Multinuclear NMR Study of the Solid Electrolyte Interface Formed in Lithium Metal Batteries

Chuan Wan, Suochang Xu, Mary Y. Hu, Ruiguo Cao, Jiangfeng Qian, Zhaohai Qin, Jun Liu, Karl Todd Mueller, Ji Guang Zhang, Jian Zhi Hu

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

The composition of the solid electrolyte interphase (SEI) layers formed in Cu|Li cells using lithium bis(fluorosulfonyi)imide (LiFSI) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in 1,2-dimethoxyethane (DME) electrolytes is determined by a multinuclear solid-state MAS NMR study at high magnetic field. It is found that the "dead" metallic Li is largely reduced in the SEI layers formed in a 4 M LiFSI-DME electrolyte system compared with those formed in a 1 M LiFSI-DME electrolyte system. This finding relates directly to the safety of Li metal batteries, as one of the main safety concerns for these batteries is associated with the "dead" metallic Li formed after long-term cycling. It is also found that a large amount of LiF, which exhibits superior mechanical strength and good Li + ionic conductivity, is observed in the SEI layer formed in the concentrated 4 M LiFSI-DME and 3 M LiTFSI-DME systems but not in the diluted 1 M LiFSI-DME system. Quantitative 6 Li MAS NMR results indicate that the SEI associated with the 4 M LiFSI-DME electrolyte is denser than those formed in the 1 M LiFSI-DME and 3 M LiTFSI-DME systems. These studies reveal the fundamental mechanisms behind the excellent electrochemical performance associated with higher concentration LiFSI-DME electrolyte systems.

Original languageEnglish (US)
Pages (from-to)14741-14748
Number of pages8
JournalACS Applied Materials and Interfaces
Volume9
Issue number17
DOIs
StatePublished - May 3 2017

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Solid electrolytes
Lithium
Metals
Electrolytes
Nuclear magnetic resonance
Ionic conductivity
Strength of materials
1,2-dimethoxyethane
Magnetic fields
Imides
Chemical analysis

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Cite this

Wan, Chuan ; Xu, Suochang ; Hu, Mary Y. ; Cao, Ruiguo ; Qian, Jiangfeng ; Qin, Zhaohai ; Liu, Jun ; Mueller, Karl Todd ; Zhang, Ji Guang ; Hu, Jian Zhi. / Multinuclear NMR Study of the Solid Electrolyte Interface Formed in Lithium Metal Batteries. In: ACS Applied Materials and Interfaces. 2017 ; Vol. 9, No. 17. pp. 14741-14748.
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abstract = "The composition of the solid electrolyte interphase (SEI) layers formed in Cu|Li cells using lithium bis(fluorosulfonyi)imide (LiFSI) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in 1,2-dimethoxyethane (DME) electrolytes is determined by a multinuclear solid-state MAS NMR study at high magnetic field. It is found that the {"}dead{"} metallic Li is largely reduced in the SEI layers formed in a 4 M LiFSI-DME electrolyte system compared with those formed in a 1 M LiFSI-DME electrolyte system. This finding relates directly to the safety of Li metal batteries, as one of the main safety concerns for these batteries is associated with the {"}dead{"} metallic Li formed after long-term cycling. It is also found that a large amount of LiF, which exhibits superior mechanical strength and good Li + ionic conductivity, is observed in the SEI layer formed in the concentrated 4 M LiFSI-DME and 3 M LiTFSI-DME systems but not in the diluted 1 M LiFSI-DME system. Quantitative 6 Li MAS NMR results indicate that the SEI associated with the 4 M LiFSI-DME electrolyte is denser than those formed in the 1 M LiFSI-DME and 3 M LiTFSI-DME systems. These studies reveal the fundamental mechanisms behind the excellent electrochemical performance associated with higher concentration LiFSI-DME electrolyte systems.",
author = "Chuan Wan and Suochang Xu and Hu, {Mary Y.} and Ruiguo Cao and Jiangfeng Qian and Zhaohai Qin and Jun Liu and Mueller, {Karl Todd} and Zhang, {Ji Guang} and Hu, {Jian Zhi}",
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Wan, C, Xu, S, Hu, MY, Cao, R, Qian, J, Qin, Z, Liu, J, Mueller, KT, Zhang, JG & Hu, JZ 2017, 'Multinuclear NMR Study of the Solid Electrolyte Interface Formed in Lithium Metal Batteries', ACS Applied Materials and Interfaces, vol. 9, no. 17, pp. 14741-14748. https://doi.org/10.1021/acsami.6b15383

Multinuclear NMR Study of the Solid Electrolyte Interface Formed in Lithium Metal Batteries. / Wan, Chuan; Xu, Suochang; Hu, Mary Y.; Cao, Ruiguo; Qian, Jiangfeng; Qin, Zhaohai; Liu, Jun; Mueller, Karl Todd; Zhang, Ji Guang; Hu, Jian Zhi.

In: ACS Applied Materials and Interfaces, Vol. 9, No. 17, 03.05.2017, p. 14741-14748.

Research output: Contribution to journalArticle

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T1 - Multinuclear NMR Study of the Solid Electrolyte Interface Formed in Lithium Metal Batteries

AU - Wan, Chuan

AU - Xu, Suochang

AU - Hu, Mary Y.

AU - Cao, Ruiguo

AU - Qian, Jiangfeng

AU - Qin, Zhaohai

AU - Liu, Jun

AU - Mueller, Karl Todd

AU - Zhang, Ji Guang

AU - Hu, Jian Zhi

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AB - The composition of the solid electrolyte interphase (SEI) layers formed in Cu|Li cells using lithium bis(fluorosulfonyi)imide (LiFSI) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in 1,2-dimethoxyethane (DME) electrolytes is determined by a multinuclear solid-state MAS NMR study at high magnetic field. It is found that the "dead" metallic Li is largely reduced in the SEI layers formed in a 4 M LiFSI-DME electrolyte system compared with those formed in a 1 M LiFSI-DME electrolyte system. This finding relates directly to the safety of Li metal batteries, as one of the main safety concerns for these batteries is associated with the "dead" metallic Li formed after long-term cycling. It is also found that a large amount of LiF, which exhibits superior mechanical strength and good Li + ionic conductivity, is observed in the SEI layer formed in the concentrated 4 M LiFSI-DME and 3 M LiTFSI-DME systems but not in the diluted 1 M LiFSI-DME system. Quantitative 6 Li MAS NMR results indicate that the SEI associated with the 4 M LiFSI-DME electrolyte is denser than those formed in the 1 M LiFSI-DME and 3 M LiTFSI-DME systems. These studies reveal the fundamental mechanisms behind the excellent electrochemical performance associated with higher concentration LiFSI-DME electrolyte systems.

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