Gold as Hydrogen. An Experimental and Theoretical Study of the Structures and Bonding in Disilicon Gold Clusters Si2Aun‐ and Si2Aun (n = 2 and 4) and Comparisons to Si2H2 and Si2H4.

Li, Xi; Kiran, Boggavarapu; Wang, Lai‐Sheng

doi:10.1002/chin.200534001

Cited by 7 publications

(9 citation statements)

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“…The electronic binding energies of C 2 HAg n -(n=1-4) well fall within the energy range of conventional excitation lasers used in PES measurements (266 nm, 4.661 eV) [45][46][47][48]. We notice that the difference between ADE and VDE of C 2 HAg 4 -is the largest (0.73 eV).…”

Section: Electron Detachment Energiessupporting

confidence: 76%

A Density-Functional Study on the Interaction of C2H Radical with Silver Clusters Agn0/-(n =1–4)

Xu¹,

Li²,

Song³

et al. 2013

J Chem Eng Process Technol

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The interaction between C 2 H radical and silver clusters Ag n 0/-(n=1-4) has been studied based on a systematic density functional theory (DFT) investigation. The DFT calculated results show that C 2 H radical inclines to interact with silver clusters Ag n 0/-(n =1-4) as an integrity in the most stable structures of C 2 HAg n 0/-(n=1-4) rather than being divided by Ag n clusters. The Ag n 0/-(n =1-4) clusters remain their structural integrities as units in the ground states of C 2 HAg n 0/-(n=1-4). Detailed natural resonance theory (NRT) and natural bond order analyses show that the interaction between the C 2 H radical and the Ag n 0/-(n =1-4) in the most stable structures of C 2 HAg n 0/-(n = 1-4) are mainly ionic. Compared with that of C 2 H radical and the Au n 0/-(n = 1-4), the electronic component in C 2 HAg n 0/-(n = 1-4) increased due to the strong relativistic effects of Au. The stretching vibrational frequencies of C≡C and C-H in the ground states of C 2 HAg n 0/-(n =1-4) occur red shifts compared with those of the C 2 H radical due to the interaction between the Ag n 0/-clusters and C2H radical. The photoelectron spectra (PES) of the most stable structures of C 2 HAg n 0/-(n=1-4) have been simulated to facilitate their future experimental characterizations.

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Section: Electron Detachment Energiessupporting

confidence: 76%

A Density-Functional Study on the Interaction of C2H Radical with Silver Clusters Agn0/-(n =1–4)

Xu¹,

Li²,

Song³

et al. 2013

J Chem Eng Process Technol

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“…There have been a relatively fewer number of studies on the silicon-doped gold clusters. One of the fascinating findings reported on the silicon-doped gold clusters is the gold–hydrogen analogy. , Recently, on the other hand, Pal et al have carried a systematic study on the structural evolution of silicon-doped gold clusters and have shown that silicon-doped gold clusters have a significantly different structure. Although the reactivity of gold clusters strongly depends on their shape and electronic distribution, , little is known about the catalytic activity of silicon-doped gold clusters that show contrastingly different structures and electronic structures as compared to the pristine gold clusters.…”

Section: Introductionmentioning

confidence: 99%

Effect of Silicon Doping on the Reactivity and Catalytic Activity of Gold Clusters

2014

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Doping is known to be an excellent and simple way of catalyst design. Although notable progress has been made in understanding the reactivity and catalytic activity of gas-phase and supported gold clusters, very few studies have been carried out on the doped gold clusters. In the present work, we have carried out density functional theory calculations to investigate the effect of silicon doping on the reactivity and catalytic activity of gold nanoclusters. The present work particularly focuses on the adsorption and activation of molecular oxygen on the pristine and silicon-doped gold clusters. The results confirm that the silicon-doped Au7Si cluster shows considerable binding and activation of the O2 molecule in comparison to the pristine Au8 cluster as reflected in the relevant geometrical parameters (O–O and Au–O bond lengths) and O–O stretching frequency. However, silicon doping has no contrasting effect on the reactivity and catalytic activity of the Au7 cluster. In addition to the stronger binding and activation of the O2 molecule, the doped Au7Si cluster leads to a significant reduction in the activation barrier (0.57 eV) for the environmentally important CO oxidation reaction in contrast to the catalytically inactive pristine Au8 cluster (1.22 eV). Thus, our results highlight the critical role of doping foreign impurities for future endeavors in the field of gold nanocatalysis.

