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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.
Nitrous Oxide (N2O) is a greenhouse gas with a Global Warming Potential (GWP) of 298-310 [1,2] (298-310 times more potent than carbon dioxide (CO2)). As a result, any aftertreatment system that generates N2O must be well understood to be used effectively. Under low temperature conditions, N2O can be produced by Selective Catalytic Reduction (SCR) catalysts. The chemistry is reasonably well understood with N2O formed by the thermal decomposition of ammonium nitrate [3]. Ammonium nitrate and N2O form in oxides of nitrogen (NOx) gas mixtures that are high in nitrogen dioxide (NO2)[4]. This mechanism occurs at a relatively low temperature of about 200°C, and can be controlled by maintaining the nitric oxide (NO)/NO2 ratio above 1. However, N2O has also been observed at relatively high temperatures, in the region of 500°C.
Four-way, integrated, diesel emission control systems that combine selective catalytic reduction for NOx control with a continuously regenerating trap to remove diesel particulate matter were evaluated under real-world, on-road conditions. Tests were conducted using a semi-tractor with an emissions year 2000, 6-cylinder, 12 L, Volvo engine rated at 287 kW at 1800 rpm and 1964 N-m. The emission control system was certified for retrofit application on-highway trucks, model years 1994 through 2002, with 4-stroke, 186-373 kW (250-500 hp) heavy-duty diesel engines without exhaust gas recirculation. The evaluations were unique because the mobile laboratory platform enabled evaluation under real-world exhaust plume dilution conditions as opposed to laboratory dilution conditions. Real-time plume measurements for NOx, particle number concentration and size distribution were made and emission control performance was evaluated on-road.
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.

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