Selective Catalytic Reduction (SCR) of Nitric Oxide (NO) with Ammonia Over Vanadia-based and Pillared Interlayer Clay-based Catalysts PDF Download
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Author: Hyuk Jin Oh Publisher: ISBN: Category : Languages : en Pages :
Book Description
The selective catalytic reduction (SCR) of nitric oxide (NO) with ammonia over vanadia-based (V2O5-WO3/TiO2) and pillared interlayer clay-based (V2O5/Ti-PILC) monolithic honeycomb catalysts using a laboratory laminar-flow reactor was investigated. The experiments used a number of gas compositions to simulate different combustion gases. A Fourier transform infrared (FTIR) spectrometer was used to determine the concentrations of the product species. The major products were nitric oxide (NO), ammonia (NH3), nitrous oxide (N2O), and nitrogen dioxide (NO2). The aim was to delineate the effect of various parameters including reaction temperature, oxygen concentration, NH3-to-NO ratio, space velocity, heating area, catalyst arrangement, and vanadium coating on the removal of nitric oxide. The investigation showed that the change of the parameters significantly affected the removals of NO and NH3 species, the residual NH3 concentration (or NH3 slip), the temperature of the maximum NO reduction, and the temperature of complete NH3 conversion. The reaction temperature was increased from the ambient temperature (25°C) to 450°C. For both catalysts, high NO and NH3 removals were obtained in the presence of a small amount of oxygen, but no significant influence was observed from 0.1 to 3.0% O2. An increase in NH3-to-NO ratio increased NO reduction but decreased NH3 conversions. For V2O5-WO3/TiO2, the decrease of space velocity increased NO and NH3 removals and broadened the active temperature window (based on NO> 88% and NH3> 87%) about 50°C. An increase in heating area decreased the reaction temperature of the maximum NO reduction from 350 to 300 ʻC, and caused the active reaction temperature window (between 250 and 400 ʻC) to shift toward 50 ʻC lower reaction temperatures (between 200 and 350°C). The change of catalyst arrangements resulted slight improvement for NO and NH3 removals, therefore, the change might contribute to more gas removals. The catalyst with extra vanadium coating showed higher NO reductions and NH3 conversions than the catalyst without the extra vanadium coating.
Author: Hyuk Jin Oh Publisher: ISBN: Category : Languages : en Pages :
Book Description
The selective catalytic reduction (SCR) of nitric oxide (NO) with ammonia over vanadia-based (V2O5-WO3/TiO2) and pillared interlayer clay-based (V2O5/Ti-PILC) monolithic honeycomb catalysts using a laboratory laminar-flow reactor was investigated. The experiments used a number of gas compositions to simulate different combustion gases. A Fourier transform infrared (FTIR) spectrometer was used to determine the concentrations of the product species. The major products were nitric oxide (NO), ammonia (NH3), nitrous oxide (N2O), and nitrogen dioxide (NO2). The aim was to delineate the effect of various parameters including reaction temperature, oxygen concentration, NH3-to-NO ratio, space velocity, heating area, catalyst arrangement, and vanadium coating on the removal of nitric oxide. The investigation showed that the change of the parameters significantly affected the removals of NO and NH3 species, the residual NH3 concentration (or NH3 slip), the temperature of the maximum NO reduction, and the temperature of complete NH3 conversion. The reaction temperature was increased from the ambient temperature (25°C) to 450°C. For both catalysts, high NO and NH3 removals were obtained in the presence of a small amount of oxygen, but no significant influence was observed from 0.1 to 3.0% O2. An increase in NH3-to-NO ratio increased NO reduction but decreased NH3 conversions. For V2O5-WO3/TiO2, the decrease of space velocity increased NO and NH3 removals and broadened the active temperature window (based on NO> 88% and NH3> 87%) about 50°C. An increase in heating area decreased the reaction temperature of the maximum NO reduction from 350 to 300 ʻC, and caused the active reaction temperature window (between 250 and 400 ʻC) to shift toward 50 ʻC lower reaction temperatures (between 200 and 350°C). The change of catalyst arrangements resulted slight improvement for NO and NH3 removals, therefore, the change might contribute to more gas removals. The catalyst with extra vanadium coating showed higher NO reductions and NH3 conversions than the catalyst without the extra vanadium coating.
Author: Giriraj Sharma Publisher: ISBN: Category : Languages : en Pages :
Book Description
In this work, the steady-state performance of zeolite-based Cu-ZSM-5, vanadium based honeycomb monolith catalysts (V), vanadium-titanium based pillared inter layered clay catalyst (V-Ti PLIC) and vanadium-titanium-tungsten-based honeycomb monolith catalysts (V-Ti-W) was investigated in the selective catalytic reduction process (SCR) for NO removal using NH3 in presence of oxygen. The objective is to obtain the expression that would predict the conversion performance of the catalysts for different values of the SCR process parameters, namely temperature, inlet oxygen concentration and inlet ammonia concentration. The NO[subscript]x emission, its formation and control methods are discussed briefly and then the fundamentals of the SCR process are described. Heat transfer based and chemical kinetics based SCR process models are discussed and widely used rate order based model are reviewed. Based on the experimental data, regression analysis was performed that gives an expression for predicting the SCR rate for the complete temperature range and the rate order with respect to inlet oxygen and ammonia concentration. The average activation energy for the SCR process was calculated and optimum operating conditions were determined for each of the catalyst. The applicable operating range for the catalyst depends on the NO conversion as well as on the ammonia slip and the N2O and NO2 emission. The regression analysis was repeated for the applicable range and an expression was obtained that can be used to estimate the catalyst performance. For the Cu-ZSM-5, the best performance was observed for 400°C, 660 ppm inlet ammonia concentration and 0.1% inlet oxygen concentration. For the V based honeycomb monolith catalyst, the best performance was observed for 300°C, 264 ppm inlet ammonia concentration and 3% inlet oxygen concentration. For the V-Ti based PLIC catalyst, the best performance was observed for 350°C, 330 ppm inlet ammonia concentration and 3% inlet oxygen concentration. For the V-Ti-W based honeycomb monolith catalyst, the best performance was observed for 300°C, 330 ppm inlet ammonia concentration and 3% inlet oxygen concentration. The conversion performance of all of these catalysts is satisfactory for the industrial application. At the operating conditions listed above, the N2O emission is less than 20 ppm and the NO2 emission is less than 10 ppm. The results were validated by comparing the findings with the similar work by other research groups. The mechanism of SCR process is discussed for each of the catalyst. The probable reactions are listed and adsorption and desorption process are studied. The various mechanisms proposed by the researchers are discussed briefly. It is concluded that V-Ti-W and Cu-ZSM-5 catalyst are very promising for SCR of NO[subscript]x. The expressions can be used to estimate the conversion performance and can be utilized for optimal design and operation. The expressions relate the SCR rate to the input parameters such as temperature and inlet oxygen and ammonia concentration hence by controlling these parameters desired NO[subscript]x reduction can be achieved with minimal cost and emission.
