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  Steering Hydrocarbon Selectivity in CO2 Electroreduction over Soft-Landed CuOx Nanoparticle-Functionalized Gas Diffusion Electrodes

Daems, N., Choukroun, D., Merino, P., Rettenmaier, C., Pacquets, L., Bergmann, A., et al. (2022). Steering Hydrocarbon Selectivity in CO2 Electroreduction over Soft-Landed CuOx Nanoparticle-Functionalized Gas Diffusion Electrodes. ACS Applied Materials and Interfaces, 14(2), 2691-2702. doi:10.1021/acsami.1c17998.

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 Creators:
Daems, Nick1, Author
Choukroun, Daniel1, Author
Merino, Pablo2, Author
Rettenmaier, Clara3, Author              
Pacquets, Lien1, 4, Author
Bergmann, Arno3, Author              
Santoro, Gonzalo2, Author
Vázquez, Luis2, Author
Martínez, Lidia2, Author
Roldan Cuenya, Beatriz3, Author              
Martín Gago, Jose Angel2, Author
Breugelmans, Tom1, Author
Affiliations:
1Applied Electrochemistry and Catalysis (ELCAT), University of Antwerp, 2610 Wilrijk, Belgium, ou_persistent22              
2ESISNA Research Group, Institute of Materials Science of Madrid (CSIC), 28049 Madrid, Spain, ou_persistent22              
3Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
4Electron Microscopy for Materials Science (EMAT), University of Antwerp, 2020 Antwerp, Belgium, ou_persistent22              

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 Abstract: The use of physical vapor deposition methods in the fabrication of catalyst layers holds promise for enhancing the efficiency of future carbon capture and utilization processes such as the CO2 reduction reaction (CO2RR). Following that line of research, we report in this work the application of a sputter gas aggregation source (SGAS) and a multiple ion cluster source type apparatus, for the controlled synthesis of CuOx nanoparticles (NPs) atop gas diffusion electrodes. By varying the mass loading, we achieve control over the balance between methanation and multicarbon formation in a gas-fed CO2 electrolyzer and obtain peak CH4 partial current densities of −143 mA cm−2 (mass activity of 7.2 kA/g) with a Faradaic efficiency (FE) of 48% and multicarbon partial current densities of −231 mA cm−2 at 76% FE (FEC2H4 = 56%). Using atomic force microscopy, electron microscopy, and quasi in situ X-ray photoelectron spectroscopy, we trace back the divergence in hydrocarbon selectivity to differences in NP film morphology and rule out the influence of both the NP size (3−15 nm, >20 μg cm −2) and in situ oxidation state. We show that the combination of the O2 flow rate to the aggregation zone during NP growth and deposition time, which affect the NP production rate and mass loading, respectively, gives rise to the formation of either densely packed CuOx NPs or rough three-dimensional networks made from CuOx NP building blocks, which in turn affects the governing CO2RR mechanism. This study highlights the potential held by SGAS-generated NP films for future CO2RR catalyst layer optimization and upscaling, where the NPs’ tunable properties, homogeneity, and the complete absence of organic capping agents may prove invaluable.

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Language(s): eng - English
 Dates: 2021-09-172021-12-262022-01-052022-01-19
 Publication Status: Published in print
 Pages: 12
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acsami.1c17998
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: ACS Applied Materials and Interfaces
  Abbreviation : ACS Appl. Mater. Interfaces
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 12 Volume / Issue: 14 (2) Sequence Number: - Start / End Page: 2691 - 2702 Identifier: ISSN: 1944-8244
CoNE: https://pure.mpg.de/cone/journals/resource/1944-8244