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

Erlend Bertheussen, Arnau Verdaguer Casadevall, Davide Ravasio, Joseph H. Montoya, Daniel Bøndergaard Trimarco, Claudie Roy, Sebastian Meier, Jürgen Wendland, Jens K. Nørskov, Ifan E. L. Stephens, Ib Chorkendorff

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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.
Original languageEnglish
JournalAngewandte Chemie
Volume128
Issue number4
Pages (from-to)1472-1476
Number of pages5
ISSN0044-8249
DOIs
Publication statusPublished - 2016

Bibliographical note

© 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.

Keywords

  • Analytische Chemie
  • Elektrochemie
  • Energieumwandlung; Katalyse
  • Materialwissenschaften

Cite this

Bertheussen, Erlend ; Verdaguer Casadevall, Arnau ; Ravasio, Davide ; H. Montoya, Joseph ; Trimarco, Daniel Bøndergaard ; Roy, Claudie ; Meier, Sebastian ; Wendland, Jürgen ; Nørskov, Jens K. ; E. L. Stephens, Ifan ; Chorkendorff, Ib. / Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper. In: Angewandte Chemie. 2016 ; Vol. 128, No. 4. pp. 1472-1476.
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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.",
keywords = "Analytische Chemie, Elektrochemie, Energieumwandlung; Katalyse, Materialwissenschaften",
author = "Erlend Bertheussen and {Verdaguer Casadevall}, Arnau and Davide Ravasio and {H. Montoya}, Joseph and Trimarco, {Daniel B{\o}ndergaard} and Claudie Roy and Sebastian Meier and J{\"u}rgen Wendland and N{\o}rskov, {Jens K.} and {E. L. Stephens}, Ifan and Ib Chorkendorff",
note = "{\circledC} 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.",
year = "2016",
doi = "10.1002/ange.201508851",
language = "English",
volume = "128",
pages = "1472--1476",
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Bertheussen, E, Verdaguer Casadevall, A, Ravasio, D, H. Montoya, J, Trimarco, DB, Roy, C, Meier, S, Wendland, J, Nørskov, JK, E. L. Stephens, I & Chorkendorff, I 2016, 'Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper', Angewandte Chemie, vol. 128, no. 4, pp. 1472-1476. https://doi.org/10.1002/ange.201508851

Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper. / Bertheussen, Erlend; Verdaguer Casadevall, Arnau; Ravasio, Davide; H. Montoya, Joseph; Trimarco, Daniel Bøndergaard; Roy, Claudie; Meier, Sebastian; Wendland, Jürgen; Nørskov, Jens K.; E. L. Stephens, Ifan; Chorkendorff, Ib.

In: Angewandte Chemie, Vol. 128, No. 4, 2016, p. 1472-1476.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper

AU - Bertheussen, Erlend

AU - Verdaguer Casadevall, Arnau

AU - Ravasio, Davide

AU - H. Montoya, Joseph

AU - Trimarco, Daniel Bøndergaard

AU - Roy, Claudie

AU - Meier, Sebastian

AU - Wendland, Jürgen

AU - Nørskov, Jens K.

AU - E. L. Stephens, Ifan

AU - Chorkendorff, Ib

N1 - © 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.

PY - 2016

Y1 - 2016

N2 - 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.

AB - 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.

KW - Analytische Chemie

KW - Elektrochemie

KW - Energieumwandlung; Katalyse

KW - Materialwissenschaften

U2 - 10.1002/ange.201508851

DO - 10.1002/ange.201508851

M3 - Journal article

VL - 128

SP - 1472

EP - 1476

JO - Angewandte Chemie

JF - Angewandte Chemie

SN - 0044-8249

IS - 4

ER -