Author: Publisher: ISBN: Category : Languages : en Pages : 77
Book Description
The most advanced and proven technology for NO(subscript x) control for stationary sources is Selective Catalytic Reduction (SCR). In SCR, NO(subscript x) is reduced by NH3 to N2 and H2O. The commercial catalysts are based on V2O5/TiO2, and the vanadium-based catalysts are patented by the Japanese (Mitsubishi). However, there are three main advantages for the vanadium-based SCR catalyst: (a) a tendency to be poisoned in the flue gas; (b) oxidation of SO2 to SO3 by V2O5, this is a particularly severe problem due to the higher sulfur content of American coals compared with coals used in Japan (from Australia) and in Europe; (c) environmental problems involved in the disposal of the spent catalyst (due to the toxicity of vanadium). In order to overcome these problems, in addition to the undesirable dominance by the Japanese patent position, the authors have studied in this project a new type of catalyst for the SCR reaction; namely, pillared clays, which have adjustable, unique structures and acidity. Three types of catalysts were developed and tested for this reaction, i.e. Fe2O3-pillared clays, delaminated Fe2O3-pillared clays, and ion-exchanged pillared clays. The project was divided into sixteen tasks, and will be reported as such.
Author: Publisher: ISBN: Category : Languages : en Pages : 109
Book Description
Removal of NO(subscript x) (NO + NO2) from exhaust gases is a challenging subject. V2O5-based catalysts are commercial catalysts for selective catalytic reduction (SCR) with NH3 for stationary sources. However, for diesel and lean-burn gasoline engines in vehicles, hydrocarbons would be the preferred reducing agents over NH3 because of the practical problems associated with the use of NH3 (i.e., handling and slippage through the reactor). The noble-metal three-way catalysts are not effective under these conditions. The first catalyst found to be active for selective catalytic reduction of NO by hydrocarbons in the presence of excess oxygen was copper exchanged ZSM-5 and other zeolites, reported in 1990 by Iwamoto in Japan and Held et al. in Germany. Although Cu-ZSM-5 is very active and the most intensively studied catalyst, it suffers from severe deactivation in engine tests, mainly due to H2O and SO2. In this project, we found that ion-exchanged pillared clays and MCM-41 catalysts showed superior SCR activities of NO with hydrocarbon. All Cu{sup 2+}-exchanged pillared clays showed higher SCR activities than Cu-ZSM-5 reported in the literature. In particular, H2O and SO2 only slightly deactivated the SCR activity of Cu-TiO2-PILC, whereas severe deactivation was observed for Cu-ZSM-5. Moreover, Pt/MCM-41 provided the highest specific NO reduction rates as compared with other Pt doped catalysts, i.e., Pt/Al2O3, Pt/SiO2 and Pt/ZSM-5. The Pt/MCM-41 catalyst also showed a good stability in the presence of H2O and SO2.
Author: Saurabh Gupta Publisher: ISBN: Category : Languages : en Pages :
Book Description
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.
Author: Publisher: ISBN: Category : Languages : en Pages : 18
Book Description
During the past quarter, progress has been made in four tasks as summarized below: Task 1: A delaminated Fe2O3 pillared clay was synthesized and carefully characterized. The chemical composition was measured by ICP atomic emission spectrometry. The structural changes in the clay as well as the iron oxide particle sizes were characterized by X-ray diffraction techniques. Task 2: The Selective Catalytic Reduction (SCR, i.e., NO reduction with NH3) activities of the delaminated pillared clay were tested and compared with four other most active SCR catalysts: a commercial V2O5 + WO3/TiO2 catalyst, a Fe2O3-pillared clay, and two supported Fe2O3 catalysts (on Al2O3 and TiO2). The delaminated Fe2O3 pillared clay exhibited the highest SCR activities. Catalyst stability test showed that the delaminated sample was also stable. Task 3: To further increase the SCR activity of the delaminated pillared clay, Cr2O3 was doped as a promoter by incipient wetness. Task 4: Deactivation effects of SO2 and H2O on the SCR activities of the delaminated Fe2O3 pillared clay were studied, and compared with other SCR catalysts. The delaminated clay catalyst showed the least deactivation.
Author: Hyuk Jin Oh
Author: Hyuk Jin Oh
Author: Giriraj Sharma
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Author: 
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Author: Mahesh Waman Kumthekar
Author: Saurabh Gupta
Author: Hans Bosch
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Author: Yeping Cai