Role of the adsorbed oxygen species in the selective electrochemical reduction of CO2 to alcohols and carbonyls on copper electrodes

Paramaconi Rodriguez, Matthew Lawrence, Cécile Le Duff

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Abstract

The electrochemical reduction of CO2 into fuels has gained significant attention recently as source of renewable carbon-based fuels. The unique high selectivity of copper in the electrochemical reduction of CO2 to hydrocarbons has called much interest in discovering its mechanism. In order to provide significant information about the role of oxygen in the electrochemical reduction of CO2 on Cu electrodes, the conditions of the surface structure and the composition of the Cu single crystal electrodes were controlled over time. This was achieved using pulsed voltammetry, since the pulse sequence can be programmed to guarantee reproducible initial conditions for the reaction at every fraction of time and at a given frequency. In contrast to the selectivity of CO2 reduction using cyclic voltammetry and chronoamperometric methods, a large selection of oxygenated hydrocarbons was found under alternating voltage conditions. Product selectivity towards the formation of oxygenated hydrocarbon was associated to the coverage of oxygen species, which is surface-structure-and-potential dependent.
Original languageEnglish
Pages (from-to)12919–12924
JournalAngewandte Chemie (International Edition)
Volume56
Issue number42
Early online date18 Sept 2017
DOIs
Publication statusPublished - 9 Oct 2017

Keywords

  • CO2 reduction
  • selectivity
  • surface structure
  • pulse voltammetry
  • copper oxides
  • copper electrodes

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