Investigation of Aging Mechanisms in Lean NOx Traps

Investigation of Aging Mechanisms in Lean NOx Traps

Author:

Publisher:

Published: 2010

Total Pages:

ISBN-13:

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Lean NO(subscript x) traps (LNTs) represent a promising technology for the abatement of NO(subscript x) under lean conditions. Although LNTs are starting to find commercial application, the issue of catalyst durability remains problematic. LNT susceptibility to sulfur poisoning is the single most important factor determining effective catalyst lifetime. The NO(subscript x) storage element of the catalyst has a greater affinity for SO3 than it does for NO2, and the resulting sulfate is more stable than the stored nitrate. Although this sulfate can be removed from the catalyst by means of high temperature treatment under rich conditions, the required conditions give rise to deactivation mechanisms such as precious metal sintering, total surface area loss, and solid state reactions between the various oxides present. The principle objective of this project was to improve understanding of the mechanisms of lean NO(subscript x) trap aging, and to understand the effect of washcoat composition on catalyst aging characteristics. The approach utilized involved detailed characterization of model catalysts prior to and after aging, in tandem with measurement of catalyst performance in NO(subscript x) storage and reduction. In this manner, NO(subscript x) storage and reduction characteristics were correlated with the evolution of catalyst physico-chemical properties upon aging. Rather than using poorly characterized proprietary catalysts, or simple model catalysts of the Pt/BaO/Al2O3 type (representing the first generation of LNTs), Pt/Rh/BaO/Al2O3 catalysts were employed which also incorporated CeO2 or CeO2-ZrO2, representing a model system which more accurately reflects current LNT formulations. Catalysts were prepared in which the concentration of each of the main components was systematically varied: Pt (50, 75 or 100 g/ft3), Rh (10 or 20 g/ft3), BaO (15, 30 or 45 g/L), and either CeO2 (0, 50 or 100 g/L) or CeO2-ZrO2 (0, 50 or 100 g/L). A high surface area La-stabilized alumina was used to support the BaO phase. Catalysts were obtained by washcoating onto standard cordierite substrates, the total washcoat loading being set at 260 g/L. La-stabilized alumina was used as the balance. Subsequent to de-greening, the NO(subscript x) storage and reduction characteristics of the catalysts were evaluated on a bench reactor, after which the catalysts were aged on a bench reactor to the equivalent of ca. 75,000 miles of road aging using a published accelerated aging protocol. The aged catalysts were then subjected to the same evaluation proecdure used for the de-greened catalysts. In addition to the use of standard physico-chemical analytical techniques for studying the fresh and aged model catalysts, use was made of advanced analytical tools for characterizing their NO(subscript x) storage/reduction and sulfation/desulfation characteristics, such as Spatially resolved capillary-inlet Mass Spectrometry (SpaciMS) and in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS).


NOx Trap Catalysts and Technologies

NOx Trap Catalysts and Technologies

Author: Luca Lietti

Publisher: Royal Society of Chemistry

Published: 2018-06-13

Total Pages: 434

ISBN-13: 1788014758

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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.


Effect of Length on the Performance of Lean NO[subscriptx] Traps

Effect of Length on the Performance of Lean NO[subscriptx] Traps

Author:

Publisher:

Published: 2007

Total Pages: 136

ISBN-13:

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The effect of monolith length on the NO[subscriptx] performance of two different Lean NO[subscriptx] Traps has been investigated using a bench flow reactor (BFR). The washcoat composition of one of the catalysts consists of Pt/K/[gamma]-Al2O3; the major components of the other catalyst include Pt, Pd, Rh, barium, ceria and zirconia supported on [gamma]-alumina washcoat. Samples of 2.22-cm in diameter and length of 2.54, 5.08 and 7.62-cm within each LNT were evaluated with long and short-cycle experiments at a fixed gas hourly space velocity, and results were compared between samples of different lengths. No significant difference in performance was observed in long and short-cycle experiments with full regeneration. On a contrary, significant difference was observed in short-cycle experiments with partial regeneration: the longer the sample the better the performance. The intra-catalyst concentration of H2 measured at different axial locations in short-cycle experiments indicated higher H2 consumption in shorter samples. A series of experiments was carried out to ascertain different mechanisms of H2 consumption, and results indicated different degrees of lean and rich front back-mixing for samples of different sizes. Higher back-mixing in shorter samples resulted in a higher H2 loss via its oxidation by O2 and lesser H2 availability for reducing stored NO[subscriptx], which in turn affected catalyst's performance when regeneration was limited by amount of H2 available.


