Detection, role and utilization of excited molecules in catalytic reaction by means of IR chemiluminescence

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(1) Dynamics of catalytic reactions by measurement of IR emission of the vibrationally-excited product molecules(1-1) CO+O_2 reaction on Pd (110), Pd (111)Analysis method using intensities of IR emission was proposed, and changes in vibrational temperatures were measured with increasing surface temperature.(1-2) CO+NO reaction on Pd (110), Pd (111)Large structure-sensitivity in the activity of the CO+NO reaction was found for the first time. NO Dissociation does not take place on Pd (111), and nascent oxygen from NO is formed on Pd (110) because NO dissociation is limited.(1-3) CO+0_2 reaction on Pt (110), Pt (111)Activity was higher on Pt (110) than on Pt (111). Changes in vibrational temperatures were observed due to the reconstruction of (l x l) into (1 x 2) on Pt (110).(2) Direct catalytic partial oxidation of CH_4 and C_2H_6 using heatable and seeded molecular beam technique(2-1) The promoting effect of energetic activation of a methane molecular beam: production of syngasCO+H_2 (in particular H_2) were produced selectively during steady-state CH_4+O_2 reaction on Pt by exciting methane. The reaction also takes place on Rh by reducing O_2.(2-2) Comparative study between methane and ethane in the catalytic paratial reaction on Pt and RhBased on the results of the reaction order measurements one possible explanation for the promotion is that energetically activated methane and ethane react with adsorbed oxygen and produce methoxy and ethoxy species, which are regarded as precursors for hydrogen formation.