<p>CO electroreduction has recently been explored as an alternative to CO<sub>2</sub> electroreduction for multicarbon product formation, because it bypasses the large carbon loss associated with CO<sub>2</sub> electroreduction. Although ethylene is generally obtained as the major product, shifting electrolysis towards the production of alcohols is an industrially promising path forward. Here we report a trimetallic-copper-based catalyst, consisting of copper nitride doped with gold nanoparticles and isolated silver atoms, with high selectivity for the formation of C<sub>2+</sub> alcohols (Faradic efficiency for ethanol + <i>n</i>-propanol is &gt;70%), within gas-fed flow cells at high current densities. Although active sites are metallic Cu(111) copper atoms derived from copper nitride, gold and silver doping suppresses ethylene formation due to the increased carbophibicity of the catalyst surface, as shown computationally. Overall, these findings open new perspectives regarding the design of catalysts for the production of liquid products from CO.</p>

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Incorporation of isolated Ag atoms and Au nanoparticles in copper nitride for selective CO electroreduction to multicarbon alcohols

  • Hong Phong Duong,
  • Jose Guillermo Rivera de la Cruz,
  • David Portehault,
  • Andrea Zitolo,
  • Jacques Louis,
  • Sandrine Zanna,
  • Quentin Arnoux,
  • Moritz W. Schreiber,
  • Nicolas Menguy,
  • Ngoc-Huan Tran,
  • Marc Fontecave

摘要

CO electroreduction has recently been explored as an alternative to CO2 electroreduction for multicarbon product formation, because it bypasses the large carbon loss associated with CO2 electroreduction. Although ethylene is generally obtained as the major product, shifting electrolysis towards the production of alcohols is an industrially promising path forward. Here we report a trimetallic-copper-based catalyst, consisting of copper nitride doped with gold nanoparticles and isolated silver atoms, with high selectivity for the formation of C2+ alcohols (Faradic efficiency for ethanol + n-propanol is >70%), within gas-fed flow cells at high current densities. Although active sites are metallic Cu(111) copper atoms derived from copper nitride, gold and silver doping suppresses ethylene formation due to the increased carbophibicity of the catalyst surface, as shown computationally. Overall, these findings open new perspectives regarding the design of catalysts for the production of liquid products from CO.