures, the changes in peak positions and intensities being monitored in situ during Li deposition. The changes in the NMR spectra, observed as a function of separator thickness and porosity (using Celgard and Whatmann glass microfiber membranes) and different applied pressures, were correlated with changes in the type of microstructure, by using SEM. Isotopically enriched 6Li metal electrodes were used against natural abundance predominantly 7Li metal counter electrodes to investigate radiofrequency (rf) field penetration into the Li anode and to confirm the assignment of the higher frequency peak to Li dendrites. The conclusions were supported by calculations performed to explore the effect of the different microstructures on peak position/broadening, the study showing that Li NMR spectroscopy can be used as a sensitive probe of both the amount and type of microstructure formation.

AB - The growth of lithium microstructures during battery cycling has, to date, prohibited the use of Li metal anodes and raises serious safety concerns even in conventional lithium-ion rechargeable batteries, particularly if they are charged at high rates. The electrochemical conditions under which these Li microstructures grow have, therefore, been investigated by in situ nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), and susceptibility calculations. Lithium metal symmetric bag cells containing LiPF6 in EC/DMC electrolytes were used. Distinct 7Li NMR resonances were observed due to the Li metal bulk electrodes and microstructures, the changes in peak positions and intensities being monitored in situ during Li deposition. The changes in the NMR spectra, observed as a function of separator thickness and porosity (using Celgard and Whatmann glass microfiber membranes) and different applied pressures, were correlated with changes in the type of microstructure, by using SEM. Isotopically enriched 6Li metal electrodes were used against natural abundance predominantly 7Li metal counter electrodes to investigate radiofrequency (rf) field penetration into the Li anode and to confirm the assignment of the higher frequency peak to Li dendrites. The conclusions were supported by calculations performed to explore the effect of the different microstructures on peak position/broadening, the study showing that Li NMR spectroscopy can be used as a sensitive probe of both the amount and type of microstructure formation.

UR - http://www.scopus.com/inward/record.url?scp=84937826111&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84937826111&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcc.5b03396

DO - 10.1021/acs.jpcc.5b03396

M3 - Article

VL - 119

SP - 16443

EP - 16451

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 29

ER -