Hydrogen dissociative chemisorption and desorption on saturated subnano palladium clusters (Pdn, n = 2-9)

Chenggang Zhou, Shujuan Yao, Jinping Wu, Robert C. Forrey, Liang Chen, Akitomo Tachibana, Hansong Cheng

Research output: Contribution to journalArticle

41 Citations (Scopus)

Abstract

H2 sequential dissociative chemisorption on small palladium clusters was studied using density functional theory. The chosen clusters Pdn (n = 2-9) are of the lowest energy structures for each n. H 2 dissociative chemisorption and subsequent H atom migration on the bare Pd clusters were found to be nearly barrierless. The dissociative chemisorption energy of H2 and the desorption energy of H atom in general decrease with the coverage of H atoms and thus the catalytic efficiency decreases as the H loading increases. These energies at full cluster saturation were identified and found to vary in small energy ranges regardless of cluster size. As H loading increases, the clusters gradually change their bonding from metallic character to covalent character. For the selected Pd clusters, the capacity to adsorb H atoms increases almost proportionally with cluster size; however, it was found that the capacity of Pd clusters to adsorb H atoms is, on average, substantially smaller than that of small Pt clusters, suggesting that the catalytic efficiency of Pt nanoparticles is superior to Pd nanoparticles in catalyzing dissociative chemisorption of H2 molecules.

Original languageEnglish (US)
Pages (from-to)5445-5451
Number of pages7
JournalPhysical Chemistry Chemical Physics
Volume10
Issue number35
DOIs
StatePublished - Sep 10 2008

Fingerprint

Palladium
Chemisorption
chemisorption
palladium
Hydrogen
Desorption
desorption
Atoms
hydrogen
Nanoparticles
atoms
Density functional theory
energy
nanoparticles
Molecules
density functional theory
saturation

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Zhou, Chenggang ; Yao, Shujuan ; Wu, Jinping ; Forrey, Robert C. ; Chen, Liang ; Tachibana, Akitomo ; Cheng, Hansong. / Hydrogen dissociative chemisorption and desorption on saturated subnano palladium clusters (Pdn, n = 2-9). In: Physical Chemistry Chemical Physics. 2008 ; Vol. 10, No. 35. pp. 5445-5451.
@article{1ff3886811af49f88d5bae0520645c8f,
title = "Hydrogen dissociative chemisorption and desorption on saturated subnano palladium clusters (Pdn, n = 2-9)",
abstract = "H2 sequential dissociative chemisorption on small palladium clusters was studied using density functional theory. The chosen clusters Pdn (n = 2-9) are of the lowest energy structures for each n. H 2 dissociative chemisorption and subsequent H atom migration on the bare Pd clusters were found to be nearly barrierless. The dissociative chemisorption energy of H2 and the desorption energy of H atom in general decrease with the coverage of H atoms and thus the catalytic efficiency decreases as the H loading increases. These energies at full cluster saturation were identified and found to vary in small energy ranges regardless of cluster size. As H loading increases, the clusters gradually change their bonding from metallic character to covalent character. For the selected Pd clusters, the capacity to adsorb H atoms increases almost proportionally with cluster size; however, it was found that the capacity of Pd clusters to adsorb H atoms is, on average, substantially smaller than that of small Pt clusters, suggesting that the catalytic efficiency of Pt nanoparticles is superior to Pd nanoparticles in catalyzing dissociative chemisorption of H2 molecules.",
author = "Chenggang Zhou and Shujuan Yao and Jinping Wu and Forrey, {Robert C.} and Liang Chen and Akitomo Tachibana and Hansong Cheng",
year = "2008",
month = "9",
day = "10",
doi = "10.1039/b804877k",
language = "English (US)",
volume = "10",
pages = "5445--5451",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "Royal Society of Chemistry",
number = "35",

}

Hydrogen dissociative chemisorption and desorption on saturated subnano palladium clusters (Pdn, n = 2-9). / Zhou, Chenggang; Yao, Shujuan; Wu, Jinping; Forrey, Robert C.; Chen, Liang; Tachibana, Akitomo; Cheng, Hansong.

In: Physical Chemistry Chemical Physics, Vol. 10, No. 35, 10.09.2008, p. 5445-5451.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Hydrogen dissociative chemisorption and desorption on saturated subnano palladium clusters (Pdn, n = 2-9)

AU - Zhou, Chenggang

AU - Yao, Shujuan

AU - Wu, Jinping

AU - Forrey, Robert C.

AU - Chen, Liang

AU - Tachibana, Akitomo

AU - Cheng, Hansong

PY - 2008/9/10

Y1 - 2008/9/10

N2 - H2 sequential dissociative chemisorption on small palladium clusters was studied using density functional theory. The chosen clusters Pdn (n = 2-9) are of the lowest energy structures for each n. H 2 dissociative chemisorption and subsequent H atom migration on the bare Pd clusters were found to be nearly barrierless. The dissociative chemisorption energy of H2 and the desorption energy of H atom in general decrease with the coverage of H atoms and thus the catalytic efficiency decreases as the H loading increases. These energies at full cluster saturation were identified and found to vary in small energy ranges regardless of cluster size. As H loading increases, the clusters gradually change their bonding from metallic character to covalent character. For the selected Pd clusters, the capacity to adsorb H atoms increases almost proportionally with cluster size; however, it was found that the capacity of Pd clusters to adsorb H atoms is, on average, substantially smaller than that of small Pt clusters, suggesting that the catalytic efficiency of Pt nanoparticles is superior to Pd nanoparticles in catalyzing dissociative chemisorption of H2 molecules.

AB - H2 sequential dissociative chemisorption on small palladium clusters was studied using density functional theory. The chosen clusters Pdn (n = 2-9) are of the lowest energy structures for each n. H 2 dissociative chemisorption and subsequent H atom migration on the bare Pd clusters were found to be nearly barrierless. The dissociative chemisorption energy of H2 and the desorption energy of H atom in general decrease with the coverage of H atoms and thus the catalytic efficiency decreases as the H loading increases. These energies at full cluster saturation were identified and found to vary in small energy ranges regardless of cluster size. As H loading increases, the clusters gradually change their bonding from metallic character to covalent character. For the selected Pd clusters, the capacity to adsorb H atoms increases almost proportionally with cluster size; however, it was found that the capacity of Pd clusters to adsorb H atoms is, on average, substantially smaller than that of small Pt clusters, suggesting that the catalytic efficiency of Pt nanoparticles is superior to Pd nanoparticles in catalyzing dissociative chemisorption of H2 molecules.

UR - http://www.scopus.com/inward/record.url?scp=51049109183&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=51049109183&partnerID=8YFLogxK

U2 - 10.1039/b804877k

DO - 10.1039/b804877k

M3 - Article

VL - 10

SP - 5445

EP - 5451

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 35

ER -