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Title: Role of hydroxyl groups on the stability and catalytic activity of Au nanoparticles on rutile surface

Abstract

Hydroxyls are present as surface terminations of transition metal oxides under ambient conditions and may modify the properties of supported catalysts. We perform first-principles density functional theory calculations to investigate the role of hydroxyls on the catalytic activity of supported gold clusters on TiO{sub 2} (rutile). We find that they have a long-range effect increasing the adhesion of gold clusters on rutile. While hydroxyls make one gold atom more electronegative, a more complex charge-transfer scenario is observed on larger clusters which are important for catalytic applications. This enhances the molecular adsorption and coadsorption energies of CO and O{sub 2}, thereby increasing the catalytic activity of gold clusters for CO oxidation, consistent with reported experiments. Hydroxyls at the interface between gold and rutile surface are most important to this process, even when not directly bound to gold. As such, accurate models of catalytic processes on gold and other catalysts should include the effect of surface hydroxyls.

Authors:
 [1];  [1];  [1]
  1. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1033156
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Physical Chemistry Letters; Journal Volume: 2; Journal Issue: 22
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ADHESION; ADSORPTION; ATOMS; CATALYSTS; FUNCTIONALS; GOLD; HETEROGENEOUS CATALYSIS; HYDROXYLATION; OXIDATION; OXIDES; RUTILE; STABILITY; TRANSITION ELEMENTS

Citation Formats

Ganesh, Panchapakesan, Kent, Paul R, and Veith, Gabriel M. Role of hydroxyl groups on the stability and catalytic activity of Au nanoparticles on rutile surface. United States: N. p., 2011. Web. doi:10.1021/jz2013177.
Ganesh, Panchapakesan, Kent, Paul R, & Veith, Gabriel M. Role of hydroxyl groups on the stability and catalytic activity of Au nanoparticles on rutile surface. United States. doi:10.1021/jz2013177.
Ganesh, Panchapakesan, Kent, Paul R, and Veith, Gabriel M. Sat . "Role of hydroxyl groups on the stability and catalytic activity of Au nanoparticles on rutile surface". United States. doi:10.1021/jz2013177.
@article{osti_1033156,
title = {Role of hydroxyl groups on the stability and catalytic activity of Au nanoparticles on rutile surface},
author = {Ganesh, Panchapakesan and Kent, Paul R and Veith, Gabriel M},
abstractNote = {Hydroxyls are present as surface terminations of transition metal oxides under ambient conditions and may modify the properties of supported catalysts. We perform first-principles density functional theory calculations to investigate the role of hydroxyls on the catalytic activity of supported gold clusters on TiO{sub 2} (rutile). We find that they have a long-range effect increasing the adhesion of gold clusters on rutile. While hydroxyls make one gold atom more electronegative, a more complex charge-transfer scenario is observed on larger clusters which are important for catalytic applications. This enhances the molecular adsorption and coadsorption energies of CO and O{sub 2}, thereby increasing the catalytic activity of gold clusters for CO oxidation, consistent with reported experiments. Hydroxyls at the interface between gold and rutile surface are most important to this process, even when not directly bound to gold. As such, accurate models of catalytic processes on gold and other catalysts should include the effect of surface hydroxyls.},
doi = {10.1021/jz2013177},
journal = {Journal of Physical Chemistry Letters},
number = 22,
volume = 2,
place = {United States},
year = {Sat Jan 01 00:00:00 EST 2011},
month = {Sat Jan 01 00:00:00 EST 2011}
}