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Influence of Tetraalkylammonium Cation Chain Length on Gold and Glassy Carbon Electrode Interfaces for Alkali Metal-Oxygen Batteries.

Authors
  • Aldous, Iain M
  • Hardwick, Laurence J
Type
Published Article
Journal
The Journal of Physical Chemistry Letters
Publisher
American Chemical Society
Publication Date
Nov 06, 2014
Volume
5
Issue
21
Pages
3924–3930
Identifiers
DOI: 10.1021/jz501850u
PMID: 26278771
Source
Medline
Keywords
License
Unknown

Abstract

Fundamental studies of dioxygen electrochemistry relevant to metal-air batteries commonly require conductive supporting salts, such as tetraalkylammonium, to sustain redox processes in nonaqueous electrolytes. Electrochemical analysis of the formation and oxidation of superoxide on glassy carbon and gold working electrodes has shown a decrease in reversibility and lowering of the oxygen reduction rate constant when tetraalkylammonium cation alkyl chain length is increased. Probing interfacial regions on Au using in situ surface enhanced Raman spectroscopy (SERS) provides evidence that this is caused by the changing adsorption characteristics of tetralkylammonium cations under negative potentials. These effects are heightened with longer alkyl chain lengths, therefore reducing the reversibility of superoxide formation and dioxygen evolution. From these observations it can be established that shorter chain tetraalkylammonium cations while retaining necessary conductive support: (1) enhance reversibility and rate of superoxide formation and oxidation and (2) for in situ SERS, have lower preference for adsorption, thus improving experimental detection of superoxide at the Au electrode interface.

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