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Book Experimental and Kinetic Modeling Studies of Selective Catalytic Reduction of NOx with NH3 on Fe  and Cu Zeolite Monolithic Catalysts

Download or read book Experimental and Kinetic Modeling Studies of Selective Catalytic Reduction of NOx with NH3 on Fe and Cu Zeolite Monolithic Catalysts written by Pranit Subhash Metkar and published by . This book was released on 2012 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: 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.

Book Selective Catalytic Reduction of NOx

Download or read book Selective Catalytic Reduction of NOx written by Oliver Kröcher and published by MDPI. This book was released on 2018-12-14 with total page 281 pages. Available in PDF, EPUB and Kindle. Book excerpt: This book is a printed edition of the Special Issue "Selective Catalytic Reduction of NOx" that was published in Catalysts

Book Selective Catalytic Reduction of NOX by NH3 for Diesel Exhaust Aftertreatment

Download or read book Selective Catalytic Reduction of NOX by NH3 for Diesel Exhaust Aftertreatment written by Christopher Sokolowski and published by . This book was released on 2014 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: 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.

Book Urea SCR Technology for deNOx After Treatment of Diesel Exhausts

Download or read book Urea SCR Technology for deNOx After Treatment of Diesel Exhausts written by Isabella Nova and published by Springer Science & Business Media. This book was released on 2014-03-14 with total page 715 pages. Available in PDF, EPUB and Kindle. Book excerpt: 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.

Book Nitrogen  the Confer N s

    Book Details:
  • Author : K. van der Hoek
  • Publisher : Elsevier
  • Release : 2012-12-02
  • ISBN : 0080984681
  • Pages : 813 pages

Download or read book Nitrogen the Confer N s written by K. van der Hoek and published by Elsevier. This book was released on 2012-12-02 with total page 813 pages. Available in PDF, EPUB and Kindle. Book excerpt: 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.

Book New and Future Developments in Catalysis

Download or read book New and Future Developments in Catalysis written by Zdenek Sobalik and published by Elsevier Inc. Chapters. This book was released on 2013-07-17 with total page 68 pages. Available in PDF, EPUB and Kindle. Book excerpt:

Book Studies of Platinum Dispersion and Catalyst Architecture for Lean NOx Reduction

Download or read book Studies of Platinum Dispersion and Catalyst Architecture for Lean NOx Reduction written by Bijesh Man Shakya and published by . This book was released on 2013 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: The combination of NOx storage and reduction (NSR) and selective catalytic reduction (SCR) catalyst is a promising technology for the reduction of NOx emission from the exhaust of lean-burn or diesel engine vehicles. In the combined NSR/SCR system, NH3 generated in LNT during the rich phase is utilized in the SCR for additional NOx conversion. Therefore, the performance of the combined NSR/SCR depends strongly on the NH3 generating function of the NSR catalyst. Earlier studies show that lower Pt dispersion NSR catalysts give higher selectivity to NH3 making them ideal candidates for this particular application. In the first part of the work, we performed experiments on lower Pt dispersion catalysts to gain insights on the mechanistic effects of Pt dispersion on NOx conversion and selectivity. We also developed an improved crystallite-scale model of NSR that explicitly accounts for the crystallite scale gradients of the stored NOx. The calibrated model is able to capture the effects of Pt dispersion, rich phase duration and overall cycle time on cycle-averaged conversion and selectivity trends. In the second part, we carried out a simulation study of dual-layer NSR+SCR monolithic catalyst using (1+1)-D model of catalytic monolith with individually-calibrated global kinetic models. Simulations show that multiple combinations of catalyst loading can attain a given NOx conversion and N2 selectivity, and that there exists a loading of SCR washcoat for a given NSR catalyst for which the NOx conversion is maximum. Simulations of the dual-brick monolith are also performed to analyze the effects of catalyst architecture. Under identical conditions, the simulations show that dual-layer catalyst outperforms the dual-brick largely because of the better utilization of generated NH3. Finally, we performed an optimization study to identify optimal loading and configuration of combined Fe+Cu zeolite catalyst that gives overall high NOx removal efficiency over a broad range of temperature. Simulations suggest that the brick configuration in which Fe- brick is followed by Cu- catalyst is slightly better than dual-layer in which Fe- is coated on top of Cu- architecture. This is attributed to the diffusional limitations in the washcoat that is more pronounced in the dual-layer catalysts.

