Size Effect of Ruthenium Nanoparticles in Catalytic Carbon Monoxide Oxidation

Joo, Sang Hoon; Park, Jeong Young; Renzas, Russ; Butcher, Derek R.; Huang, Wenyu; Somorjai, Gábor A.

doi:10.1021/nl101700j

Cited by 390 publications

(359 citation statements)

References 36 publications

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“…The lower activity of smaller particles in the CO hydrogenation reaction (typically studied using polydispersed catalysts of different loadings to give some control of particle size) has typically been attributed to a greater susceptibility to oxidation, 18 and it is known for other metals that this is the case for colloidally prepared nanoparticles, such as Ru or Rh. 19,20 The turnover frequency (TOF) for the larger particles of around 0.1 CO 2 molecules (surface Co atom) −1 s −1 at 250°C is of a similar magnitude to the TOF data by Weatherbee and Bartholomew for their 15 wt % Co/SiO 2 catalyst prepared by incipient wetness (after extrapolation using the E a values they report for reactant pressures of 1 and 11 bar). 9 However the E a of around 75 ± 7 kJ mol −1 that is obtained for all particle sizes (by an Arrhenius fit of the data presented in Figure 4, see Supporting Information) appears lower than that reported, although direct comparison is not straightforward.…”

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confidence: 75%

Size-Controlled Model Co Nanoparticle Catalysts for CO₂ Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

et al. 2012

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Model cobalt catalysts for CO 2 hydrogenation were prepared using colloidal chemistry. The turnover frequency at 6 bar and at 200−300°C increased with cobalt nanoparticle size from 3 to 10 nm. It was demonstrated that near monodisperse nanoparticles in the size range of 3−10 nm could be generated without using trioctylphosphine oxide, a capping ligand that we demonstrate results in phosphorus being present on the metal surface and poisoning catalyst activity in our application.KEYWORDS: Cobalt nanoparticles, CO 2 hydrogenation, heterogeneous catalysis, catalytic poisoning C obalt-catalyzed processes and specifically the conversion of synthesis gas to hydrocarbons using cobalt (Co), Fischer−Tropsch synthesis, although long established, 1 have recently become a topic of renewed interest. This results from increased demand and declining fossil fuel reserves making both gas-to-liquid and biomass-to-liquid attractive routes to transportation fuels. 2 Especially when derived from biomass, the synthesis gas typically contains a significant fraction of CO 2 , however studies on CO 2 hydrogenation and its catalytic mechanism on Co are much less well developed than the analogous reaction with CO. 3,4 Because of its environmental impact through the greenhouse effect, fixation of CO 2 by reaction (rather than simply capture and storage) also makes studying the possibility of Co-catalyzed CO 2 hydrogenation a topic of considerable interest. 4 Additionally, there is an important technical precedent in terms of producing desirable oxygenated products by incorporation of CO 2 in such reactions (important in producing synthetic fuels). In the case of classical Cu/ZnO catalyzed methanol production, Chinchen et al. demonstrated using isotopic labeling studies that it is CO 2 , rather than CO, that is incorporated in the methanol produced. 5 Few kinetic studies of the chemistry of Co-catalyzed CO 2 hydrogenation exist. In our laboratory the conversion of CO 2 to CH 4 was explored at atmospheric pressure in a batch reactor over high-purity Co foil, 6 subsequently Welder and co-workers also studied the hydrogenation of CO 2 over Co foils in a flow reactor. 7,8 Wetherbee and Bartholomew however have reported on the use of a Co/SiO 2 catalyst prepared by incipient wetness impregnation to obtain various kinetic parameters, 9 although this does not contain information at the atomic scale about the nature of the Co catalyst particles, and it is this problem that we now address.In our laboratory size-and morphology-controlled nanoparticles, which are synthesized using colloidal techniques, have allowed the production of model catalysts via deposition within mesoporous silica supports. This is important because selectivity in multipath reactions has been found to vary with catalyst particle size and shape. In combination with powerful characterization techniques that provide atomic-and molecularlevel information, these model nanoparticle catalysts have been employed in studying fundamental mechanistic questions in many key chemica...

