화학공학소재연구정보센터
Journal of the American Chemical Society, Vol.129, No.11, 3420-3425, 2007
Oxidation of H-2 and CO over ion-exchanged X and Y zeolites
Zeolites X and Y exchanged with Group IA cations were synthesized by aqueous ion exchange of NaX and NaY and used as catalysts in the oxidation of H-2 and CO at temperatures ranging from 473 to 573 K. The CsX zeolite was the most active material of the series for both reactions whereas HX was the least active. Moreover, the oxidation of CO in H-2 was very selective (similar to 80%) over the alkali-metal exchanged materials. Isotopic transient analysis of CO oxidation during steady-state reaction at 573 K was used to evaluate the coverage of reactive carbon-containing intermediates that lead to product as well as the pseudo-first-order rate constant of the reaction. A factor of 4 enhancement in activity achieved by exchanging Cs for Na was attributed to a higher coverage of reactive intermediates in CsX because the pseudo-first-order rate constant was nearly same for the two materials (similar to 0.7 s(-1)). The number of reactive intermediates on both materials was orders of magnitude below the number of alkali metal cations in the zeolites but was similar to the number of impurity Fe atoms in the samples. Because the trend in Fe impurity loading was the same as that for oxidation activity, a role of transition metal impurities in zeolite oxidation catalysis is suggested.