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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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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
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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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creator	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
description	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.
doi_str_mv	10.1002/ange.201508851
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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.</description><identifier>ISSN: 0044-8249</identifier><identifier>EISSN: 1521-3757</identifier><identifier>DOI: 10.1002/ange.201508851</identifier><language>eng</language><publisher>Weinheim: Blackwell Publishing Ltd</publisher><subject>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</subject><ispartof>Angewandte Chemie, 2016-01, Vol.128 (4), p.1472-1476</ispartof><rights>2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.</rights><rights>2016 WILEY-VCH Verlag GmbH & Co. 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L.</creatorcontrib><creatorcontrib>Chorkendorff, Ib</creatorcontrib><title>Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper</title><title>Angewandte Chemie</title><addtitle>Angew. Chem</addtitle><description>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. 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L.</au><au>Chorkendorff, Ib</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper</atitle><jtitle>Angewandte Chemie</jtitle><addtitle>Angew. Chem</addtitle><date>2016-01-22</date><risdate>2016</risdate><volume>128</volume><issue>4</issue><spage>1472</spage><epage>1476</epage><pages>1472-1476</pages><issn>0044-8249</issn><eissn>1521-3757</eissn><abstract>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. 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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
title	Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper
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