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Sample records for nox trap catalysts

  1. Influence of Ceria on the NOx Storage/Reduction Behavior of Lean NOx Trap Catalysts

    SciTech Connect

    Ji, Yaying; Choi, Jae-Soon; Toops, Todd J; Crocker, Dr. Mark; Naseri, Mojghan

    2008-01-01

    The effect of La2O3-stabilized ceria incorporation on the functioning of fully formulated lean NOx trap catalysts was investigated. Monolithic catalysts were prepared, corresponding to loadings of 0, 50 and 100 g CeO2/L, together with a catalyst containing 100 g/L of ceria-zirconia (Ce0.7Zr0.3O2). Loadings of the other main components (Pt, Rh and BaO) were held constant. Catalyst evaluation was performed on a bench flow reactor under simulated diesel exhaust conditions, employing NOx storage/reduction cycles. NOx storage efficiency in the temperature range 150-350 C was observed to increase with ceria loading, resulting in higher NOx conversion levels. At 150 C, high rich phase NOx slip was observed for all of the catalysts, resulting from an imbalance in the rates of nitrate decomposition and NOx reduction. Optimal NOx conversion was obtained in the range 250-350 C for all the catalysts, while at 450 C high rich phase NOx slip from the most highly loaded ceria-containing catalyst resulted in lower NOx conversion than for the ceria-free formulation. N2O was the major NOx reduction product at 150 C over all of the catalysts, although low NOx conversion levels limited the N2O yield. At higher temperatures N2 was the main product of NOx reduction, although NH3 formation was also observed. Selectivity to NH3 decreased with increasing ceria loading, indicating that NH3 is consumed by reaction with stored oxygen in the rear of the catalyst.

  2. Mitigation of Sulfur Effects on a Lean NOx Trap Catalyst by Sorbate Reapplication

    SciTech Connect

    Parks, II, James E

    2007-01-01

    Lean NOx trap catalysis has demonstrated the ability to reduce NOx emissions from lean natural gas reciprocating engines by >90%. The technology operates in a cyclic fashion where NOx is trapped on the catalyst during lean operation and released and reduced to N2 under rich exhaust conditions; the rich cleansing operation of the cycle is referred to as "regeneration" since the catalyst is reactivated for more NOx trapping. Natural gas combusted over partial oxidation catalysts in the exhaust can be used to obtain the rich exhaust conditions necessary for catalyst regeneration. Thus, the lean NOx trap technology is well suited for lean natural gas engine applications. One potential limitation of the lean NOx trap technology is sulfur poisoning. Sulfur compounds directly bond to the NOx trapping sites of the catalyst and render them ineffective; over time, the sulfur poisoning leads to degradation in overall NOx reduction performance. In order to mitigate the effects of sulfur poisoning, a process has been developed to restore catalyst activity after sulfur poisoning has occurred. The process is an aqueous-based wash process that removes the poisoned sorbate component of the catalyst. A new sorbate component is reapplied after removal of the poisoned sorbate. The process is low cost and does not involve reapplication of precious metal components of the catalyst. Experiments were conducted to investigate the feasibility of the washing process on a lean 8.3-liter natural gas engine on a dynamometer platform. The catalyst was rapidly sulfur poisoned with bottled SO2 gas; then, the catalyst sorbate was washed and reapplied and performance was re-evaluated. Results show that the sorbate reapplication process is effective at restoring lost performance due to sulfur poisoning. Specific details relative to the implementation of the process for large stationary natural gas engines will be discussed.

  3. Ammonia reactions with the stored oxygen in a commercial lean NOx trap catalyst

    DOE PAGESBeta

    Bartova, Sarka; Mracek, David; Koci, Petr; Marek, Milos; Choi, Jae -Soon

    2014-10-12

    Ammonia is an important intermediate of the NOx reduction in a NOx storage and reduction catalyst (aka lean NOx trap). NH3 formed under rich conditions in the reduced front part of the catalyst is transported by convection downstream to the unregenerated (still oxidized) zone of the catalyst, where it further reacts with the stored oxygen and NOx. In this paper, the kinetics and selectivity of NH3 reactions with the stored oxygen are studied in detail with a commercial Ba-based NOx storage catalyst containing platinum group metals (PGM), Ba and Ce oxides. Furthermore, steady-state NH3 decomposition, NH3 oxidation by O2 andmore » NO, and N2O decomposition are examined in light-off experiments. Periodic lean/rich cycling is measured first with O2 and NH3, and then with NOx + O2 and NH3 to discriminate between the NH3 reactions with the stored oxygen and the stored NOx. The reaction of NH3 with the stored O2 is highly selective towards N2, however a certain amount of NOx and N2O is also formed. The formed NOx by-product is efficiently adsorbed on the NOx storage sites such that the NOx is not detected at the reactor outlet except at high temperatures. The stored NOx reacts with NH3 feed in the next rich phase, contributing to the N2O formation. Water inhibits the reactions of NH3 with the stored oxygen. On the contrary, the presence of CO2 increases the NH3 consumption. Furthermore, CO2 is able to provide additional oxygen for NH3 oxidation, forming –CO in analogy to the reverse water gas shift reaction.« less

  4. Characterization of Lean NOx Trap Catalysts with In-Cylinder Regeneration Strategies

    SciTech Connect

    Parks, II, James E; Huff, Shean P; Swartz, Matthew M; West, Brian H

    2008-01-01

    Lean NOx trap (LNT) catalysts with different formulations have been characterized on a light-duty diesel engine platform. Two in-cylinder regeneration strategies were used during the study. The reductant chemistry differed for both strategies with one strategy having high levels of CO and H2 and the other strategy having a higher hydrocarbon component. The matrix of LNT catalysts that were characterized included LNTs with various sorbate loads and varying ceria content; the sorbate was Ba. Intra-catalyst measurements of exhaust gas composition were obtained at one quarter, one half, and three quarters of the length of the catalysts to better understand the affect of formulation on performance. Exhaust analysis with FTIR allowed measurement of NH3 and thereby, a measurement of N2 selectivity for the catalysts. Although overall NOx conversion increased with increasing sorbate load, the formation of NH3 increased as well. Interestingly, the presence of ceria in the LNT allowed NH3 to be oxidized to N2 in the downstream half of the LNT, thereby greatly reducing the tailpipe NH3 level. Despite different capacities for NOx sorption, a similar pattern for NOx adsorption as a function of the length of the catalyst was observed for catalysts with 8% and 20% Ba load. Results from these engine based experiments will be discussed relative to the body of literature concerning fundamental and model LNT studies.

  5. Determination of the NOx Loading of an Automotive Lean NOx Trap by Directly Monitoring the Electrical Properties of the Catalyst Material Itself

    PubMed Central

    Fremerey, Peter; Reiß, Sebastian; Geupel, Andrea; Fischerauer, Gerhard; Moos, Ralf

    2011-01-01

    Recently, it has been shown that the degree of loading of several types of automotive exhaust aftertreatment devices can be directly monitored in situ and in a contactless way by a microwave-based method. The goal of this study was to clarify whether this method can also be applied to NOx storage and reduction catalysts (lean NOx traps) in order to obtain further knowledge about the reactions occurring in the catalyst and to compare the results with those obtained by wirebound NOx loading sensors. It is shown that both methods are able to detect the different catalyst loading states. However, the sensitivity of the microwave-based method turned out to be small compared to that previously observed for other exhaust aftertreatment devices. This may limit the practical applicability of the microwave-based NOx loading detection in lean NOx traps. PMID:22164074

  6. Determination of the NOx loading of an automotive lean NOx trap by directly monitoring the electrical properties of the catalyst material itself.