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“…Hydrogen in gold has a special relevance considering the so-called gold–hydrogen analogy as established by Kiran et al, − where the chemistry of the gold atom resembles that of a single hydrogen atom. Extending a step further, this Au/H analogy initially reported for mono- and disilicon gold clusters has also been extended to trisilicon gold clusters by the same authors .…”

mentioning

confidence: 99%

Beyond the Gold–Hydrogen Analogy: Doping Gold Cluster with H-atom–O₂ Activation and Reduction of the Reaction Barrier for CO Oxidation

Jena

Chandrakumar

Ghosh

2011

J. Phys. Chem. Lett.

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The gold–hydrogen analogy is well established in terms of analogous chemistry exhibited by gold and hydrogen atoms. A step beyond this analogy is demonstrated here by showing that the replacement of a Au atom with a H-atom in a gold cluster can lead to considerable enhancement in its reactivity. The present computational study reveals that while the closed-shell neutral pristine gold cluster Au8 can bind only weakly with an O2 molecule, its doped counterpart Au7H shows remarkable enhancement in its binding with molecular oxygen. It also shows an increment in O–O bond length and a red shift in vibrational frequency, indicating the activation of the O2 molecule. Furthermore, the H-doped gold cluster reduces the barrier height for the environmentally important CO oxidation reaction as compared to the pristine cluster. These observations may spur further studies in the design of a cost-effective and efficient catalyst by doping gold clusters with a cheaper element like hydrogen.

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Gold as Hydrogen. An Experimental and Theoretical Study of the Structures and Bonding in Disilicon Gold Clusters Si₂Au_n^‐ and Si₂Au_n (n = 2 and 4) and Comparisons to Si₂H₂ and Si₂H₄.

Cited by 7 publications

References 1 publication

A Density-Functional Study on the Interaction of C2H Radical with Silver Clusters Agn0/-(n =1–4)

A Density-Functional Study on the Interaction of C2H Radical with Silver Clusters Agn0/-(n =1–4)

Effect of Silicon Doping on the Reactivity and Catalytic Activity of Gold Clusters

Beyond the Gold–Hydrogen Analogy: Doping Gold Cluster with H-atom–O₂ Activation and Reduction of the Reaction Barrier for CO Oxidation

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Gold as Hydrogen. An Experimental and Theoretical Study of the Structures and Bonding in Disilicon Gold Clusters Si2Aun‐ and Si2Aun (n = 2 and 4) and Comparisons to Si2H2 and Si2H4.

Cited by 7 publications

References 1 publication

A Density-Functional Study on the Interaction of C2H Radical with Silver Clusters Agn0/-(n =1–4)

A Density-Functional Study on the Interaction of C2H Radical with Silver Clusters Agn0/-(n =1–4)

Effect of Silicon Doping on the Reactivity and Catalytic Activity of Gold Clusters

Beyond the Gold–Hydrogen Analogy: Doping Gold Cluster with H-atom–O2 Activation and Reduction of the Reaction Barrier for CO Oxidation

Contact Info

Product

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Gold as Hydrogen. An Experimental and Theoretical Study of the Structures and Bonding in Disilicon Gold Clusters Si₂Au_n^‐ and Si₂Au_n (n = 2 and 4) and Comparisons to Si₂H₂ and Si₂H₄.

Beyond the Gold–Hydrogen Analogy: Doping Gold Cluster with H-atom–O₂ Activation and Reduction of the Reaction Barrier for CO Oxidation