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A gas-phase system to oxidize and remove the platinum and palladium from automotive catalytic converter units was studied. The effects of varying reaction temperature, time and reactant gas concentration upon yields were monitored using a colorimetric procedure based on the regent p-nitroso-N, N-dimethyl amiline. Chlorine plus carbon monoxide at 700°-900°C. displayed the most promise for commercial application.

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This thesis describes an investigation into the spatial species conversion profiles of a Cu-zeolite SCR under engine conditions at low exhaust gas temperatures; this was then compared with a CFD model that models the catalyst via a porous medium measuring 5 x 5 x 91 cells assuming a uniform cross-sectional flow distribution. Species conversion rates were sampled at fixed points in the axial direction. The analysis of the spatial conversion profiles is a more rigorous method in assessing the ability of a mathematical model to predict the experimental data. It can also assist in the optimisation of the catalyst size, minimising packaging requirements and manufacturing costs. The experiments were undertaken on a light-duty diesel engine at a speed of 1500rpm, and at a load of 6bar BMEP; this provided exhaust gas temeraqtures between 200 and 220°C. NO2:NOx ratios were controlled by changing the size and position of the diesel oxidation catalyst, the inlet NH3: NOx ratio was also also varied, ammonia gas was used instead of urea for the purposes of simlicity. The advantage of testing on an actual engine over lab-babed studies is that the conditions such as exhaust gas composition are more realistic. A 1D CFD model was constructed using the ‘porous medium approach’ with kinetics obtained from open literature. Results from the simulations were then compared with the experimental data for the same engine conditions. It was observed that the majority of the NOx conversion took place in the first half of the brick for all NH3: NOx ratios investigated, and that the formation of N2O via NO2 and ammonia had the same influence as the ‘fast’ SCR reaction just after the inlet, which the CFD model failed to predict for the base case analyses. The influence of the inlet ammonia on the model was also noticed to be greater than in the experiments. Simple transient analyses were also undertaken on the short SCR bricks for NO2: NOx ratios of 0.6 and 0.07, and it was observed that the response time to steady-state was noticeably higher in the experiments than in the model. Modifications made to the model, including decreasing the influence of the ‘fast’ SCR reaction, and the addition of an empirical term onto the ammonia adsorption provided a noticeably better agreement for different NH3: NOx injection ratios. The desorption kinetics in the model were also altered by increasing the strength of the bonding of the ammonia onto the adsorption sites. This improved the transient agreement between the model and the experiments, but reduced the steady-state concentrations at the exit of the brick for all NH3:NOx ratios investigated.

Digitized by Kansas Correctional Industries

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