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Role of the Adsorbed Oxygen Species in the Selective Electrochemical Reduction of CO 2 to Alcohols and Carbonyls on Copper Electrodes
Author(s) -
Le Duff Cécile S.,
Lawrence Matthew J.,
Rodriguez Paramaconi
Publication year - 2017
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201706463
Subject(s) - chemistry , electrochemistry , selectivity , cyclic voltammetry , inorganic chemistry , copper , oxygen , electrode , hydrocarbon , adsorption , catalysis , organic chemistry
The electrochemical reduction of CO 2 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 CO 2 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 CO 2 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 CO 2 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.