    PubMed

    Fremerey, Peter; Reiss, Sebastian; Geupel, Andrea; Fischerauer, Gerhard; Moos, Ralf

    2011-01-01

    Recently, it has been shown that the degree of loading of several types of automotive exhaust aftertreatment devices can be directly monitored in situ and in a contactless way by a microwave-based method. The goal of this study was to clarify whether this method can also be applied to NOx storage and reduction catalysts (lean NOx traps) in order to obtain further knowledge about the reactions occurring in the catalyst and to compare the results with those obtained by wirebound NOx loading sensors. It is shown that both methods are able to detect the different catalyst loading states. However, the sensitivity of the microwave-based method turned out to be small compared to that previously observed for other exhaust aftertreatment devices. This may limit the practical applicability of the microwave-based NOx loading detection in lean NOx traps. PMID:22164074

  7. Characteristics of Pt-K/MgAl2O4 lean NOx trap catalysts

    SciTech Connect

    Kim, Do Heui; Mudiyanselage, Kumudu K.; Szanyi, Janos; Zhu, Haiyang; Kwak, Ja Hun; Peden, Charles HF

    2012-04-30

    We report the various characteristics of Pt-K/MgAl{sub 2}O{sub 4} lean NOx trap (LNT) catalysts including the effect of K loading on nitrate formation/decomposition, NOx storage activity and durability. Upon the adsorption of NO{sub 2} on K/MgAl{sub 2}O{sub 4} samples, potassium nitrates formed on Mg-related sites in MgAl{sub 2}O{sub 4} support are observed, in addition to the typical two potassium nitrates (ionic and bidentate) formed also on Al{sub 2}O{sub 3} supported sample. Based on NO{sub 2} TPD and FTIR results, the Mg-bound KNO{sub 3} thermally decompose at higher temperature than Al-bound KNO{sub 3}, implying its superior thermal stability. At a potassium loading of 5wt%, the temperature of maximum NOx uptake (T{sub max}) is 300 C. Increasing the potassium loading from 5wt% to 10 wt%, the T{sub max} gradually shifted from 300 C to 450 C, indicating the dependence of T{sub max} on the potassium loading. However, increase in potassium loading above 10 wt% only gives rise to the reduction in the overall NOx storage capacity. This work also underlines the obstacles these materials have prior to their practical application (e.g., durability and sulfur poisoning/ removal). This work provides fundamental understanding of Pt-K/MgAl{sub 2}O{sub 4}-based lean NOx trap catalysts, which could be good candidates for high temperature LNT applications.

  8. NOx Storage and Reduction Properties of Model Ceria-based Lean NOx Trap Catalysts

    SciTech Connect

    Shi, Chuan; Ji, Yaying; Graham, Uschi; Jacobs, Gary; Crocker, Mark; Zhang, Zhaoshun; Wang, Yu; Toops, Todd J

    2012-01-01

    Three kinds of model ceria-containing LNT catalysts, corresponding to Pt/Ba/CeO{sub 2}, Pt/CeO{sub 2}/Al{sub 2}O{sub 3} and Pt/BaO/CeO{sub 2}/Al{sub 2}O{sub 3}, were prepared for comparison with a standard LNT catalyst of the Pt/BaO/Al{sub 2}O{sub 3} type. In these catalysts ceria functioned as a No{sub x} storage component and/or a support material. The influence of ceria on the microstructure of the catalysts was investigated, in addition to the effect on No{sub x} storage capacity, regeneration behavior and catalyst performance during lean/rich cycling. The Pt/Ba/CeO{sub 2} and Pt/BaO/CeO{sub 2}/Al{sub 2}O{sub 3} catalysts exhibited higher No{sub x} storage capacity at 200 and 300 C relative to the Pt/BaO/Al{sub 2}O{sub 3} catalyst, although the latter displayed better storage capacity at 400 C. Catalyst regeneration behavior at low temperature was also improved by the presence of ceria, as reflected by TPR measurements. These factors contributed to the superior No{sub x} storage-reduction performance exhibited by the Pt/Ba/CeO{sub 2} and Pt/BaO/CeO{sub 2}/Al{sub 2}O{sub 3} catalysts under cycling conditions in the temperature range 200-300 C. Overall, Pt/BaO/CeO{sub 2}/Al{sub 2}O{sub 3} (which displayed well balanced No{sub x} storage and regeneration behavior), showed the best performance, affording consistently high No{sub x} conversion levels in the temperature range 200-400 C under lean-rich cycling conditions.

  9. NOx storage and reduction in model lean NOx trap catalysts studied by in situ DRIFTS

    SciTech Connect

    Ji, Yaying; Toops, Todd J; Pihl, Josh A; Crocker, Mark

    2009-01-01

    NO{sub x} storage and reduction on a model Pt/BaO/Al{sub 2}O{sub 3} catalyst was studied by means of in situ DRIFTS measurements. To examine the effect of ceria addition, experiments were also conducted using Pt/BaO/Al{sub 2}O{sub 3} to which Pt/CeO{sub 2} was added as a physical mixture in a 74:26 weight ratio. For the former catalyst, DRIFT spectra acquired during NO/O{sub 2} and NO{sub 2}/O{sub 2} storage indicated the formation of nitrite at 200 C during the initial stages of adsorption, while increasing the adsorption temperature appeared to facilitate the oxidation of nitrite to nitrate. The ceria-containing catalyst afforded similar DRIFT spectra under these conditions, although the presence of cerium nitrates was observed at 200 and 300 C, consistent with NO{sub x} storage on the ceria phase. DRIFT spectra acquired during NO{sub x} reduction in CO and CO/H{sub 2} showed that Ba nitrate species remained on the surface of both catalysts at 450 C, whereas the use of H{sub 2}-only resulted in complete removal of stored NO{sub x}. The observation of Ba carbonates when CO was present suggests that the inferior reduction efficiency of CO may arise from the formation of a crust of BaCO{sub 3} on the Ba phase, which inhibits further NO{sub x} reduction. DRIFT spectra acquired during lean-rich cycling (6.5 min lean, 1.0 min rich) with CO/H{sub 2} as the rich phase reductants revealed that a significant concentration of nitrates remained on the catalysts at the end of the rich phase. This implies that a large fraction of nitrate is not decomposed during cycling and thus cannot participate in NO{sub x} abatement through storage and regeneration.

  10. NOx Storage-Reduction Characteristics of Ba-Based Lean NOx Trap Catalysts Subjected to Simulated Road Aging

    SciTech Connect

    Ji, Yaying; Fisk, Courtney; Easterling, Vencon; Graham, Uschi; Poole, Adam; Crocker, Mark; Choi, Jae-Soon; Partridge Jr, William P; Wilson, Karen

    2010-01-01

    Although Lean NO{sub x} Trap (LNT) catalyst technology has made significant strides in recent years, the issue of LNT durability remains problematic. Following on from our previous research concerning the effect of ceria addition on LNT preformance, in this study we focus on the role of ceria in ameliorating the deterioration of Ba-based LNT catalysts during aging. Indeed, we have observed that spectacular improvements in LNT durability can be achieved through the incorporation of CeO{sub 2}-ZrO{sub 2} into the LNT formulation, and, to a lesser extent, La-stabilized ceria.

  11. Effect of Ceria on the Sulfation and Desulfation Characteristics of a Model Lean NOx Trap Catalyst

    SciTech Connect

    Ji, Yaying; Toops, Todd J; Crocker, Mark

    2009-01-01

    The effect of ceria addition on the sulfation and desulfation characteristics of a model Ba-based lean NO{sub x} trap (LNT) catalyst was studied. According to DRIFTS and NO{sub x} storage capacity measurements, ceria is able to store sulfur during catalyst exposure to SO{sub 2}, thereby helping to limit sulfation of the main (Ba) NO{sub x} storage phase and maintain NO{sub x} storage capacity. Temperature programmed desulfation experiments revealed that desulfation of a model ceria-containing catalyst occurred in two stages, corresponding to sulfur elimination from the ceria phase at {approx}450 C, followed by sulfur loss from the Ba phase at {approx}650 C. Significantly, the ceria-containing catalyst displayed relatively lower sulfur evolution from the Ba phase than its non-ceria analog, confirming that the presence of ceria lessened the degree of sulfur accumulation on the Ba phase.

  12. Effect of Aging on the NOx Storage and Regeneration Characteristics of Fully Formulated Lean NOx Trap Catalysts

    SciTech Connect

    Ji, Yaying; Easterling, Vencon; Graham, Uschi; Fisk, Courtney; Crocker, Mark; Choi, Jae-Soon

    2011-01-01

    In order to elucidate the effect of washcoat composition on lean NO{sub x} trap (LNT) aging characteristics, fully formulated monolithic LNT catalysts containing varying amounts of Pt, Rh and BaO were subjected to accelerated aging on a bench reactor. Subsequent catalyst evaluation revealed that in all cases aging resulted in deterioration of the NO{sub x} conversion as a consequence of impaired NO{sub x} storage and NO{sub x} reduction functions, while increased selectivity to NH{sub 3} was observed in the temperature range 250--450 C. Elemental analysis, H{sub 2} chemisorption and TEM data revealed two main changes which account for the degradation in LNT performance. First, residual sulfur in the catalysts, associated with the Ba phase, decreased catalyst NO{sub x} storage capacity. Second, sintering of the precious metals in the washcoat occurred, resulting in decreased contact between the Pt and Ba, and hence in less efficient NO{sub x} spillover from Pt to Ba during NO{sub x} adsorption, as well as decreased rates of reductant spillover from Pt to Ba and reverse NO{sub x} spillover during catalyst regeneration. For the aged catalysts, halving the Pt loading from 100 to 50 g/ft{sup 3} was found to result in a significant decrease in overall NO{sub x} conversion, while for catalysts with the same 100 g/ft{sup 3} Pt loading, increasing the relative amount of Pt on the NO{sub x} storage components (BaO and La-stabilized CeO{sub 2}), as opposed to an Al{sub 2}O{sub 3} support material (where it was co-located with Rh), was found to be beneficial. The effect of Rh loading on aged catalyst performance was found to be marginal within the range studied (10--20 g/ft{sup 3}), as was the effect of BaO loading in the range 30--45 g/L.

