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  Segregation Phenomena in Size-selected Bimetallic CuNi Nanoparticle Catalysts

Pielsticker, L., Zegkinoglou, I., Divins, N. J., Mistry, H., Chen, Y.-T., Kostka, A., et al. (2018). Segregation Phenomena in Size-selected Bimetallic CuNi Nanoparticle Catalysts. The Journal of Physical Chemistry B, 122(2), 919-926. doi:10.1021/acs.jpcb.7b06984.

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 Urheber:
Pielsticker, Lukas1, Autor
Zegkinoglou, Ioannis1, Autor
Divins, Nuria J.1, Autor
Mistry, Hemma2, Autor
Chen, Yen-Ting1, Autor
Kostka, Aleksander3, Autor           
Boscoboinik, Jorge Anibal4, Autor
Roldan Cuenya, Beatriz5, Autor           
Affiliations:
1Department of Physics, Ruhr University Bochum, 44780 Bochum, Germany, ou_persistent22              
2Department of Physics, University of Central Florida, Orlando, Florida 32816, United States, ou_persistent22              
3Center for Interface-Dominated High Performance Materials (ZGH), Ruhr-Universität Bochum, 44780 Bochum, Germany, persistent22              
4Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973- 5000, United States, ou_persistent22              
5Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Zusammenfassung: Surface segregation, restructuring and sintering phenomena in size-selected copper-nickel nanoparticles (NPs) supported on silicon dioxide substrates were systematically investigated as a function of temperature, chemical state and reactive gas environment. Using near-ambient pressure (NAP-XPS) and ultra-high vacuum X-ray photoelectron spectroscopy (XPS), we showed that nickel tends to segregate to the surface of the NPs at elevated temperatures in oxygen- or hydrogencontaining atmospheres. It was found that the NP pre-treatment, gaseous environment and oxide formation free energy are the main driving forces of the restructuring and segregation trends observed, overshadowing the role of the surface free energy. The depth profile of the elemental composition of the particles was determined under operando CO2 hydrogenation conditions by varying the energy of the X-ray beam. The temperature dependence of the chemical state of the two metals was systematically studied, revealing the high stability of nickel oxides on the NPs and the important role of high valence oxidation states in the segregation behavior. Atomic force microscopy (AFM) studies revealed a remarkable stability of the NPs against sintering at temperatures as high as 700 °C. The results provide new insights into the complex interplay of the various factors which affect alloy formation and segregation phenomena in bimetallic NP systems, often in ways different from those previously known for their bulk counterparts. This leads to new routes for tuning the surface composition of nanocatalysts, for example through plasma and annealing pre-treatments.

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Sprache(n): eng - English
 Datum: 2017-07-152017-10-252018-01-18
 Publikationsstatus: Erschienen
 Seiten: 8
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acs.jpcb.7b06984
 Art des Abschluß: -

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Projektname : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Förderprogramm : H2020
Förderorganisation : -

Quelle 1

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Titel: The Journal of Physical Chemistry B
  Andere : J. Phys. Chem. B
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Washington, D.C. : American Chemical Society
Seiten: 8 Band / Heft: 122 (2) Artikelnummer: - Start- / Endseite: 919 - 926 Identifikator: ISSN: 1520-6106
CoNE: https://pure.mpg.de/cone/journals/resource/1000000000293370_1