Reactivity of molecular oxygen with aluminum clusters: Density functional and Ab Initio molecular dynamics simulation study

Joonghan Kim, Selvarengan Paranthaman, Jiwon Moon, Kiryong Hong, Jeongho Kim, Dong Eon Kim, Tae Kyu Kim

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

Dissociative adsorption of molecular oxygen (O2) on aluminum (Al) clusters has attracted much interest in the field of surface science and catalysis, but theoretical predictions of the reactivity of this reaction in terms of barrier height is still challenging. In this regard, we systematically investigate the reactivity of O2 with Al clusters using density functional theory (DFT) and atom-centered density matrix propagation (ADMP) simulations. We also calculate potential energy surfaces (PESs) of the reaction between O2 and Al clusters to estimate the barrier energy of this reaction. The M06-2X functional gives the barrier energy in agreement with the one calculated by coupled cluster singles and doubles with perturbed triples (CCSD(T)) while the TPSSh functional significantly underestimates the barrier height. The ADMP simulation using the M06-2X functional predicts the reactivity of O2 with the Al cluster in agreement with the experimental findings, that is, singlet O2 readily reacts with Al clusters but triplet O2 is less reactive. We found that the ability of a DFT functional to describe the charge transfer appropriately is critical for calculating the barrier energy and the reactivity of the reaction of O2 with Al clusters. The M06-2X functional is relevant for investigating chemical reactions involving Al and O2.

Original languageEnglish
Pages (from-to)547-554
Number of pages8
JournalInternational Journal of Quantum Chemistry
Volume116
Issue number7
DOIs
Publication statusPublished - 2016 Apr 5

Fingerprint

Molecular oxygen
Aluminum
Molecular dynamics
reactivity
molecular dynamics
aluminum
Computer simulation
oxygen
Energy barriers
simulation
Density functional theory
density functional theory
Atoms
Potential energy surfaces
propagation
Catalysis
catalysis
atoms
energy
Charge transfer

All Science Journal Classification (ASJC) codes

  • Atomic and Molecular Physics, and Optics
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry

Cite this

Kim, Joonghan ; Paranthaman, Selvarengan ; Moon, Jiwon ; Hong, Kiryong ; Kim, Jeongho ; Kim, Dong Eon ; Kim, Tae Kyu. / Reactivity of molecular oxygen with aluminum clusters : Density functional and Ab Initio molecular dynamics simulation study. In: International Journal of Quantum Chemistry. 2016 ; Vol. 116, No. 7. pp. 547-554.
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abstract = "Dissociative adsorption of molecular oxygen (O2) on aluminum (Al) clusters has attracted much interest in the field of surface science and catalysis, but theoretical predictions of the reactivity of this reaction in terms of barrier height is still challenging. In this regard, we systematically investigate the reactivity of O2 with Al clusters using density functional theory (DFT) and atom-centered density matrix propagation (ADMP) simulations. We also calculate potential energy surfaces (PESs) of the reaction between O2 and Al clusters to estimate the barrier energy of this reaction. The M06-2X functional gives the barrier energy in agreement with the one calculated by coupled cluster singles and doubles with perturbed triples (CCSD(T)) while the TPSSh functional significantly underestimates the barrier height. The ADMP simulation using the M06-2X functional predicts the reactivity of O2 with the Al cluster in agreement with the experimental findings, that is, singlet O2 readily reacts with Al clusters but triplet O2 is less reactive. We found that the ability of a DFT functional to describe the charge transfer appropriately is critical for calculating the barrier energy and the reactivity of the reaction of O2 with Al clusters. The M06-2X functional is relevant for investigating chemical reactions involving Al and O2.",
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Reactivity of molecular oxygen with aluminum clusters : Density functional and Ab Initio molecular dynamics simulation study. / Kim, Joonghan; Paranthaman, Selvarengan; Moon, Jiwon; Hong, Kiryong; Kim, Jeongho; Kim, Dong Eon; Kim, Tae Kyu.

In: International Journal of Quantum Chemistry, Vol. 116, No. 7, 05.04.2016, p. 547-554.

Research output: Contribution to journalArticle

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AU - Kim, Joonghan

AU - Paranthaman, Selvarengan

AU - Moon, Jiwon

AU - Hong, Kiryong

AU - Kim, Jeongho

AU - Kim, Dong Eon

AU - Kim, Tae Kyu

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