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The performance of a commercial Cu-zeolite SCR catalyst after differing degrees of hydrothermal aging (aged for 72 hours at 500, 700 and 800°C with 10% moisture balanced with air) was studied by spatially resolving different key reactions using gas-phase FTIR measurements. Gases were sampled along a channel at different positions and analyzed using FTIR, which overcomes the interference of water and nitrogen on ammonia concentration detection encountered in standard mass spectrometer-based spatial resolution measurements. The NO:NO₂ concentration ratio was changed so that the standard (NO:NO₂ = 1:0), fast (NO:NO₂ = 1:1) and NO₂ (NO:NO₂ = 0:1) SCR reactions could be investigated as a function of the catalyst's hydrothermal aging extent. In addition, the effects of hydrothermal aging on the activity of NH₃ and NO oxidation were also investigated. Hydrothermal aging had little effect on NO oxidation activity.

Diesel engines have the potential to significantly increase vehicle fuel economy and decrease CO₂ emissions; however, efficient removal of NOx and particulate matter from the engine exhaust is required to meet stringent emission standards. A conventional diesel aftertreatment system consists of a Diesel Oxidation Catalyst (DOC), a urea-based Selective Catalyst Reduction (SCR) catalyst and a diesel particulate filter (DPF), and is widely used to meet the most recent NOx (nitrogen oxides comprising NO and NO₂) and particulate matter (PM) emission standards for medium- and heavy-duty sport utility and truck vehicles. The increasingly stringent emission targets have recently pushed this system layout towards an increase in size of the components and consequently higher system cost. An emerging technology developed recently involves placing the SCR catalyst onto the conventional wall-flow filter.

With a tighter regulatory environment, reduction of hydrocarbon emissions has emerged as a major concern for advanced low-temperature combustion engines. Currently precious metal-based diesel oxidation catalysts (DOC) containing platinum (Pt) and palladium (Pd) are most commonly used for diesel exhaust hydrocarbon oxidation. The efficiency of hydrocarbon oxidation is greatly enhanced by employing both Pt and Pd together compared to the case with Pt or Pd alone. However, there have been few systematic studies to investigate the effects of the ratio of platinum to palladium on catalytic oxidation over the DOC. The present study illustrates the relationship between the Pt-Pd ratio and catalyst activity and stability by evaluating a series of catalysts with various Pt to Pd ratios (1:0, 7:1, 2:1, 1:2, 1:5, 0:1). These catalysts were tested for their CO and hydrocarbon light-off temperatures under simulated conditions where both unburned and partially burned hydrocarbons were present.

Unique silver/alumina (Ag-Al₂O₃) catalysts developed using high-throughput discovery techniques in collaboration with BASF Corporation were investigated at General Motors Corporation under simulated lean-burn engine exhaust feed conditions for the selective catalytic reduction of NOx using hydrocarbons (HC-SCR). Hydrocarbon mixtures were used as the reductant to model the multi-component nature of diesel fuel and gasoline. Previous work has shown promising HC-SCR results in both laboratory reactor and engine dynamometer testing. This report investigates several aspects of HC-SCR catalyst durability, including thermal durability, sulfur tolerance, and hydrocarbon deactivation.

Unique silver/alumina catalysts developed in collaboration with BASF Corporation were investigated at General Motors under simulated lean-burn engine exhaust feed conditions for the selective catalytic reduction of NOx using hydrocarbons as reductant (HC-SCR). Catalysts were evaluated using a laboratory fixed-bed flow reactor system over a wide range of temperatures relevant to light-duty and heavy-duty exhaust conditions for CIDI (compression ignition direct injection – diesel) and SIDI (spark ignition direct injection – gasoline) applications. This report investigates the effects of silver content (i.e., wt.% Ag2O) and reductant composition (i.e., simulated diesel fuel, simulated gasoline, ethanol, and ethanol/simulated gasoline mixtures) on the steady-state NOx reduction activity. A dual catalyst approach using a HC-SCR catalyst followed by an NH3-SCR catalyst was also investigated.

A unique catalyst developed using high-throughput discovery techniques in collaboration with BASF Corporation and Accelrys, Inc. was investigated at General Motors under simulated diesel engine exhaust feed conditions for the selective catalytic reduction of NOx. A hydrocarbon mixture was used as the reductant to model the multi-component nature of diesel fuel and the catalyst was evaluated over a wide range of temperatures (150 - 550°C) relevant to light-duty diesel exhaust. This report investigates the effects of NOx (as NO or NO2), hydrocarbon concentration level (HC:NOx ratio), oxygen concentration, NO concentration, catalyst space velocity, catalyst temperature, and the co-presence of hydrogen on steady-state NOx reduction activity. Using these results, a control strategy was developed to maximize NOx conversion over the wide-ranging exhaust conditions likely to be encountered in light-duty diesel applications.

The selective catalytic reduction of NO using urea (urea-SCR) is one of the promising technologies for removing NOx from diesel engine exhaust. The engine-out NOx is reduced by ammonia (NH3) derived from urea over a catalyst to environmentally benign N2. In this paper, we investigate the effect of various reactor operating conditions on the NOx reduction performance of three different catalyst formulations (e.g., Cu-zeolite, Fe-zeolite, Vanadium-based) to obtain useful guidance in the design and operation of urea-SCR lean NOx emission control systems. We examine the effects of NO:NO2 ratio on the steady-state NOx reduction activity at typical diesel engine exhaust temperatures (150-550°C). Transient measurements were also performed to determine the impact of NH3:NOx ratio and NH3 storage on catalyst performance. The impacts of hydrocarbon poisoning and sulfur poisoning/regeneration were also examined.

The steady-state reduction of NOx at temperatures between 150-300°C has been investigated under simulated lean-burn conditions using a two-stage transient flow reactor system consisting of non-thermal plasma in combination with a sodium Y zeolite catalyst. Reactivity comparisons were made with and without plasma operation in order to identify the plasma-generated hydrocarbon species necessary for the selective catalytic reduction (SCR) of NOx. With propene as the hydrocarbon in the feed, NO is completely oxidized to NO2 in the plasma and the formation of oxidized carbon-containing species include formaldehyde, acetaldehyde, carbon monoxide, carbon dioxide, and methanol. Fourier transform infrared (FTIR) measurements indicate a close carbon balance between plasma inlet and outlet gas feed concentrations, signifying the major species have been identified.

We have prepared and tested laboratory scale monoliths wash-coated with 10, 20 and 30 wt% of either CeO2 or Ce.75Zr.25O2 (remainder is alumina). Wet impregnation was used to load the wash-coated monoliths with 50g/ft Pt:Rh at a 5:1 ratio. The catalyst were aged at temperatures between 825°C and 950°C using a cycled redox aging. The catalysts were then tested in a full-feed simulated exhaust laboratory reactor with air-to-fuel ratio (A/F) perturbations (frequencies at 1 and 3 Hz and amplitudes up to +/- 0.8 A/F). Even the lowest loading of Ce.75Zr.25O2 outperformed all three loadings of CeO2 over a full range of reaction temperatures, A/F perturbations, and catalyst space velocity (SV). Our data indicates that the ceria-zirconia catalysts can tolerate cycled redox aging at sustained bed temperatures at least 25°C higher (∼925°C vs. < 900°C) than can ceria. For the CeO2 catalysts aged at or above 900°C we observed an inverse correlation of catalyst activity to CeO2 loading.