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Controlling Hydrogen Activation, Spillover, and Desorption with Pd-Au Single-Atom Alloys

Lucci, FR; Darby, MT; Mattera, MF; Ivimey, CJ; Therrien, AJ; Michaelides, A; Stamatakis, M; (2016) Controlling Hydrogen Activation, Spillover, and Desorption with Pd-Au Single-Atom Alloys. Journal of Physical Chemistry Letters , 7 (3) pp. 480-485. 10.1021/acs.jpclett.5b02400. Green open access

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Abstract

Key descriptors in hydrogenation catalysis are the nature of the active sites for H2 activation and the adsorption strength of H atoms to the surface. Using atomically resolved model systems of dilute Pd-Au surface alloys and density functional theory calculations, we determine key aspects of H2 activation, diffusion, and desorption. Pd monomers in a Au(111) surface catalyze the dissociative adsorption of H2 at temperatures as low as 85 K, a process previously expected to require contiguous Pd sites. H atoms preside at the Pd sites and desorb at temperatures significantly lower than those from pure Pd (175 versus 310 K). This facile H2 activation and weak adsorption of H atom intermediates are key requirements for active and selective hydrogenations. We also demonstrate weak adsorption of CO, a common catalyst poison, which is sufficient to force H atoms to spill over from Pd to Au sites, as evidenced by low-temperature H2 desorption.

Type: Article
Title: Controlling Hydrogen Activation, Spillover, and Desorption with Pd-Au Single-Atom Alloys
Location: United States
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.jpclett.5b02400
Publisher version: http://dx.doi.org/10.1021/acs.jpclett.5b02400
Language: English
Additional information: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal Physical Chemistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/acs.jpclett.5b02400.
Keywords: Bimetallic alloys, temperature programmed desorption, scanning tunneling microscopy, density functional theory, hydrogenation
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
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery.ucl.ac.uk/id/eprint/1475584
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