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Title: 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 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 indicate an important step towards understanding the CO reduction mechanism on OD-Cu electrodes.
Authors:
ORCiD logo [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [4] ;  [5] ; ORCiD logo [6] ; ORCiD logo [1]
  1. Technical University of Denmark, Lyngby (Denmark)
  2. Carlsberg Lab., København V, (Denmark)
  3. Stanford Univ., Stanford, CA (United States)
  4. Carlsberg Lab., København V (Denmark)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. Technical University of Denmark, Lyngby (Denmark); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 4; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1240104

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., and Chorkendorff, Ib. Acetaldehyde as an intermediate in the electroreduction of carbon monoxide to ethanol on oxide-derived copper. United States: N. p., Web. doi:10.1002/anie.201508851.
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. Acetaldehyde as an intermediate in the electroreduction of carbon monoxide to ethanol on oxide-derived copper. United States. doi:10.1002/anie.201508851.
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., and Chorkendorff, Ib. 2015. "Acetaldehyde as an intermediate in the electroreduction of carbon monoxide to ethanol on oxide-derived copper". United States. doi:10.1002/anie.201508851. https://www.osti.gov/servlets/purl/1240104.
@article{osti_1240104,
title = {Acetaldehyde as an intermediate in the electroreduction of carbon monoxide to ethanol on oxide-derived copper},
author = {Bertheussen, Erlend and Verdaguer-Casadevall, Arnau and Ravasio, Davide and Montoya, Joseph H. and Trimarco, Daniel B. and Roy, Claudie and Meier, Sebastian and Wendland, Jürgen and Nørskov, Jens K. and Stephens, Ifan E. L. and Chorkendorff, Ib},
abstractNote = {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 indicate an important step towards understanding the CO reduction mechanism on OD-Cu electrodes.},
doi = {10.1002/anie.201508851},
journal = {Angewandte Chemie (International Edition)},
number = 4,
volume = 55,
place = {United States},
year = {2015},
month = {12}
}