4.7 Article

Copper sulfide derived nanoparticles supported on carbon for the electrochemical reduction of carbon dioxide

Journal

CATALYSIS TODAY
Volume 377, Issue -, Pages 157-165

Publisher

ELSEVIER
DOI: 10.1016/j.cattod.2020.09.020

Keywords

Copper sulfide; Nanoparticles; Carbon support; Sulfidation; In situ X-ray absorption spectroscopy; CO(2 r)eduction

Funding

  1. Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC)
  2. NWO Gravitation program - Ministry of Education, Culture and Science of the government of the Netherlands
  3. European Research Council [648991]
  4. Dutch Research Council (NWO)
  5. European Research Council (ERC) [648991] Funding Source: European Research Council (ERC)

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The study introduces a novel strategy for preparing Cu nanoparticle catalysts and investigates the evolution of Cu species under CO2 reduction conditions, revealing the selectivity and efficiency of the catalysts.
The electrocatalytic reduction of CO2 to produce sustainable fuels and chemicals is attracting great attention. Cubased catalysts can lead to the production of a range of different molecules, and interestingly the product selectivity strongly depends on the preparation history, although it is not fully understood yet why. We report a novel strategy that allowed us to prepare Cu nanoparticle on carbon catalysts with similar morphologies, but prepared by in-situ reduction of either supported CuS, Cu2S or CuO nanoparticles. For the first time the evolution of the Cu species was followed under CO2 and H+ reduction conditions using in-situ X-ray absorption spectroscopy. Excellent electrochemical contact between the Cu-based nanoparticles, the carbon support and the carbon-paper substrate was observed, resulting in metallic Cu as the predominant phase under typical electrochemical CO2 reduction conditions. Even covering less than 4% of the H2 producing carbon support with Cusulfide derived nanoparticles allowed to steer the selectivity to a maximum of 12% Faradaic efficiency for the production of formate. Clear differences between the catalysts derived from CuS, Cu2S or CuO nanoparticles were observed, which was ascribed to the presence of residual sulfur in the catalysts.

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