Enhanced Electrocatalytic Activity of Pt Subnanoclusters on Graphene Nanosheet Surface

Yoo, Eunjoo; Okata, Tatsuhiro; Akita, Tornoki; Kohyama, Masanori; Nakamura, Junji; Honma, Itaru

doi:10.1021/nl900397t

Cited by 1,060 publications

(761 citation statements)

References 18 publications

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“…Due to high surface-to-volume ratio (theoretical value of 2630 m 2 /g), graphene is a promising candidate as a substrate for stabilizing metal nanoparticles in heterogeneous catalysis. 7,8 Progress in experimental techniques has made it possible to study the properties of graphene-supported metal nanoparticles such as Pt, Pd and Au, [9][10][11][12] which may offer a new type of carbon-based metal nanocomposite for the next generation of catalysts. 9 Besides the key electrocatalytic role of the Pt catalysts in fuel cells, they have long been used as a promoter in the Fischer-Tropsch (FT) synthesis for conversion of syngas (CO + H 2 ) to liquid fuels.…”

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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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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“…We conclude that the development of more reliable damping functions may warrant better agreement with experimental data. Among the studied vdW corrections, the TS, TS+SCS, and D2, in that order, yield the best estimates for C 33 . We next compare the C 333 coefficients from vdW corrections with the RPA result, 530 GPa.…”

Section: Curvature Of the Interlayer Binding Energymentioning

confidence: 91%

“…33,[128][129][130] The resulting samples have been characterized via X-ray diffraction (XRD) and spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning tunneling microscopy (STM), and transmission electron microscopy (TEM). 129,130 For example, stable Ru and Rh nanoparticles on Gr in the 2 nm to 3 nm range resulted from decomposition of metal carbonyl precursors under rapid microwave irradiation of a graphene suspension in the ionic liquid 1-butyl-3-methylimidazolium tetrafluoroborate.…”

Section: Graphenementioning

confidence: 99%

“…We are considering a normal collision of a hydrogen atom with a flat metallic surface. Our simplified model is defined by the following Hamiltonian: 33) here the nuclear kinetic energy term is given byK n = −∇ 2 n /2M n , where M n is the nuclear mass. The physics of this phenomenon is dominated by the electron-hole excitation, which will cause one PES be close to the other PES.…”

Section: Connection Between Nrg and Exact Factorizationmentioning

confidence: 99%

“…The adsorption properties of the material being likewise extraordinary, transitionmetal (TM) clusters on Gr support emerge as promising candidates for a wide range of applications, from catalysis to spintronics. For example, in many reactions the catalytic activity of TM atoms and nanoparticles adsorbed on Gr is much higher than that of standard catalysts, such as methanol oxidation, 33 or hydrogenation of 1,3-Butadiene. 34 Vacancies in Gr sheets supporting adsorbed TM clusters enhance their stability and chemical activity 9 and increase their hydrogen-storage capacity.…”

Section: Introductionmentioning

confidence: 99%

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Since the breakthrough work by Geim and Novosolov in 2004, the investigation on graphene has grown as a result of graphene's unique electronic, mechanical, and chemical properties. To characterize single‐layer graphene, interfacial diffraction‐induced color difference was the first milestone in the graphene adventure, and then Raman spectroscopy, scanning probe microscopy, and transmission electron microscopy were used to identify the graphene layers. Apart from the Scotch tap legend, the massive production of graphene is important for graphene research and applications. The current preparation methods can be classified into top‐down (eg, chemical intercalation and liquid exfoliation) and bottom‐up (eg, chemical vapor deposition and, chemical total synthesis) strategies. The massive production of graphene has enabled researchers to explore graphene in a variety of applications, for instance, energy conversion and storage, sensor, reinforcement, catalysis, separation, and so on. Meanwhile, inspired by the legend of graphene, other layered materials are being investigated. Challenges and future perspectives in the studies of graphene and other quasi‐two‐dimensional nanomaterials are discussed.

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Enhanced Electrocatalytic Activity of Pt Subnanoclusters on Graphene Nanosheet Surface

Cited by 1,060 publications

References 18 publications

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

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

Ab-<i>initio</i> studies of adsorbate-surface interactions

Graphene: Synthesis, Characterization, and Applications

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