Thermal stability and catalytic activity of gold nanoparticles supported on silica

Gabriel M. Veith; Andrew R. Lupini; Sergey Rashkeev; Stephen J. Pennycook; David R. Mullins; Viviane Schwartz; Craig A. Bridges; Nancy J. Dudney

doi:10.1016/j.jcat.2008.12.005

Thermal stability and catalytic activity of gold nanoparticles supported on silica

Gabriel M. Veith, Andrew R. Lupini, Sergey Rashkeev, Stephen J. Pennycook, David R. Mullins, Viviane Schwartz, Craig A. Bridges, Nancy J. Dudney

Research output: Contribution to journal › Article › peer-review

170 Scopus citations

Abstract

2.5 nm gold nanoparticles were grown on a fumed silica support, using the physical vapor deposition technique of magnetron sputtering, that are thermally stable when annealed in an oxygen containing environment up to at least 500 °C. Traditional Au/TiO₂ catalysts rapidly sinter to form large 13.9 nm gold clusters under these annealing conditions. This surprising stability of Au/SiO₂ is attributed to the absence of residual impurities (ensured by the halide-free production method) and a strong bond between gold and defects at the silica surface (about 3 eV per bond) estimated from density functional theory (DFT) calculations. The Au/SiO₂ catalysts are less active for CO oxidation than the prototypical Au/TiO₂ catalysts, however they can be regenerated far more easily, allowing the activity of a catalyst to be fully recovered after deactivation.

Original language	English
Pages (from-to)	92-101
Number of pages	10
Journal	Journal of Catalysis
Volume	262
Issue number	1
DOIs	https://doi.org/10.1016/j.jcat.2008.12.005
State	Published - Feb 15 2009

Funding

The authors thank Professor Craig Barnes and Dr. Jason Clarke (University of Tennessee Chemistry Department) for collecting and analyzing the 29 Si-NMR data, Ben Jang (University Texas, Commerce) and Wenfu Yan (ORNL) for assistance with some catalytic measurements as well as Steven Overbury (ORNL) and Sokrates Pantelides (Vanderbilt) for many helpful discussions. The calculation portion of this work is supported in part by a grant of computer time from the DoD High Performance Computing Modernization Program at the Maui High Performance Computer Center (MHPCC), Naval Oceanographic Office (NAVO) and the U.S. Army Engineer Research and Development Center (ERDC). A portion of this research (Hitachi STEM) was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities, U.S. Department of Energy. Use of the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886. This research was also sponsored by the U.S. Department of Energy's Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (G.M.V., A.R.L., S.J.P., C.A.B., N.J.D.), and the Division of Chemical Sciences (D.R.M., V.S.).

Funders	Funder number
A.R.L.
Division of Chemical Sciences
Division of Scientific User Facilities
National Synchrotron Light Source
Naval Oceanographic Office
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Brookhaven National Laboratory
Engineer Research and Development Center
Hitachi
Division of Materials Sciences and Engineering

Keywords

DFT calculations
Gold catalyst
Gold reference catalyst
Gold-support interaction
Silica
Sputtering
Tammann temperature
Thermal stability
Titania

Access to Document

10.1016/j.jcat.2008.12.005

Cite this

@article{1a48a451ae3b4c1b8f11d409ac79dcc1,

title = "Thermal stability and catalytic activity of gold nanoparticles supported on silica",

abstract = "2.5 nm gold nanoparticles were grown on a fumed silica support, using the physical vapor deposition technique of magnetron sputtering, that are thermally stable when annealed in an oxygen containing environment up to at least 500 °C. Traditional Au/TiO2 catalysts rapidly sinter to form large 13.9 nm gold clusters under these annealing conditions. This surprising stability of Au/SiO2 is attributed to the absence of residual impurities (ensured by the halide-free production method) and a strong bond between gold and defects at the silica surface (about 3 eV per bond) estimated from density functional theory (DFT) calculations. The Au/SiO2 catalysts are less active for CO oxidation than the prototypical Au/TiO2 catalysts, however they can be regenerated far more easily, allowing the activity of a catalyst to be fully recovered after deactivation.",

keywords = "DFT calculations, Gold catalyst, Gold reference catalyst, Gold-support interaction, Silica, Sputtering, Tammann temperature, Thermal stability, Titania",

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

year = "2009",

month = feb,

day = "15",

doi = "10.1016/j.jcat.2008.12.005",

language = "English",

volume = "262",

pages = "92--101",

journal = "Journal of Catalysis",

issn = "0021-9517",

publisher = "Elsevier",

number = "1",

}

TY - JOUR

T1 - Thermal stability and catalytic activity of gold nanoparticles supported on silica

AU - Veith, Gabriel M.

AU - Lupini, Andrew R.

AU - Rashkeev, Sergey

AU - Pennycook, Stephen J.

AU - Mullins, David R.

AU - Schwartz, Viviane

AU - Bridges, Craig A.

AU - Dudney, Nancy J.

PY - 2009/2/15

Y1 - 2009/2/15

N2 - 2.5 nm gold nanoparticles were grown on a fumed silica support, using the physical vapor deposition technique of magnetron sputtering, that are thermally stable when annealed in an oxygen containing environment up to at least 500 °C. Traditional Au/TiO2 catalysts rapidly sinter to form large 13.9 nm gold clusters under these annealing conditions. This surprising stability of Au/SiO2 is attributed to the absence of residual impurities (ensured by the halide-free production method) and a strong bond between gold and defects at the silica surface (about 3 eV per bond) estimated from density functional theory (DFT) calculations. The Au/SiO2 catalysts are less active for CO oxidation than the prototypical Au/TiO2 catalysts, however they can be regenerated far more easily, allowing the activity of a catalyst to be fully recovered after deactivation.

AB - 2.5 nm gold nanoparticles were grown on a fumed silica support, using the physical vapor deposition technique of magnetron sputtering, that are thermally stable when annealed in an oxygen containing environment up to at least 500 °C. Traditional Au/TiO2 catalysts rapidly sinter to form large 13.9 nm gold clusters under these annealing conditions. This surprising stability of Au/SiO2 is attributed to the absence of residual impurities (ensured by the halide-free production method) and a strong bond between gold and defects at the silica surface (about 3 eV per bond) estimated from density functional theory (DFT) calculations. The Au/SiO2 catalysts are less active for CO oxidation than the prototypical Au/TiO2 catalysts, however they can be regenerated far more easily, allowing the activity of a catalyst to be fully recovered after deactivation.

KW - DFT calculations

KW - Gold catalyst

KW - Gold reference catalyst

KW - Gold-support interaction

KW - Silica

KW - Sputtering

KW - Tammann temperature

KW - Thermal stability

KW - Titania

UR - http://www.scopus.com/inward/record.url?scp=63749128006&partnerID=8YFLogxK

U2 - 10.1016/j.jcat.2008.12.005

DO - 10.1016/j.jcat.2008.12.005

M3 - Article

AN - SCOPUS:63749128006

SN - 0021-9517

VL - 262

SP - 92

EP - 101

JO - Journal of Catalysis

JF - Journal of Catalysis

IS - 1

ER -

Thermal stability and catalytic activity of gold nanoparticles supported on silica

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this