Molecular Dynamics Simulations of the Interactions between Platinum Clusters and Carbon Platelets

Sanz-Navarro, Carlos F.; Åstrand, Per‐Olof; Chen, De; Rønning, Magnus; Duin, Adri C. T. van; Jacob, Timo; Goddard, William A.

doi:10.1021/jp074806y

Cited by 87 publications

(122 citation statements)

References 78 publications

(128 reference statements)

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“…According to our calculations, the reported parameters in Ref. [18] well represent the binding energy of Pt crystals.…”

Section: Pt 5 On Graphenesupporting

confidence: 65%

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Graphdiyne as a promising substrate for stabilizing Pt nanoparticle catalyst

Lin

2015

Carbon

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PACS 61.46.-w Structure of nanoscale materials PACS 68.65.-k Low-dimensional, mesoscopic, nanoscale and other related systems: structure and nonelectronic properties Abstract -At present, Pt nanoparticle catalysts in fuel cells suffer from aggregation and loss of chemical activity. In this work, graphdiyne, which has natural porous structure, was proposed as substrate with high adsorption ability to stabilize Pt nanoparticles. Using multiscale calculations by ab initio method and the ReaxFF potential, geometry optimizations, molecular dynamics simulations, Metropolis Monte Carlo simulations and minimum energy paths calculations were performed to investigate the adsorption energy and the rates of desorption and migration of Pt nanoparticles on graphdiyne and graphene. According to the comparison between graphdiyne and graphene, it was found that the high adsorption ability of graphdiyne can avoid Pt nanoparticle migration and aggregation on substrate. Then, simulations indicated the potential catalytic ability of graphdiyne-Pt-nanoparticle system to the oxygen reduction reaction in fuel cells. In summary, graphdiyne should be an excellent material to replace graphite or amorphous carbon matrix for stabilizing Pt nanoparticle catalysts.

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“…According to our calculations, the reported parameters in Ref. [18] well represent the binding energy of Pt crystals.…”

Section: Pt 5 On Graphenesupporting

confidence: 65%

“…To obtain more information on Pt clusters adsorbed on graphene or graphdiyne surface, the ReaxFF potential [15,16] for C-Pt systems [17,18] was employed. The…”

Section: Simulation Methodsmentioning

confidence: 99%

Graphdiyne as a promising substrate for stabilizing Pt nanoparticle catalyst

Lin

2015

Carbon

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“…4), the Pt-Pt bond distance has to be slightly elongated to fit the binding sites on the PAH, which gives a slight destabilization of the Pt-Pt interaction. This change in the PtPt bond length has an important role in the enhancement of its catalytic activity 35 . In contrast to the Pt/PAH system, the interaction of Pt dimer with the PAH surface is not accompanied by a change of spin state, and the most stable spin state is still a triplet state.…”

Section: Pt Dimer On the Pah Surfacementioning

confidence: 99%

“…In this regard, it is necessary to understand the microstructure of Pt/C to analyze the interaction between the Pt atoms and the carbon surface, and to investigate the stability of Pt nano-particles on carbon materials. There are several theoretical efforts devoted to an improved understanding of the Pt-C interaction [10][11][12][13][14][15][26][27][28][29][30][31][32][33][34][35][36][37] . Kong et al, investigated the single Pt-atom adsorption on a carbon nanotubes (CNTs) and graphite nano-fibers (GNFs) 27 , and observed strong adsorption on atomic vacant sites or graphene edges.…”

Section: Introductionmentioning

confidence: 99%

Structural and electronic properties of the Pt_n–PAH complex (n = 1, 2) from density functional calculations

Mahmoodinia

Ebadi

Åstrand

et al. 2014

Phys. Chem. Chem. Phys.

