Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper

Oxide‐derived copper (OD‐Cu) electrodes exhibit unprecedented CO reduction performance towards liquid fuels, producing ethanol and acetate with >50 % Faradaic efficiency at −0.3 V (vs. RHE). By using static headspace‐gas chromatography for liquid phase analysis, we identify acetaldehyde as a mino...

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Bibliographic Details
Published in:Angewandte Chemie 2016-01, Vol.128 (4), p.1472-1476
Main Authors: Bertheussen, Erlend, Verdaguer-Casadevall, Arnau, Ravasio, Davide, Montoya, Joseph H., Trimarco, Daniel B., Roy, Claudie, Meier, Sebastian, Wendland, Jürgen, Nørskov, Jens K., Stephens, Ifan E. L., Chorkendorff, Ib
Format: Article
Language:English
Subjects:
Acetaldehyde
ALDEHYDES
Analytische Chemie
Carbon
CARBON MONOXIDE
Chemistry
Chromatography
Copper
Efficiency
Electrodes
Electrowinning
Elektrochemie
Energieumwandlung
Ethanol
ETHYL ALCOHOL
Fuels
Gas chromatography
Headspace
Katalyse
Liquid fuels
Magnetic resonance spectroscopy
Materialwissenschaften
NMR spectroscopy
OXIDES
Reduction
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Summary:Oxide‐derived copper (OD‐Cu) electrodes exhibit unprecedented CO reduction performance towards liquid fuels, producing ethanol and acetate with >50 % Faradaic efficiency at −0.3 V (vs. RHE). By using static headspace‐gas chromatography for liquid phase analysis, we identify acetaldehyde as a minor product and key intermediate in the electroreduction of CO to ethanol on OD‐Cu electrodes. Acetaldehyde is produced with a Faradaic efficiency of ≈5 % at −0.33 V (vs. RHE). We show that acetaldehyde forms at low steady‐state concentrations, and that free acetaldehyde is difficult to detect in alkaline solutions using NMR spectroscopy, requiring alternative methods for detection and quantification. Our results represent an important step towards understanding the CO reduction mechanism on OD‐Cu electrodes. Kupfer & CO: Acetaldehyd wurde als ein Produkt und Schlüsselintermediat der Reduktion von CO zu Ethanol auf Oxid‐abgeleitetem Kupfer identifiziert. Die Detektion von Acetaldehyd mit NMR‐Spektroskopie in alkalischer Lösung erwies sich als anspruchsvoll und erforderte den Einsatz komplementärer Techniken.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201508851