Catalyst and electrolyte synergy in Li-O2 batteries

Forrest S. Gittleson, Ryan C. Sekol, Gustavo Doubek, Marcelo Linardi, Andre Taylor

Research output: Contribution to journalArticle

Abstract

Understanding the interactions between catalyst and electrolyte in Li-O2 systems is crucial to improving capacities, efficiencies, and cycle life. In this study, supported noble metal catalysts Pt/C, Pd/C, and Au/C were paired with popular Li-O2 electrolyte solvents dimethoxyethane (DME), tetraglyme (TEGDME), and dimethyl sulfoxide (DMSO). The effects of these combinations on stability, kinetics, and activity were assessed. We show evidence of a synergistic effect between Pt and Pd catalysts and a DMSO-based electrolyte which enhances the kinetics of oxygen reduction and evolution reactions. DME and TEGDME are more prone to decomposition and less kinetically favorable for oxygen reduction and evolution than DMSO. While the order of oxygen reduction onset potentials with each catalyst was found to be consistent across electrolyte (Pd > Pt > Au), larger overpotentials with DME and TEGDME, and negative shifts in onset after only five cycles favor the stability of a DMSO electrolyte. Full cell cycling experiments confirm that catalyst-DMSO combinations produce up to 9 times higher discharge capacities than the same with TEGDME after 20 cycles (∼707.4 vs. 78.8 mA h g-1 with Pd/C). Ex situ EDS and in situ EIS analyses of resistive species in the cathode suggest that improvements in capacity with DMSO are due to a combination of greater electrolyte conductivity and catalyst synergies. Our findings demonstrate that co-selection of catalyst and electrolyte is necessary to exploit chemical synergies and improve the performance of Li-O2 cells. This journal is

Original languageEnglish (US)
Pages (from-to)3230-3237
Number of pages8
JournalPhysical Chemistry Chemical Physics
Volume16
Issue number7
DOIs
StatePublished - Feb 21 2014

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Electrolytes
electric batteries
Dimethyl Sulfoxide
electrolytes
catalysts
Catalysts
cycles
Oxygen
oxygen
Kinetics
kinetics
Precious metals
noble metals
cells
Life cycle
Energy dispersive spectroscopy
Cathodes
cathodes
Decomposition
decomposition

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Gittleson, F. S., Sekol, R. C., Doubek, G., Linardi, M., & Taylor, A. (2014). Catalyst and electrolyte synergy in Li-O2 batteries. Physical Chemistry Chemical Physics, 16(7), 3230-3237. https://doi.org/10.1039/c3cp54555e

Catalyst and electrolyte synergy in Li-O2 batteries. / Gittleson, Forrest S.; Sekol, Ryan C.; Doubek, Gustavo; Linardi, Marcelo; Taylor, Andre.

In: Physical Chemistry Chemical Physics, Vol. 16, No. 7, 21.02.2014, p. 3230-3237.

Research output: Contribution to journalArticle

Gittleson, FS, Sekol, RC, Doubek, G, Linardi, M & Taylor, A 2014, 'Catalyst and electrolyte synergy in Li-O2 batteries', Physical Chemistry Chemical Physics, vol. 16, no. 7, pp. 3230-3237. https://doi.org/10.1039/c3cp54555e
Gittleson FS, Sekol RC, Doubek G, Linardi M, Taylor A. Catalyst and electrolyte synergy in Li-O2 batteries. Physical Chemistry Chemical Physics. 2014 Feb 21;16(7):3230-3237. https://doi.org/10.1039/c3cp54555e
Gittleson, Forrest S. ; Sekol, Ryan C. ; Doubek, Gustavo ; Linardi, Marcelo ; Taylor, Andre. / Catalyst and electrolyte synergy in Li-O2 batteries. In: Physical Chemistry Chemical Physics. 2014 ; Vol. 16, No. 7. pp. 3230-3237.
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