Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111)

Höcker, Jan; Duchoň, Tomáš; Veltruská, Kateřina; Matolín, Vladimír; Falta, Jens; Senanayake, Sanjaya D.; Flege, J. Ingo

doi:10.1021/acs.jpcc.5b11066

Title: Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111)

Abstract

We present a novel and simple method for the preparation of a well-defined CeO₂(100) model system on Cu(111) based on the adjustment of the Ce/O ratio during growth. The method yields micrometer-sized, several nanometers high, single-phase CeO₂(100) islands with controllable size and surface termination that can be benchmarked against the known (111) nanostructured islands on Cu(111). We also demonstrate the ability to adjust the Ce to O stoichiometry from CeO₂(100) (100% Ce⁴⁺) to c-Ce₂O₃(100) (100% Ce³⁺), which can be readily recognized by characteristic surface reconstructions observed by low-energy electron diffraction. Finally, the discovery of the highly stable CeO_x(100) phase on a hexagonally close packed metal surface represents an unexpected growth mechanism of ceria on Cu(111), and it provides novel opportunities to prepare more elaborate models, benchmark surface chemical reactivity, and thus gain valuable insights into the redox chemistry of ceria in catalytic processes.

Authors:

Höcker, Jan ^[1]; Duchoň, Tomáš ^[2]; Veltruská, Kateřina ^[2]; Matolín, Vladimír ^[2]; Falta, Jens ^[3]; Senanayake, Sanjaya D. ^[4]; Flege, J. Ingo ^[1]

Univ. of Bremen (Germany)
Charles Univ., Prague (Czech Republic). Faculty of Mathematics and Physics
Univ. of Bremen (Germany). MAPEX Center for Materials and Processes and Inst. of Solid State Physics
Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Wed Jan 06 00:00:00 EST 2016

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1303025

Report Number(s):: BNL-112522-2016-JA
Journal ID: ISSN 1932-7447; R&D Project: CO009; KC0302010

Grant/Contract Number:: SC00112704

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 120; Journal Issue: 9; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Höcker, Jan, Duchoň, Tomáš, Veltruská, Kateřina, Matolín, Vladimír, Falta, Jens, Senanayake, Sanjaya D., and Flege, J. Ingo. Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111).  United States: N. p., 2016. 
Web.  doi:10.1021/acs.jpcc.5b11066.

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                    Höcker, Jan, Duchoň, Tomáš, Veltruská, Kateřina, Matolín, Vladimír, Falta, Jens, Senanayake, Sanjaya D., & Flege, J. Ingo. Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111).  United States.  https://doi.org/10.1021/acs.jpcc.5b11066

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                    Höcker, Jan, Duchoň, Tomáš, Veltruská, Kateřina, Matolín, Vladimír, Falta, Jens, Senanayake, Sanjaya D., and Flege, J. Ingo. Wed .  
"Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111)".  United States.  https://doi.org/10.1021/acs.jpcc.5b11066.  https://www.osti.gov/servlets/purl/1303025.

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@article{osti_1303025,

  title        = {Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111)},

  author       = {Höcker, Jan and Duchoň, Tomáš and Veltruská, Kateřina and Matolín, Vladimír and Falta, Jens and Senanayake, Sanjaya D. and Flege, J. Ingo},

  abstractNote = {We present a novel and simple method for the preparation of a well-defined CeO2(100) model system on Cu(111) based on the adjustment of the Ce/O ratio during growth. The method yields micrometer-sized, several nanometers high, single-phase CeO2(100) islands with controllable size and surface termination that can be benchmarked against the known (111) nanostructured islands on Cu(111). We also demonstrate the ability to adjust the Ce to O stoichiometry from CeO2(100) (100% Ce4+) to c-Ce2O3(100) (100% Ce3+), which can be readily recognized by characteristic surface reconstructions observed by low-energy electron diffraction. Finally, the discovery of the highly stable CeOx(100) phase on a hexagonally close packed metal surface represents an unexpected growth mechanism of ceria on Cu(111), and it provides novel opportunities to prepare more elaborate models, benchmark surface chemical reactivity, and thus gain valuable insights into the redox chemistry of ceria in catalytic processes.},

  doi          = {10.1021/acs.jpcc.5b11066},

  journal      = {Journal of Physical Chemistry. C},

  number       = 9,

  volume       = 120,

  place        = {United States},

  year         = {Wed Jan 06 00:00:00 EST 2016},

  month        = {Wed Jan 06 00:00:00 EST 2016}

}

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Works referencing / citing this record:

Growth and characterization of epitaxially stabilized ceria(001) nanostructures on Ru(0001)
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Mandziak, Anna; D. Soria, Guiomar; Prieto, José Emilio
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Title: Controlling Heteroepitaxy by Oxygen Chemical Potential: Exclusive Growth of (100) Oriented Ceria Nanostructures on Cu(111)

Abstract

Citation Formats

Shape-Selective Synthesis and Oxygen Storage Behavior of Ceria Nanopolyhedra, Nanorods, and Nanocubes journal, December 2005

Enhanced catalytic activity of ceria nanorods from well-defined reactive crystal planes journal, January 2005

Morphology-dependent redox and catalytic properties of CeO2 nanostructures: Nanowires, nanorods and nanoparticles journal, October 2009

Opposite Face Sensitivity of CeO 2 in Hydrogenation and Oxidation Catalysis journal, August 2014

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Morphological effects of the nanostructured ceria support on the activity and stability of CuO/CeO 2 catalysts for the water-gas shift reaction journal, January 2014

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Polarity driven morphology of CeO2(100) islands on Cu(111) journal, November 2013

Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2 journal, July 2014

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Stability and morphology of cerium oxide surfaces in an oxidizing environment: A first-principles investigation journal, January 2009

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Growth, Structure, and Stability of the High-Index TbO x (112) Surface on Cu(111) journal, June 2015

Adjusting Morphology and Surface Reduction of CeO 2 (111) Thin Films on Cu(111) journal, March 2011

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Growth and characterization of epitaxially stabilized ceria(001) nanostructures on Ru(0001) journal, January 2016

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Surface properties of ${CeO}_{2}$ from first principles
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