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A detailed density functional study of the Pt atom and Pt dimer adsorption on a polyaromatic hydrocarbon (PAH) is presented. The preferred adsorption site for a Pt atom is confirmed to be the bridge site. Upon adsorption of a single Pt atom, however, it is found here that the electronic ground state changes from the triplet state (5d 9 6s 1 configuration) to the closed-shell singlet state (5d 10 6s 0 configuration), which consequently will affect the catalytic activity of Pt when single Pt atoms bind to a carbon surface. The preferred adsorption site for the Pt dimer in the upright configuration is the hollow site. In contrast to the adsorption of a single Pt atom, the formation of a Pt-C bond in the adsorption of a Pt dimer is not accompanied by a change in the spin state, so the most stable electronic state is still the triplet state. While the atomic charge on the Pt atoms and dimers (in parallel configuration) in the Pt n /PAH complex is positive, a negative charge is found on the upper Pt atom for the upright configuration, indicating that single layers of Pt atoms will have a different catalytic activity as compared to Pt clusters on a carbon surface. Comparing the Pt-C bond length and the charge transfer on different sites, the magnitude of the charge transfer decreases with bond elongation, indicating that the catalytic activity of the Pt atom and dimer can be changed by modifying its chemical surroundings. The adsorption energy for the Pt dimer on a PAH surface is larger than for two individual Pt atoms on the surface indicating that aggregation of Pt atoms on the PAH surface is favorable.

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“…13,14 Interfaces between transition metals (TM) and graphene have been investigated extensively by several theoretical and experimental techniques. [16][17][18][19][20][21][22] Müller et al investigated a single Pt atom, Pt dimers and trimers on highly oriented pyrolytic graphite using a scanning tunneling microscope (STM) in air. 21 The Pt particles were produced by evaporation of platinum onto the surface and the position of the Pt atoms were stable, without changes for many scans.…”

Section: Introductionmentioning

confidence: 99%

Influence of Carbon Support on Electronic Structure and Catalytic Activity of Pt Catalysts: Binding to the CO Molecule

2016

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Single-atom catalysts, especially with single Pt atoms, exhibit potentially improved catalytic activity as compared to metal clusters and metal surfaces. Here, the atop and bridged bondings of the CO molecule on the Pt/C system are studied. Vibrational frequencies, Mulliken populations, charge transfer, charge density differences and density of states are examined to determine the influence of the carbon support on electronic properties and catalytic activity of the Pt adatom and dimer. Comparing orbital populations and the amount of electron transfer to/from the CO molecule show that the net amount of electron transfer to the anti-bonding 2π * orbitals of the CO molecule is higher for the supported Pt dimer than for the substrate-free Pt dimer which leads to a lower vibrational frequency and a larger C−O bond distance. The hybridization between the π orbitals of the polycyclic aromatic hydrocarbons surface and the d orbitals of the Pt adatoms is responsible for enhancing the back donation of electrons to the 2π * orbitals of the CO molecule which results in a larger peak below the Fermi level for the 2π * states of the CO molecule in the corresponding density of state analysis. Therefore, it can be concluded that the carbon support significantly enhances the catalytic activity of the Pt atoms in contact with the surface for activating the CO molecule. The calculated C−O vibrational stretching frequencies provide valuable guidance for experiments considering the use of atom-type catalyst as building blocks for designing new catalysts.

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Molecular Dynamics Simulations of the Interactions between Platinum Clusters and Carbon Platelets

Cited by 87 publications

References 78 publications

Graphdiyne as a promising substrate for stabilizing Pt nanoparticle catalyst

Graphdiyne as a promising substrate for stabilizing Pt nanoparticle catalyst

Structural and electronic properties of the Pt_n–PAH complex (n = 1, 2) from density functional calculations

Influence of Carbon Support on Electronic Structure and Catalytic Activity of Pt Catalysts: Binding to the CO Molecule

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Molecular Dynamics Simulations of the Interactions between Platinum Clusters and Carbon Platelets

Cited by 87 publications

References 78 publications

Graphdiyne as a promising substrate for stabilizing Pt nanoparticle catalyst

Graphdiyne as a promising substrate for stabilizing Pt nanoparticle catalyst

Structural and electronic properties of the Ptn–PAH complex (n = 1, 2) from density functional calculations

Influence of Carbon Support on Electronic Structure and Catalytic Activity of Pt Catalysts: Binding to the CO Molecule

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Structural and electronic properties of the Pt_n–PAH complex (n = 1, 2) from density functional calculations