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Isolated metal atom geometries as a strategy for selective heterogeneous hydrogenations

Boucher, Matthew B.; Kyriakou, G.; Jewell, April D.; Lewis, Emily A.; Sykes, E. Charles H.; Baber, Ashleigh E.; Flytzani-Stephanopoulos, Maria; Lawton, Timothy J.; Tierney, Heather L.

Authors

Matthew B. Boucher

G. Kyriakou

April D. Jewell

Emily A. Lewis

E. Charles H. Sykes

Ashleigh E. Baber

Maria Flytzani-Stephanopoulos

Timothy J. Lawton

Heather L. Tierney



Abstract

Facile dissociation of reactants and weak binding of intermediates are key requirements for efficient and selective catalysis. However, these two variables are intimately linked in a way that does not generally allow the optimization of both properties simultaneously. By using desorption measurements in combination with high-resolution scanning tunneling microscopy, we show that individual, isolated Pd atoms in a Cu surface substantially lower the energy barrier to both hydrogen uptake on and subsequent desorption from the Cu metal surface. This facile hydrogen dissociation at Pd atom sites and weak binding to Cu allow for very selective hydrogenation of styrene and acetylene as compared with pure Cu or Pd metal alone.

Citation

Boucher, M. B., Kyriakou, G., Jewell, A. D., Lewis, E. A., Sykes, E. C. H., Baber, A. E., …Tierney, H. L. (2012). Isolated metal atom geometries as a strategy for selective heterogeneous hydrogenations. Science, 335(6073), 1209-1212. https://doi.org/10.1126/science.1215864

Journal Article Type Article
Acceptance Date Jan 30, 2012
Online Publication Date Mar 8, 2012
Publication Date Mar 9, 2012
Deposit Date Nov 13, 2014
Journal Science
Print ISSN 0036-8075
Electronic ISSN 1095-9203
Publisher American Association for the Advancement of Science
Peer Reviewed Peer Reviewed
Volume 335
Issue 6073
Pages 1209-1212
DOI https://doi.org/10.1126/science.1215864
Keywords Multidisciplinary
Public URL https://hull-repository.worktribe.com/output/466682
Publisher URL http://science.sciencemag.org/content/335/6073/1209