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  • 1
    Electronic Resource
    Electronic Resource
    On the nature of the active state of silver during catalytic oxidation of methanol (1993)
    Springer
    Catalysis letters 22 (1993), S. 215-225 
    Details
    ISSN: 1572-879X
    Keywords: Ion-scattering spectroscopy (ISS) ; methanol oxidation ; oxygen ; Raman spectroscopy ; reflection electron microscopy (REM) ; silver ; X-ray photoelectron spectroscopy (XPS)
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Under the applied high reaction temperatures (∼900 K) the Ag surface is restructured and a tightly held oxygen species is formed on the surface (Oγ) apart from O atoms dissolved in the bulk (Oβ). Methanol oxidation to formaldehyde proceeds through this Oγ species as demonstrated by application of a variety of spectroscopic techniques.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00810368
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  • 2
    Electronic Resource
    Electronic Resource
    The dissociative adsorption of N2 on a multiply promoted iron catalyst used for ammonia synthesis: a temperature-programmed desorption study (1994)
    Springer
    Catalysis letters 24 (1994), S. 317-331 
    Details
    ISSN: 1572-879X
    Keywords: Nitrogen adsorption ; N2 TPD ; iron-based catalyst ; ammonia synthesis ; microkinetic analysis
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The temperature-programmed desorption (TPD) of N2 from a multiply promoted iron catalyst used for ammonia synthesis has been studied in a microreactor system at atmospheric pressure. From TPD experiments with various heating rates a preexponential factorA = 2 × 109 molecules/site s and an activation energyE = 146 kJ/mol was derived assuming second-order desorption. The observed dependence of the TPD peak shapes on the heating rates indicated the influence of readsorption of N2 in agreement with the results obtained for various initial coverages. Simulating the N2 TPD curves using the model by Stoltze and Nørskov revealed that the calculated TPD curves were not influenced by the molecular precursor to desorption. However, the calculated rate of readsorption was found to be overestimated at high coverage compared with the experimental results. A coverage-dependent net activation energy for dissociative chemisorption (E*) was introduced as the simplest assumption rendering the dissociative chemisorption of N2 activated at high coverage. The best fit of the experimental data yieldedE* = (−15+30θ) kJ/mol using only a single type of atomic nitrogen species. These findings are in satisfactory agreement with the parameters underlying the Stoltze-Nørskov model for the kinetics of ammonia synthesis as well as with the data reported for Fe(111) single crystal surfaces.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00811804
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  • 3
    Electronic Resource
    Electronic Resource
    Oxidative coupling of methane on silver catalysts (1995)
    Springer
    Catalysis letters 32 (1995), S. 185-194 
    Details
    ISSN: 1572-879X
    Keywords: methane ; silver ; oxidative coupling ; C2 selectivity
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Bulk silver catalysts were found to be active for the oxidative coupling of methane to ethane and ethylene if operated under oxygen-limited conditions at atmospheric pressure and at temperatures above 1020 K. The addition of small amounts of sodium phosphate as promoter increases markedly the C2 selectivity (to values above 90%) and yield (〉10%) by efficient suppression of reaction steps leading to total oxidation. Further improvement of the yields might be achieved by more appropriate reactor design.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00806113
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  • 4
    Electronic Resource
    Electronic Resource
    The effect of water on the formation of strongly bound oxygen on silver surfaces (1995)
    Springer
    Catalysis letters 32 (1995), S. 171-183 
    Details
    ISSN: 1572-879X
    Keywords: oxygen ; partial oxidation ; reconstruction ; reflection electron microscopy ; Raman spectroscopy ; silver ; water
