The selective catalytic reduction (SCR) of NOx with NH3 is considered to be the most promising technique for the efficient reduction of highly detrimental NOx (to N2) emitted from diesel engine vehicles. Amongst the various catalysts available for SCR, Fe- and Cu-zeolite catalysts are found to be highly stable and efficient towards maximum NOx reduction over a wide temperature range. Cu-zeolites are more active at low temperatures ( 350 oC) while Fe-zeolites are more active at high temperatures ( 400 oC). We carried out a comprehensive experimental and kinetic modeling study of key SCR reactions on Fe- and Cu-zeolite catalysts and present a detailed understanding of mass transfer limitations and kinetics and mechanistic aspects of various SCR reactions on these catalysts. Experiments carried out on monolith catalysts having different washcoat loadings, washcoat thicknesses and lengths indicate the presence of washcoat (or pore) diffusion limitations at intermediate to high temperature range in all the SCR reactions. A detailed analysis of the effect of temperature on the transitions between various controlling regimes (kinetic, washcoat diffusion and external mass transfer) is presented. Agreement in the differential kinetics studies of NO oxidation and standard SCR (NO + O2 + NH3) reactions indicates NO oxidation is the rate determining step for standard SCR. A detailed kinetic model capturing key features of all the SCR reactions is developed. This model accurately predicts the experimentally observed NOx conversions over a wide temperature range and different feed conditions. Finally, a systematic study of various SCR reactions is carried out on a combined system of Fe- and Cu-zeolite monolithic catalysts to determine if a high NOx conversion could be sustained over a wider temperature range than with individual Fe- and Cu-zeolite catalysts. Amongst various configurations, a dual-layer catalyst with a thin Fe-zeolite layer on top of a thick Cu-zeolite layer resulted in a very high NOx removal efficiency over a broad temperature range of practical interest. The kinetic model accurately captures the experimental data with a combined system of Fe- and Cu-zeolite catalysts and provides further insights into the catalyst arrangements for maximum NOx reduction efficiency.

This book is a printed edition of the Special Issue "Selective Catalytic Reduction of NO_x" that was published in Catalysts

The increasing price of liquid fuels and an increased focus on fuel efficiency has driven vehicle engine manufacturers toward diesel and other lean burn engines at the cost of increased emissions of nitrogen oxides (NOX), which contribute to pollution such as smog, ground level ozone, and acid deposition. Within the past thirty years, increasingly stringent NOX emission standards have forced engine manufacturers to develop novel ways to reduce these emissions. With the implementation of the latest American and European NOX emission standards, Selective Catalytic Reduction (SCR) has become the most prominent NOX reduction method in lean-burn engines.In the present work, a method is developed to test the performance of commercial SCR catalyst coated monoliths and probe the deactivation mechanisms. A monolith testing apparatus is constructed for these purposes. Necessary design features included a programmable gas mixing system, a steam generator, a temperature control system, and an analysis system based upon Fourier-transformed infrared spectroscopy. It is found that a high flow rate of carrier gas as well as a method to generate a water mist and prevent dripping is essential to ensure a stable supply of steam and repeatable results.Important SCR reactions, namely the standard, fast, and slow SCR reactions as well as NH3 adsorption and performance of a zeolite catalyst coated monolith were investigated at three temperatures -- 250 and 300 °C representing engine operation at normal operating conditions and 400 °C representing engine operation at high load. The amount of NH3 adsorbed decreased with temperature in line with previous studies while NOX reduction performance increased with higher temperatures at all inlet compositions tested. A transient drop in NO conversion performance was observed upon introduction of NH3 without the presence of NO2 consistent with previous studies suggesting an NH3 inhibition mechanism. When supplied with 1:1 and 1:3 ratios of NO:NO2 at 250 °C, the catalyst reduced more NOX than NH3 suggesting that part of the NOX reduction was proceeding through an ammonium nitrate intermediate and generating nitric acid. In addition, NH3 oxidation into N2O was prevalent at 300°C in an excess of NO2. The SCR reaction results indicate that both transient effects and side reactions play an important role in an NH3 SCR system, particularly one that is designed to operate under continuously changing conditions.Catalyst aging mechanisms were investigated by comparing catalytic performance, material structure, and surface composition of a new and a used zeolite catalyst monolith for the fast SCR reaction. Physical analysis of the catalyst monoliths through X-ray Photoelectron Spectroscopy (XPS), X-ray Diffraction (XRD), and Scanning Electron Microscopy (SEM) with Energy-Dispersive X-ray Spectroscopy (EDS) indicated four aging mechanisms. Both the new and used catalyst monoliths performed at least 95% NOX reduction in the fast reaction at all temperatures tested. Despite the similar NOX reduction performance, the used catalyst monolith exhibited lower NO oxidation performance, increased NH3 oxidation, and a lower quantity of adsorbed NH3 compared to the new catalyst monolith. Dealumination is likely the primary cause of the used catalyst monolith's lower NOX reduction performance with promoter metal deactivation, poisoning by sulfur and phosphorous, and mechanical failure of the catalyst coating on the monolith also contributing to the decreased performance. The results do not find evidence of carbon coking. This investigation into catalyst aging mechanisms confirms the efficacy of the commercial SCR catalyst monolith over long time periods.

Urea-SCR Technology for deNOx After Treatment of Diesel Exhausts presents a complete overview of the selective catalytic reduction of NOx by ammonia/urea. The book starts with an illustration of the technology in the framework of the current context (legislation, market, system configurations), covers the fundamental aspects of the SCR process (catalysts, chemistry, mechanism, kinetics) and analyzes its application to useful topics such as modeling of full scale monolith catalysts, control aspects, ammonia injections systems and integration with other devices for combined removal of pollutants.

The First International Nitrogen Conference provided an opportunity for researchers and decision-makers to exchange information on environmental pollution by nitrogen compounds on three scales: global, continental/regional and local. The main topics were air, ground water and surface water pollution; emission sources, atmospheric chemistry, deposition processes and effects; disturbance of nitrogen cycles, critical loads and levels; assessments, policy development and evaluation; target groups and abatement techniques; and new approaches leading to an integrated abatement strategy.The peer-reviewed papers from the Conference presented in this volume will provide readers with a comprehensive review of the transport, deposition and impact on ecosystems of nitrogen.