Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm: Relative Stability and Catalytic Activity for CO Oxidation

Tutkimustuotos: Lehtiartikkeli

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Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm : Relative Stability and Catalytic Activity for CO Oxidation. / Li, Hui; Li, Lei; Pedersen, Andreas; Gao, Yi; Khetrapal, Navneet; Jonsson, Hannes; Zeng, Xiao Cheng.

julkaisussa: Nano Letters, Vuosikerta 15, Nro 1, 01.2015, s. 682-688.

Tutkimustuotos: Lehtiartikkeli

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Li, Hui ; Li, Lei ; Pedersen, Andreas ; Gao, Yi ; Khetrapal, Navneet ; Jonsson, Hannes ; Zeng, Xiao Cheng. / Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm : Relative Stability and Catalytic Activity for CO Oxidation. Julkaisussa: Nano Letters. 2015 ; Vuosikerta 15, Nro 1. Sivut 682-688.

Bibtex - Lataa

@article{acd6b2254765446c9e1a9961a0e51fc6,
title = "Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm: Relative Stability and Catalytic Activity for CO Oxidation",
abstract = "Relative stability of geometric magic-number gold nanoclusters with high point-group symmetry (I-h, D-5h, O-h) and size up to 3.5 nm, as well as structures obtained by global optimization using an empirical potential, is investigated using density functional theory (DFT) calculations. Among high-symmetry nanoclusters, our calculations suggest that from Au(147) to Au(923), the stability follows the order I-h > D-5h > O-h. However, at the largest size of Au(923), the computed cohesive energy differences among high-symmetry I-h, D-5h and O-h isomers are less than 4 meV/atom (at PBE level of theory), suggesting the larger high-symmetry clusters are similar in stability. This conclusion supports a recent experimental demonstration of controlling morphologies of high-symmetry Au(923) clusters (Plant, S. R.; Cao, L.; Palmer, R. E. J. Am. Chem. Soc. 2014, 136, 7559). Moreover, at and beyond the size of Au(549), the face-centered cubic-(FCC)-based structure appears to be slightly more stable than the Ih structure with comparable size, consistent with experimental observations. Also, for the Au clusters with the size below or near Au(561), reconstructed icosahedral and decahedral clusters with lower symmetry are slightly more stable than the corresponding high-symmetry isomers. Catalytic activities of both high-symmetry and reconstructed I-h-Au(147) and both I-h-Au(309) clusters are examined. CO adsorption on Au(309) exhibits less sensitivity on the edge and vertex sites compared to Au(147), whereas the CO/O2 coadsorption is still energetically favorable on both gold nanoclusters. Computed activation barriers for CO oxidation are typically around 0.2 eV, suggesting that the gold nanoclusters of similar to 2 nm in size are highly effective catalysts for CO oxidation.",
keywords = "gold nanoclusters, magic number, relative stability, surface reconstruction, CO oxidation, SPACE GAUSSIAN PSEUDOPOTENTIALS, LOW-SYMMETRY STRUCTURES, SUPPORTED AU CATALYSTS, STRUCTURAL EVOLUTION, THEORETICAL CHEMISTRY, SYNCHRONOUS-TRANSIT, SELECTIVE OXIDATION, ATOMIC STRUCTURES, COMBINING THEORY, GAS-PHASE",
author = "Hui Li and Lei Li and Andreas Pedersen and Yi Gao and Navneet Khetrapal and Hannes Jonsson and Zeng, {Xiao Cheng}",
year = "2015",
month = "1",
doi = "10.1021/nl504192u",
language = "English",
volume = "15",
pages = "682--688",
journal = "Nano Letters",
issn = "1530-6984",
publisher = "AMERICAN CHEMICAL SOCIETY",
number = "1",

}

RIS - Lataa

TY - JOUR

T1 - Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm

T2 - Relative Stability and Catalytic Activity for CO Oxidation

AU - Li, Hui

AU - Li, Lei

AU - Pedersen, Andreas

AU - Gao, Yi

AU - Khetrapal, Navneet

AU - Jonsson, Hannes

AU - Zeng, Xiao Cheng

PY - 2015/1

Y1 - 2015/1

N2 - Relative stability of geometric magic-number gold nanoclusters with high point-group symmetry (I-h, D-5h, O-h) and size up to 3.5 nm, as well as structures obtained by global optimization using an empirical potential, is investigated using density functional theory (DFT) calculations. Among high-symmetry nanoclusters, our calculations suggest that from Au(147) to Au(923), the stability follows the order I-h > D-5h > O-h. However, at the largest size of Au(923), the computed cohesive energy differences among high-symmetry I-h, D-5h and O-h isomers are less than 4 meV/atom (at PBE level of theory), suggesting the larger high-symmetry clusters are similar in stability. This conclusion supports a recent experimental demonstration of controlling morphologies of high-symmetry Au(923) clusters (Plant, S. R.; Cao, L.; Palmer, R. E. J. Am. Chem. Soc. 2014, 136, 7559). Moreover, at and beyond the size of Au(549), the face-centered cubic-(FCC)-based structure appears to be slightly more stable than the Ih structure with comparable size, consistent with experimental observations. Also, for the Au clusters with the size below or near Au(561), reconstructed icosahedral and decahedral clusters with lower symmetry are slightly more stable than the corresponding high-symmetry isomers. Catalytic activities of both high-symmetry and reconstructed I-h-Au(147) and both I-h-Au(309) clusters are examined. CO adsorption on Au(309) exhibits less sensitivity on the edge and vertex sites compared to Au(147), whereas the CO/O2 coadsorption is still energetically favorable on both gold nanoclusters. Computed activation barriers for CO oxidation are typically around 0.2 eV, suggesting that the gold nanoclusters of similar to 2 nm in size are highly effective catalysts for CO oxidation.

AB - Relative stability of geometric magic-number gold nanoclusters with high point-group symmetry (I-h, D-5h, O-h) and size up to 3.5 nm, as well as structures obtained by global optimization using an empirical potential, is investigated using density functional theory (DFT) calculations. Among high-symmetry nanoclusters, our calculations suggest that from Au(147) to Au(923), the stability follows the order I-h > D-5h > O-h. However, at the largest size of Au(923), the computed cohesive energy differences among high-symmetry I-h, D-5h and O-h isomers are less than 4 meV/atom (at PBE level of theory), suggesting the larger high-symmetry clusters are similar in stability. This conclusion supports a recent experimental demonstration of controlling morphologies of high-symmetry Au(923) clusters (Plant, S. R.; Cao, L.; Palmer, R. E. J. Am. Chem. Soc. 2014, 136, 7559). Moreover, at and beyond the size of Au(549), the face-centered cubic-(FCC)-based structure appears to be slightly more stable than the Ih structure with comparable size, consistent with experimental observations. Also, for the Au clusters with the size below or near Au(561), reconstructed icosahedral and decahedral clusters with lower symmetry are slightly more stable than the corresponding high-symmetry isomers. Catalytic activities of both high-symmetry and reconstructed I-h-Au(147) and both I-h-Au(309) clusters are examined. CO adsorption on Au(309) exhibits less sensitivity on the edge and vertex sites compared to Au(147), whereas the CO/O2 coadsorption is still energetically favorable on both gold nanoclusters. Computed activation barriers for CO oxidation are typically around 0.2 eV, suggesting that the gold nanoclusters of similar to 2 nm in size are highly effective catalysts for CO oxidation.

KW - gold nanoclusters

KW - magic number

KW - relative stability

KW - surface reconstruction

KW - CO oxidation

KW - SPACE GAUSSIAN PSEUDOPOTENTIALS

KW - LOW-SYMMETRY STRUCTURES

KW - SUPPORTED AU CATALYSTS

KW - STRUCTURAL EVOLUTION

KW - THEORETICAL CHEMISTRY

KW - SYNCHRONOUS-TRANSIT

KW - SELECTIVE OXIDATION

KW - ATOMIC STRUCTURES

KW - COMBINING THEORY

KW - GAS-PHASE

U2 - 10.1021/nl504192u

DO - 10.1021/nl504192u

M3 - Article

VL - 15

SP - 682

EP - 688

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

IS - 1

ER -

ID: 10259013