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Interaction of water with an oxygenated Ag(111) surface leads to an enhancement of the surface restructuring and an activated formation of hydroxyl groups (OH) located stably on the surface and incorporated in the subsurface region, as evidenced by means of reflection electron microscopy (REM) and in situ Raman spectroscopy. Dehydroxylation of OHads at elevated temperatures releases the strongly bound oxygen species labelled Oγ at the surface, and offers an alternative to the energetically less favorable pathway for the direct formation of the Oγ species from molecular oxygen.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00806112
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  • 5
    Electronic Resource
    Electronic Resource
    The temperature-programmed desorption of N2 from a Ru/MgO catalyst used for ammonia synthesis (1996)
    Springer
    Catalysis letters 36 (1996), S. 229-235 
    Details
    ISSN: 1572-879X
    Keywords: N2 TPD ; N2 adsorption ; Ru ; MgO ; NH3 synthesis ; microkinetic analysis
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The temperature-programmed desorption (TPD) of N2 from a Ru/MgO catalyst used for ammonia synthesis was studied in a microreactor flow system operating at atmospheric pressure. Saturation with chemisorbed atomic nitrogen (N-*) was achieved by exposure to N2 at 573 K for 14 h and subsequent cooling in N2 to room temperature. With a heating rate of 5 K/min in He, a narrow and fairly symmetric N2 TPD peak at about 640 K results. From experiments with varying heating rates a preexponential factor Ades = 1.5×1010 molecules/(site s) and an activation energy Edes = 158 kJ/mol was derived assuming secondorder desorption. This rate constant of desorption is in good agreement with results obtained with a Ru(0001) single crystal surface in ultra-high vacuum (UHV). The rate of dissociative chemisorption was determined by varying the N2 exposure conditions. Determination of the coverage of N-* was based on the integration of the subsequently recorded N2 TPD traces yielding Aads = 2×10−6 (Pa s)−1 and Eads = 27 kJ/mol. The corresponding sticking coefficient of about 10−14 at 300 K is in agreement with the inertness of Ru(0001) in UHV towards dissociative chemisorption of N2. However, if the whole catalytic surface were in this state, then the resulting rate of N2 dissociation would be several orders of magnitude lower than the observed rate of NH3 formation. Hence only a small fraction of the total Rumetal surface area of Ru/MgO seems to be highly active dominating the rate of ammonia formation.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1007/BF00807624
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  • 6
    Electronic Resource
    Electronic Resource
    The reduction of NO with H2 over Ru/MgO (1998)
    Springer
    Catalysis letters 53 (1998), S. 77-81 
    Details
    ISSN: 1572-879X
    Keywords: SCR of NO ; Ru ; MgO ; frontal chromatography ; TPD ; TPSR
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Ruthenium supported on magnesia was found to be a highly active and selective catalyst for the reduction of NO to N2 with H2. The adsorption of NO on Ru/MgO was studied at room temperature by applying frontal chromatography with a mixture of 2610 ppm NO in He. Subsequently, temperature‐programmed desorption (TPD) and temperature‐programmed surface reaction (TPSR) experiments in H2 were performed. The adsorption of NO was observed to occur partly dissociatively as indicated by the formation of molecular nitrogen. The TPD spectrum exhibited a minor NO peak at 340 K indicating additional molecular adsorption of NO during the exposure to NO at room temperature, and two N2 peaks at 480 K and 625 K, respectively. The latter data are in good agreement with previous results with Ru(0001) single‐crystal samples, where the interaction with NH3 was found to lead to two N2 thermal desorption states with a maximum coverage of atomic nitrogen of about 0.38. Heating up the catalyst after saturation with NO at room temperature in a H2 atmosphere revealed the self‐accelerated formation of NH3 after partial desorption of N2, whereby sites for reaction with H2 become available. As a consequence, the observed high selectivity towards N2 under steady‐state reduction conditions is ascribed to the presence of a saturated N+O coadsorbate layer resulting in an enhanced rate of N2 desorption from this layer and a very low steady‐state coverage of atomic hydrogen. The formation of H2O by reduction of adsorbed atomic oxygen is the slow step of the overall reaction which determines the minimum temperature required for full conversion of NO.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1023/A:1019072915187
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