Citation: Yaroslava Lykhach, Tomáš Skála, Armin Neitzel, Nataliya Tsud, Klára Beranová, Kevin C. Prince, Vladimír Matolín, Jörg Libuda. Nanoscale architecture of ceria-based model catalysts: Pt-Co nanostructures on well-ordered CeO₂(111) thin films[J]. Chinese Journal of Catalysis, ;2020, 41(6): 985-997. doi: S1872-2067(19)63462-5 shu

Nanoscale architecture of ceria-based model catalysts: Pt-Co nanostructures on well-ordered CeO₂(111) thin films

a Interface Research and Catalysis, Erlangen Catalysis Resource Center, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstrasse 3, 91058 Erlangen, Germany;
b Charles University, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holešovičkách 2, 18000 Prague, Czech Republic;
c Elettra-Sincrotrone Trieste SCpA, Strada Statale 14, km 163. 5, 34149 Basovizza-Trieste, Italy

Received Date: 3 July 2019
Revised Date: 12 August 2019

We have prepared and characterized atomically well-defined model systems for ceria-supported Pt-Co core-shell catalysts. Pt@Co and Co@Pt core-shell nanostructures were grown on well-ordered CeO₂(111) films on Cu(111) by physical vapour deposition of Pt and Co metals in ultrahigh vacuum and investigated by means of synchrotron radiation photoelectron spectroscopy and resonant photoemission spectroscopy. The deposition of Co onto CeO₂(111) yields Co-CeO₂(111) solid solution at low Co coverage (0.5 ML), followed by the growth of metallic Co nanoparticles at higher Co coverages. Both Pt@Co and Co@Pt model structures are stable against sintering in the temperature range between 300 and 500 K. After annealing at 500 K, the Pt@Co nanostructure contains nearly pure Co-shell while the Pt-shell in the Co@Pt is partially covered by metallic Co. Above 550 K, the re-ordering in the near surface regions yields a subsurface Pt-Co alloy and Pt-rich shells in both Pt@Co and Co@Pt nanostructures. In the case of Co@Pt nanoparticles, the chemical ordering in the near surface region depends on the initial thickness of the deposited Pt-shell. Annealing of the Co@Pt nanostructures in the presence of O₂ triggers the decomposition of Pt-Co alloy along with the oxidation of Co, regardless of the thickness of the initial Pt-shell. Progressive oxidation of Co coupled with adsorbate-induced Co segregation leads to the formation of thick CoO layers on the surfaces of the supported Co@Pt nanostructures. This process is accompanied by the disintegration of the CeO₂(111) film and encapsulation of oxidized Co@Pt nanostructures by CeO₂ upon annealing in O₂ above 550 K. Notably, during oxidation and reduction cycles with O₂ and H₂ at different temperatures, the changes in the structure and chemical composition of supported Co@Pt nanostructures were driven mainly by oxidation while reduction treatments had little effect regardless of the initial thickness of the Pt-shell.
- Core-shell nanoparticles,
- Model catalyst,
- Pt-Co,
- Cerium oxide,
- Chemical ordering,
- Synchrotron radiation photoelectron
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沈阳化工大学材料科学与工程学院沈阳 110142

Nanoscale architecture of ceria-based model catalysts: Pt-Co nanostructures on well-ordered CeO2(111) thin films

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通讯作者: 陈斌, bchen63@163.com

Nanoscale architecture of ceria-based model catalysts: Pt-Co nanostructures on well-ordered CeO₂(111) thin films