Surface reactions of ethylene and oxygen on Pt(111)

Steininger, Harald; Ibach, H.; Lehwald, S.

doi:10.1016/0039-6028(82)90549-0

Cited by 417 publications

(228 citation statements)

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“…C 2 H 4 + Pt-H → CH 3 CH 2 Pt (1) CH 3 CH 2 Pt + Pt-H → C 2 H 6 + Pt (2) Adsorbed ethylene is known to exist in a weakly π-bonded or more strongly di-σ-bonded form based on reflection-absorption infrared and HREELS studies on Pt(111) surfaces, [4][5][6][7][8] and transmission IR spectroscopy of supported metal particle catalysts. 9,10 Various experimental studies have provided convincing evidence that the hydrogenation step (1) involves π-C 2 H 4 species.…”

Section: Introductionmentioning

confidence: 99%

Direct Observation of Surface Ethyl to Ethane Interconversion upon C₂H₄ Hydrogenation over Pt/Al₂O₃ Catalyst by Time-Resolved FT-IR Spectroscopy

Wasylenko

Frei

2005

J. Phys. Chem. B

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Section: Introductionmentioning

confidence: 99%

Direct Observation of Surface Ethyl to Ethane Interconversion upon C₂H₄ Hydrogenation over Pt/Al₂O₃ Catalyst by Time-Resolved FT-IR Spectroscopy

Wasylenko

Frei

2005

J. Phys. Chem. B

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“…Scanning tunneling microscopy has made dramatic advances in many areas of surface science since its introduction by Binnig and Rohrer in 1982 [11], allowing direct observation of dynamic processes such as adatom diffusion [12], chemical reactions [13], and adsorbate restructuring of surfaces [14], on both model surfaces and supported catalysts [15]. Clearly, its direct real space observation at extremely high resolution, in comparison to averaged information obtained by diffraction techniques, allows one to monitor atomic features from adsorbates, defects (vacancies, interstitials, impurities, steps, dislocations, and grain boundaries), to molecular processes such as adsorbate mobility and surface reconstruction.…”

Section: List Of Figures and Tablesmentioning

confidence: 99%

“…The adsorption of ethylene on Pt(111) is well documented [12][13][14][15][16][17][18][19][20][21]. At temperatures below 50 K, ethylene is physisorbed with its C-C bond parallel to the surface [12].…”

Section: Co Poisoning Of Ethylene Hydrogenation On Pt(111)mentioning

confidence: 99%

“…At temperatures below 50 K, ethylene is physisorbed with its C-C bond parallel to the surface [12]. Above 60 K it rehybridizes to form a di-σ-bonded state on fcc hollow sites [13][14][15][16]. The di-σ-bonded ethylene forms ethylidyne readily near room temperature through the loss of one hydrogen and transfer of another to the other carbon to form a methyl group [22][23][24].…”

Section: Co Poisoning Of Ethylene Hydrogenation On Pt(111)mentioning

confidence: 99%

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High Pressure Scanning Tunneling Microscopy Studies of AdsorbateStructure and Mobility during Catalytic Reactions: Novel Design of anUltra High Pressure, High Temperature Scanning Tunneling MicroscopeSystem for Probing Catalytic Conversions

Tang¹

2005

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The aim of the work presented therein is to take advantage of scanning tunneling microscope's (STM) capability for operation under a variety of environments under real time and at atomic resolution to monitor adsorbate structures and mobility under high pressures, as well as to design a new generation of STM systems that allow imaging in situ at both higher pressures (35 atm) and temperatures (350 °C).The design of a high pressure, high temperature scanning tunneling microscope system, that is capable of monitoring reactions in situ at conditions from UHV and ambient temperature up to 1 atm and 250 °C, is briefly presented along with vibrational 2 and thermal analysis, as this system serves as a template to improve upon during the design of the new ultra high pressure, high temperature STM.Using this existing high pressure scanning tunneling microscope we monitored the co-adsorption of hydrogen, ethylene and carbon dioxide on platinum (111) and rhodium (111) crystal faces in the mTorr pressure range at 300 K in equilibrium with the gas phase. During the catalytic hydrogenation of ethylene to ethane in the absence of CO the metal surfaces are covered by an adsorbate layer that is very mobile on the time scale of STM imaging. We found that the addition of CO poisons the hydrogenation reaction and induces ordered structures on the single crystal surfaces. Several ordered structures were observed upon CO addition to the surfaces pre-covered with hydrogen and ethylene: a rotated (√19 x √19)R23.4° on Pt(111), and domains of c(4 x 2)-CO+C 2 H 3 , previously unobserved (4 x 2)-CO+3C 2 H 3 , and (2 x 2)-3CO on Rh(111). A mechanism for CO poisoning of ethylene hydrogenation on the metal single crystals was proposed, in which CO blocks surface metal sites and reduces adsorbate mobility to limit adsorption and reaction rate of ethylene and hydrogen.In order to observe heterogeneous catalytic reactions that occur well above ambient pressure and temperature that more closely resemble industrial settings, a custom STM motor has been designed and constructed in-house. The new STM design features a much reduced size and a rigid coupling to the sample, and has been tested to show considerably higher resonance frequency than conventional tripod designs, providing the ability to image faster and yielding smaller susceptibility to noise. A flow reactor cell of much reduced volume for pressures up to 35 atmospheres has also been designed and 3 constructed to house the new STM. The small volume reduces gas consumption and sensitivity to impurities in high pressure gases, as well as maximizes product concentration and reduces response time. The ability to flow reactant gases also allows for continuous monitoring of reaction mixture by mass spectrometry or gas chromatography, and permits correlation of structural information from STM and reaction kinetics. The reactor cell containing the STM is placed inside an UHV system to allow cleaning and characterization of sample before and after experiments, as well as continuous monitoring by m...

