Density functional study of the interactions between dihydrogen and Pdn (n = 1-4) clusters

Irena Efremenko; Ernst D. German; Moshe Sheintuch

doi:10.1021/jp0009195

Density functional study of the interactions between dihydrogen and Pd_n (n = 1-4) clusters

Irena Efremenko^*, Ernst D. German, Moshe Sheintuch

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

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Abstract

The dihydrogen interactions with Pd_n (n = 1-4) clusters was investigated using hybrid density functional Becke3LYP method and two ECP basis sets. The local minima configurations for a number of H₂ molecule approach modes toward Pd_n clusters are presented. Some of these states may be interpreted as a physical adsorption and others as dissociative interaction of the H₂ molecule with the palladium cluster. Both geometric and energetic characteristics of weakly bonded pre-dissociated complexes on Pd_3-4 clusters are very close to those on a bulk Pd (111) surface, while the stable states with dissociated hydrogen molecules show significant differences. In contrast to the bulk surface, 2-fold coordination positions exhibit slightly higher stability of hydrogen bonding in Pd₄ and Pd₄ clusters than 3-fold ones. The binding energy is significantly higher for small clusters than for the bulk surface. The Pd₂ cluster was found to be the most active toward hydrogen capture in accordance with the experimental results.

Original language	English
Pages (from-to)	8089-8096
Number of pages	8
Journal	Journal of Physical Chemistry A
Volume	104
Issue number	34
DOIs	https://doi.org/10.1021/jp0009195
State	Published - 31 Aug 2000
Externally published	Yes

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@article{e0462f704f1e4b65bffc467bf71c6ba5,

title = "Density functional study of the interactions between dihydrogen and Pdn (n = 1-4) clusters",

abstract = "The dihydrogen interactions with Pdn (n = 1-4) clusters was investigated using hybrid density functional Becke3LYP method and two ECP basis sets. The local minima configurations for a number of H2 molecule approach modes toward Pdn clusters are presented. Some of these states may be interpreted as a physical adsorption and others as dissociative interaction of the H2 molecule with the palladium cluster. Both geometric and energetic characteristics of weakly bonded pre-dissociated complexes on Pd3-4 clusters are very close to those on a bulk Pd (111) surface, while the stable states with dissociated hydrogen molecules show significant differences. In contrast to the bulk surface, 2-fold coordination positions exhibit slightly higher stability of hydrogen bonding in Pd4 and Pd4 clusters than 3-fold ones. The binding energy is significantly higher for small clusters than for the bulk surface. The Pd2 cluster was found to be the most active toward hydrogen capture in accordance with the experimental results.",

author = "Irena Efremenko and German, {Ernst D.} and Moshe Sheintuch",

year = "2000",

month = aug,

day = "31",

doi = "10.1021/jp0009195",

language = "英语",

volume = "104",

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journal = "Journal of Physical Chemistry A",

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publisher = "American Chemical Society",

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TY - JOUR

T1 - Density functional study of the interactions between dihydrogen and Pdn (n = 1-4) clusters

AU - Efremenko, Irena

AU - German, Ernst D.

AU - Sheintuch, Moshe

PY - 2000/8/31

Y1 - 2000/8/31

N2 - The dihydrogen interactions with Pdn (n = 1-4) clusters was investigated using hybrid density functional Becke3LYP method and two ECP basis sets. The local minima configurations for a number of H2 molecule approach modes toward Pdn clusters are presented. Some of these states may be interpreted as a physical adsorption and others as dissociative interaction of the H2 molecule with the palladium cluster. Both geometric and energetic characteristics of weakly bonded pre-dissociated complexes on Pd3-4 clusters are very close to those on a bulk Pd (111) surface, while the stable states with dissociated hydrogen molecules show significant differences. In contrast to the bulk surface, 2-fold coordination positions exhibit slightly higher stability of hydrogen bonding in Pd4 and Pd4 clusters than 3-fold ones. The binding energy is significantly higher for small clusters than for the bulk surface. The Pd2 cluster was found to be the most active toward hydrogen capture in accordance with the experimental results.

AB - The dihydrogen interactions with Pdn (n = 1-4) clusters was investigated using hybrid density functional Becke3LYP method and two ECP basis sets. The local minima configurations for a number of H2 molecule approach modes toward Pdn clusters are presented. Some of these states may be interpreted as a physical adsorption and others as dissociative interaction of the H2 molecule with the palladium cluster. Both geometric and energetic characteristics of weakly bonded pre-dissociated complexes on Pd3-4 clusters are very close to those on a bulk Pd (111) surface, while the stable states with dissociated hydrogen molecules show significant differences. In contrast to the bulk surface, 2-fold coordination positions exhibit slightly higher stability of hydrogen bonding in Pd4 and Pd4 clusters than 3-fold ones. The binding energy is significantly higher for small clusters than for the bulk surface. The Pd2 cluster was found to be the most active toward hydrogen capture in accordance with the experimental results.

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U2 - 10.1021/jp0009195

DO - 10.1021/jp0009195

M3 - 文章

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SN - 1089-5639

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SP - 8089

EP - 8096

JO - Journal of Physical Chemistry A

JF - Journal of Physical Chemistry A

IS - 34

ER -

Density functional study of the interactions between dihydrogen and Pd_n (n = 1-4) clusters

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