  13. Effect of Ceria on the Storage and Regeneration Behavior of a Model Lean NOx Trap Catalyst

    SciTech Connect

    Ji, Yaying; Toops, Todd J; Crocker, Dr. Mark

    2007-01-01

    In this study the effect of ceria addition on the performance of a model Ba-based lean NO{sub x} trap (LNT) catalyst was examined. The presence of ceria improved NO{sub x} storage capacity in the temperature range 200-400 C under both continuous lean and lean-rich cycling conditions. Temperature-programmed experiments showed that NO{sub x} stored in the ceria-containing catalyst was thermally less stable and more reactive to reduction with both H{sub 2} and CO as reductants, albeit at the expense of additional reductant consumed by reduction of the ceria. These findings demonstrate that the incorporation of ceria in LNTs not only improves NO{sub x} storage efficiency but also positively impacts LNT regeneration behavior.

  14. New operation strategy for driving the selectivity of NOx reduction to N2, NH3 or N2O during lean/rich cycling of a lean NOx trap catalyst

    DOE PAGESBeta

    Mráček, David; Koci, Petr; Choi, Jae -Soon; Partridge, Jr., William P.

    2015-09-08

    Periodical regeneration of NOx storage catalyst (also known as lean NOx trap) by short rich pulses of CO, H2 and hydrocarbons is necessary for the reduction of nitrogen oxides adsorbed on the catalyst surface. Ideally, the stored NOx is converted into N2, but N2O and NH3 by-products can be formed as well, particularly at low-intermediate temperatures. The N2 and N2O products are formed concurrently in two peaks. The primary peaks appear immediately after the rich-phase inception, and tail off with the breakthrough of the reductant front accompanied by NH3 product. In addition, the secondary N2 and N2O peaks then appearmore » at the rich-to-lean transition as a result of reactions between surface-deposited reductants/intermediates (CO, HC, NH3, — NCO) and residual stored NOx under increasingly lean conditions.« less

  15. Effects of Potassium loading and thermal aging on K/Pt/Al2O3 high-temperature lean NOx trap catalysts

    SciTech Connect

    Luo, Jinyong; Gao, Feng; Kim, Do Heui; Peden, Charles HF

    2014-03-31

    The effects of K loading and thermal aging on the structural properties and high temperature performance of Pt/K/Al2O3 lean NOx trap (LNT) catalysts were investigated using in situ X-ray diffraction (XRD), temperature-programmed decomposition/desorption of NOx (NOx-TPD), transmission electron microscopy (TEM), NO oxidation and NOx storage tests. In situ XRD results demonstrate that KNO3 becomes extremely mobile on the Al2O3 surface, and experiences complex transformations between orthorhombic and rhombohedral structures, accompanied by sintering, melting and thermal decomposition upon heating. NOx storage results show an optimum K loading around 10% for the best performance at high temperatures. At lower K loadings where the majority of KNO3 stays as a surface layer, the strong interaction between KNO3 and Al2O3 promotes KNO3 decomposition and deteriorates high-temperature performance. At K loadings higher than 10%, the performance drop is not caused by NOx diffusion limitations as for the case of barium-based LNTs, but rather from the blocking of Pt sites by K species, which adversely affects NO oxidation. Thermal aging at 800 ºC severely deactivates the Pt/K/Al2O3 catalysts due to Pt sintering. However, in the presence of potassium, some Pt remains in a dispersed and oxidized form. These Pt species interact strongly with K and, therefore, do not sinter. After a reduction treatment, these Pt species remain finely dispersed, contributing to a partial recovery of NOx storage performance.

  16. Effect of sulfur loading on the desulfation chemistry of a commercial lean NOx trap catalyst

    SciTech Connect

    Kim, Do Heui; Yezerets, Aleksey; Li, Junhui; Currier, Neal; Chen, Haiying; Hess, Howard ..; Engelhard, Mark H.; Muntean, George G.; Peden, Charles HF

    2012-12-15

    We investigate the effects of initial sulfur loadings on the desulfation chemistry and the subsequent final activity of a commercial LNT catalyst. Identical total amounts of SO2 are applied to the samples, albeit with the frequency of desulfation varied. The results indicate that performance is better with less frequent desulfations. The greater the amount of sulfur deposited before desulfation, the more amount of SO2 evolution before H2S is observed during desulfation, which can be explained by two sequential reactions; initial conversion of sulfate to SO2, followed by the reduction of SO2 to H2S. After completing all sulfation/desulfation steps, the sample with only a single desulfation results in a fairly uniform sulfur distribution along the z-axis inside of the monolith. We expect that the results obtained in this study will provide useful information for optimizing regeneration strategies in vehicles that utilize the LNT technology.

  17. Carbonates-based noble metal-free lean NOx trap catalysts MOx-K2CO3/K2Ti8O17 (M = Ce, Fe, Cu, Co) with superior catalytic performance

    NASA Astrophysics Data System (ADS)

    Zhang, Yuxia; You, Rui; Liu, Dongsheng; Liu, Cheng; Li, Xingang; Tian, Ye; Jiang, Zheng; Zhang, Shuo; Huang, Yuying; Zha, Yuqing; Meng, Ming

    2015-12-01

    A series of base metal-based lean NOx trap (LNT) catalysts MOx-K2CO3/K2Ti8O17 (M = Ce, Fe, Cu, Co) were synthesized by successive impregnations and employed for the storage and reduction of NOx in the emissions of lean-burn engines at 350 °C. The XRD and XANES/EXAFS results reveal that the active phases in the corresponding catalysts exist as CeO2, Fe2O3, CuO and Co3O4, respectively. Among all the catalysts, CoOx-K2CO3/K2Ti8O17 exhibits the best performance, which cannot only trap the NOx quickly and completely at lean condition, giving the highest storage capacity (3.32 mmol/g) reported so far, but also reduce the NOx at rich condition, showing a NOx reduction percentage as high as 99.0%. Meanwhile, this catalyst displays an ultralow NOx to N2O selectivity (0.3%) during NOx reduction. The excellent performance of CoOx-K2CO3/K2Ti8O17 results from its largest amount of surface active oxygen species as revealed by XPS, O2-TPD and NO-TPD. HRTEM, FT-IR and CO2-TPD results illustrate that several kinds of K species such as sbnd OK groups, K2O, surface carbonates and bulk or bulk-like carbonates coexist in the catalysts. Based upon the in situ DRIFTS results, the participation of K2CO3 in NOx storage is confirmed, and the predominant NOx storage species is revealed as bidentate nitrites formed via multiple kinetic pathways. The low cost and high catalytic performance of the CoOx-based LNT catalyst make it most promising for the substitution of noble metal-based LNT catalysts.

  18. Enhanced high temperature performance of MgAl2O4-supported Pt-BaO lean NOx trap catalysts

    SciTech Connect

    Kwak, Ja Hun; Kim, Do Heui; Szanyi, Janos; Cho, Sung June; Peden, Charles HF

    2012-03-05

    The structural and chemical characteristics of Pt/BaO lean-NO{sub x} trap (LNT) catalysts supported on {gamma}-Al{sub 2}O{sub 3} and MgAl{sub 2}O{sub 4} are compared in this study. The Pt-BaO/MgAl{sub 2}O{sub 4} sample shows relatively low NO{sub x} uptake at temperatures below 300 C, and the temperature of maximum NO{sub x} uptake (T{sub max}) is shifted to 350 C in comparison to that of Pt-BaO/Al{sub 2}O{sub 3} (T{sub max} {approx}250 C). More importantly, the NO{sub x} uptake over the MgAl{sub 2}O{sub 4}-supported catalyst at 350 C is twice that of the alumina-based one. The shift toward the higher temperature NO{sub x} uptake is explained by the larger interfacial area between Pt and BaO, due to smaller Pt clusters as evidenced by TEM and Pt L3 EXAFS. In situ TR-XRD results demonstrate that the formation of a BaAl{sub 2}O{sub 4} phase in the BaO/MgAl{sub 2}O{sub 4} LNT catalyst occurs at a temperature about 100 C higher than on BaO/Al{sub 2}O{sub 3}, which may also represent a beneficial attribute of the BaO/MgAl{sub 2}O{sub 4} LNT with respect to catalyst stability.

