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  • 18-Jun-2012 12:02 EDT

SCR Deactivation Kinetics for Model-Based Control and Accelerated Aging Applications


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Selective Catalytic Reduction (SCR) catalysts are used to reduce NOx emissions from internal combustion engines in a variety of applications [1,2,3,4]. Southwest Research Institute (SwRI) performed an Internal Research & Development project to study SCR catalyst thermal deactivation. The study included a V/W/TiO2 formulation, a Cu-zeolite formulation and a Fe-zeolite formulation. This work describes NH3 storage capacity measurement data as a function of aging time and temperature. Addressing one objective of the work, these data can be used in model-based control algorithms to calculate the current NH3 storage capacity of an SCR catalyst operating in the field, based on time and temperature history. The model-based control then uses the calculated value for effective DEF control and prevention of excessive NH3 slip. Addressing a second objective of the work, accelerated thermal aging of SCR catalysts may be achieved by elevating temperatures above normal operating temperatures. Time and temperature correlations use the Arrhenius equation[5], which requires a formulation-specific deactivation energy value (Ed). The NH3 storage capacity data generated in this work were used to calculate an Ed value for each of the three SCR catalyst formulations.

Gordon J. Bartley, Southwest Research Institute

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TECH PPR 2012 CONG SP-2324
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Currently, two consolidated aftertreatment technologies are available for the reduction of NOx emissions from diesel engines: Urea SCR (Selective Catalytic Reduction) systems and LNT (Lean NOx Trap) systems. Urea SCR technology, which has been widely used for many years at stationary sources, is becoming nowadays an attractive alternative also for light-duty diesel applications. However, SCR systems are much more effective in NOx reduction efficiency at high load operating conditions than light load condition, characterized by lower exhaust gas temperatures.
OBD requirements for aftertreatment system components require monitoring of the individual system components. One such component can be an NH3-SCR catalyst for NOx reduction. An OBD method that has been suggested is to generate positive or negative spikes in the inlet NH3 concentration, and monitor the outlet NOx transient response. A slow response indicates that the catalyst is maintaining its NH3 storage capacity, and therefore it is probably not degraded. A fast response indicates the catalyst has lost NH3 storage capacity, and may be degraded. The purpose of the work performed at Southwest Research Institute was to assess this approach for feasibility, effectiveness and practicality. The presentation will describe the work performed, results obtained, and implications for applying this method in test laboratory and real-world situations. Presenter Gordon J. Bartley, Southwest Research Institute
The combination of advanced combustion with advanced selective catalytic reduction (SCR) catalyst formulations was studied in the work presented here to determine the impact of the unique hydrocarbon (HC) emissions from premixed charge compression ignition (PCCI) combustion on SCR performance. Catalyst core samples cut from full size commercial Fe- and Cu-zeolite SCR catalysts were exposed to a slipstream of raw engine exhaust from a 1.9-liter 4-cylinder diesel engine operating in conventional and PCCI combustion modes. The zeolites which form the basis of these catalysts are different with the Cu-based catalyst made on a chabazite zeolite which las smaller pore structures relative to the Fe-based catalyst. Subsequent to exposure, bench flow reactor characterization of performance and hydrocarbon release and oxidation enabled evaluation of overall impacts from the engine exhaust.
In this project funded by the Bayerische Forschungsstiftung two fundamental investigations had been carried out: first a new N-rich liquid ammonia precursor solution based on guanidine salts had been completely characterized and secondly a new type of side-flow reactor for the controlled catalytic decomposition of aqueous NH3 precursor to ammonia gas has been designed, applied and tested in a 3 liter passenger car diesel engine. Guanidine salts came into the focus due to the fact of a high nitrogen-content derivate of urea (figure 1). Specially guanidinium formate has shown extraordinary solubility in water (more than 6 kg per 1 liter water at room temperature) and therefore a possible high ammonia potential per liter solution compared to the classical 32.5% aqueous urea solution (AUS32) standardized in ISO 22241 and known as DEF (diesel emission fluid), ARLA32 or AdBlue®. Additionally a guanidine based formulation could be realized with high freezing stability down to almost ?30 °C (?

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