Journal of the Chemical Society - Faraday Transactions p. 1267 - 1275 (1996)
Update date:2022-08-29
Topics:
Genta, Minoru
Nishiyama, Satoru
Tsuruya, Shigeru
Masai, Mitsuo
Alkali-metal addition to Cu-NaZSM-5 zeolite promotes oxidation activity (mainly partial oxidation rather than complete oxidation) using benzyl alcohol oxidation as a model reaction. The alkali-metal added to Cu-NaZSM-5 is present as the corresponding oxide, such as Na2O. The percentage of Cu ion exchanged and the added Na/Cu atomic ratio in Na-added Cu-NaZSM-5 are important factors governing the oxidation activity. The added alkali-metal is suggested to be located in the neighbourhood of the Cu species as ligands, rather than covering the Cu species in Cu-NaZSM-5 zeolite. The influence of added Na on the adsorption and redox properties of Cu-NaZSM-5 zeolite were investigated to shed light on the role of the added alkali-metal during oxidation by means of ethanol and CO adsorptions, O2 uptake, TPD of ethanol and temperature-programmed reaction, in addition to the results of the oxidation reaction. The amounts of O2 uptake by the prereduced Naadded Cu-NaZSM-5 were considerably larger than those by the corresponding Cu-NaZSM-5 without alkali-metal. The added alkali-metal is considered to help accommodate the adsorbed oxygen species, which is dissociated and is responsible for the partial oxidation of benzyl alcohol. The added alkali-metal also allows the Cu1 species to be more easily oxidized and to adsorb greater amounts of reactant alcohol; this explains the promotion effect of the added alkali-metal observed in the gas-phase catalytic oxidation of benzyl alcohol.
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