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  • 1
    ISSN: 1572-879X
    Keywords: N2O decomposition ; molecular beam ; nozzle heating ; Pt ; Rh ; translational energy ; vibrational energy
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Steady‐state N2O decomposition reaction on polycrystalline Pt and Rh surfaces has been studied using a supersonic free‐jet molecular beam (2.1 × 1018 molecules/cm2 s). The energy of the incident N2O beam was controlled by a nozzle heating technique in conjunction with a seeding technique. The decomposition rate shows both translational and vibrational energy dependence on the Pt surface. However, there is also the surface temperature dependence of the decomposition rate even varying the incident beam energy, indicating precursor‐mediated dissociation of N2O on the Pt surface. On the other hand, no energy dependence was observed on the Rh surface, suggesting that the decomposition dynamics are different between Pt and Rh surfaces.
    Type of Medium: Electronic Resource
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  • 2
    ISSN: 1572-879X
    Keywords: SCR of N2O ; CH4 ; greenhouse‐effect gas ; simultaneous removal ; Fe‐BEA zeolite
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Simultaneous catalytic removal of N2O and CH4 as the strong greenhouse‐effect gases was found to be possible over an Fe‐ion‐exchanged BEA zeolite (Fe‐BEA) by the selective catalytic reduction (SCR) of N2O with CH4. The direct decomposition of N2O (2N2O → 2N2 + O2) and the oxidation of CH4 (CH4 + 2O2 → CO2 + 2H2O) over Fe‐BEA zeolite required high temperature above 400 and 450 °C, respectively. Nevertheless, the catalytic reduction of N2O by adding CH4 over Fe‐BEA zeolite readily occurred at much lower temperatures (ca. 250–350 °C) whether in the presence of O2 or not. No oxidation of CH4 by O2 took place at these temperatures. On the basis of these results and the kinetic studies, it was concluded that CH4 reacted selectively with N2O to produce N2, CO2 and H2O over Fe‐BEA zeolite even in the presence of excess O2. Overall stoichiometry of the SCR of N2O with CH4 was determined as follows: 4N2O + CH4 → 4N2 + CO2 + 2H2O.
    Type of Medium: Electronic Resource
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  • 3
    ISSN: 1572-879X
    Keywords: 18O isotope ; N2O decomposition ; oxidized Rh catalyst ; reaction mechanism
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract N2O decomposition on an oxidized Rh catalyst (unsupported) has been studied using a tracer technique in order to reveal the reaction mechanism. N2 16O was pulsed onto an 18O/oxidized Rh catalyst at 493 K and desorbed O2 molecules were monitored. The 18O fraction in the desorbed oxygen had the same value as that on the surface oxygen. The result shows that the oxygen molecules do not desorb via the Eley–Rideal mechanism, but via the Langmuir–Hinshelwood mechanism. On the other hand, desorption of oxygen from Rh surfaces (in vacuum or in He) occurs at higher temperatures, which suggests reaction-assisted desorption of oxygen during the N2O decomposition reaction at low temperature.
    Type of Medium: Electronic Resource
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