  19. NOx Reduction with Natural Gas for Lean Large-Bore Engine Applications Using Lean NOx Trap Aftertreatment

    SciTech Connect

    Parks, JE

    2005-02-11

    Large-bore natural gas engines are used for distributed energy and gas compression since natural gas fuel offers a convenient and reliable fuel source via the natural gas pipeline and distribution infrastructure. Lean engines enable better fuel efficiency and lower operating costs; however, NOx emissions from lean engines are difficult to control. Technologies that reduce NOx in lean exhaust are desired to enable broader use of efficient lean engines. Lean NOx trap catalysts have demonstrated greater than 90% NOx reduction in lean exhaust from engines operating with gasoline, diesel, and natural gas fuels. In addition to the clean nature of the technology, lean NOx traps reduce NOx with the fuel source of the engine thereby eliminating the requirement for storage and handling of secondary fuels or reducing agents. A study of lean NOx trap catalysts for lean natural gas engines is presented here. Testing was performed on a Cummins C8.3G (CG-280) engine on a motor dynamometer. Lean NOx trap catalysts were tested for NOx reduction performance under various engine operating conditions, and the utilization of natural gas as the reductant fuel source was characterized. Engine test results show that temperature greatly affects the catalytic processes involved, specifically methane oxidation and NOx storage on the lean NOx trap. Additional studies on a bench flow reactor demonstrate the effect of precious metal loading (a primary cost factor) on lean NOx trap performance at different temperatures. Results and issues related to the potential of the lean NOx trap technology for large-bore engine applications will be discussed.

  20. THE EFFECT OF SULFUR ON METHANE PARTIAL OXIDATION AND REFORMING PROCESSES FOR LEAN NOX TRAP CATALYSIS

    SciTech Connect

    Parks, II, James E; Ponnusamy, Senthil

    2006-01-01

    Lean NOx trap catalysis has demonstrated the ability to reduce NOx emissions from lean natural gas reciprocating engines by >90%. The technology operates in a cyclic fashion where NOx is trapped on the catalyst during lean operation and released and reduced to N2 under rich exhaust conditions; the rich cleansing operation of the cycle is referred to as "regeneration" since the catalyst is reactivated for more NOx trapping after NOx purge. Creating the rich exhaust conditions for regeneration can be accomplished by catalytic partial oxidation of methane in the exhaust system. Furthermore, catalytic reforming of partial oxidation exhaust can enable increased quantities of H2 which is an excellent reductant for lean NOx trap regeneration. It is critical to maintain clean and efficient partial oxidation and reforming processes to keep the lean NOx trap functioning properly and to reduce extra fuel consumption from the regeneration process. Although most exhaust constituents do not impede partial oxidation and reforming, some exhaust constituents may negatively affect the catalysts and result in loss of catalytic efficiency. Of particular concern are common catalyst poisons sulfur, zinc, and phosphorous. These poisons form in the exhaust through combustion of fuel and oil, and although they are present at low concentrations, they can accumulate to significant levels over the life of an engine system. In the work presented here, the effects of sulfur on the partial oxidation and reforming catalytic processes were studied to determine any durability limitations on the production of reductants for lean NOx trap catalyst regeneration.

  1. Lean Gasoline Engine Reductant Chemistry During Lean NOx Trap Regeneration

    SciTech Connect

    Choi, Jae-Soon; Prikhodko, Vitaly Y; Partridge Jr, William P; Parks, II, James E; Norman, Kevin M; Huff, Shean P; Chambon, Paul H; Thomas, John F

    2010-01-01

    Lean NOx Trap (LNT) catalysts can effectively reduce NOx from lean engine exhaust. Significant research for LNTs in diesel engine applications has been performed and has led to commercialization of the technology. For lean gasoline engine applications, advanced direct injection engines have led to a renewed interest in the potential for lean gasoline vehicles and, thereby, a renewed demand for lean NOx control. To understand the gasoline-based reductant chemistry during regeneration, a BMW lean gasoline vehicle has been studied on a chassis dynamometer. Exhaust samples were collected and analyzed for key reductant species such as H2, CO, NH3, and hydrocarbons during transient drive cycles. The relation of the reductant species to LNT performance will be discussed. Furthermore, the challenges of NOx storage in the lean gasoline application are reviewed.

  2. Development of a Desulfurization Strategy for a NOx Adsorber Catalyst

    SciTech Connect

    Tomazic, Dean

    2000-08-20

    Improve NOx regeneration calibration developed in DECSE Phase I project to understand full potential of NOx adsorber catalyst over a range of operating temperatures. Develop and demonstrate a desulfurization process to restore NOx conversion efficiency lost to sulfur contamination. Investigate effect of desulfurization process on long-term performance of the NOx adsorber catalyst.

  3. Spatiotemporal distribution of NOx storage and impact on NH3 and N2O selectivities during lean/rich cycling of a Ba-based lean NOx trap catalyst

    SciTech Connect

    Choi, Jae-Soon; Partridge Jr, William P; Pihl, Josh A; Kim, Miyoung; Koci, Petr; Daw, C Stuart

    2012-01-01

    We summarize results from an investigation of the spatiotemporal distribution of NO{sub x} storage and intermediate gas species in determining the performance of a fully formulated, Ba-based, lean NO{sub x} trap catalyst under lean/rich cycling conditions. By experimentally resolving spatiotemporal profiles of gas composition, we found that stored NO{sub x} was significantly redistributed along the monolith axis during the rich phase of the cycle by release and subsequent downstream re-adsorption. Sulfur poisoning of upstream NO{sub x} storage sites caused the active NO{sub x}-storage zone to be displaced downstream. This axial displacement in turn influenced rich-phase NO{sub x} release and re-adsorption. As sulfur poisoning increased, NH3 slip at the catalyst exit also increased due to its formation closer to the catalyst outlet and decreased exposure to downstream oxidation by surface oxygen. N{sub 2}O formation was found to be associated with nitrate reduction rather than oxidation of NH3 by stored oxygen. We propose that the observed evolution of N{sub 2}O selectivity with sulfation can be explained by changes in the spatiotemporal distribution of NO{sub x} storage resulting in either increased or decreased number of precious-metal sites surrounded by nitrates.

  4. Lean NOx Trap Catalysis for Lean Natural Gas Engine Applications

    SciTech Connect

    Parks, II, James E; Storey, John Morse; Theiss, Timothy J; Ponnusamy, Senthil; Ferguson, Harley Douglas; Williams, Aaron M; Tassitano, James B

    2007-09-01

    efficiency and emissions of natural gas reciprocating engines are being pursued. Approaches include: stoichiometric engine operation with exhaust gas recirculation and three-way catalysis, advanced combustion modes such as homogeneous charge compression ignition, and extension of the lean combustion limit with advanced ignition concepts and/or hydrogen mixing. The research presented here addresses the technical approach of combining efficient lean spark-ignited natural gas combustion with low emissions obtained from a lean NOx trap catalyst aftertreatment system. This approach can be applied to current lean engine technology or advanced lean engines that may result from related efforts in lean limit extension. Furthermore, the lean NOx trap technology has synergy with hydrogen-assisted lean limit extension since hydrogen is produced from natural gas during the lean NOx trap catalyst system process. The approach is also applicable to other lean engines such as diesel engines, natural gas turbines, and lean gasoline engines; other research activities have focused on those applications. Some commercialization of the technology has occurred for automotive applications (both diesel and lean gasoline engine vehicles) and natural gas turbines for stationary power. The research here specifically addresses barriers to commercialization of the technology for large lean natural gas reciprocating engines for stationary power. The report presented here is a comprehensive collection of research conducted by Oak Ridge National Laboratory (ORNL) on lean NOx trap catalysis for lean natural gas reciprocating engines. The research was performed in the Department of Energy's ARES program from 2003 to 2007 and covers several aspects of the technology. All studies were conducted at ORNL on a Cummins C8.3G+ natural gas engine chosen based on industry input to simulate large lean natural gas engines. Specific technical areas addressed by the research include: NOx reduction efficiency, partial

  5. Alkali- and Sulfur-Resistant Tungsten-Based Catalysts for NOx Emissions Control.

    PubMed

    Huang, Zhiwei; Li, Hao; Gao, Jiayi; Gu, Xiao; Zheng, Li; Hu, Pingping; Xin, Ying; Chen, Junxiao; Chen, Yaxin; Zhang, Zhaoliang; Chen, Jianmin; Tang, Xingfu

