Controlling the catalytic bond-breaking selectivity of Ni surfaces by step blocking
Vang, Ronnie T. ; Honkala, Karoliina ; Dahl, Søren ; Vestergaard, Ebbe K. ; Schnadt, Joachim LU
; Lægsgaard, Erik
; Clausen, Bjerne S.
; Nørskov, Jens K.
and Besenbacher, Flemming
(2005)
In Nature Materials
4(2).
p.160-162
- Abstract
The reactivity of catalytic surfaces is often dominated by very reactive low-coordinated atoms such as step-edge sites1-11. However, very little knowledge exists concerning the influence of step edges on the selectivity in reactions involving multiple reaction pathways. Such detailed information could be very valuable in rational design of new catalysts with improved selectivity. Here we show, from an interplay between scanning tunnelling microscopy experiments and density functional theory calculations, that the activation of ethylene on Ni(111) follows the trend of higher reactivity for decomposition at step edges as compared with the higher-coordinated terrace sites. The step-edge effect is considerably more pronounced for... (More)
The reactivity of catalytic surfaces is often dominated by very reactive low-coordinated atoms such as step-edge sites1-11. However, very little knowledge exists concerning the influence of step edges on the selectivity in reactions involving multiple reaction pathways. Such detailed information could be very valuable in rational design of new catalysts with improved selectivity. Here we show, from an interplay between scanning tunnelling microscopy experiments and density functional theory calculations, that the activation of ethylene on Ni(111) follows the trend of higher reactivity for decomposition at step edges as compared with the higher-coordinated terrace sites. The step-edge effect is considerably more pronounced for the C-C bond breaking than for the C-H bond breaking, and thus steps play an important role in the bond-breaking selectivity. Furthermore, we demonstrate how the number of reactive step sites can be controlled by blocking the steps with Ag. This approach to nanoscale design of catalysts is exploited in the synthesis of a new high-surface-area AgNi alloy catalyst, which is tested in hydrogenolysis experiments.
(Less)
- author
- Vang, Ronnie T.
; Honkala, Karoliina
; Dahl, Søren
; Vestergaard, Ebbe K.
; Schnadt, Joachim
LU
; Lægsgaard, Erik
; Clausen, Bjerne S.
; Nørskov, Jens K.
and Besenbacher, Flemming
- publishing date
- 2005-01-01
- type
- Contribution to journal
- publication status
- published
- in
- Nature Materials
- volume
- 4
- issue
- 2
- pages
- 3 pages
- publisher
- Nature Publishing Group
- external identifiers
-
- scopus:13144306103
- ISSN
- 1476-1122
- DOI
- 10.1038/nmat1311
- language
- English
- LU publication?
- no
- id
- cf774b4d-67c5-411b-a1ba-474dfeb37943
- date added to LUP
- 2018-08-07 22:07:38
- date last changed
- 2022-04-10 00:53:27
@article{cf774b4d-67c5-411b-a1ba-474dfeb37943,
abstract = {{<p>The reactivity of catalytic surfaces is often dominated by very reactive low-coordinated atoms such as step-edge sites<sup>1-11</sup>. However, very little knowledge exists concerning the influence of step edges on the selectivity in reactions involving multiple reaction pathways. Such detailed information could be very valuable in rational design of new catalysts with improved selectivity. Here we show, from an interplay between scanning tunnelling microscopy experiments and density functional theory calculations, that the activation of ethylene on Ni(111) follows the trend of higher reactivity for decomposition at step edges as compared with the higher-coordinated terrace sites. The step-edge effect is considerably more pronounced for the C-C bond breaking than for the C-H bond breaking, and thus steps play an important role in the bond-breaking selectivity. Furthermore, we demonstrate how the number of reactive step sites can be controlled by blocking the steps with Ag. This approach to nanoscale design of catalysts is exploited in the synthesis of a new high-surface-area AgNi alloy catalyst, which is tested in hydrogenolysis experiments.</p>}},
author = {{Vang, Ronnie T. and Honkala, Karoliina and Dahl, Søren and Vestergaard, Ebbe K. and Schnadt, Joachim and Lægsgaard, Erik and Clausen, Bjerne S. and Nørskov, Jens K. and Besenbacher, Flemming}},
issn = {{1476-1122}},
language = {{eng}},
month = {{01}},
number = {{2}},
pages = {{160--162}},
publisher = {{Nature Publishing Group}},
series = {{Nature Materials}},
title = {{Controlling the catalytic bond-breaking selectivity of Ni surfaces by step blocking}},
url = {{http://dx.doi.org/10.1038/nmat1311}},
doi = {{10.1038/nmat1311}},
volume = {{4}},
year = {{2005}},
}