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.

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Air pollution is a threat to the environment and human health. Freight trucking in particular is the main source of freight transportation emissions. Heavy-duty trucks emit large amounts of toxic air pollutants that cause serious diseases and harm public health. In addition, heavy-duty trucks emit great amounts of greenhouse gas (GHG), which is the leading cause of global warming. Despite increased environmental restrictions on air pollution and rising trucking greenhouse gas emissions in the past decades, no economic study has examined the potential GHG and air pollution reductions in the trucking sector and the associated private abatement costs to the industry. This study accounts for GHG emissions and toxic air pollutants in measuring and evaluating efficiency and productivity for the trucking industry in the 48 contiguous states. Moreover, the private costs of abatement to the industry were also estimated. When only GHG was incorporated in the production model, the results showed that each state could expand desirable output and reduce GHG by an average of 11 percent per year between 2000 and 2007. The Malmquist-Luenberger productivity indexes showed that omitting or ignoring GHG in trucking service production yielded biased estimates. On the other hand, due to increased environmental regulations, most of the toxic air pollutants decreased dramatically between 2002 and 2005. The analytical results showed that inefficiency decreased during this period. The private costs of abatement averaged $73 million per state in 2005. When GHG and six toxic air pollutants were incorporated in the production model, the estimated private abatement cost was $76 million per state, which was equivalent to 0.7 percent of the industry output in 2005.

La Réduction Catalytique Sélective (SCR) par l'ammoniac, ou l'urée, est un procédé connu de post-traitement permettant de réduire efficacement les oxydes d'azote émis par les motorisations Diesel, en azote et en eau. Les zéolithes échangées au cuivre sont parmi les meilleures formulations pour une application sur véhicules légers, puisque efficaces sur une large zone de température. Le but de cette thèse était d'étudier la stabilité hydrothermale de ce type de catalyseur. L'approche utilisée au cours de ce travail repose sur l'étude des différentes fonctionnalités d'un catalyseur commercial de NH3-SCR présent sous forme de monolithe, à l'état frais et pour différentes conditions de vieillissement, au Banc Gaz Synthétique couplée à une analyse physico-chimique précise de la phase active du catalyseur. Ceci nous a permis de comprendre les phénomènes de désactivation intervenant au cours d'un vieillissement hydrothermal et de mesurer leur impact sur l'activité et la sélectivité de ce type de catalyseur. Après traitement hydrothermal, on assiste à une désalumination plus ou moins importante de la zéolithe, pouvant conduire à l'effondrement de sa structure, ainsi que d'importantes modifications au niveau du cuivre dès les plus faibles températures de vieillissements. Les résultats ont montré l'importance de maintenir une teneur minimal de cuivre en position d'échange, afin de conserver une capacité de stockage en ammoniac suffisante, mais surtout pour garantir une bonne efficacité à basse température en SCR du NO. Le maintien de la structure de la zéolithe semble essentiel pour que le catalyseur conserve une bonne efficacité et sélectivité au cours du temps. / The Selective Catalytic Reduction (SCR) by ammonia, or urea, is a well-known after-treatment process used for converting efficiently the nitrogen oxides, emitted by Diesel engines, into nitrogen and water. Copper-exchanged zeolites are among the most efficient formulations for light-duty applications, since effective over a wide temperature-range. The aim of this thesis is to study the hydrothermal stability of this type of catalyst. The approach used is this work is based on the study of the catalytic properties of a fresh commercial monolith catalyst for NH3-SCR in fresh and after different ageing conditions, at synthetic gas test bench, coupled with a comprehensive physicochemical analysis of the catalyst active phase. This allowed us to understand the deactivation phenomena occurring during a hydrothermal ageing and the impact on the catalyst activity and selectivity. A hydrothermal treatment induces a dealumination of the zeolite, into a more or less significant extent, which can lead to its collapse, as well as important modifications of the copper sites, even at low ageing. The results showed the importance to maintain a minimal copper content into exchanged sites, in order to retain a sufficient ammonia storage capacity, and especially to provide a good efficiency for the SCR of NO at low temperature. The preservation of the zeolite structure seems to be essential in order to maintain the catalyst efficiency and selectivity over time.

The growing municipal solid waste generation rates have necessitated more efficient, optimized waste collection facilities. The majority of the US collection fleet is composed of diesel-fueled vehicles which contribute significant atmospheric emissions including greenhouse gases. In order to reduce emissions to the atmosphere, more collection agencies are investigating alternative fuel technologies such as natural gas, biofuels (bio-gas and bio-diesel), and hybrid electric technology. This research is an in-depth environmental analysis of potential alternative fuel technologies for waste collection vehicles. This study will evaluate the use of alternative fuels by waste collection vehicles. Lifecycle emissions, cost, fuel and energy consumption were evaluated for a wide range of fossil and bio-fuel technologies. Moreover, the energy consumption and the tail-pipe emissions of dieselfueled waste collection vehicles were estimated using MOVES 2010a software. Emission factors were calculated for a typical waste collection driving cycle as well as constant speed. Finally, the selection of fuel type by the waste collection industry requires consideration of environmental, security, financial, operational, and safety issues. In this study, a qualitative comparison between alternative fuels was performed; a multifactorial assessment of these factors was conducted taking into account the opinion of the waste collection industry of the importance of each factor. Liquid-petroleum fuels have higher life-cycle emissions compared to natural gas; however landfill natural gas has the lowest life-cycle emissions compared to all other fuel categories. Compressed natural gas waste collection vehicles have the lowest fuel cost per collection vehicle mile travel compared to other fuel categories. Moreover, the actual driving cycle of waste collection vehicles consists of repetitive stops and starts during waste collection; iv this generates more emissions than constant speed driving. Finally, the multifactorial assessment indicates that natural gas and landfill gas have better environmental, economical, and energy security performance than current liquid-petroleum fuels.

No description available.