    2015-12-15

    The development of catalysts with simultaneous resistance to alkalis and sulfur poisoning is of great importance for efficiently controlling NOx emissions using the selective catalytic reduction of NOx with NH3 (SCR), because the conventional V2O5/WO3-TiO2 catalysts often suffer severe deactivation by alkalis. Here, we support V2O5 on a hexagonal WO3 (HWO) to develop a V2O5/HWO catalyst, which has exceptional resistance to alkali and sulfur poisoning in the SCR reactions. A 350 μmol g(-1) K(+) loading and the presence of 1,300 mg m(-3) SO2 do not almost influence the SCR activity of the V2O5/HWO catalyst, and under the same conditions, the conventional V2O5/WO3-TiO2 catalysts completely lost the SCR activity within 4 h. The strong resistance to alkali and sulfur poisoning of the V2O5/HWO catalysts mainly originates from the hexagonal structure of the HWO. The HWO allows the V2O5 to be highly dispersed on the external surfaces for catalyzing the SCR reactions and has the relatively smooth surfaces and the size-suitable tunnels specifically for alkalis' diffusion and trapping. This work provides a useful strategy to develop SCR catalysts with exceptional resistance to alkali and sulfur poisoning for controlling NOx emissions from the stationary source and the mobile source. PMID:26587749

  6. DYNAMOMETER EVALUATION OF PLASMA-CATALYST FOR DIESEL NOX REDUCTION

    SciTech Connect

    Hoard, J; Schmieg, S; Brooks, D; Peden, C; Barlow, S; Tonkyn, R

    2003-08-24

    A three-stage plasma-catalyst system was developed and tested on an engine dynamometer. Previous laboratory testing suggested high NOx efficiency could be obtained. With hexene reductant added to the exhaust, over 90% NOx reduction was observed. However, with diesel or Fischer-Tropsch reductant the catalyst efficiency rapidly dropped off. Heating the catalyst in air removed brown deposit from the surface and restored conversion efficiency. Following the engine tests, the used catalysts were evaluated. BET surface area decreased, and TPD revealed significant storage. This storage appears to be partly unburned diesel fuel that can be removed by heating to around 250-300 C, and partly hydrocarbons bonded to the surface that remain in place until 450-500 C. Laboratory testing with propene reductant demonstrated that the catalyst regains efficiency slowly even when operating temperature does not exceed 300 C. This suggests that control strategies may be able to regenerate the catalyst by occasional moderate heating.

  7. Kinetic and Performance Studies of the Regeneration Phase of Model Pt/Ba/Rh NOx Traps for Design and Optimization

    SciTech Connect

    Michael Harold; Vemuri Balakotaiah

    2010-05-31

    In this project a combined experimental and theoretical approach was taken to advance our understanding of lean NOx trap (LNT) technology. Fundamental kinetics studies were carried out of model LNT catalysts containing variable loadings of precious metals (Pt, Rh), and storage components (BaO, CeO{sub 2}). The Temporal Analysis of Products (TAP) reactor provided transient data under well-characterized conditions for both powder and monolith catalysts, enabling the identification of key reaction pathways and estimation of the corresponding kinetic parameters. The performance of model NOx storage and reduction (NSR) monolith catalysts were evaluated in a bench scale NOx trap using synthetic exhaust, with attention placed on the effect of the pulse timing and composition on the instantaneous and cycle-averaged product distributions. From these experiments we formulated a global model that predicts the main spatio-temporal features of the LNT and a mechanistic-based microkinetic models that incorporates a detailed understanding of the chemistry and predicts more detailed selectivity features of the LNT. The NOx trap models were used to determine its ability to simulate bench-scale data and ultimately to evaluate alternative LNT designs and operating strategies. The four-year project led to the training of several doctoral students and the dissemination of the findings as 47 presentations in conferences, catalysis societies, and academic departments as well 23 manuscripts in peer-reviewed journals. A condensed review of NOx storage and reduction was published in an encyclopedia of technology.

  8. Enhanced High Temperature Performance of NOx Reduction Catalyst Materials

    SciTech Connect

    Gao, Feng; Kim, Do Heui; Luo, Jinyong; Muntean, George G.; Peden, Charles HF; Howden, Ken; Currier, Neal; Kamasamudram, Krishna; Kumar, Ashok; Li, Junhui; Stafford, Randy; Yezerets, Aleksey; Castagnola, Mario; Chen, Hai Ying; Hess, Howard ..

    2012-12-31

    Two primary NOx after-treatment technologies have been recognized as the most promising approaches for meeting stringent NOx emission standards for diesel vehicles within the Environmental Protection Agency’s (EPA’s) 2007/2010 mandated limits, NOx Storage Reduction (NSR) and NH3 selective catalytic reduction (SCR); both are, in fact being commercialized for this application. However, in looking forward to 2015 and beyond with expected more stringent regulations, the continued viability of the NSR technology for controlling NOx emissions from lean-burn engines such as diesels will require at least two specific, significant and inter-related improvements. First, it is important to reduce system costs by, for example, minimizing the precious metal content while maintaining, even improving, performance and long-term stability. A second critical need for future NSR systems, as well as for NH3 SCR, will be significantly improved higher and lower temperature performance and stability. Furthermore, these critically needed improvements will contribute significantly to minimizing the impacts to fuel economy of incorporating these after-treatment technologies on lean-burn vehicles. To meet these objectives will require, at a minimum an improved scientific understanding of the following things: i) the various roles for the precious and coinage metals used in these catalysts; ii) the mechanisms for these various roles; iii) the effects of high temperatures on the active metal performance in their various roles; iv) mechanisms for higher temperature NOx storage performance for modified and/or alternative storage materials; v) the interactions between the precious metals and the storage materials in both optimum NOx storage performance and long term stability; vi) the sulfur adsorption and regeneration mechanisms for NOx reduction materials; vii) materials degradation mechanisms in CHA-based NH3 SCR catalysts. The objective of this CRADA project between PNNL and Cummins, Inc

  9. Congressionally Directed Project for Passive NOx Removal Catalysts Research

    SciTech Connect

    Schneider, William

    2014-08-29

    The Recipient proposes to produce new scientific and technical knowledge and tools to enable the discovery and deployment of highly effective materials for the selective catalytic reduction (SCR) of nitrogen oxides (NOx) from lean combustion exhaust. A second goal is to demonstrate a closely coupled experimental and computational approach to heterogeneous catalysis research. These goals will be met through the completion of four primary technical objectives: First, an in-depth kinetic analysis will be performed on two prominent classes of NOx SCR catalysts, Fe- and Cu-exchanged beta and ZSM-5 zeolites, over a wide range of catalyst formulation and under identical, high conversion conditions as a function of gas phase composition. Second, the nanoscale structure and adsorption chemistry of these high temperature (HT) and low temperature (LT) catalysts will be determined using in situ and operando spectroscopy under the same reaction conditions. Third, first-principles molecular simulations will be used to model the metal-zeolite active sites, their adsorption chemistry, and key steps in catalytic function. Fourth, this information will be integrated into chemically detailed mechanistic and kinetic descriptions and models of the operation of these well- defined NOx SCR catalysts under practically relevant reaction conditions. The new knowledge and models that derive from this work will be published in the scientific literature.

  10. Hydrophobic Catalysts For Removal Of NOx From Flue Gases

    NASA Technical Reports Server (NTRS)

    Sharma, Pramod K.; Hickey, Gregory S.; Voecks, Gerald E.

    1995-01-01

    Improved catalysts for removal of nitrogen oxides (NO and NO2) from combustion flue gases formulated as composites of vanadium pentoxide in carbon molecular sieves. Promotes highly efficient selective catalytic reduction of NOx at relatively low temperatures while not being adversely affected by presence of water vapor and sulfur oxide gases in flue gas. Apparatus utilizing catalyst of this type easily integrated into exhaust stream of power plant to remove nitrogen oxides, generated in combustion of fossil fuels and contribute to formation of acid rain and photochemical smog.

  11. Investigation of Aging Mechanisms in Lean NOx Traps

    SciTech Connect

    Mark Crocker

    2010-03-31

    Lean NO{sub x} traps (LNTs) represent a promising technology for the abatement of NO{sub 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{sub x} storage element of the catalyst has a greater affinity for SO{sub 3} than it does for NO{sub 2}, 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{sub 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{sub x} storage and reduction. In this manner, NO{sub 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/Al{sub 2}O{sub 3} type (representing the first generation of LNTs), Pt/Rh/BaO/Al{sub 2}O{sub 3} catalysts were employed which also incorporated CeO{sub 2} or CeO{sub 2}-ZrO{sub 2}, 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/ft{sup 3}), Rh (10 or 20 g/ft{sup 3}), BaO (15, 30 or 45 g/L), and either CeO{sub 2} (0, 50 or 100 g/L) or CeO{sub 2}-ZrO{sub 2} (0, 50

  12. Axial length effects on lean NOx trap performance

    SciTech Connect

    Prikhodko, Vitaly Y; Nguyen, Ke; Choi, Jae-Soon; Daw, C Stuart

    2009-01-01

    The effect of axial length on the NO{sub x} reduction performance of two different commercial Lean NO{sub x} Trap (LNT) monolithic catalysts was experimentally investigated in a bench flow reactor. The washcoat composition of one of the catalysts consisted of Pt and K on {gamma}-Al{sub 2}O{sub 3}; whereas the other catalyst contained a complex mixture of Pt, Pd, Rh, Ba, Ce, Zr, Mg, Al and others. The NO{sub x} removal characteristics of cylindrical monolith segments of constant diameter (2.22 cm) and axial lengths of 2.54, 5.08 and 7.62 cm were evaluated using a simulated lean engine exhaust containing water and carbon dioxide at a constant space velocity of 30,000 h{sup -1}. No significant effects of length were observed when the catalysts were fully reduced with hydrogen between NO{sub x} capture phases. However when the catalysts were only partially regenerated NO{sub x} reduction efficiency increased with monolith length. Intra-catalyst H{sub 2} measurements at different axial locations indicated that at least some of the efficiency loss during partial regeneration occurred when back-mixed H{sub 2} was directly oxidized and became unavailable for nitrate reduction.