Book Selective Catalytic Reduction of NOx

Download or read book Selective Catalytic Reduction of NOx written by Oliver Kröcher and published by . This book was released on 2018 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: The most efficient process to reduce NOx emissions from lean exhaust gases, selective catalytic reduction (SCR) with ammonia, has undergone tremendous development over the past decades. Originally only applied in stationary power plants and industrial installations, SCR systems are now installed in millions of mobile diesel engines, ranging from off-road machineries, to heavy-duty and light-duty trucks and passenger cars, to locomotives and ships. All of these applications involve specific challenges due to tighter emission limits, new internal combustion engine technologies, or alternative fuels. Three review articles and 14 research articles in this book describe recent results and research trends of various aspects of the SCR process. Reaction engineering aspects, such as the proper dosage of ammonia or urea, respectively, are as important as further developments of the different SCR catalysts, by deepening the understanding of their functionality or by systematic improvements of their properties, such as low-temperature activity, selectivity, or poisoning-resistance. Another covered aspect is cost reduction through the use of cheaper base materials for the production is active and stable SCR catalysts. Finally, research efforts are reported to develop SCR processes with different reducing agents, which would open doors to new applications in the future. The range of topics addressed in this book will stimulate the reader's interest as well as provide a valuable source of information for researchers in academia and industry.

Book Selective Catalytic Reduction  SCR  of Nitric Oxide with Ammonia Using Cu ZSM 5 and Va based Honeycomb Monolith Catalysts

Download or read book Selective Catalytic Reduction SCR of Nitric Oxide with Ammonia Using Cu ZSM 5 and Va based Honeycomb Monolith Catalysts written by Saurabh Gupta and published by . This book was released on 2003 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: In this work, the steady-state performance of zeolite-based (Cu-ZSM-5) and vanadium-based honeycomb monolith catalysts was investigated in the selective catalytic reduction process (SCR) for NO removal using NH3. The aim was to delineate the effect of various parameters including pretreatment of the catalyst sample with H2, NH3-to-NO ratio, inlet oxygen concentration, and space velocity. The concentrations of the species (e.g. NO, NH3, and others) were determined using a Fourier Transform Infrared (FTIR) spectrometer. The temperature was varied from ambient (25 C) to 500 C. The investigation showed that all of the above parameters (except pre-treatment with H2) significantly affected the peak NO reduction, the temperature at which peak NO reduction occurred, and residual ammonia left at higher temperatures (also known as 'NH3 slip'). Depending upon the particular values of the parameters, a peak NO reduction of around 90% was obtained for both the catalysts. However, an accompanied generation of N2O and NO2 species was observed as well, being much higher for the vanadium-based catalyst than for the Cu-ZSM-5 catalyst. For both catalysts, the peak NO reduction decreased with an increase in space velocity, and did not change significantly with an increase in oxygen concentration. The temperatures at which peak NO reduction and complete NH3 removal occurred increased with an increase in space velocity but decreased with an increase in oxygen concentration. The presence of more ammonia at the inlet (i.e. higher NH3-to-NO ratio) improved the peak NO reduction but simultaneously resulted in an increase in residual ammonia. Pretreatment of the catalyst sample with H2 (performed only for the Cu-ZSM-5 catalyst) did not produce any perceivable difference in any of the results for the conditions of these experiments.

Book Selective Catalytic Reduction of NOx by NH3  NH3 SCR  in Small Pore Cu exchanged Chabazite  CHA  Catalysts

