In this review, we examine the role of oxide support defects, cluster
size-dependence, cluster structural fluxionality, and impurity doping
on the catalytic properties of size-selected metal clusters on surfaces.
By combining experimental results from the oxidation of CO on size-selected
gold clusters with ab-initio calculations, a detailed picture emerges
of the electronic and structural dynamics of this process. For Au8,
Au4, and Au3Sr clusters on F-center defects on MgO(100), optimized
atomic structures and local density of states calculations support
the experimental results for the oxidation of CO. Fundamental aspects
such as charge transfer from oxide defect sites and the adsorption
and activation of reactant molecules are elucidated. Using a pulsed
molecular beam set up, turnover frequencies for the oxidation of
CO and the reduction of NO on Pd clusters were determined. This new
experimental scheme allows for the determination of mechanistic details
of much greater sophistication than with one-cycle experiments. Isolating
known catalytic phenomena such as spillover, reverse spillover, and
adlineation should be attainable at the atomic level using these
pulsed molecular beam experiments on size-selected metal clusters
on surfaces.
%0 Journal Article
%1 Heiz2004
%A Heiz, U
%A Bullock, E. L.
%D 2004
%J J. Mater. Chem.
%K science surface
%N 4
%P 564-577
%R 10.1039/b313560h
%T Fundamental aspects of catalysis on supported metal clusters
%U http://tinyurl.sfx.mpg.de/q8z6
%V 14
%X In this review, we examine the role of oxide support defects, cluster
size-dependence, cluster structural fluxionality, and impurity doping
on the catalytic properties of size-selected metal clusters on surfaces.
By combining experimental results from the oxidation of CO on size-selected
gold clusters with ab-initio calculations, a detailed picture emerges
of the electronic and structural dynamics of this process. For Au8,
Au4, and Au3Sr clusters on F-center defects on MgO(100), optimized
atomic structures and local density of states calculations support
the experimental results for the oxidation of CO. Fundamental aspects
such as charge transfer from oxide defect sites and the adsorption
and activation of reactant molecules are elucidated. Using a pulsed
molecular beam set up, turnover frequencies for the oxidation of
CO and the reduction of NO on Pd clusters were determined. This new
experimental scheme allows for the determination of mechanistic details
of much greater sophistication than with one-cycle experiments. Isolating
known catalytic phenomena such as spillover, reverse spillover, and
adlineation should be attainable at the atomic level using these
pulsed molecular beam experiments on size-selected metal clusters
on surfaces.
@article{Heiz2004,
abstract = {In this review, we examine the role of oxide support defects, cluster
size-dependence, cluster structural fluxionality, and impurity doping
on the catalytic properties of size-selected metal clusters on surfaces.
By combining experimental results from the oxidation of CO on size-selected
gold clusters with ab-initio calculations, a detailed picture emerges
of the electronic and structural dynamics of this process. For Au8,
Au4, and Au3Sr clusters on F-center defects on MgO(100), optimized
atomic structures and local density of states calculations support
the experimental results for the oxidation of CO. Fundamental aspects
such as charge transfer from oxide defect sites and the adsorption
and activation of reactant molecules are elucidated. Using a pulsed
molecular beam set up, turnover frequencies for the oxidation of
CO and the reduction of NO on Pd clusters were determined. This new
experimental scheme allows for the determination of mechanistic details
of much greater sophistication than with one-cycle experiments. Isolating
known catalytic phenomena such as spillover, reverse spillover, and
adlineation should be attainable at the atomic level using these
pulsed molecular beam experiments on size-selected metal clusters
on surfaces.},
added-at = {2009-10-30T10:04:05.000+0100},
author = {Heiz, U and Bullock, E. L.},
biburl = {https://www.bibsonomy.org/bibtex/2662c6dd31ed1bfccba8783af7351d6eb/jfischer},
doi = {10.1039/b313560h},
interhash = {0d798bc2de2aa721191534a661f3abf3},
intrahash = {662c6dd31ed1bfccba8783af7351d6eb},
issn = {0959-9428},
journal = {J. Mater. Chem.},
keywords = {science surface},
number = 4,
pages = {564-577},
timestamp = {2009-10-30T10:04:13.000+0100},
title = {Fundamental aspects of catalysis on supported metal clusters},
url = {http://tinyurl.sfx.mpg.de/q8z6},
volume = 14,
year = 2004
}