  13. Nitrogen Release from a NOx Storage and Reduction Catalyst

    SciTech Connect

    Tonkyn, Russell G.; Disselkamp, Robert S.; Peden, C. H.

    2006-04-30

    In a NOx storage and reduction (NSR) catalyst the release and reduction of NOx occurs over a very short period. The speed of the NOx release and reduction creates difficulties in analyzing the chemistry using normal analytical techniques, which are typically better suited to slower, steady state studies. We have investigated the time dependence of NO, NO2, NH3, N2O and N2 released by an NSR catalyst using a combination of FTIR and gas chromatographic techniques. Nitrogen was detected with the GC by using He rather than N2 as the background gas. The FTIR was used not only to monitor NO, NO2, NH3 and N2O, but also to establish cycle-to-cycle reproducibility. Under these conditions we used the GC to sample the effluent at multiple times over many lean-rich cycles. To the extent that the chemistry was truly periodic and reproducible, we obtained the time dependence of the release of nitrogen after the lean-to-rich transition. Similar information was obtained for O2, H2 and N2O. Combining the FTIR and GC data we obtained good cycle averaged nitrogen balances, indicating that all the major products were accounted for.

  14. Advantages of MgAlOx over gamma-Al2O3 as a support material for potassium-based high temperature lean NOx traps

    SciTech Connect

    Luo, Jinyong; Gao, Feng; Karim, Ayman M.; Xu, Pinghong; Browning, Nigel D.; Peden, Charles HF

    2015-08-07

    MgAlOx mixed oxides were employed as supports for potassium-based lean NOx traps (LNTs) targeted for high temperature applications. Effects of support compositions, K/Pt loadings, thermal aging and catalyst regeneration on NOx storage capacity were systematically investigated. The catalysts were characterized by XRD, NOx-TPD, TEM, STEM-HAADF and in-situ XAFS. The results indicate that MgAlOx mixed oxides have significant advantages over conventional gamma-Al2O3-supports for LNT catalysts, in terms of high temperature NOx trapping capacity and thermal stability. First, as a basic support, MgAlOx stabilizes stored nitrates (in the form of KNO3) to much higher temperatures than mildly acidic gamma-Al2O3. Second, MgAlOx minimizes Pt sintering during thermal aging, which is not possible for gamma-Al2O3 supports. Notably, combined XRD, in-situ XAFS and STEM-HAADF results indicate that Pt species in the thermally aged Pt/MgAlOx samples are finely dispersed in the oxide matrix as isolated atoms. This strong metal-support interaction stabilizes Pt and minimizes the extent of sintering. However, such strong interactions result in Pt oxidation via coordination with the support so that NO oxidation activity can be adversely affected after aging which, in turn, decreases NOx trapping ability for these catalysts. Interestingly, a high-temperature reduction treatment regenerates essentially full NOx trapping performance. In fact, regenerated Pt/K/MgAlOx catalyst exhibits much better NOx trapping performance than fresh Pt/K/Al2O3 LNTs over the entire temperature range investigated here. In addition to thermal aging, Pt/K loading effects were systemically studied over the fresh samples. The results indicate that NOx trapping is kinetically limited at low temperatures, while thermodynamically limited at high temperatures. A simple conceptual model was developed to explain the Pt and K loading effects on NOx storage. An optimized K loading, which allows balancing between the

  15. EVALUATION OF NOX EMISSION CONTROL CATALYSTS FOR POWER PLANT SCR INSTALLATIONS

    EPA Science Inventory

    The paper gives results of an evaluation of nitrogen oxide (NOx) emission control catalysts commercially developed for power plant selective catalytic reduction (SCR) installations. ith the objective of establishing the performance of SCR catalysts and related technology, control...

  16. Diesel Fuel Sulfur Effects on the Performance of Lean NOx Catalysts

    SciTech Connect

    Ren, Shouxian

    2000-08-20

    Evaluate the effects of diesel fuel sulfur on the performance of low temperature and high temperature Lean-NOx Catalysts. Evaluate the effects of up to 250 hours of aging on the performance of the Lean-NOx Catalysts with different fuel sulfur contents.

  17. Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process.

    PubMed

    Guo, Yufang; Liao, Xiaobin; Fu, Mingli; Huang, Haibao; Ye, Daiqi

    2015-02-01

    Characteristics of toluene decomposition and formation of nitrogen oxide (NOx) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al2O3/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO2 selectivity. In addition, NOx was suppressed with the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NOx suppression. The MnOx catalyst exhibited the lowest concentration of O3 and highest CO2 selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression. PMID:25662254

  18. Method of preparing doped oxide catalysts for lean NOx exhaust

    DOEpatents

    Park, Paul W.

    2004-03-09

    The lean NOx catalyst includes a substrate, an oxide support material, preferably .gamma.-alumina deposited on the substrate and a metal or metal oxide promoter or dopant introduced into the oxide support material. The metal promoters or dopants are selected from the group consisting of indium, gallium, tin, silver, germanium, gold, nickel, cobalt, copper, iron, manganese, molybdenum, chromium cerium, and vanadium, and oxides thereof, and any combinations thereof. The .gamma.-alumina preferably has a pore volume of from about 0.5 to about 2.0 cc/g; a surface area of between 80 and 350 m.sup.2 /g; an average pore size diameter of between about 3 to 30 nm; and an impurity level of less than or equal to about 0.2 weight percent. In a preferred embodiment the .gamma.-alumina is prepared by a sol-gel method, with the metal doping of the .gamma.-alumina preferably accomplished using an incipient wetness impregnation technique.

  19. Discovery of New NOx Reduction Catalysts for CIDI Engines Using Combinatorial Techniques

    SciTech Connect

    Blint, Richard J

    2005-08-15

    This project for the discovery of new lean reduction NOx catalysts was initiated on August 16th, 2002 and is now into its fourth year. Several materials have already been identified as NOx reduction catalysts for possible future application. NOx reduction catalysts are a critical need in the North American vehicle market since these catalysts are needed to enable both diesels and lean gasoline engines to meet the 2007-2010 emission standards. Hydrocarbon selective catalytic reduction (SCR) is a preferred technology since it requires no infrastructure changes (as may be expected for urea SCR) and most likely has the simplest engine control strategy of the three proposed NOx reduction approaches. The use of fast throughput techniques and informatics greatly enhances the possibility of discovering new NOx reduction catalysts. Using fast throughput techniques this project has already screened over 3000 new materials and evaluates hundreds of new materials a month. Evaluating such a high number of new materials puts this approach into a very different paradigm than previous discovery approaches for new NOx reduction catalysts. With so much data on materials it is necessary to use statistical techniques to identify the potential catalysts and these statistical techniques are needed to optimize compositions of the multi-component materials that are identified under the program as possible new lean NOx catalysts. Several new materials have conversions in excess of 80% at temperatures above 300 C. That is more than twice the activity of previous HC SCR materials. These materials are candidates for emission control on heavy-duty systems (i.e.; over 8500 pounds gross weight). Tests of one of the downselected materials on an engine dynamometer show NOx reductions greater than 80% under some conditions even though the net NOx reductions on the HWFET and the US06 cycles were relatively low. The program is scheduled to continue until the end of the 2006 calendar year. Work in the

  20. Discovery of Novel NOx Catalysts for CIDI Applications by High-throughput Methods

    SciTech Connect

    Blint, Richard

    2007-12-31

    DOE project DE-PS26-00NT40758 has developed very active, lean exhaust, NOx reduction catalysts that have been tested on the discovery system, laboratory reactors and engine dynamometer systems. The goal of this project is the development of effective, affordable NOx reduction catalysts for lean combustion engines in the US light duty vehicle market which can meet Tier II emission standards with hydrocarbons based reductants for reducing NOx. General Motors (prime contractor) along with subcontractors BASF (Engelhard) (a catalytic converter developer) and ACCELRYS (an informatics supplier) carried out this project which began in August of 2002. BASF (Engelhard) has run over 16,000 tests of 6100 possible catalytic materials on a high throughput discovery system suitable for automotive catalytic materials. Accelrys developed a new database informatics system which allowed material tracking and data mining. A program catalyst was identified and evaluated at all levels of the program. Dynamometer evaluations of the program catalyst both with and without additives show 92% NOx conversions on the HWFET, 76% on the US06, 60% on the cold FTP and 65% on the Set 13 heavy duty test using diesel fuel. Conversions of over 92% on the heavy duty FTP using ethanol as a second fluid reductant have been measured. These can be competitive with both of the alternative lean NOx reduction technologies presently in the market. Conversions of about 80% were measured on the EUDC for lean gasoline applications without using active dosing to adjust the C:N ratio for optimum NOx reduction at all points in the certification cycle. A feasibility analysis has been completed and demonstrates the advantages and disadvantages of the technology using these materials compared with other potential technologies. The teaming agreements among the partners contain no obstacles to commercialization of new technologies to any potential catalyst customers.

