Simulating gold's structure-dependent reactivity

Nonlocal density functional theory studies of hydrogen activation by gold clusters, nanowires, and surfaces

John J. Determan, Salvador Moncho Escriva, Edward Brothers, Benjamin G. Janesko

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Gold's structure-dependent catalytic activity motivates the study of reactions on a range of gold nanostructures. Electronic structure methods used to model gold catalysis should be capable of treating atoms, clusters, nanostructures, and surfaces on an equal theoretical footing. We extend our previous density functional theory (DFT) studies of a model reaction, H 2 adsorption and dissociation on unsupported Au3 clusters [J. Phys. Chem. C 2013, 117, 7487], to larger clusters, quasi-one-dimensional nanowires and nanoribbons, and surfaces. We focus on trends in DFT predictions made using various approximate exchange-correlation functionals. Most functionals predict qualitatively reasonable trends, i.e., decreasing adsorption energies and increasing dissociation barriers with increasing Au coordination number. However, significant quantitative differences motivate continued exploration of methods beyond the generalized gradient approximation.

Original languageEnglish
Pages (from-to)15693-15704
Number of pages12
JournalJournal of Physical Chemistry C
Volume118
Issue number29
DOIs
Publication statusPublished - 24 Jul 2014
Externally publishedYes

Fingerprint

Gold
Nanowires
Density functional theory
Hydrogen
nanowires
reactivity
Chemical activation
activation
gold
density functional theory
functionals
Nanostructures
hydrogen
dissociation
trends
Adsorption
Nanoribbons
Carbon Nanotubes
adsorption
coordination number

ASJC Scopus subject areas

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

Cite this

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AU - Janesko, Benjamin G.

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