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Controlling a spillover pathway with the molecular cork effect

Lewis, Ellen; Marcinkowski, Matthew D.; Boucher, Matthew; Jewell, April D.; Jewell, April; Stamatakis, Michail; Marcinkowski, Matthew; Boucher, Matthew B.; Murphy, Colin; Lewis, Emily A.; Murphy, Colin J.; Sykes, Charles; Kyriakou, Georgios; Sykes, E. Charles H.


Ellen Lewis

Matthew D. Marcinkowski

Matthew Boucher

April D. Jewell

April Jewell

Michail Stamatakis

Matthew Marcinkowski

Matthew B. Boucher

Colin Murphy

Emily A. Lewis

Colin J. Murphy

Charles Sykes

Georgios Kyriakou

E. Charles H. Sykes


Spillover of reactants from one active site to another is important in heterogeneous catalysis and has recently been shown to enhance hydrogen storage in a variety of materials. The spillover of hydrogen is notoriously hard to detect or control. We report herein that the hydrogen spillover pathway on a Pd/Cu alloy can be controlled by reversible adsorption of a spectator molecule. Pd atoms in the Cu surface serve as hydrogen dissociation sites from which H atoms can spillover onto surrounding Cu regions. Selective adsorption of CO at these atomic Pd sites is shown to either prevent the uptake of hydrogen on, or inhibit its desorption from, the surface. In this way, the hydrogen coverage on the whole surface can be controlled by molecular adsorption at a minority site, which we term a ‘molecular cork’ effect. We show that the molecular cork effect is present during a surface catalysed hydrogenation reaction and illustrate how it can be used as a method for controlling uptake and release of hydrogen in a model storage system


Marcinkowski, M. D., Jewell, A. D., Stamatakis, M., Boucher, M. B., Lewis, E. A., Murphy, C. J., …Sykes, E. C. H. (2013). Controlling a spillover pathway with the molecular cork effect. Nature Materials, 12(6), (523-528). doi:10.1038/nmat3620. ISSN 1476-1122

Journal Article Type Article
Acceptance Date Mar 5, 2013
Online Publication Date Apr 21, 2013
Publication Date Jun 1, 2013
Deposit Date Nov 13, 2014
Publicly Available Date Nov 23, 2017
Journal Nature materials
Print ISSN 1476-1122
Electronic ISSN 1476-4660
Publisher Nature Publishing Group
Peer Reviewed Peer Reviewed
Volume 12
Issue 6
Pages 523-528
Keywords Heterogeneous catalysis; Surfaces, interfaces and thin films
Public URL
Publisher URL
Copyright Statement ©2016 University of Hull
Additional Information Author's accepted manuscript of article published in: Nature materials, 2013, v.12, issue 6


Marcinkowski_-_Nat_Mater_2013_-_Controlling_a_Spillover_Pathway_with_the_Molecular_Cork_Effect.pdf (9.2 Mb)

Copyright Statement
©2016 University of Hull

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