ChemInform Abstract: 1,3‐Bitadiene Hydrogenation on Single Crystals of Platinum. Part 2. Sulfur Poisoning of Pt(110).

Oudar, J.; Piñol, S.; Pradier, C. M.; Berthier, Yves

doi:10.1002/chin.198805087

Cited by 3 publications

(44 citation statements)

References 1 publication

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“…Low-energy electron diffraction (LEED) results indicate that at coverages up to 1 monolayer the Ni and Co films grow pseudomorphically with respect to the W(110) and W(100) substrates. 165,182 This growth pattern leads to Ni and CO monolayer densities on W(110) and W(100) which are significantly less than the corresponding monolayer densities for the corresponding (111) and (100) surfaces. However, the specific rates for CO methanation on the Ni/W(110), Ni/W(100) and Co/W(100), Co/W(110) catalysts correlate well with those observed on the corresponding supported Ni and Co catalysts.…”

Section: Mixed-metal Surfaces As Model Alloy Catalystsmentioning

confidence: 91%

“…Oxygen dissolved on Ag(111) promotes selective oxidation. 42 Kinetic data for Ag (110) 48,49 and Ag (111) 41,50 indicate that adsorbed chlorine reduces the activity and increases the selectivity of these surfaces toward ethylene epoxidation. It has been proposed 49,50 that this occurs mainly via an ensemble effect, in which the chlorine blocks the Ag sites that are necessary for fragmentation and full combustion of the intermediate.…”

Section: Metal Single Crystals As Model Catalystsmentioning

confidence: 95%

“…A comparison of the turnover frequencies (TOF) at P H2 ) 100 Torr, P ethane ) 1 Torr, and T ) 575 K gives the following order of catalytic activity: Ir(110)-(1×2) > Ir-(111) > Ru(001) > Ni(100) > Re(001) > Ni(111) > W(100) > Pt (111). In this series the TOF varies from ∼ 0.001 CH 4 molecules site -1 s -1 on Pt (111) 89 to ∼ 2 CH 4 molecules site -1 s -1 on Ir(110)-(1×2). 88 These studies show unambiguously that ethane hydrogenolysis can be classified as a structure sensitive reaction.…”

Section: Metal Single Crystals As Model Catalystsmentioning

confidence: 99%

“…213 For reference, data are displayed for a saturation coverage of CO on Pd (111) and P(100) single-crystal surfaces. 213 The Pd particle sizes of the model catalysts were determined by chemisorption methods 214,215 and verified using scanning probe techniques (see, for example, Figure 13).…”

Section: Model Oxide-supported Metal Catalystsmentioning

confidence: 99%

“…Comparison of the specific rates of the CO + O2 reaction measured over Rh(100), Rh(111), and Rh/Al2O3 (from refs 107 and 108).…”

mentioning

confidence: 99%

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Correlations between Surface Science Models and “Real-World” Catalysts

Goodman

1996

J. Phys. Chem.

157

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Over the past two decades the "pressure and material gaps" separating ultrahigh-vacuum surface science and technical catalysis has been bridged by coupling an apparatus for the measurement of reaction kinetics at elevated pressures with an ultrahigh-vacuum system for surface analysis. Studies with this combined methodology have provided an atomic-level understanding of various aspects of heterogeneous catalysis such as structure/activity relationships, the role of promoters and inhibitors on catalytic activity, and the nature of the metal-metal bond in mixed-metal catalysts. These investigations have demonstrated the relevance of single-crystal studies for modeling the behavior of high surface area supported catalysts as well as the power of surface analytical techniques for characterizing adsorbed reactants and intermediates.

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Section: Mixed-metal Surfaces As Model Alloy Catalystsmentioning

confidence: 91%

Section: Metal Single Crystals As Model Catalystsmentioning

confidence: 95%

Section: Metal Single Crystals As Model Catalystsmentioning

confidence: 99%

Section: Model Oxide-supported Metal Catalystsmentioning

confidence: 99%

“…Comparison of the specific rates of the CO + O2 reaction measured over Rh(100), Rh(111), and Rh/Al2O3 (from refs 107 and 108).…”

mentioning

confidence: 99%

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Correlations between Surface Science Models and “Real-World” Catalysts

Goodman

1996

J. Phys. Chem.

157

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Hydrogen Diffusion Guided Design of Pt‐Based Alloys for Inhibition of Butadiene Over‐Hydrogenation

Sun

Wang

et al. 2019

ChemPhysChem

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Alloying Pt with other metals is an effective strategy to tune its performance towards selective hydrogenation reactions. Herein, we have demonstrated a process to screen Pt‐based alloys for inhibition of butadiene over‐hydrogenation with a model comprising isolated single atoms (ISA) embedded into Pt(111). DFT calculations reveal that the diffusion energy barrier of H co‐adsorbed with 1‐butene is a key parameter for the screening. The output from the ISA model was validated by testing several typical Pt‐based alloys towards butadiene hydrogenation. Furthermore, an unexpected higher selectivity to cis‐2‐butene compared to the trans isomer and 1‐butene over the PtZn alloy was explored employing the ISA model.

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Structure Sensitivity in Pt Nanoparticle Catalysts for Hydrogenation of 1,3-Butadiene:In SituStudy of Reaction Intermediates Using SFG Vibrational Spectroscopy

et al. 2013

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The product selectivity during 1,3-butadiene hydrogenation on monodisperse, colloidally synthesized, Pt nanoparticles was studied under reaction conditions with kinetic measurements and in situ sum frequency generation (SFG) vibrational spectroscopy. SFG was performed with the capping ligands intact in order to maintain nanoparticle size by reduced sintering. Four products are formed at 75 °C: 1-butene, cis-2-butene, trans-2-butene, and n-butane. Ensembles of Pt nanoparticles with average diameters of 0.9 and 1.8 nm exhibit a ∼30% and ∼20% increase in the full hydrogenation products, respectively, as compared to Pt nanoparticles with average diameters of 4.6 and 6.7 nm. Methyl and methylene vibrational stretches of reaction intermediates observed under working conditions using SFG were used to correlate the stable reaction intermediates with the product distribution. Kinetic and SFG results correlate with previous DFT predictions for two parallel reaction pathways of 1,3-butadiene hydrogenation. Hydrogenation of 1,3-butadiene can initiate with H-addition at internal or terminal carbons leading to the formation of 1-buten-4-yl radical (metallocycle) and 2-buten-1-yl radical intermediates, respectively. Small (0.9 and 1.8 nm) nanoparticles exhibited vibrational resonances originating from both intermediates, while the large (4.6 and 6.7 nm) particles exhibited vibrational resonances originating predominately from the 2-buten-1-yl radical. This suggests each reaction pathway competes for partial and full hydrogenation and the nanoparticle size affects the kinetic preference for the two pathways. The reaction pathway through the metallocycle intermediate on the small nanoparticles is likely due to the presence of low-coordinated sites.

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ChemInform Abstract: 1,3‐Bitadiene Hydrogenation on Single Crystals of Platinum. Part 2. Sulfur Poisoning of Pt(110).

Cited by 3 publications

References 1 publication

Correlations between Surface Science Models and “Real-World” Catalysts

Correlations between Surface Science Models and “Real-World” Catalysts

Hydrogen Diffusion Guided Design of Pt‐Based Alloys for Inhibition of Butadiene Over‐Hydrogenation

Structure Sensitivity in Pt Nanoparticle Catalysts for Hydrogenation of 1,3-Butadiene:In SituStudy of Reaction Intermediates Using SFG Vibrational Spectroscopy

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