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Controlling a spillover pathway with the molecular cork effect

Marcinkowski, MD; Jewell, AD; Stamatakis, M; Boucher, MB; Lewis, EA; Murphy, CJ; Kyriakou, G; (2013) Controlling a spillover pathway with the molecular cork effect. Nature Materials , 12 (6) 523 - 528. 10.1038/NMAT3620. Green open access

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Abstract

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.

Type: Article
Title: Controlling a spillover pathway with the molecular cork effect
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/NMAT3620
Publisher version: http://dx.doi.org/10.1038/NMAT3620
Language: English
Additional information: PubMed ID: 23603849
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/1394895
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