A benchmark study of H2 activation by Au3 and Ag 3 clusters

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Abstract

We present a high-level computational study of the activation and disassociation of H2 on triatomic gold and silver clusters as well as benchmarks of various density functional theory (DFT) approximations. The reaction was modeled using complete basis set (CBS) extrapolated CCSD(T) energies at MP2/def2-QZVPP geometries. Our calculations considered several isomers of dissociated H2 on the metal trimer as well as transition states between them. High-level results were then used to benchmark 30 different semilocal, hybrid, double hybrid, and Rung 3.5 DFT functionals as well as Hartree-Fock and MP2 theory. The effect of optimizing the geometries using DFT was also studied with a smaller set of functionals. The results indicate that double-hybrid functionals, especially mPW2PLYP, accurately model this class of reactions, albeit at computational cost higher than standard DFT. The range-separated (screened) hybrids HSE06 and HISSb are also successful and provide a reasonable balance of computational cost and accuracy. These methods are particularly promising for treatments of coinage metal clusters and surfaces.

Original languageEnglish
Pages (from-to)7487-7496
Number of pages10
JournalJournal of Physical Chemistry C
Volume117
Issue number15
DOIs
Publication statusPublished - 18 Apr 2013

Fingerprint

Density functional theory
Chemical activation
functionals
activation
density functional theory
Coinage
costs
Geometry
metal clusters
trimers
geometry
Silver
Gold
Isomers
metal surfaces
Transition metals
Costs
isomers
Metals
silver

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Cite this

A benchmark study of H2 activation by Au3 and Ag 3 clusters. / Moncho Escriva, Salvador; Brothers, Edward; Janesko, Benjamin G.

In: Journal of Physical Chemistry C, Vol. 117, No. 15, 18.04.2013, p. 7487-7496.

Research output: Contribution to journalArticle

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