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confidence: 75%

Size-Controlled Model Co Nanoparticle Catalysts for CO₂ Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

et al. 2012

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“…17 Ruthenium has interesting catalytic properties for CO oxidation if prepared in the form of nanoparticles of diameter between 2 nm and 6 nm. 18 The reason for size dependence is still not entirely clear and has been debated for a long time. However, there are cases in which a combination of theoretical and experimental work has elucidated the role of different types of sites in the catalytic activity, whose abundance is related to particle size and structure.…”

Section: Introductionmentioning

confidence: 99%

Exploring the phase space of time of flight mass selected Pt_xY nanoparticles

Masini

Hernández-Fernández

Deiana³

et al. 2014

Phys. Chem. Chem. Phys.

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Mass-selected nanoparticles can be conveniently produced using magnetron sputtering and aggregation techniques. However, numerous pitfalls can compromise the quality of the samples, e.g. double or triple mass production, dendritic structure formation or unpredicted particle composition. We stress the importance of transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and ion scattering spectroscopy (ISS) for verifying the morphology, size distribution and chemical composition of the nanoparticles. Furthermore, we correlate the morphology and the composition of the Pt x Y nanoparticles with their catalytic properties for the oxygen reduction reaction. Finally, we propose a completely general diagnostic method, which allows us to minimize the occurrence of undesired masses.

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“…The available uniform nanoparticles will allow one to carry out more precise measurements of size dependence in catalytic tests in future work. Joo et al [104] synthesized uniform Ru nanoparticles ranging from 2.1 to 6.0 nm by a polyol reduction of Ru(acac) 3 precursor in the presence of a PVP stabilizer and further investigated their catalytic activity for CO oxidation. The CO oxidation activity was interestingly found to increase with particle size (as opposed to the common observation -the smaller the better -in many reactions), with the 6.0-nm Ru nanoparticle catalyst showing an 8-fold higher activity than the 2.1-nm catalysts.…”

Section: Size Control Of Metal Nanoparticles and Effects On Catalysismentioning

confidence: 99%

The impacts of nanotechnology on catalysis by precious metal nanoparticles

Jin

2012

Nanotechnology Reviews

139

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This review article focuses on the impacts of recent advances in solution phase precious metal nanoparticles on heterogeneous catalysis. Conventional nanometal catalysts suffer from size polydispersity. The advent of nanotechnology has signifi cantly advanced the techniques for preparing uniform nanoparticles, especially in solution phase synthesis of precious metal nanoparticles with excellent control over size, shape, composition and morphology, which have opened up new opportunities for catalysis. This review summarizes some recent catalytic research by using well-defi ned nanoparticles, including shape-controlled nanoparticles, high index-faceted polyhedral nanocrystals, nanostructures of different morphology (e.g., coreshell, hollow, etc.), bi-and multi-metallic nanoparticles, as well as atomically precise nanoclusters. Such well-defi ned nanocatalysts provide many exciting opportunities, such as identifying the types of active surface atoms (e.g., corner and edge atoms) in catalysis, the effect of surface facets on catalytic performance, and obtaining insight into the effects of size-induced electron energy quantization in ultra-small metal nanoparticles on catalysis. With well-defi ned metal nanocatalysts, many fundamentally important issues are expected to be understood much deeper in future research, such as the nature of the catalytic active sites, the metalsupport interactions, the effect of surface atom arrangement, and the atomic origins of the structure-activity and the structure-selectivity relationships.

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Size Effect of Ruthenium Nanoparticles in Catalytic Carbon Monoxide Oxidation

Cited by 390 publications

References 36 publications

Size-Controlled Model Co Nanoparticle Catalysts for CO₂ Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

Size-Controlled Model Co Nanoparticle Catalysts for CO₂ Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

Exploring the phase space of time of flight mass selected Pt_xY nanoparticles

The impacts of nanotechnology on catalysis by precious metal nanoparticles

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Size Effect of Ruthenium Nanoparticles in Catalytic Carbon Monoxide Oxidation

Cited by 390 publications

References 36 publications

Size-Controlled Model Co Nanoparticle Catalysts for CO2 Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

Size-Controlled Model Co Nanoparticle Catalysts for CO2 Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

Exploring the phase space of time of flight mass selected PtxY nanoparticles

The impacts of nanotechnology on catalysis by precious metal nanoparticles

Contact Info

Product

Resources

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Size-Controlled Model Co Nanoparticle Catalysts for CO₂ Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

Size-Controlled Model Co Nanoparticle Catalysts for CO₂ Hydrogenation: Synthesis, Characterization, and Catalytic Reactions

Exploring the phase space of time of flight mass selected Pt_xY nanoparticles