Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage

doi:10.1016/j.susc.2015.10.002

Title: Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeO_x–TiO₂(110) surfaces: Effects of high ceria coverage

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Abstract

We used scanning tunnelling microscopy to study the morphology of an overlayer of ceria in contact with a TiO₂(110) substrate. Two types of domains were observed after ceria deposition. An ordered ceria film covered half of the surface and high-resolution imaging suggested a near-c(6 × 2) relationship to the underlying TiO₂(110)-(1 × 1). For the other half of the surface, it comprised CeO_x nanoparticles and reconstructed TiOx supported on TiO₂(110)-(1 × 1). Exposure to a small amount of gold resulted in the formation of isolated gold atoms and small clusters on the ordered ceria film and TiO₂(110)-(1 × 1) areas, which exhibited significant sintering at 500 K and showed strong interaction between the sintered gold clusters and the domain boundaries of the ceria film. The Au/CeO_x/TiO₂(110) model system proved to be a good catalyst for the water–gas shift (WGS) exhibiting much higher turnover frequencies (TOFs) than Cu(111) and Pt(111) benchmarks, or the individual Au/TiO₂(110) and Au/CeO₂(111) systems. Finally, for Au/CeO_x/TiO₂(110) catalysts, there was a decrease in catalytic activity with increasing ceria coverage that correlates with a reduction in the concentration of Ce^{3 +} formed during WGS reaction conditions.

Authors:

Grinter, D. C. ^[1]; Park, J. B. ^[1]; Agnoli, S. ^[1]; Evans, J. ^[2]; Hrbek, J. ^[1]; Stacchiola, D. J. ^[1]; Senanayake, S. D. ^[1]; Rodriguez, J. A. ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Central Univ. of Venezuela, Caracas (Venezuela)

Publication Date:: 2016-08-01

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI Identifier:: 1303023

Alternate Identifier(s):: OSTI ID: 1333203; OSTI ID: 1373613

Report Number(s):: BNL-112519-2016-JA; BNL-113208-2016-JA
Journal ID: ISSN 0039-6028; R&D Project: CO009; KC0302010

Grant/Contract Number:: SC00112704; SC0012704

Resource Type:: Accepted Manuscript

Journal Name:: Surface Science

Additional Journal Information:: Journal Volume: 650; Journal Issue: C; Journal ID: ISSN 0039-6028

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; STM; TiO2 (110); CeO2; gold; water-gas shift; TiO2(110); water–gas shift

Citation Formats


                    Grinter, D. C., Park, J. B., Agnoli, S., Evans, J., Hrbek, J., Stacchiola, D. J., Senanayake, S. D., and Rodriguez, J. A. Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage.  United States: N. p., 2016. 
        Web.  doi:10.1016/j.susc.2015.10.002.

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                    Grinter, D. C., Park, J. B., Agnoli, S., Evans, J., Hrbek, J., Stacchiola, D. J., Senanayake, S. D., & Rodriguez, J. A. Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage.  United States.  doi:10.1016/j.susc.2015.10.002.

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                    Grinter, D. C., Park, J. B., Agnoli, S., Evans, J., Hrbek, J., Stacchiola, D. J., Senanayake, S. D., and Rodriguez, J. A. Mon .  
        "Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage".  United States.  doi:10.1016/j.susc.2015.10.002.  https://www.osti.gov/servlets/purl/1303023.

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@article{osti_1303023,

  title        = {Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage},

  author       = {Grinter, D. C. and Park, J. B. and Agnoli, S. and Evans, J. and Hrbek, J. and Stacchiola, D. J. and Senanayake, S. D. and Rodriguez, J. A.},

  abstractNote = {We used scanning tunnelling microscopy to study the morphology of an overlayer of ceria in contact with a TiO2(110) substrate. Two types of domains were observed after ceria deposition. An ordered ceria film covered half of the surface and high-resolution imaging suggested a near-c(6 × 2) relationship to the underlying TiO2(110)-(1 × 1). For the other half of the surface, it comprised CeOx nanoparticles and reconstructed TiOx supported on TiO2(110)-(1 × 1). Exposure to a small amount of gold resulted in the formation of isolated gold atoms and small clusters on the ordered ceria film and TiO2(110)-(1 × 1) areas, which exhibited significant sintering at 500 K and showed strong interaction between the sintered gold clusters and the domain boundaries of the ceria film. The Au/CeOx/TiO2(110) model system proved to be a good catalyst for the water–gas shift (WGS) exhibiting much higher turnover frequencies (TOFs) than Cu(111) and Pt(111) benchmarks, or the individual Au/TiO2(110) and Au/CeO2(111) systems. Finally, for Au/CeOx/TiO2(110) catalysts, there was a decrease in catalytic activity with increasing ceria coverage that correlates with a reduction in the concentration of Ce3 + formed during WGS reaction conditions.},

  doi          = {10.1016/j.susc.2015.10.002},

  journal      = {Surface Science},

  number       = C,

  volume       = 650,

  place        = {United States},

  year         = {2016},

  month        = {8}

}

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DOI: 10.1016/j.susc.2015.10.002

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Title: Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage

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Title: Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeO_x–TiO₂(110) surfaces: Effects of high ceria coverage