  1. Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts

    DOE PAGESBeta

    Brookshear, Daniel William; Nam, Jeong -Gil; Nguyen, Ke; Toops, Todd J.; Binder, Andrew J.

    2015-06-05

    This bench reactor study investigates the impact of gaseous sulfur on the NOx reduction activity of Cu-chabazite SCR (Cu-CHA) catalysts at SO2 concentrations representative of marine diesel engine exhaust. After two hours of 500 ppm SO2 exposure at 250 and 400 °C in the simulated diesel exhaust gases, the NOx reduction activity of the sulfated Cu-CHA SCR catalysts is severely degraded at evaluation temperatures below 250 °C; however, above 250 °C the impact of sulfur exposure is minimal. EPMA shows that sulfur is located throughout the washcoat and along the entire length of the sulfated samples. Interestingly, BET measurements revealmore » that the sulfated samples have a 20% decrease in surface area. Moreover, the sulfated samples show a decrease in NOx/nitrate absorption during NO exposure in a DRIFTS reactor which suggests that Cu sites in the catalyst are blocked by the presence of sulfur. SO2 exposure also results in an increase in NH3 storage capacity, possibly due to the formation of ammonium sulfate species in the sulfated samples. In all cases, lean thermal treatments as low as 500 °C reverse the effects of sulfur exposure and restore the NOx reduction activity of the Cu-CHA catalyst to that of the fresh condition.« less

  2. Metal/metal oxide doped oxide catalysts having high deNOx selectivity for lean NOx exhaust aftertreatment systems

    DOEpatents

    Park, Paul W.

    2004-03-16

    A lean NOx catalyst and method of preparing the same is disclosed. The lean NOx catalyst includes a ceramic substrate, an oxide support material, preferably .gamma.-alumina, deposited on the substrate and a metal promoter or dopant introduced into the oxide support material. The metal promoters or dopants are selected from the group consisting of indium, gallium, tin, silver, germanium, gold, nickel, cobalt, copper, iron, manganese, molybdenum, chromium, cerium, vanadium, oxides thereof, and combinations thereof. The .gamma.-alumina preferably has a pore volume of from about 0.5 to about 2.0 cc/g; a surface area of between about 80 to 350 m.sup.2 /g; an average pore size diameter of between about 3 to 30 nm; and an impurity level of less than or equal to 0.2 weight percent. In a preferred embodiment the .gamma.-alumina is prepared by a sol-gel method, with the metal doping of the .gamma.-alumina preferably accomplished using an incipient wetness impregnation technique.

  3. Sulfur and temperature effects on the spatial distribution of reactions inside a lean NOx trap and resulting changes in global performance

    SciTech Connect

    Choi, Jae-Soon; Partridge Jr, William P; Pihl, Josh A; Daw, C Stuart

    2008-01-01

    We experimentally studied the influence of temperature and sulfur loading on the axial distribution of reactions inside a commercial lean NOx trap (LNT) catalyst to better understand the global performance trends. Our measurements were made on a monolith core, bench-flow reactor under cycling conditions (60-s lean/5-s rich) at 200, 325, and 400 C with intra-catalyst and reactor-outlet gas speciation. Postmortem elemental and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses of the catalyst also supplemented our gas species measurements. For the unsulfated catalyst, the NOx storage/reduction (NSR) reactions were localized in the front (upstream) portion of the monolith, whereas oxygen storage/reduction reactions were distributed more evenly along the entire catalyst length. As a result, two axially distinct reaction zones were developed inside the working catalyst: an upstream 'NSR zone' where both NOx and oxygen storage/reduction took place and a downstream oxygen storage capacity (OSC)-only zone where the NSR reactions did not penetrate. The NSR zone involved less than half the LNT at 325 and 400 C, but it included almost the entire length at 200 C. Sulfation poisoned both the NSR and OSC reactions beginning at the catalyst upstream edge, with the NSR degradation occurring more rapidly and distinctly than the OSC. As sulfation proceeded, a third zone (the sulfated zone) developed and the NSR zone moved downstream, with a concomitant decrease in both the OSC-only zone and global NOx conversion. The sulfation impact on NOx conversion was greatest at 200 C, when the NSR zone was largest. Ammonia selectivity increased with sulfation, which we attributed to a shortened OSC-only zone and resultantly reduced consumption of NH{sub 3}, slipping from the NSR zone, by downstream OSC. Lower temperatures also increased NH{sub 3} selectivity. Nitrous oxide selectivity also increased with decreasing temperature but showed little dependence on

  4. MODELING COMPETITIVE ADSORPTION IN UREA-SCR CATALYSTS FOR EFFECTIVE LOW TEMPERATURE NOX CONTROL

    SciTech Connect

    Devarakonda, Maruthi N.; Tonkyn, Russell G.; Tran, Diana N.; Lee, Jong H.; Herling, Darrell R.

    2010-09-17

    Although the SCR technology exhibits higher NOx reduction efficiency over a wider range of temperatures among the lean NOx reduction technologies, further improvement in low-temperature performance is required to meet the future emission standards and to lower the system cost. In order to improve the catalyst technologies and optimize the system performance, it is critical to understand the reaction mechanisms and catalyst behaviors with respect to operating conditions. For example, it is well known that the ammonia coverage on catalyst surface is critical for NOx reduction efficiency. However, the level of ammonia storage is influenced by competitive adsorption by other species, such as H2O and NO2. Moreover, hydrocarbon species that slip through the upstream DOC during the cold-start period can also inhibit the SCR performance, especially at low temperatures. Therefore, a one-dimensional detailed kinetic model that can account for the effects of such competitive adsorption has been developed based on steady state surface isotherm tests on a commercial Fe-zeolite catalyst. The model is developed as a C language S-function and implemented in Matlab/Simulink environment. Rate kinetics of adsorption and desorption of each of the adsorbents are determined from individual adsorption tests and validated for a set of test conditions that had all the adsorbents in the feed gas.

  5. Sulfate Storage and Stability on Common Lean NOx Trap Components

    SciTech Connect

    Ottinger, Nathan A; Toops, Todd J; Pihl, Josh A; Roop, Justin T; Choi, Jae-Soon; Partridge Jr, William P

    2012-01-01

    Components found in a commercial lean NO{sub x} trap have been studied in order to determine their impact on sulfate storage and release. A micro-reactor and a diffuse reflectance infrared Fourier transform spectrometer (DRIFTS) were used to compare components MgAl{sub 2}O{sub 4}, Pt/MgAl{sub 2}O{sub 4}, Pt/Al{sub 2}O{sub 3}, Pt/Ba/Al{sub 2}O{sub 3}, Pt/CeO{sub 2}-ZrO{sub 2}, and Pt/Ba/CeO{sub 2}-ZrO{sub 2}, as well as physical mixtures of Pt/Al{sub 2}O{sub 3} + MgAl{sub 2}O{sub 4} and Pt/Ba/CeO{sub 2}-ZrO{sub 2} + MgAl{sub 2}O{sub 4}. Desulfation temperature profiles as well as DRIFTS NO{sub x} and SO{sub x} storage spectra are presented for all components. This systematic approach highlighted the ability of the underlying support to impact sulfate stability, in particular when Ba was supported on ceria-zirconia rather than alumina the desulfation temperature decreased by 60-120 C. A conceptual model of sulfation progression on the ceria-zirconia support is proposed that explains the high uptake of sulfur and low temperature release when it is employed. It was also determined that the close proximity of platinum is not necessary for much of the sulfation and desulfation chemistry that occurs, as physical mixtures with platinum dispersed on only one phase displayed similar behavior to samples with platinum dispersed on both phases.

