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  Shape-Dependent CO2 Hydrogenation to Methanol over Cu2O Nanocubes Supported on ZnO

Kordus, D., Jelic, J., Lopez-Luna, M., Divins, N. J., Timoshenko, J., Chee, S. W., et al. (2023). Shape-Dependent CO2 Hydrogenation to Methanol over Cu2O Nanocubes Supported on ZnO. Journal of the American Chemical Society, 145(5), 3016-3030. doi:10.1021/jacs.2c11540.

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jacs.2c11540.pdf (Verlagsversion), 6MB
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2023
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 Urheber:
Kordus, David1, Autor           
Jelic, Jelena, Autor
Lopez-Luna, Mauricio1, Autor           
Divins, Núria J., Autor
Timoshenko, Janis1, Autor           
Chee, See Wee1, Autor           
Rettenmaier, Clara1, Autor           
Kröhnert, Jutta2, Autor           
Kühl, Stefanie1, Autor           
Trunschke, Annette2, Autor           
Schlögl, Robert2, Autor           
Studt , Felix, Autor
Roldan Cuenya, Beatriz1, Autor           
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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 Zusammenfassung: The hydrogenation of CO2 to methanol over Cu/ZnO-based catalysts is highly sensitive to the surface composition and catalyst structure. Thus, its optimization requires a deep understanding of the influence of the pre-catalyst structure on its evolution under realistic reaction conditions, including the formation and stabilization of the most active sites. Here, the role of the pre-catalyst shape (cubic vs spherical) in the activity and selectivity of ZnO-supported Cu nanoparticles was investigated during methanol synthesis. A combination of ex situ, in situ, and operando microscopy, spectroscopy, and diffraction methods revealed drastic changes in the morphology and composition of the shaped pre-catalysts under reaction conditions. In particular, the rounding of the cubes and partial loss of the (100) facets were observed, although such motifs remained in smaller domains. Nonetheless, the initial pre-catalyst structure was found to strongly affect its subsequent transformation in the course of the CO2 hydrogenation reaction and activity/selectivity trends. In particular, the cubic Cu particles displayed an increased activity for methanol production, although at the cost of a slightly reduced selectivity when compared to similarly sized spherical particles. These findings were rationalized with the help of density functional theory calculations.

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Sprache(n): eng - English
 Datum: 2022-10-312023-01-302023-02-08
 Publikationsstatus: Erschienen
 Seiten: 15
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/jacs.2c11540
 Art des Abschluß: -

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Projektname : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)

Quelle 1

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Titel: Journal of the American Chemical Society
  Andere : JACS
  Kurztitel : J. Am. Chem. Soc.
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: 15 Band / Heft: 145 (5) Artikelnummer: - Start- / Endseite: 3016 - 3030 Identifikator: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870