Title

Factors Controlling The Reactivity Of Catalytically Active Monolayers On Metal Substrates

Keywords

active element monolayer; density functional theory; electrocatalysts; electronic structure; substrate; surface reactivity

Abstract

The focus of this work is on the Pt/MS structures (MS = Au, Ir, Ru, or Pt substrate), as promising electrocatalysts and a prototype for more general systems: (active element monolayer)/(metal substrate) (AE/MS). We evaluate from first principles the effects of AE monolayer strain and the interlayer AE-MS electronic state hybridization on surface reactivity and reveal rationale for the interlayer hybridization to dominate over the strain effect in determining the AE/MS surface reactivity. We find, however, that, if AE is weakly bound to MS, the surface electronic structure does not suffice to characterize the surface reactivity, because of involvement of other factors related to lattice response to adsorption of a reaction intermediate. Guided by our findings, we trace surface reactivity to a newly introduced hybridization parameter that reflects important features of the electronic structure of the AE/MS surface, which are not taken into account in the original d-band center model. © 2013 American Chemical Society.

Publication Date

5-2-2013

Publication Title

Journal of Physical Chemistry Letters

Volume

4

Issue

9

Number of Pages

1537-1540

Document Type

Article

Personal Identifier

scopus

DOI Link

https://doi.org/10.1021/jz4005174

Socpus ID

84877127307 (Scopus)

Source API URL

https://api.elsevier.com/content/abstract/scopus_id/84877127307

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