Emissions Control Catalysis

Emissions Control Catalysis

Author: Ioannis V. Yentekakis

Publisher: MDPI

Published: 2020-06-18

Total Pages: 448

ISBN-13: 3039360361

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The important advances achieved over the past years in all technological directions (industry, energy, and health) contributing to human well-being are unfortunately, in many cases, accompanied by a threat to the environment, with photochemical smog, stratospheric ozone depletion, acid rain, global warming, and finally climate change being the most well-known major issues. These are the results of a variety of pollutants emitted through these human activities. The indications show that we are already at a tipping point that might lead to non-linear and sudden environmental change on a global scale. Aiming to tackle these adverse effects in an attempt to mitigate any damage that has already occurred and to ensure that we are heading toward a cleaner (green) and sustainable future, scientists around the world are developing tools and techniques to understand, monitor, protect, and improve the environment. Emissions control catalysis is continuously advancing, providing novel, multifunctional, and optimally promoted using a variety of methods, nano-structured catalytic materials, and strategies (e.g., energy chemicals recycling, cyclic economy) that enable us to effectively control emissions, either of mobile or stationary sources, improving the quality of air (outdoor and indoor) and water and the energy economy. Representative cases include the abatement and/or recycling of CO2, CO, NOx, N2O, NH3, CH4, higher hydrocarbons, volatile organic compounds (VOCs), particulate matter, and specific industrial emissions (e.g., SOx, H2S, dioxins aromatics, and biogas). The “Emissions Control Catalysis” Special Issue has succeeded in collecting 22 high-quality contributions, included in this MDPI open access book, covering recent research progress in a variety of fields relevant to the above topics and/or applications, mainly on: (i) NOx catalytic reduction from cars (i.e., TWC) and industry (SCR) emissions; (ii) CO, CH4, and other hydrocarbons removal, and (iii) CO2 capture/recirculation combining emissions control with added-value chemicals production.


Past and Present in DeNOx Catalysis: From Molecular Modelling to Chemical Engineering

Past and Present in DeNOx Catalysis: From Molecular Modelling to Chemical Engineering

Author: Pascal Granger

Publisher: Elsevier

Published: 2007-12-15

Total Pages: 419

ISBN-13: 0080554059

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This book offers an overview of the state of the art in the field of DeNOx catalysis in order to focus novel orientations, new technological developments, from laboratory to industrial scale. A particular attention has been paid towards the implementation of catalytic processes for minimising NOx emissions either from stationary or mobile sources under lean condition to meet future standard regulations of NOx emissions. In the first part of this book, critical aspects reported in the literature which usually make difficult the achievement of efficient catalytic technologies in those conditions are summarised and analysed in order two separate new perspectives. The second part deals with fundamental aspects at molecular level. A better understanding of the reactions involved under unsteady-state conditions is probably a pre-requisite step for improving the performances of the actual processes or developing original ones. The development of powerful in situ spectroscopic techniques is of fundamental interest for kinetic modelling. Correlations between spectroscopic and kinetic data with those obtained from theoretical calculations are reported. Some illustrations emphasise the fact that these comparisons may help in determining the nature of the catalytic active sites and building predictive tools for simulations under running conditions. The latter part of this book will be illustrated by different practical approaches covering various aspects related to the catalysts preparation and the development of alternative technologies which include industrial considerations. - New technological developments for investigating catalytic reactions in transient conditions (in situ and operando spectroscopic techniques) - Concerted approaches in DeNOx catalysis - How academic aspects (kinetic, in situ spectroscopic measurements) can provide useful information for practical applications - Comparison of different approaches provided by academic and industrial partners


Handbook of Clean Energy Systems, 6 Volume Set

Handbook of Clean Energy Systems, 6 Volume Set

Author: Jinyue Yan

Publisher: John Wiley & Sons

Published: 2015-06-22

Total Pages: 4038

ISBN-13: 1118388585

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The Handbook of Clean Energy Systems brings together an international team of experts to present a comprehensive overview of the latest research, developments and practical applications throughout all areas of clean energy systems. Consolidating information which is currently scattered across a wide variety of literature sources, the handbook covers a broad range of topics in this interdisciplinary research field including both fossil and renewable energy systems. The development of intelligent energy systems for efficient energy processes and mitigation technologies for the reduction of environmental pollutants is explored in depth, and environmental, social and economic impacts are also addressed. Topics covered include: Volume 1 - Renewable Energy: Biomass resources and biofuel production; Bioenergy Utilization; Solar Energy; Wind Energy; Geothermal Energy; Tidal Energy. Volume 2 - Clean Energy Conversion Technologies: Steam/Vapor Power Generation; Gas Turbines Power Generation; Reciprocating Engines; Fuel Cells; Cogeneration and Polygeneration. Volume 3 - Mitigation Technologies: Carbon Capture; Negative Emissions System; Carbon Transportation; Carbon Storage; Emission Mitigation Technologies; Efficiency Improvements and Waste Management; Waste to Energy. Volume 4 - Intelligent Energy Systems: Future Electricity Markets; Diagnostic and Control of Energy Systems; New Electric Transmission Systems; Smart Grid and Modern Electrical Systems; Energy Efficiency of Municipal Energy Systems; Energy Efficiency of Industrial Energy Systems; Consumer Behaviors; Load Control and Management; Electric Car and Hybrid Car; Energy Efficiency Improvement. Volume 5 - Energy Storage: Thermal Energy Storage; Chemical Storage; Mechanical Storage; Electrochemical Storage; Integrated Storage Systems. Volume 6 - Sustainability of Energy Systems: Sustainability Indicators, Evaluation Criteria, and Reporting; Regulation and Policy; Finance and Investment; Emission Trading; Modeling and Analysis of Energy Systems; Energy vs. Development; Low Carbon Economy; Energy Efficiencies and Emission Reduction. Key features: Comprising over 3,500 pages in 6 volumes, HCES presents a comprehensive overview of the latest research, developments and practical applications throughout all areas of clean energy systems, consolidating a wealth of information which is currently scattered across a wide variety of literature sources. In addition to renewable energy systems, HCES also covers processes for the efficient and clean conversion of traditional fuels such as coal, oil and gas, energy storage systems, mitigation technologies for the reduction of environmental pollutants, and the development of intelligent energy systems. Environmental, social and economic impacts of energy systems are also addressed in depth. Published in full colour throughout. Fully indexed with cross referencing within and between all six volumes. Edited by leading researchers from academia and industry who are internationally renowned and active in their respective fields. Published in print and online. The online version is a single publication (i.e. no updates), available for one-time purchase or through annual subscription.