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Published: 2005

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As lean-burn engines are being introduced in the United States, both advantages and disadvantages arise. Lean-burn engines can operate at a high efficiency, and are developed for a wide range of power supplies. Unfortunately, due to the low temperature at which these engines operate, NO[subscript x] formation becomes an issue. Forthcoming legislation pertaining to heavy-duty lean-burn engines aimed at reducing both particulate matter emissions and emissions of nitric oxides has brought about a need for a better method for reducing NO[subscript x] from lean exhaust gases at moderate temperatures. It is generally accepted that current fuel treatment processes alone will be unable to accommodate emission standards proposed for upcoming years. While the current 3-way catalyst is ineffective in reducing NO[subscript x] under lean conditions, many new strategies are being developed. The Lean NO[subscript x] Catalyst (LNC), Lean NO[subscript x] Trap (LNT), and Selective Catalytic Reduction (SCR) catalyst are all viable methods with research underway. Currently, the selective catalytic reduction (SCR) of nitrogen oxides by N-containing reducing agents is one of the most powerful methods for accomplishing the removal of NO[subscript x] from an exhaust stream. This technology has been in place in steady state power plants, but has yet to be fully implemented in mobile engines. This is due in part to the problems encountered in the automated control of ammonia addition to the exhaust gas. In steady state operation, a relatively constant amount of NO[subscript x] is produced over a given amount of time. Thus, to provide a stoichiometric amount of ammonia only the steady state concentration of NO[subscript x] must be known. In an automotive application the NO[subscript x] produced is not constant and the addition of ammonia must vary accordingly. The purpose of this thesis is to explore the SCR process of the reaction between NO and NH3 through an experimental matrix and also through a kinetic study extracted from the results. These results are used in a simple theoretical model of the SCR reaction. The use of NO as the only form of NO[subscript x] allows for the kinetics of the NO reaction to be studied separately from the NO2 kinetics. This will be a first step in understanding the overall SCR process involving both NO and NO2. The SCR process for the reaction between NO and NH3, while understood on a global scale, is still under debate at the elementary level. It is currently thought that the reaction occurs according to an Eley-Rideal mechanism, where strongly absorbed ammonia reacts with weakly absorbed or gas phase NO to produce nitrogen and water. It is generally accepted that this reaction proceeds in first order with respect to nitric oxide and zero order with respect to ammonia and oxygen.