Mechanism of the reduction of nitric oxide with ammonia over Cu(II) ion-exchanged zeolites.
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The catalytic NO reduction with NH<SUB>3</SUB> over Cu(II) ion-exchanged zeolite was studied with special attention to the temperature dependence of catalytic activity which reaches maximum at <I>ca.</I> 120 °C. ESR study showed that in the catalytic system all the exchanged copper ions exist as Cu(II) up to <I>ca.</I> 120 °C, above which Cu(II) ions decrease with a rise in temperature. The reaction rates measured at 110 and 140 °C were found to show similar dependence on both NO and NH<SUB>3</SUB> partial pressures, indicating that the reaction mechanism does not differ much. By lowering temperature the Cu(I) ions formed at higher temperatures were reoxidized to Cu(II), accompanied by N<SUB>2</SUB>O formation due to the disproportionation of NO. From the results and the IR spectroscopic data a reaction mechanism was proposed. It includes a step in which NO reacts with NH<SUB>3</SUB> adsorbed to Cu(II) ions to give rise to the evolution of N<SUB>2</SUB> and the reduction of Cu(II) ions, and steps in which Cu(II) ions are regenerated accompanying the evolution of N<SUB>2</SUB>+N<SUB>2</SUB>O.
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