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  Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO2 electroreduction: Size and Support Effects

Grosse, P., Gao, D., Scholtenn, F., Sinev, I., Mistry, H., & Roldan Cuenya, B. (2018). Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO2 electroreduction: Size and Support Effects. Angewandte Chemie, 130(21), 6300-6305. doi:10.1002/ange.201802083.

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manuscript_2567165.pdf (beliebiger Volltext), 3MB
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2018
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Wiley-VCH
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 Urheber:
Grosse, Philipp1, Autor
Gao, Dunfeng1, Autor
Scholtenn, Fabian1, Autor
Sinev, Ilya1, Autor           
Mistry, Hemma1, 2, Autor           
Roldan Cuenya, Beatriz1, 2, 3, Autor           
Affiliations:
1Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, persistent22              
2Department of Physics, University of Central Florida, Orlando, Florida 32816, USA, ou_persistent22              
3Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Zusammenfassung: In situ and operando spectroscopic and microscopic methods were used to gain insight into the correlation between the structure, chemical state, and reactivity of size‐ and shape‐controlled ligand‐free Cu nanocubes (Cu‐cubes) during CO2 electroreduction (CO2RR). Dynamic changes in the morphology and composition of Cu‐cubes supported on carbon were monitored under potential control via electrochemical atomic force microscopy, X‐ray absorption fine‐structure spectroscopy and X‐ray photoelectron spectroscopy. Under reaction conditions, the roughening of the nanocube surface, disappearance of the (100) facets, formation of pores, loss of Cu and reduction of CuOx species observed were found to lead to a suppression of the selectivity for multi‐carbon products (i.e. C2H4 and ethanol) versus CH4. A comparison with Cu‐cubes supported on Cu foils revealed an enhanced morphological stability and persistence of Cu(I) species under CO2RR. Both factors are held responsible for the higher C2/C1 product ratio observed for the Cu cubes/Cu as compared to Cu cubes/C. Our findings highlight the importance of the structure of the active nanocatalyst but also its interaction with the underlying substrate in CO2RR selectivity.

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Sprache(n): eng - English
 Datum: 2018-03-252018-02-152018-03-262018-03-262018-05-22
 Publikationsstatus: Erschienen
 Seiten: 6
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1002/ange.201802083
 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: Angewandte Chemie
  Kurztitel : Angew. Chem.
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Weinheim : Wiley-VCH
Seiten: 6 Band / Heft: 130 (21) Artikelnummer: - Start- / Endseite: 6300 - 6305 Identifikator: ISSN: 0044-8249
CoNE: https://pure.mpg.de/cone/journals/resource/954926979058_1