Surface reactions of nitrogen oxide and ethylene on rhodium (111)

Hardeveld, R.M. van; Schmidt, A.; Niemantsverdriet, J.W.

doi:10.1007/bf00811478

Cited by 25 publications

(24 citation statements)

References 27 publications

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“…46 van Hardeveld and Hartog established the relationship between metal particle size and crystallite morphology. 24 More recently, Schimpf et al have used such concepts to evaluate the structure/activity relationships for supported gold catalysts applied to selective hydrogenation reactions. 65 Investigations on model alumina-supported palladium catalysts have been able to refine the description of adsorption sites on well-defined nanoparticles.…”

Section: A Adsorption Isotherms and Transmission Electron Microscopymentioning

confidence: 99%

“…In these cases the spectrum of chemisorbed CO is characterized by an abnormally strong linear CO band between 2070 and 2110 cm −1 , relative to the bridged CO bands. 24,25 Additionally, this latter group of catalysts is thought to be sensitive to support effects. 26 Finalizing the comments related to metal single crystals ͑surface area ca.…”

Section: Introductionmentioning

confidence: 99%

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The application of infrared spectroscopy to probe the surface morphology of alumina-supported palladium catalysts

Lear

Marshall

López-Sánchez

et al. 2005

The Journal of Chemical Physics

281

188

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Five alumina-supported palladium catalysts have been prepared from a range of precursor compounds [palladium(II) nitrate, palladium(II) chloride, palladium(II) acetylacetonate, and tetraamminepalladium(II) tetraazidopalladate(II)] and at different metal loadings (1-7.3 wt %). Collectively, this series of catalysts provides a range of metal particle sizes (1.2-8.5 nm) that emphasize different morphological aspects of the palladium crystallites. The infrared spectra of chemisorbed CO applied under pulse-flow conditions reveal distinct groupings between metal crystallites dominated by low index planes and those that feature predominantly corner/edge atoms. Temperature-programmed infrared spectroscopy establishes that the linear CO band can be resolved into contributions from corner atoms and a combination of (111)(111) and (111)(100) particle edges. Propene hydrogenation has been used as a preliminary assessment of catalytic performance for the 1 wt % loaded catalysts, with the relative inactivity of the catalyst prepared from palladium(II) chloride attributed to a diminished hydrogen supply due to decoration of edge sites by chlorine originating from the preparative process. It is anticipated that refinements linking the vibrational spectrum of a probe molecule with surface structure and accessible adsorption sites for such a versatile catalytic substrate provide a platform against which structure/reactivity relationships can be usefully developed.

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Section: A Adsorption Isotherms and Transmission Electron Microscopymentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

The application of infrared spectroscopy to probe the surface morphology of alumina-supported palladium catalysts

Lear

Marshall

López-Sánchez

et al. 2005

The Journal of Chemical Physics

281

188

View full text Add to dashboard Cite

show abstract

“…3,4 Carbon-nitrogen bond formation was reported in the reaction of NO with carbidic carbon on Pt(111) 5 and on Rh(331). 6 HCN formation in the reaction of NO with ethylene (C 2 H 4 ) on Rh(111) was reported by van Hardeveld et al 7,8 They also reported both HCN and C 2 N 2 formation in the reaction of atomic N with C 2 H 4 on Rh-(111). 9 In the latter case, the surface reactions were thought to involve only carbon atoms or CH x species but not C 2 H x species.…”

Section: Introductionmentioning

confidence: 61%

Carbon−Nitrogen Bond Formation from the Reaction of Ammonia with Dicarbon on the Pt(111) Surface

Deng

Trenary

2007

J. Phys. Chem. C

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The reaction of NH 3 with C 2 molecules on a Pt(111) surface was investigated using temperature programmed desorption, X-ray photoelectron spectroscopy (XPS), and reflection absorption infrared spectroscopy. Surface C 2 , which was prepared by dissociative adsorption of acetylene (C 2 H 2 ) at 750 K, reacts with NH 3 to form C-N bonds as revealed by the desorption of HCN and C 2 N 2 at 570 and 650 K, respectively. The formation of C-N bonds was also detected with XPS when the NH 3 /C 2 layer was annealed from 85 to 200 K through the appearance of a chemically shifted C 1s peak at 286.5 eV, which is well-resolved from the unreacted C 1s peak at 284.3 eV. Comparison of calculated and experimental RAIRS data indicates that C-N bond formation involves an HCCNH 2 surface intermediate.

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“…Insight into the nature of the intermediate fragments during the decomposition reaction of these hydrocarbons is important when investigating surface reactions of these intermediates with other species such as nitrogen atoms. These reactions can lead to the formation of products with CÀN bonds; for example, Van Hardeveld et al [1][2][3] showed that all N atoms co-adsorbed to CH species on a Rh-A C H T U N G T R E N N U N G (111) surface reacted to HCN at temperatures that are substantially below those employed in industrial HCN synthesis. We are currently exploring similar reactions between hydrocarbon species that are larger than CH on a range of surfaces including RhA C H T U N G T R E N N U N G (100).…”

Section: Introductionmentioning

confidence: 99%

Acetylene Decomposition on Rh(100): Theory and Experiment

et al. 2006

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The decomposition of acetylene on a Rh(100) single crystal was studied by a combination of experimental techniques [static secondary ion mass spectrometry (SSIMS), temperature-programmed desorption (TPD), and low-energy electron diffraction (LEED)] to gain insight into the reaction pathway and the nature of the reaction intermediates. The experimental techniques were combined with a computational approach using density functional theory (DFT). Acetylene adsorbs irreversibly on the Rh(100) surface and eventually decomposes to atomic carbon and gas-phase hydrogen. The combination of experimental and computational results enabled us to determine the most likely reaction pathway for the decomposition process.

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Surface reactions of nitrogen oxide and ethylene on rhodium (111)

Cited by 25 publications

References 27 publications

The application of infrared spectroscopy to probe the surface morphology of alumina-supported palladium catalysts

The application of infrared spectroscopy to probe the surface morphology of alumina-supported palladium catalysts

Carbon−Nitrogen Bond Formation from the Reaction of Ammonia with Dicarbon on the Pt(111) Surface

Acetylene Decomposition on Rh(100): Theory and Experiment

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