Adsorption and Reaction of C2H4 and O2 on a Nanosized Gold Cluster: A Computational Study

Lee, Chen-Chi; Chen, Hsin‐Tsung

doi:10.1021/acs.jpca.5b04737

Cited by 16 publications

(22 citation statements)

References 52 publications

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“…Using DFT calculations, we found that O 2 is strongly chemisorbed on the C 59 N (–0.32 ∼ −0.84 eV for CN site and −0.66 ∼ −0.99 eV for CC site depending on the various adsorption sites, see Figure S1 and Table S1 in Supporting Information). Compared to those on Pt(111) (–0.58 ∼ −0.72 eV), Pt(110) (–1.48 eV), Pt(001) (–1.30 eV), Pt clusters (–0.72 eV for Pt 2 and −1.08 eV for Pt 3 ), Au clusters (–0.24 eV for Au 4 , ∼ −0.50 eV for Au 7 and Au 9 , −0.60 eV for Au 29 , −0.99 eV for Au 38 ), Pt‐embedded graphene (–1.34 eV), Cu‐embedded graphene (–2.67 eV), Fe‐embedded graphene (–2.09 eV), Au‐embedded graphene (–1.34 eV), the strong ability of C 59 N fullerene for O 2 adsorption (–0.32 ∼ −0.99 eV) creates its possibility as a high active and metal‐free catalyst for ORR and CO oxidation. Two species of O 2 activation on the C 59 N fullerene can be examined: superoxide and peroxide.…”

Section: Resultsmentioning

confidence: 99%

Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation

Lin

Chen

2017

J Comput Chem

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The O activation and CO oxidation on nitrogen-doped C N fullerene are investigated using first-principles calculations. The calculations indicate that the C N fullerene is able to activate O molecules resulting in the formation of superoxide species ( O2-) both kinetically and thermodynamically. The active superoxide can further react with CO to form CO via the Eley-Rideal mechanism by passing a stepwise reaction barrier of only 0.20 eV. Ab initio molecular dynamics (AIMD) simulation is carried out to evidence the feasibility of the Eley-Rideal mechanism. In addition, the second CO oxidation takes place with the remaining atomic O without any activation energy barrier. The full catalytic reaction cycles can occur energetically favorable and suggest a two-step Eley-Rideal mechanism for CO oxidation with O catalyzed by the C N fullerene. The catalytic properties of high percentage nitrogen-doped fullerene (C N ) is also examined. This work contributes to designing higher effective carbon-based materials catalysts by a dependable theoretical insight into the catalytic properties of the nitrogen-doped fullerene. © 2017 Wiley Periodicals, Inc.

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Section: Resultsmentioning

confidence: 99%

Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation

Lin

Chen

2017

J Comput Chem

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“…Günay et al investigated O 2 adsorption on a gold cluster and found that stable O 2 adsorption required the presence of an unpaired electron on the gold cluster. Lee et al , calculated O 2 and O adsorption on Au 38 and found that the most stable sites for O 2 and O adsorption are the bridge and hexagonal sites. These investigations showed that only negatively charged even-numbered gold clusters bind a single O 2 molecule in a superoxo-like configuration , and that negatively charged free gold clusters are catalytically active for the CO-combustion reaction, whereas positively charged clusters are inert for the reaction because oxygen cannot be adsorbed …”

Section: Resultsmentioning

confidence: 99%

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Zhao

et al. 2021

J. Phys. Chem. C

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Controlling the charge types of metal clusters on supports is of great importance in designing a noble-metal-free catalyst. Here, we designed two different types of N-doped graphene surfaces, the graphitic-like nitrogen-doped graphene G nN and the pyridinic-like nitrogen-doped graphene G nN,n′V. We found that in the Au28/G nN system, the Au atoms interact with C atoms. However, in the Au28/G nN,n′V system, the Au atoms interact with the N atoms. Specifically, the different bonding modes result in the charge state of the Au cluster being negative on the G nN surface, whereas on the G nN,n′V surface, the Au cluster is of positive charge. Therefore, it is possible to change the type of carbon–nitrogen bonding structure to control the charge types of gold clusters on nitrogen-doped graphene. In these two systems, the O2 molecules prefer to be activated at the unsaturated and electron-rich bridge sites of the Au cluster. O2 adsorption further enhances the charge transfer along the original directions at the Au28 cluster/N-doped graphene substrate interfaces. However, the charge states of Au clusters slightly affect the activation of O–O bonds. The negatively charged Au cluster surface (Au28/G nN) exhibits better catalytic activity to CO oxidation under the trimolecular Eley–Rideal (3ER) mechanism and electrocatalytic reduction of CO2 compared with the positively charged Au cluster surface (Au28/G nN,n′V). Our results are beneficial for accelerating the industrial application of nanometer-sized gold catalysts and provide a theoretical basis for the design and development of new catalysts.

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“…Furthermore, some theoretical studies employing clusters as structural models for gold surfaces have been reported. Au 25 and Au 32 , serving as models for Au(111) and Au(100) surfaces, respectively, were found to adsorb ethylene in a di--bonded configuration [20], whereas Au 38 adsorbs C 2 H 4 in a di-bonded configuration on an fcc(100) surface but in abonded configuration on an fcc(111) surface [21]. Additionally, it was shown that C 2 H 4 prefers to bind to corner Au atoms in Au 79 and Au 140 in a -bonded configuration [22,23].…”

Section: Introductionmentioning

confidence: 99%

The interaction of ethylene with free gold cluster cations: infrared photodissociation spectroscopy combined with electronic and vibrational structure calculations

Lang

Bernhardt

Bakker

et al. 2018

J. Phys.: Condens. Matter

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The interaction of ethylene with free gold clusters of different sizes and charge states has been previously shown theoretically to involve two different adsorption modes of the C 2 H 4 molecule, namely: the di-and-bonded ethylene adsorption configurations. Here, we present the first experimental investigation of the structure of a series of gas-phase gold-ethylene complexes, Au x (C 2 H 4) y + (x =2-4, y =1-3). By employing infrared multiple-photon dissociation spectroscopy (IR-MPD) in conjunction with first-principles calculations it is uncovered that up to three C 2 H 4 molecules bind to gold cations exclusively in a-bonded configuration. The binding of all ethylene molecules is found to be dominated by partial electron donation from the ethylene molecules to the gold clusters leading to an activation of the CC bond. The cooperative action of multiple coadsorbed C 2 H 4 on Au 4 + is shown to enable additional charge back-donation and an enhanced CC bond activation. In contrast, the strong C-H bond is not weakened and the experimental spectra do not give any indication for C-H bond dissociation. The possible correlations of the CC bond stretch vibration with the CC bond length and the net charge transfer are discussed.

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Adsorption and Reaction of C₂H₄ and O₂ on a Nanosized Gold Cluster: A Computational Study

Cited by 16 publications

References 52 publications

Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation

Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

The interaction of ethylene with free gold cluster cations: infrared photodissociation spectroscopy combined with electronic and vibrational structure calculations

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Adsorption and Reaction of C2H4 and O2 on a Nanosized Gold Cluster: A Computational Study

Cited by 16 publications

References 52 publications

Nitrogen‐doped C60 as a robust catalyst for CO oxidation

Nitrogen‐doped C60 as a robust catalyst for CO oxidation

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

The interaction of ethylene with free gold cluster cations: infrared photodissociation spectroscopy combined with electronic and vibrational structure calculations

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Product

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Adsorption and Reaction of C₂H₄ and O₂ on a Nanosized Gold Cluster: A Computational Study

Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation

Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation