Properties of High Na-Ion Content N-Propyl-N-Methylpyrrolidinium Bis(Fluorosulfonyl)Imide -Ethylene Carbonate Electrolytes

S. A.M. Noor, N. C. Su, L. T. Khoon, N. S. Mohamed, Azizan Ahmad, M. Z.A. Yahya, H. Zhu, M. Forsyth, D. R. MacFarlane

Research output: Contribution to journalArticle

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Abstract

Sodium-based batteries have emerged as promising alternatives to Li-based batteries for future safe, high energy-density energy storage. They are expected to be cheaper, due to the greater abundance of Na and likely reduction in raw material costs. In this study, we investigate the properties of superconcentrated sodium bis(fluorosulfonyl)amide (NaFSI) mixtures with the ionic liquid (IL) methylpropylpyrrolinium (C3mpyr) FSI in the presence of ethylene carbonate (EC) in the liquid and gel states. Ionic conductivity and thermal stability are evaluated through electrochemical impedance spectroscopy (EIS) and differential scanning calorimetry (DSC), respectively. NaFSI is soluble in the IL up to 55 mol% Na; adding EC (30 wt.%) to the IL almost doubles the ionic conductivity at ambient temperature. The temperature dependence of conductivity is well described by the Vogel-Tamman-Fulcher equation. NMR spectroscopy and Pulse Field Gradient NMR diffusion were employed to investigate transport in these electrolyte systems, while the chemical interactions were also studied using ATR-FTIR. Stable plasticized gel electrolytes were observed, even at 30 wt. % EC; the formation of the gel does not significantly affect the liquid-like ion dynamics in these materials, as shown by DSC and FTIR analysis. The Na+ transference number of Na0.55[C3mpyr]0.45[FSI] + 30 wt.% EC was up to 0.32, and deposition and dissolution of sodium metal were observed in cyclic voltammetry around 0 V vs. Na/Na+. Moreover, the suitability of the prepared electrolyte is preliminarily verified in half-cells at room temperature using Na3V2(PO4)3 as a cathode. The cells delivered capacity of 52.4 mAhg−1 at C/20.

Original languageEnglish
Pages (from-to)983-993
Number of pages11
JournalElectrochimica Acta
Volume247
DOIs
Publication statusPublished - 1 Sep 2017

Fingerprint

Imides
Ionic Liquids
Electrolytes
Carbonates
Ethylene
Ionic liquids
Ions
Gels
Sodium
Ionic conductivity
Differential scanning calorimetry
Liquids
Electrochemical impedance spectroscopy
Amides
Temperature
Energy storage
Nuclear magnetic resonance spectroscopy
Cyclic voltammetry
Raw materials
Dissolution

Keywords

  • ethylene carbonate
  • ionic liquid
  • sodium ion conductors
  • superconcentrated sodium electrolyte

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Electrochemistry

Cite this

Properties of High Na-Ion Content N-Propyl-N-Methylpyrrolidinium Bis(Fluorosulfonyl)Imide -Ethylene Carbonate Electrolytes. / Noor, S. A.M.; Su, N. C.; Khoon, L. T.; Mohamed, N. S.; Ahmad, Azizan; Yahya, M. Z.A.; Zhu, H.; Forsyth, M.; MacFarlane, D. R.

In: Electrochimica Acta, Vol. 247, 01.09.2017, p. 983-993.

Research output: Contribution to journalArticle

Noor, S. A.M. ; Su, N. C. ; Khoon, L. T. ; Mohamed, N. S. ; Ahmad, Azizan ; Yahya, M. Z.A. ; Zhu, H. ; Forsyth, M. ; MacFarlane, D. R. / Properties of High Na-Ion Content N-Propyl-N-Methylpyrrolidinium Bis(Fluorosulfonyl)Imide -Ethylene Carbonate Electrolytes. In: Electrochimica Acta. 2017 ; Vol. 247. pp. 983-993.
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AU - Su, N. C.

AU - Khoon, L. T.

AU - Mohamed, N. S.

AU - Ahmad, Azizan

AU - Yahya, M. Z.A.

AU - Zhu, H.

AU - Forsyth, M.

AU - MacFarlane, D. R.

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AB - Sodium-based batteries have emerged as promising alternatives to Li-based batteries for future safe, high energy-density energy storage. They are expected to be cheaper, due to the greater abundance of Na and likely reduction in raw material costs. In this study, we investigate the properties of superconcentrated sodium bis(fluorosulfonyl)amide (NaFSI) mixtures with the ionic liquid (IL) methylpropylpyrrolinium (C3mpyr) FSI in the presence of ethylene carbonate (EC) in the liquid and gel states. Ionic conductivity and thermal stability are evaluated through electrochemical impedance spectroscopy (EIS) and differential scanning calorimetry (DSC), respectively. NaFSI is soluble in the IL up to 55 mol% Na; adding EC (30 wt.%) to the IL almost doubles the ionic conductivity at ambient temperature. The temperature dependence of conductivity is well described by the Vogel-Tamman-Fulcher equation. NMR spectroscopy and Pulse Field Gradient NMR diffusion were employed to investigate transport in these electrolyte systems, while the chemical interactions were also studied using ATR-FTIR. Stable plasticized gel electrolytes were observed, even at 30 wt. % EC; the formation of the gel does not significantly affect the liquid-like ion dynamics in these materials, as shown by DSC and FTIR analysis. The Na+ transference number of Na0.55[C3mpyr]0.45[FSI] + 30 wt.% EC was up to 0.32, and deposition and dissolution of sodium metal were observed in cyclic voltammetry around 0 V vs. Na/Na+. Moreover, the suitability of the prepared electrolyte is preliminarily verified in half-cells at room temperature using Na3V2(PO4)3 as a cathode. The cells delivered capacity of 52.4 mAhg−1 at C/20.

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