Download or read book Selective Catalytic Reduction of NOx by NH3 NH3 SCR in Small Pore Cu exchanged Chabazite CHA Catalysts written by Di Wang and published by . This book was released on 2014 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Nitrogen oxides, NOx (NO+NO2), are considered significant air pollutants. Selective catalytic reduction of NOx with NH3 (NH3-SCR) is a leading technology candidate for NOx emissions control for diesel engine vehicles. Recently, the Cu-exchanged chabazite framework type zeolite with small pores, such as SAPO-34 and SSZ-13, has received a great deal of attention due to exceptional hydrothermal durability and enhanced SCR activity. I have carried out a systematic study over both Cu-SAPO-34 and Cu-SSZ-13 catalysts to elucidate the reaction mechanisms, acid properties, Cu structures, active centers and deactivation modes. First, the intrinsic mechanism of the SCR reaction over a Cu-exchanged SAPO-34 catalyst at low temperature was studied by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), coupled with a mass spectrometer to measure inlet and outlet gas concentrations. The evolution of the surface intermediates, as well as the reactivity of NH3 with surface NOx species and NOx with surface NH3 species, was evaluated. Second, a series of SAPO-34 catalysts with various Cu loadings (ranging 0.7-3.0 wt%) was prepared by a solid state ion exchange method (SSIE). The acid properties as well as the Cu structures were characterized by XRD, NH3-TPD, UV-vis, DRIFTS and H2-TPR. Third, a SSIE method was developed to synthesize Cu-SSZ-13 catalysts with excellent NH3-SCR performance and durable hydrothermal stability. After the SSIE process, the SSZ framework structure and surface area was maintained. DRIFTS and NH3-TPD experiments provide evidence that Cu ions were successfully exchanged with Brønsted acid protons in the pores. Fourth, the hydrothermal stability of Cu-SAPO-34 and Cu-SSZ-13 was studied. Their different evolutions of zeolite framework, acidity and Cu structure during the hydrothermal aging were probed by XRD, DRIFTS and NH3-TPD. The results suggest that Cu-SAPO-34 is more resistant to hydrothermal aging in comparison to Cu-SSZ-13. Last, the SO2 poisoning effect over Cu-SAPO-34 catalyst was investigated by using in-situ DRIFTS combined with temperature programmed desorption (TPD) experiments. It was found that the low temperature deactivation mechanism involved the formation of ammonium sulfate species as well as the competitive adsorption SO2 with NOx.

Book Computational Insights Into the Mechanism of the Selective Catalytic Reduction of NOx  Fe  Versus Cu Exchanged Zeolite Catalysts

Download or read book Computational Insights Into the Mechanism of the Selective Catalytic Reduction of NOx Fe Versus Cu Exchanged Zeolite Catalysts written by Julian Rudolph and published by . This book was released on 2019 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: We computationally investigate the mechanism of the reduction half-cycle of the selective catalytic reduction of nitrogen oxides with ammonia. We compare both Fe- and Cu-exchanged zeolite catalysts and aim at exploring all accessible reaction pathways. From our calculations, a comprehensive picture emerges that unifies several previous mechanistic proposals. We find that both for Fe and for Cu catalysts different reaction pathways are feasible but some of the possible reaction pathways differ in these two cases. Our computational results provide a basis for the interpretation of in situ spectroscopic investigations that can possibly distinguish the different mechanistic pathways.

Book Selective catalytic reduction of NOx with NH3

Download or read book Selective catalytic reduction of NOx with NH3 written by Hanna Sjövall and published by . This book was released on 2009 with total page 68 pages. Available in PDF, EPUB and Kindle. Book excerpt:

Book Catalyst and Method for Reduction of Nitrogen Oxides

Download or read book Catalyst and Method for Reduction of Nitrogen Oxides written by and published by . This book was released on 2008 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub. 2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub. 2O was not detected (detection limit: 0.6 percent N.sub. 2O).

Book Characterization and Performances of Nanosized Bi metallic Fe based Zeolite Catalysts During Selective Catalytic Reduction  SCR  of NO by NH3

Download or read book Characterization and Performances of Nanosized Bi metallic Fe based Zeolite Catalysts During Selective Catalytic Reduction SCR of NO by NH3 written by 莎亞達 and published by . This book was released on 2013 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt:

Book NOx Trap Catalysts and Technologies

Download or read book NOx Trap Catalysts and Technologies written by Luca Lietti and published by Royal Society of Chemistry. This book was released on 2018-06-13 with total page 434 pages. Available in PDF, EPUB and Kindle. Book excerpt: Vehicle exhaust emissions, particularly from diesel cars, are considered to be a significant problem for the environment and human health. Lean NOx Trap (LNT) or NOx Storage/Reduction (NSR) technology is one of the current techniques used in the abatement of NOx from lean exhausts. Researchers are constantly searching for new inexpensive catalysts with high efficiency at low temperatures and negligible fuel penalties, to meet the challenges of this field. This book will be the first to comprehensively present the current research on this important area. Covering the technology used, from its development in the early 1990s up to the current state-of-the-art technologies and new legislation. Beginning with the fundamental aspects of the process, the discussion will cover the real application standard through to the detailed modelling of full scale catalysts. Scientists, academic and industrial researchers, engineers working in the automotive sector and technicians working on emission control will find this book an invaluable resource.