Applied Catalysis B: Environmental, Vol.11, No.1, 81-98, 1996
Kinetics of the Catalytic Liquid-Phase Hydrogenation of Aqueous Nitrate Solutions
Liquid-phase reduction using a solid Pd/Cu bimetallic catalyst provides a potential technique for the removal of nitrates from waters. Kinetic measurements were performed for a wide range of reactant concentrations and reaction conditions in an isothermal semi-batch slurry reactor operating at atmospheric pressure. The effects of catalyst loading and initial nitrate concentration on the reaction rate were also investigated. The proposed intrinsic rate expression for nitrate disappearance is based on the conventional Langmuir-Hinshelwood kinetic approach, considering both equilibrium nitrate as well as dissociative hydrogen adsorption processes to different types of active sites, and assuming an irreversible bimolecular surface reaction between adsorbed reactant species to be the rate-controlling step. The apparent activation energy for catalytic liquid-phase nitrate reduction and the heat of nitrate adsorption, in the temperature range 280.5-293 K, were found to be 47 and 22 kJ/mol, respectively, It is confirmed that the process of catalytic liquid-phase hydrogenation of aqueous nitrate solutions undergoes a redox mechanism.