Insight into the Solid Electrolyte Interphase Formation in Bis(fluorosulfonyl)Imide Based Ionic Liquid Electrolytes
Abstract
Abstract The formation of the solid electrolyte interphase (SEI) in an ionic liquid electrolyte of 0.5 m lithium bis(fluorosulfonyl)imide (LiFSI) in 1‐ethyl‐3‐methylimidazolium bis(fluorosulfonyl)imide at high cell voltages (1.7–1.9 V) is investigated in ordered mesoporous carbon (OMC) based Li metal cells using an operando small‐angle neutron scattering (SANS) technique coupled with electrochemical impedance spectroscopy and ex situ X‐ray photoelectron spectroscopy (XPS). It is demonstrated that discharging the OMC Li metal cells to ≈2 V and holding the cell voltage constant induces a rapid current increase with time, confirming extensive reduction and SEI formation. XPS analysis reveals that LiF is formed at open cell voltage (OCV), which is attributed to the carbenes generated at the lithium negative electrode because of its reaction with EMIm cation diffusing to and initiating the reaction with FSI − anions at the carbon positive electrode. It is confirmed that the chemical reaction at OCV and electrochemical reduction at high cell voltage of the FSI − anion plays a protective role against EMIm cation co‐intercalation into the carbon positive electrode during the initial discharge. Operando SANS studies also suggest that slight differences occur in the surface composition and reaction mechanism as a function of cell voltage.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States)
- ORNLOak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- ORNLOak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1822082
- Alternate Identifier(s):
- OSTI ID: 1785742
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 31; Journal Issue: 23; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Ionic liquids; neutron scattering; lithium bis(fluorosulfonyl)imide; 1-ethyl-3- methylimidazolium bis(fluorosulfonyl)imide; solid electrolyte interphase (SEI); operando characterization
Citation Formats
Jafta, Charl, Sun, Xiao-Guang, Lyu, Hailong, Chen, Hao, Thapaliya, Bishnu, Heller, William T., Cuneo, Matthew, Mayes, Richard, Paranthaman, Parans, Dai, Sheng, and Bridges, Craig A. Insight into the Solid Electrolyte Interphase Formation in Bis(fluorosulfonyl)Imide Based Ionic Liquid Electrolytes. United States: N. p., 2021.
Web. doi:10.1002/adfm.202008708.
Jafta, Charl, Sun, Xiao-Guang, Lyu, Hailong, Chen, Hao, Thapaliya, Bishnu, Heller, William T., Cuneo, Matthew, Mayes, Richard, Paranthaman, Parans, Dai, Sheng, & Bridges, Craig A. Insight into the Solid Electrolyte Interphase Formation in Bis(fluorosulfonyl)Imide Based Ionic Liquid Electrolytes. United States. https://doi.org/10.1002/adfm.202008708
Jafta, Charl, Sun, Xiao-Guang, Lyu, Hailong, Chen, Hao, Thapaliya, Bishnu, Heller, William T., Cuneo, Matthew, Mayes, Richard, Paranthaman, Parans, Dai, Sheng, and Bridges, Craig A. Wed .
"Insight into the Solid Electrolyte Interphase Formation in Bis(fluorosulfonyl)Imide Based Ionic Liquid Electrolytes". United States. https://doi.org/10.1002/adfm.202008708. https://www.osti.gov/servlets/purl/1822082.
@article{osti_1822082,
title = {Insight into the Solid Electrolyte Interphase Formation in Bis(fluorosulfonyl)Imide Based Ionic Liquid Electrolytes},
author = {Jafta, Charl and Sun, Xiao-Guang and Lyu, Hailong and Chen, Hao and Thapaliya, Bishnu and Heller, William T. and Cuneo, Matthew and Mayes, Richard and Paranthaman, Parans and Dai, Sheng and Bridges, Craig A.},
abstractNote = {Abstract The formation of the solid electrolyte interphase (SEI) in an ionic liquid electrolyte of 0.5 m lithium bis(fluorosulfonyl)imide (LiFSI) in 1‐ethyl‐3‐methylimidazolium bis(fluorosulfonyl)imide at high cell voltages (1.7–1.9 V) is investigated in ordered mesoporous carbon (OMC) based Li metal cells using an operando small‐angle neutron scattering (SANS) technique coupled with electrochemical impedance spectroscopy and ex situ X‐ray photoelectron spectroscopy (XPS). It is demonstrated that discharging the OMC Li metal cells to ≈2 V and holding the cell voltage constant induces a rapid current increase with time, confirming extensive reduction and SEI formation. XPS analysis reveals that LiF is formed at open cell voltage (OCV), which is attributed to the carbenes generated at the lithium negative electrode because of its reaction with EMIm cation diffusing to and initiating the reaction with FSI − anions at the carbon positive electrode. It is confirmed that the chemical reaction at OCV and electrochemical reduction at high cell voltage of the FSI − anion plays a protective role against EMIm cation co‐intercalation into the carbon positive electrode during the initial discharge. Operando SANS studies also suggest that slight differences occur in the surface composition and reaction mechanism as a function of cell voltage.},
doi = {10.1002/adfm.202008708},
journal = {Advanced Functional Materials},
number = 23,
volume = 31,
place = {United States},
year = {Wed Feb 17 00:00:00 EST 2021},
month = {Wed Feb 17 00:00:00 EST 2021}
}
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