Author: Bijesh Man Shakya
Publisher:
ISBN:
Category : Chemical engineering
Languages : en
Pages :
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Book Description
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.
Author: Luca Lietti
Publisher: Royal Society of Chemistry
ISBN: 1788013239
Category : Science
Languages : en
Pages : 514
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Book Description
This book will be the first to comprehensively present the current research on catalysts used for NOx abatement in lean exhausts.
Author: Crystle Constantinou
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
Increases in vehicle exhaust emission regulations have led to research, development and improvements in catalytic converter technologies for gasoline-powered vehicles since the 1970s. Nowadays, there are strict regulations and standards for diesel engines as well, and one of the regulated species is nitrogen oxides (NOX). The lean NOX trap (LNT) catalyst has been studied and developed for use in lean burn (of which diesel is an example) engine exhaust as a technology to reduce NOX to N2. Typical LNT catalysts contain Pt, which catalyzes NO oxidation and NOX reduction, and an alkali or alkaline earth material for NOX storage via nitrate formation. The catalyst is operated in a cyclic mode, with one phase of the cycle under oxidizing conditions where NOX is trapped, and a second phase, which is reductant-rich relative to O2, where stored NOX is reduced to N2. A recently developed catalyst uses a perovskite material as part of the LNT formulation for the oxidation reactions thereby eliminating the need for Pt in a LNT. This catalyst does include Pd and Rh, added to accommodate hydrocarbon oxidation and NO reduction, respectively. Ba was used as the trapping component, and Ce was also part of the formulation. NO oxidation kinetics over the fully-formulated and bare perovskite material were determined, with NO, O2 and NO2 orders being at or near 1, 1 and -1, respectively for both samples. The fully-formulated sample, which contains Ba supported on the perovskite, was evaluated in terms of NOX trapping ability and NOX reduction as a function of temperature and reduction phase properties. Trapping and overall performance increased with temperature to 375°C, primarily due to improved NO oxidation, as NO2 is more readily trapped, or better diffusion of nitrates away from the initial trapping sites. At higher temperatures nitrate stability decreased, thus decreasing the trapping ability. At these higher temperatures, a more significant amount of unreduced NOX formed during the reduction phase, primarily due to nitrate instability and decomposition and the relative rates of the NOX and oxygen storage (OS) components reduction reactions. Most of the chemistry observed was similar to that observed over Pt-based LNT catalysts. However, there were some distinct differences, including a stronger nitrate diffusion resistance at low temperature and a more significant reductant-induced nitrate decomposition reaction. The perovskite-based lean NOX trap (LNT) catalyst was also evaluated after thermal aging and sulfur exposure. NO oxidation, NOX trapping ability and NOX reduction as a function of temperature and reduction phase properties were evaluated. Similar overall performance trends were seen before and after degradation, however lower performance after thermal aging and sulfur exposure were seen due to sintering effects and possible build-up of S species. Although performance results show that most of the sulfur was removed after desulfation, some sulfur remained affecting the trapping and reduction capabilities as well as the water gas shift (WGS) extent at lower temperatures. The Oxygen storage capacity (OSC) on the other hand was maintained after the catalyst was exposed to thermal aging and sulfur poisoning then desulfation, all of which suggest that the perovskite or Pd components were irreversibly poisoned to some extent.
Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 10
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Book Description
The original goal of this program was the identification and design of new noble-metal-based catalysts for the selective catalytic reduction of nitric oxide by hydrocarbons under excess oxygen (i.e., ''lean'') conditions (HC-SCR). Work conducted in the first funding cycle of this award (i.e., 1997-2000) was successful in allowing us to develop an understanding of the fundamental surface chemistry taking place during the adsorption and reaction of nitrogen oxides and propylene on the surface of supported noble metal catalysts. Both experimental results collected in our own group as well as molecular simulation results published by Professor Neurock suggested that in order to improve the performance of the Pt catalysts--in terms of the nitrogen selectivity and the temperature window of operation-- it was necessary to introduce a second metal. However, synthesizing such catalysts with the metals of interest (i.e., Pt-Au, Pt-Ru, Pt-Rh, etc.) with some degree of control of the structure and composition of the resulting supported metal particles is in itself a research challenge. Consequently, the bulk of our efforts during the second funding cycle of this award (covered by this report) was shifted to the use of organometallic cluster precursors for the synthesis on novel bimetallic catalysts. During this time we have also continued to maintain an interest in NOx abatement, but have redirected our efforts from the HC-SCR process to the more promising from a commercial standpoint NOx Storage Reduction (NSR) approach.
Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Recent developments in catalytic control of NOx are revealing the significance of NO2 as an intermediary for achieving higher NOx removal efficiencies. This paper discusses the combination of the plasma with a catalyst to improve the selective reduction of NOx under lean-burn conditions. It is shown that the main effect of the plasma is to enhance the gas-phase oxidation of NO to NO2. The reduction of NOx to N2 is then accomplished by the heterogeneous reaction of NO2 with activated hydrocarbons on the catalyst surface. By using a plasma, one can take advantage of a new class of catalysts that are potentially more durable, more active, more selective and more sulfur-tolerant compared to conventional lean-NOx catalysts. The plasma-assisted catalytic reduction process can be implemented with any type of plasma reactor and does not require a specific type of electrical power supply. It can also easily accommodate any type of catalyst support structure.
Author: ASTM International
Publisher:
ISBN:
Category : Catalysis
Languages : en
Pages : 18
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Author: Karen Susan Kabin
Publisher:
ISBN:
Category : Catalysts
Languages : en
Pages : 394
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Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 6
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Book Description
The control of NOx (NO and NO2) emissions from so-called ''lean-burn'' vehicle engines remains a challenge. In recent years, there have been a number of reports that show that a plasma device combined with a catalyst can reduce as high as 90% or more of NOx in simulated diesel and other ''lean-burn'' exhaust. In the case of propylene containing simulated diesel exhaust, the beneficial role of a plasma treatment is now thought to be due to oxidation of NO to NO2, and the formation of partially oxidized hydrocarbons that are more active for the catalytic reduction of NO2 than propylene. Thus, the overall system can be most usefully described as hydrocarbon selective catalytic reduction (SCR) enhanced by 'reforming' the exhaust with a non-thermal plasma (NTP) device. For plasma-enhanced catalysis, both zeolite- and alumina-based materials have shown high activity, albeit in somewhat different temperature ranges, when preceded by an NTP reactor. This paper will briefly describe our research efforts aimed at optimizing the catalyst materials for NTP-catalysis devices based, in part, on our continuing studies of the NTP- and catalytic-reaction mechanisms. Various alkali- and alkaline earth-cation-exchanged Y zeolites have been prepared, their material properties characterized, and they have been tested as catalytic materials for NOx reduction in laboratory NTP-catalysis reactors. Interestingly, NO2 formed in the plasma and not subsequently removed over these catalysts, will back-convert to NO, albeit to varying extents depending upon the nature of the cation. Besides this comparative reactivity, we will also discuss selected synthesis strategies for enhancing the performance of these zeolite-based catalyst materials. A particularly important result from our mechanistic studies is the observation that aldehydes, formed during the plasma treatment of simulated diesel exhaust, are the important species for the reduction of NOx to N2. Indeed, acetaldehyde has been found to be especially effective in the thermal reduction of both NO and NO2 over Ba- and Na-Y zeolite catalysts.
Author: Aline Auroux
Publisher: Springer Science & Business Media
ISBN: 3642119549
Category : Technology & Engineering
Languages : en
Pages : 569
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Book Description
The book is about calorimetry and thermal analysis methods, alone or linked to other techniques, as applied to the characterization of catalysts, supports and adsorbents, and to the study of catalytic reactions in various domains: air and wastewater treatment, clean and renewable energies, refining of hydrocarbons, green chemistry, hydrogen production and storage. The book is intended to fill the gap between the basic thermodynamic and kinetics concepts acquired by students during their academic formation, and the use of experimental techniques such as thermal analysis and calorimetry to answer practical questions. Moreover, it supplies insights into the various thermal and calorimetric methods which can be employed in studies aimed at characterizing the physico-chemical properties of solid adsorbents, supports and catalysts, and the processes related to the adsorption desorption phenomena of the reactants and/or products of catalytic reactions. The book also covers the basic concepts for physico-chemical comprehension of the relevant phenomena. Thermodynamic and kinetic aspects of the catalytic reactions can be fruitfully investigated by means of thermal analysis and calorimetric methods, in order to better understand the sequence of the elemental steps in the catalysed reaction. So the fundamental theory behind the various thermal analysis and calorimetric techniques and methods also are illustrated.
Author:
Publisher:
ISBN:
Category : Chemistry
Languages : en
Pages : 2726
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