Understanding support mediated activity by investigating highly active, thermally stable, silica supported gold catalysts

Veith, Gabriel M; Lupini, Andrew R; Rashkeev, Sergey; Pennycook, Stephen J; Schwartz, Viviane; Mullins, David R; Dudney, Nancy J

doi:10.1016/j.jcat.2008.12.005

Title: Understanding support mediated activity by investigating highly active, thermally stable, silica supported gold catalysts

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Abstract

2.5 nm gold nanoparticles were grown on a fumed silica support using the physical vapor deposition technique magnetron sputtering. Combining electron microscopy, extended X-ray absorption fine structure (EXAFS) spectroscopy, and catalytic studies revealed that the silica supported gold catalysts are thermally stable when annealed in an oxygen containing environment up to at least 500oC. This surprising stability is attributed to the absence of residual halide impurities and a strong bond between gold and defects at the silica surface (2.7 - 3.8 eV), as estimated from density functional theory (DFT) calculations. The Au/SiO2 catalysts are slightly less active for CO oxidation than the prototypical Au/TiO2 catalysts, however they can be regenerated far more easily, fully recovering the activity of a freshly prepared catalyst after deactivation.

Authors:

Veith, Gabriel M ^[1]; Lupini, Andrew R ^[1]; Rashkeev, Sergey ^[1]; Pennycook, Stephen J ^[1]; Schwartz, Viviane ^[1]; Mullins, David R ^[1]; Dudney, Nancy J ^[1]

ORNL

Publication Date:: Thu Jan 01 00:00:00 EST 2009

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 947576

DOE Contract Number:: DE-AC05-00OR22725

Resource Type:: Journal Article

Journal Name:: Journal of Catalysis

Additional Journal Information:: Journal Volume: 262; Journal Issue: 1; Journal ID: ISSN 0021-9517

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; GOLD; CATALYSTS; SILICA; CATALYST SUPPORTS; PHYSICAL VAPOR DEPOSITION; STABILITY; DENSITY FUNCTIONAL METHOD; CARBON MONOXIDE; OXIDATION; CATALYTIC EFFECTS; REGENERATION; gold; catalyst; silica; oxidation; sputtering

Citation Formats


                    Veith, Gabriel M, Lupini, Andrew R, Rashkeev, Sergey, Pennycook, Stephen J, Schwartz, Viviane, Mullins, David R, and Dudney, Nancy J. Understanding support mediated activity by investigating highly active, thermally stable, silica supported gold catalysts.  United States: N. p., 2009. 
        Web.  doi:10.1016/j.jcat.2008.12.005.

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                    Veith, Gabriel M, Lupini, Andrew R, Rashkeev, Sergey, Pennycook, Stephen J, Schwartz, Viviane, Mullins, David R, & Dudney, Nancy J. Understanding support mediated activity by investigating highly active, thermally stable, silica supported gold catalysts.  United States.  https://doi.org/10.1016/j.jcat.2008.12.005

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                    Veith, Gabriel M, Lupini, Andrew R, Rashkeev, Sergey, Pennycook, Stephen J, Schwartz, Viviane, Mullins, David R, and Dudney, Nancy J. 2009.  
        "Understanding support mediated activity by investigating highly active, thermally stable, silica supported gold catalysts".  United States.  https://doi.org/10.1016/j.jcat.2008.12.005.

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@article{osti_947576,

  title        = {Understanding support mediated activity by investigating highly active, thermally stable, silica supported gold catalysts},

  author       = {Veith, Gabriel M and Lupini, Andrew R and Rashkeev, Sergey and Pennycook, Stephen J and Schwartz, Viviane and Mullins, David R and Dudney, Nancy J},

  abstractNote = {2.5 nm gold nanoparticles were grown on a fumed silica support using the physical vapor deposition technique magnetron sputtering. Combining electron microscopy, extended X-ray absorption fine structure (EXAFS) spectroscopy, and catalytic studies revealed that the silica supported gold catalysts are thermally stable when annealed in an oxygen containing environment up to at least 500oC. This surprising stability is attributed to the absence of residual halide impurities and a strong bond between gold and defects at the silica surface (2.7 - 3.8 eV), as estimated from density functional theory (DFT) calculations. The Au/SiO2 catalysts are slightly less active for CO oxidation than the prototypical Au/TiO2 catalysts, however they can be regenerated far more easily, fully recovering the activity of a freshly prepared catalyst after deactivation.},

  doi          = {10.1016/j.jcat.2008.12.005},

  url          = {https://www.osti.gov/biblio/947576},
  journal      = {Journal of Catalysis},

  issn         = {0021-9517},

  number       = 1,

  volume       = 262,

  place        = {United States},

  year         = {Thu Jan 01 00:00:00 EST 2009},

  month        = {Thu Jan 01 00:00:00 EST 2009}

}

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