Transient response method applied to the kinetic analysis of the DeNOx–SCR reaction

The dynamics of the selective catalytic reduction (SCR) reaction over a commercial V 2 O 5 -WO 3 /TiO 2 catalyst is investigated by concentration programmed surface reaction (CPSR), i.e. a modified transient response method based on linear temporal evolution of the reactant feed concentrations. The adsorption-desorption of the reactants NH 3 and NO and their surface reaction are addressed independently. The data confirm that over the investigated catalyst NH 3 is stored on the catalyst surface, and that the reaction occurs between adsorbed NH 3 and gaseous or weakly adsorbed NO. H 2 O significantly inhibits the SCR reaction, but this effect is not due to competition with NH 3 for the adsorption on the surface acid sites at any surface coverage. A slight inhibiting effect of adsorbed NH 3 on the SCR reaction is also evident. The whole set of data is quantitatively described according to a dynamic kinetic model which superimposes the surface reaction of NO reduction to the NH 3 adsorption-desorption processes, and accounts for NH 3 oxidation at high temperatures. It is also shown that the transient SCR-DeNO x data, as well as the related kinetic analysis, approach steady-state data in the limit of slow variations.

[1]  P. Forzatti,et al.  Characterization and Reactivity of V2O5–MoO3/TiO2 De-NOx SCR Catalysts , 1999 .

[2]  Ken Nobe,et al.  Kinetics of nitric oxide reduction with ammonia on "chemical mixed" and impregnated vanadium(V) oxide-titanium(IV) oxide catalysts , 1984 .

[3]  James A. Dumesic,et al.  Vanadia-Titania Catalysts for Selective Catalytic Reduction of Nitric-Oxide by Ammonia , 1995 .

[4]  M. D. Amiridis,et al.  The effect of metal oxide additives on the activity of V2O5/TiO2 catalysts for the selective catalytic reduction of nitric oxide by ammonia , 1999 .

[5]  E. Moroz,et al.  The Influence of Support on the Activity of Monolayer Vanadia-Titania Catalysts for Selective Catalytic Reduction of NO with Ammonia , 1995 .

[6]  P. Berge,et al.  The preparation of WO3/TiO2 and Wo3/Al2O3 and characterization by temperature-programmed reduction , 1989 .

[7]  G. Bond,et al.  Vanadium oxide monolayer catalysts Preparation, characterization and catalytic activity , 1991 .

[8]  E. Tronconi,et al.  Transient kinetics of SO2 oxidation over SCR-DeNO(x) monolith catalysts , 1999 .

[9]  A. Hindmarsh LSODE and LSODI, two new initial value ordinary differential equation solvers , 1980, SGNM.

[10]  Guido Busca,et al.  Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts: A review , 1998 .

[11]  A. Wokaun,et al.  In Situ Diffuse Reflectance FTIR Study of the Selective Catalytic Reduction of NO by NH3 over Vanadia-Titania Aerogels , 1994 .

[12]  Pio Forzatti,et al.  Unsteady Analysis of NO Reduction over Selective Catalytic Reduction−De-NOx Monolith Catalysts , 1998 .

[13]  P. Forzatti,et al.  Chemical, structural and mechanistic aspects on NOx SCR over commercial and model oxide catalysts , 1998 .

[14]  T. Srnak,et al.  Temperature-programmed desorption/reaction and in situ spectroscopic studies of vanadia/titania for catalytic reduction of nitric oxide , 1992 .

[15]  G. Ramis On the consistency of data obtained from different techniques concerning the surface structure of vanadia-titania catalysts: Reply to the comment of Israel E. Wachs , 1990 .

[16]  Pio Forzatti,et al.  Steady-State and Transient Reactivity Study of TiO2-Supported V2O5−WO3 De-NOx Catalysts: Relevance of the Vanadium−Tungsten Interaction on the Catalytic Activity , 1996 .

[17]  E. Tronconi,et al.  Experimental and theoretical investigation of the dynamics of the SCR - DeNOx reaction , 1996 .