Infrared chemiluminescence study of CO2 Formation in CO + NO reaction on Pd(110) and Pd(111) surfaces

Kenji Nakao, Shin Ichi Ito, Keiichi Tomishige, Kimio Kunimori

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25 Citations (Scopus)

Abstract

Infrared (IR) chemiluminescence studies of CO2 formed during steady-state CO + NO reaction over Pd(110) and Pd(111) surfaces were carried out. Kinetics of the CO + NO reaction were studied over Pd(110) using a molecular-beam reaction system in the pressure range of 10-2-10 -1 Torr. The activity of the CO + NO reaction on Pd(110) was much higher than that of Pd(111), which was quite different from the result of other experiments under a higher pressure range. On the basis of the experimental data on the dependence of the reaction rate on CO and NO pressures and the reaction rate constants obtained by using a reaction model, the coverage of NO, CO, N, and O was calculated under various flux conditions. From the analysis of IR emission spectra in the CO + O2 reaction on Pd(110) and Pd(111), the antisymmetric vibrational temperature (TVAS) was seen to be higher than the bending vibrational temperature (TVB) on Pd(110). In contrast, TVB was higher than T VAS on Pd(111). These behaviors suggest that the activated complex for CO2 formation is more bent on Pd(111) than that on Pd(110), which is reflected by the surface structure. Both TV B and TVAS for the CO + O2 reaction on Pd(110) and Pd(111) increased gradually with increasing surface temperature (TS). On the other hand, in the case of the CO + NO reaction on Pd(110) and Pd(111), TVAS decreased and TV B increased significantly with increasing TS. T VB was lower than TVAS at lower TS, while TVB was higher than T VAS at higher TS. Comparison of the data obtained for the two reactions indicates that TVB in the CO + NO reaction on Pd(110) at TS = 800 and 850 K is much higher than that in the CO + O2 reaction on Pd(110).

Original languageEnglish
Pages (from-to)17579-17586
Number of pages8
JournalJournal of Physical Chemistry B
Volume109
Issue number37
DOIs
Publication statusPublished - 2005 Sep 22
Externally publishedYes

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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