Abstract
The electrocatalytic reduction of CO2 to produce sustainable fuels and chemicals is attracting great attention. Cu-based 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 Cu-sulfide 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.
Original language | English |
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Pages (from-to) | 157-165 |
Number of pages | 9 |
Journal | Catalysis Today |
Volume | 377 |
Early online date | 1 Oct 2020 |
DOIs | |
Publication status | Published - 1 Oct 2021 |
Bibliographical note
Funding Information:This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the government of the Netherlands, and by the European Research Council, project number ERC-2014-CoG 648991. MTR acknowledges the NWO-EleReCet project, which is part of the Solar-to-Products program funded by the Dutch Research Council (NWO), for funding. We are grateful to Alessandro Longo at the ESRF for providing assistance in using beamline 26 ? The Dutch-Belgian Beam Line (DUBBLE). Fei Chang is thanked for his help during the XAS beamtime. Sneh Sameer is thanked for his help on the electrochemical cell design. Kai Han, Francesco Mattarozzi and Jan Willem de Rijk are acknowledged for useful discussions on the electrochemical set-up and measurements.
Funding Information:
This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC) , a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the government of the Netherlands, and by the European Research Council, project number ERC-2014-CoG 648991. MTR acknowledges the NWO-EleReCet project, which is part of the Solar-to-Products program funded by the Dutch Research Council (NWO), for funding. We are grateful to Alessandro Longo at the ESRF for providing assistance in using beamline 26 – The Dutch-Belgian Beam Line (DUBBLE). Fei Chang is thanked for his help during the XAS beamtime. Sneh Sameer is thanked for his help on the electrochemical cell design. Kai Han, Francesco Mattarozzi and Jan Willem de Rijk are acknowledged for useful discussions on the electrochemical set-up and measurements.
Publisher Copyright:
© 2020 The Authors
Funding
This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC) , a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the government of the Netherlands, and by the European Research Council, project number ERC-2014-CoG 648991. MTR acknowledges the NWO-EleReCet project, which is part of the Solar-to-Products program funded by the Dutch Research Council (NWO), for funding. We are grateful to Alessandro Longo at the ESRF for providing assistance in using beamline 26 – The Dutch-Belgian Beam Line (DUBBLE). Fei Chang is thanked for his help during the XAS beamtime. Sneh Sameer is thanked for his help on the electrochemical cell design. Kai Han, Francesco Mattarozzi and Jan Willem de Rijk are acknowledged for useful discussions on the electrochemical set-up and measurements.
Keywords
- Carbon support
- CO reduction
- Copper sulfide
- In situ X-ray absorption spectroscopy
- Nanoparticles
- Sulfidation