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“…An EELS study of ethylene chemisorbed on Pt͑111͒ has been carried out and it was concluded that ethylene is sp 3 hybridized on the surface, namely it is bonded in the di-configuration. 12 The near edge x-rayabsorption fine-structure ͑NEXAFS͒ spectra of ethylene on Pt͑111͒, when compared to the spectra calculated using the multiple-scattering X␣ method for a cluster model of adsorbed ethylene, indicate that ethylene is adsorbed on Pt͑111͒ in the di-configuration. 13 A similar NEXAFS study of ethylene on Ni͑111͒ "Ni͑110͒… indicates that ethylene is also adsorbed on Ni͑111͒ "Ni͑110͒… in the diconfiguration.…”

Section: Introductionmentioning

confidence: 98%

Theoretical study of the valence level photoemission spectrum of C2H2 adsorbed on a Ni metal surface

Ohno

Niessen

1996

Surface Science

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In order to investigate the valence-level photoemission spectrum of C 2 H 4 adsorbed on a Ni metal surface, we calculated the valence-hole spectral functions of NiC 2 H 4 ͑ bonding͒ using the ab initio third-order algebraicdiagrammatic-construction "ADC͑3͒… Green-function method using an extended basis set. We obtained an overall good agreement with experiment. The changes in the spectral features such as the changes in the separations of the ionization energies from the gas phase to the chemisorbed phase are due to the metal ligand bonding exerted via the charge-transfer excitations and do not arise from the distortion of the molecule, which occurs upon chemisorption. ͓S0163-1829͑97͒01004-7͔

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Surface reactions of ethylene and oxygen on Pt(111)

Cited by 417 publications

References 17 publications

Direct Observation of Surface Ethyl to Ethane Interconversion upon C₂H₄ Hydrogenation over Pt/Al₂O₃ Catalyst by Time-Resolved FT-IR Spectroscopy

Direct Observation of Surface Ethyl to Ethane Interconversion upon C₂H₄ Hydrogenation over Pt/Al₂O₃ Catalyst by Time-Resolved FT-IR Spectroscopy

High Pressure Scanning Tunneling Microscopy Studies of AdsorbateStructure and Mobility during Catalytic Reactions: Novel Design of anUltra High Pressure, High Temperature Scanning Tunneling MicroscopeSystem for Probing Catalytic Conversions

Theoretical study of the valence level photoemission spectrum of C2H2 adsorbed on a Ni metal surface

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Surface reactions of ethylene and oxygen on Pt(111)

Cited by 417 publications

References 17 publications

Direct Observation of Surface Ethyl to Ethane Interconversion upon C2H4 Hydrogenation over Pt/Al2O3 Catalyst by Time-Resolved FT-IR Spectroscopy

Direct Observation of Surface Ethyl to Ethane Interconversion upon C2H4 Hydrogenation over Pt/Al2O3 Catalyst by Time-Resolved FT-IR Spectroscopy

High Pressure Scanning Tunneling Microscopy Studies of AdsorbateStructure and Mobility during Catalytic Reactions: Novel Design of anUltra High Pressure, High Temperature Scanning Tunneling MicroscopeSystem for Probing Catalytic Conversions

Theoretical study of the valence level photoemission spectrum of C2H2 adsorbed on a Ni metal surface

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Direct Observation of Surface Ethyl to Ethane Interconversion upon C₂H₄ Hydrogenation over Pt/Al₂O₃ Catalyst by Time-Resolved FT-IR Spectroscopy

Direct Observation of Surface Ethyl to Ethane Interconversion upon C₂H₄ Hydrogenation over Pt/Al₂O₃ Catalyst by Time-Resolved FT-IR Spectroscopy