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Electrochemical Reduction of Carbon Dioxide to 1-Butanol on Oxide-Derived Copper.

  • Ting LRL Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
  • García-Muelas R Institute of Chemical Research of Catalonia, The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.
  • Martín AJ Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.
  • Veenstra FLP Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.
  • Chen ST Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
  • Peng Y Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
  • Per EYX Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
  • Pablo-García S Institute of Chemical Research of Catalonia, The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.
  • López N Institute of Chemical Research of Catalonia, The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.
  • Pérez-Ramírez J Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.
  • Yeo BS Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
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  • 2020-07-25
Published in:
  • Angewandte Chemie (International ed. in English). - 2020
1-butanol
carbon dioxide reduction
density functional theory
electrochemistry
reaction mechanisms
English The electroreduction of carbon dioxide using renewable electricity is an appealing strategy for the sustainable synthesis of chemicals and fuels. Extensive research has focused on the production of ethylene, ethanol and n-propanol, but more complex C4 molecules have been scarcely reported. Herein, we report the first direct electroreduction of CO2 to 1-butanol in alkaline electrolyte on Cu gas diffusion electrodes (Faradaic efficiency=0.056 %, j1-Butanol =-0.080 mA cm-2 at -0.48 V vs. RHE) and elucidate its formation mechanism. Electrolysis of possible molecular intermediates, coupled with density functional theory, led us to propose that CO2 first electroreduces to acetaldehyde-a key C2 intermediate to 1-butanol. Acetaldehyde then undergoes a base-catalyzed aldol condensation to give crotonaldehyde via electrochemical promotion by the catalyst surface. Crotonaldehyde is subsequently electroreduced to butanal, and then to 1-butanol. In a broad context, our results point to the relevance of coupling chemical and electrochemical processes for the synthesis of higher molecular weight products from CO2 .
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  • English
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hybrid
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https://sonar.ch/global/documents/241278
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