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The infrared chemiluminescence technique was applied to catalytic oxidation of CH3OH, HCOOH and i-C4H10 on a Pd surface, and the reaction dynamics and mechanism were discussed in terms of internal energy states of nascent product CO2 and CO molecules. The vibrational and rotational states of CO2 produced by CH3OH oxidation were quite similar to those of CO2 produced by CO oxidation, indicating that the final step of the CO2 formation in the CH3OH oxidation involved a bimolecular process (i.e., COad+Oad). On the contrary, the intensity of IR emission of CO2 produced by HCOOH oxidation was very weak, suggesting that most of CO2 was not so vibrationally excited and that CO2 was formed via decomposition of HCOOad (unimolecular decomposition of formate). The selective production of CO and H2O was observed by the partial oxidation of i-C4H10 on Pd, and the vibrational state of product CO was very different between the Pd and Pt surfaces. These differences in internal energy states of the CO and CO2 products can provide us with new information on the dynamics and mechanism of catalytic reactions.

hyōmen kagaku/hyoumen kagaku

Molecular-Beam Infrared Chemiluminescence Study of the Dynamics of Catalytic Reactions: Decomposition and Oxidation of Methanol and Formic Acid and Partial Oxidation of Butane on Pd Surface.