Infrared spectroelectrochemical study of dissociation and oxidation of methanol at a palladium electrode in alkaline solution

Langmuir. 2013 Feb 5;29(5):1709-16. doi: 10.1021/la305141q. Epub 2013 Jan 25.

Abstract

The dissociative adsorption and electrooxidation of CH(3)OH at a Pd electrode in alkaline solution are investigated by using in situ infrared spectroscopy with both internal and external reflection modes. The former (ATR-SEIRAS) has a higher sensitivity of detecting surface species, and the latter (IRAS) can easily detect dissolved species trapped in a thin-layer-structured electrolyte. Real-time ATR-SEIRAS measurement indicates that CH(3)OH dissociates to CO(ad) species at a Pd electrode accompanied by a "dip" at open circuit potential, whereas deuterium-replaced CH(3)OH doesn't, suggesting that the breaking of the C-H bond is the rate-limiting step for the dissociative adsorption of CH(3)OH. Potential-dependent ATR-SEIRAS and IRAS measurements indicate that CH(3)OH is electrooxidized to formate and/or (bi)carbonate, the relative concentrations of which depend on the potential applied. Specifically, at potentials negative of ca. -0.15 V (vs Ag/AgCl), formate is the predominant product and (bi)carbonate (or CO(2) in the thin-layer structure of IRAS) is more favorable at potentials from -0.15 to 0.10 V. Further oxidation of the CO(ad) intermediate species arising from CH(3)OH dissociation is involved in forming (bi)carbonate at potentials above -0.15 V. Although the partial transformation from interfacial formate to (bi)carbonate may be justified, no bridge-bonded formate species can be detected over the potential range under investigation.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Electrochemical Techniques*
  • Electrodes
  • Methanol / chemistry*
  • Oxidation-Reduction
  • Palladium / chemistry*
  • Sodium Hydroxide / chemistry*
  • Solutions
  • Spectrophotometry, Infrared

Substances

  • Solutions
  • Sodium Hydroxide
  • Palladium
  • Methanol