Search Results

Selective Catalytic Reduction (SCR) systems are nowadays widely applied for the reduction of NOx emitted from Diesel engines. The typical process is based on the injection of aqueous urea in the exhaust gases before the SCR catalyst, which determines the production of the ammonia needed for the catalytic reduction of NOx. However, this technology is affected by two main limitations: a) the evaporation of the urea water solution (UWS) requires a sufficiently high temperature of the exhaust gases and b) the formation of solid deposits during the UWS evaporation is a frequent phenomenon which compromise the correct operation of the system. In this context, to overcome these issues, a technology based on the injection of gaseous ammonia has been recently proposed: in this case, ammonia is stored at the solid state in a cartridge containing a Strontium Chloride salt and it is desorbed by means of electrical heating.

NH₃/urea SCR is a very effective and widely used technology for the abatement of NOx from diesel exhaust. The SCR mechanism is well understood and the catalyst behavior can be predicted by mathematical models - as long as operation above the temperature limit for AdBlue® injection is considered. The behavior below this level is less understood. During the first seconds up to minutes after cold start, complete NOx abatement can be observed over an SCR catalyst in test bench experiments, together with a significant increase in temperature after the converter (ca. 100 K). In this work these effects have been investigated over a monolith Cu-zeolite SCR catalyst. Concentration step experiments varying NO, NO₂ and H₂O have been carried out in lab scale, starting from room temperature. Further, the interaction of C₃H₆ and CO with NOx over the SCR has been investigated.

Transient and steady-state kinetic data are herein presented to analyze the inhibiting effect of ammonia on the NH₃-SCR of NO at low temperatures over a Fe-zeolite commercial catalyst for vehicles. It is shown that in SCR converter models a rate expression accounting for NH₃ inhibition of the Standard SCR reaction is needed in order to predict the specific dynamics observed both in lab-scale and in engine test bench runs upon switching on and off the ammonia feed. Two redox, dual site kinetic models are developed which ascribe such inhibition to the spill-over of ammonia from its adsorption sites, associated with the zeolite, to the redox sites, associated with the Fe promoter. Better agreement both with lab-scale intrinsic kinetic runs and with engine test-bench data, particularly during transients associated with dosing of ammonia to the SCR catalyst, is obtained assuming slow migration of NH₃ between the two sites.

Ammonia/urea-SCR is a mature technology, applied worldwide for the control of NOx emissions in combustion exhausts from thermal power plants, cogeneration units, incinerators and stationary diesel engines and more recently also from mobile sources. However a greater DeNOx activity at low temperatures is desired in order to meet more and more restrictive legislations. In this paper we report transient and steady state data collected over commercial Fe-ZSM-5 and V₂O₅-WO₃/TiO₂ catalysts showing high NOx reduction efficiencies in the 200 - 350°C T-range when NO and ammonia react with nitrates, e.g., in the form of an aqueous solution of ammonium nitrate. Under such conditions a new reaction occurs, the so-called "Enhanced SCR" reaction, 2 NH₃ + 2 NO + NH₄NO₃ → 3 N₂ + 5 H₂O.

A numerical model describing the ammonia based SCR process of NOX on zeolite catalysts is presented. The model is able to simulate coated and extruded monoliths. The development of the reaction kinetics is based on a study which compares the activity of zeolite and vanadium based catalysts. This study was conducted in a microreactor loaded with washcoat powder and with crushed coated monoliths. A model for the SCR reaction kinetics on zeolite catalysts is presented. After the parameterization of the reaction mechanism the reaction kinetics were coupled with models for heat and mass transport. The model is validated with laboratory data and engine test bench measurement data over washcoated monolith catalysts. A numerical simulation study is presented, aiming to reveal the differences between zeolite and vanadium based SCR catalysts.

In this paper the low temperature reduction process of nitrates stored at high temperatures over model Pt-Ba/Al2O3 LNT catalysts using both H2 and C3H6 is analyzed. The results indicate that over the Pt-Ba/Al2O3 catalyst the reduction of stored NOx with both H2 and C3H6 occurs at temperature below those corresponding to their thermal stability. Accordingly, the reduction process occurs through a Pt-catalyzed surface reaction, which does not involve, as a preliminary step, the thermal decomposition of the adsorbed NOx species. The occurrence of such a pathway also requires the co-presence of the storage element and of the noble metal on the same support.

A 1D+1D numerical model describing the ammonia based SCR process of NO and NO2 on vanadia-titania catalysts is presented. The model is able to simulate coated and extruded monoliths. Basing on a fundamental investigation of the catalytic processes a reaction mechanism for the NO/NO2 - NH3 reacting system is proposed and modeled. After the parameterization of the reaction mechanism the reaction kinetics have been coupled with models for heat and mass transport. Model validation has been performed with engine test bench experiments. Finally the model has been applied to study the influence of NO2 on SCR efficiency within ETC and ESC testcycles, Additional simulations have been conducted to identify the potential for catalyst volume reduction if NO2 is present in the inlet feed.

A two-dimensional numerical model describing the ammonia based SCR-process on vanadia-titania catalysts is presented. The model is able to simulate coated and extruded monoliths. For the determination of the intrinsic kinetics of the various NH3-NOx reactions, unsteady microreactor experiments were used. In order to account for the influence of transport effects the kinetics were coupled with a fully transient two-phase 1D+1D monolith channel model. The model has been validated extensively with laboratory data and engine test bench measurements. After validation the model has been applied to calculate catalyst NOx conversion maps, which were used to define catalyst sizes. Additional simulations were conducted studying the influence of cell density and NH3-dosage ratio.

In a previous systematic investigation on the adsorption of NOx/O2 over Pt/Al2O3, Ba/Al2O3 and Pt-Ba/Al2O3 samples, a novel pathway for NOx storage was proposed that implies the direct uptake of NO in the presence of oxygen in the form of nitrites at Ba sites nearby Pt. In order to better elucidate the role of the Pt-Ba interaction on NOx storage and reduction, in the present study the adsorption of NOx/O2 and their subsequent reduction was further investigated over Pt-Ba/Al2O3 samples having different Ba loadings; a physical mixture Pt/Al2O3+Ba/Al2O3 was also considered for comparison purposes. A kinetic literature model has been adapted to our catalytic system in order to simulate the transient NOx adsorption over a wide range of operating conditions.