  6. Control of diesel soot and NOx emissions with a particulate trap and EGR.

    PubMed

    Liu, Rui-xiang; Gao, Xi-yan; Yang, De-sheng; Xu, Xiao-guang

    2005-01-01

    The exhaust gas recirculation (EGR), coupled with a high-collection efficiency particulate trap to simultaneously control smoke and NOx emissions from diesel engines were studied. This ceramic trap developed previously provided the soot cleaning efficiency of 99%, the regeneration efficiency reaches 80% and the ratio of success reaches 97%, which make EGR used in diesel possible. At the presence of EGR, opening of the regeneration control valve of the trap was over again optimized to compensate for the decrease of the oxygen concentration in the exhaust gas resulted from EGR. The results indicated the cleaning efficiency and regeneration performance of the trap were maintained at the same level except that the back pressure increased faster. A new EGR system was developed, which is based on a wide range oxygen (UEGO) sensor. Experiments were carried out under steady state conditions while maintaining the engine speed at 1600 r/min, setting the engine loads at 0%, 25%, 50%, 75% and 100% respectively. Throughout each test the EGR rate was kept at nine different settings and data were taken with the gas analyzer and UEGO sensor. Then, the EGR rate and engine load maps, which showed the tendencies of NOx, CO and HC emissions from diesel engine, were made using the measured data. Using the maps, the author set up the EGR regulation, the relationship between the optimal amounts of EGR flow and the equivalence ratio, sigma, where sigma = 14.5/AFR. PMID:16295898

  7. Alkali-Resistant Mechanism of a Hollandite DeNOx Catalyst.

    PubMed

    Hu, Pingping; Huang, Zhiwei; Gu, Xiao; Xu, Fei; Gao, Jiayi; Wang, Yue; Chen, Yaxin; Tang, Xingfu

    2015-06-01

    A thorough understanding of the deactivation mechanism by alkalis is of great importance for rationally designing improved alkali-resistant deNOx catalysts, but a traditional ion-exchange mechanism cannot often accurately describe the nature of the deactivation, thus hampering the development of superior catalysts. Here, we establish a new exchange-coordination mechanism on the basis of the exhaustive study on the strong alkali resistance of a hollandite manganese oxide (HMO) catalyst. A combination of isothermal adsorption measurements of ammonia with X-ray absorption near-edge structure spectra and X-ray photoelectron spectra reveals that alkali metal ions first react with protons from Brønsted acid sites of HMO via the ion exchange. Synchrotron X-ray diffraction patterns and extended X-ray absorption fine structure spectra coupled with theoretical calculations demonstrate that the exchanged alkali metal ions are subsequently stabilized at size-suitable cavities in the HMO pores via a coordination model with an energy savings. This exchange-coordination mechanism not only gives a wholly convincing explanation for the intrinsic nature of the deactivation of the reported catalysts by alkalis but also provides a strategy for rationally designing improved alkali-resistant deNOx catalysts in general. PMID:25941972

  8. New catalyst for NO(x) control. Phase 1. Final report, August 1988-March 1989

    SciTech Connect

    Nelson, B.W.; Nelson, S.G.; Higgins, M.O.; Brandum, P.A.

    1989-06-01

    During static firing tests, aircraft engines are subject to regulation as fixed sources of air pollution. Present best available technology (BAT) to control NOx emissions in exhaust gases from jet-engine test cells (JETCs) is selective catalytic reduction (SCR). SCR is effective at a narrow range of high temperatures, requires elaborate process controls to minimize emissions of ammonia reagent, and consumes precious metal catalysts. This Phase I SBIR project tested vermiculite (a common silicate mineral) as a catalyst for reducing NOx to oxygen and nitrogen. Efficient reduction (50-98%) of NOx was observed over a practical range of operating temperatures (200->850 F) and gas flow rates (5,000-60,000 bed volumes/hr). The vermiculite test bed also efficiently scavenges carbon particulates and reduces part of the CO and CO{sub 2} from the exhaust stream. Used catalyst was regenerated by heating to 930 F in an air stream; it was also judged to be a disposable solid.

  9. Thermal Durability of Cu-CHA NH3-SCR Catalysts for Diesel NOx Reduction

    SciTech Connect

    Schmieg, Steven J.; Oh, Se H.; Kim, Chang H.; Brown, David B.; Lee, Jong H.; Peden, Charles HF; Kim, Do Heui

    2012-04-30

    Multiple catalytic functions (NOx conversion, NO and NH3 oxidation, NH3 storage) of a commercial Cu-zeolite urea/NH3-SCR catalyst were assessed in a laboratory fixed-bed flow reactor system after differing degrees of hydrothermal aging. Catalysts were characterized by using x-ray diffraction (XRD), 27Al solid state nuclear magnetic resonance (NMR) and transmission electron microscopy (TEM) / energy dispersive X-ray (EDX) spectroscopy to develop an understanding of the degradation mechanisms during catalyst aging. The catalytic reaction measurements of laboratory-aged catalysts were performed, which allows us to obtain a universal curve for predicting the degree of catalyst performance deterioration as a function of time at each aging temperature. Results show that as the aging temperature becomes higher, the zeolite structure collapses in a shorter period of time after an induction period. The decrease in SCR performance was explained by zeolite structure destruction and/or Cu agglomeration, as detected by XRD/27Al NMR and by TEM/EDX, respectively. Destruction of the zeolite structure and agglomeration of the active phase also results in a decrease in the NO/NH3 oxidation activity and the NH3 storage capacity of the catalyst. Selected laboratory aging conditions (16 h at 800oC) compare well with a 135,000 mile vehicle-aged catalyst for both performance and characterization criteria.

  10. Impact of oxidation catalysts on exhaust NO2/NOx ratio from lean-burn natural gas engines.

    PubMed

    Olsen, Daniel B; Kohls, Morgan; Arney, Gregg

    2010-07-01

    Oxides of nitrogen (NOx) emitted from internal combustion engines are composed primarily of nitric oxide (NO) and nitrogen dioxide (NO2). Exhaust from most combustion sources contains NOx composed primarily of NO. There are two important scenarios specific to lean-burn natural gas engines in which the NO2/NOx ratio can be significant: (1) when the engine is operated at ultralean conditions and (2) when an oxidation catalyst is used. Large NO2/NOx ratios may result in additional uncertainty in NOx emissions measurements because the most common technique (chemiluminescence) was developed for low NO2/NOx ratios. In this work, scenarios are explored in which the NO2/NOx ratio can be large. Additionally, three NOx measurement approaches are compared for exhaust with various NO2/NOx ratios. The three measurement approaches are chemiluminescence, chemical cell, and Fourier-transform infrared spectroscopy. A portable analyzer with chemical cell technology was found to be the most accurate for measuring exhaust NOx with large NO2/NOx ratios. PMID:20681434

  11. Modeling Species Inhibition of NO Oxidation in Urea-SCR Catalysts for Diesel Engine NOx Control

    SciTech Connect

    Devarakonda, Maruthi N.; Tonkyn, Russell G.; Tran, Diana N.; Lee, Jong H.; Herling, Darrell R.

    2011-04-20

    Urea-selective catalytic reduction (SCR) catalysts are regarded as the leading NOx aftertreatment technology to meet the 2010 NOx emission standards for on-highway vehicles running on heavy-duty diesel engines. However, issues such as low NOx conversion at low temperature conditions still exist due to various factors, including incomplete urea thermolysis, inhibition of SCR reactions by hydrocarbons and H2O. We have observed a noticeable reduction in the standard SCR reaction efficiency at low temperature with increasing water content. We observed a similar effect when hydrocarbons are present in the stream. This effect is absent under fast SCR conditions where NO ~ NO2 in the feed gas. As a first step in understanding the effects of such inhibition on SCR reaction steps, kinetic models that predict the inhibition behavior of H2O and hydrocarbons on NO oxidation are presented in the paper. A one-dimensional SCR model was developed based on conservation of species equations and was coded as a C-language S-function and implemented in Matlab/Simulink environment. NO oxidation and NO2 dissociation kinetics were defined as a function of the respective adsorbate’s storage in the Fe-zeolite SCR catalyst. The corresponding kinetic models were then validated on temperature ramp tests that showed good match with the test data. Such inhibition models will improve the accuracy of model based control design for integrated DPF-SCR aftertreatment systems.

  12. Modeling Species Inhibition of NO oxidation in Urea-SCR Catalysts for Diesel Engine NOx Control

    SciTech Connect

    Devarakonda, Maruthi N.; Tonkyn, Russell G.; Tran, Diana N.; Lee, Jong H.; Herling, Darrell R.

    2010-09-15

    Urea-selective catalytic reduction (SCR) catalysts are regarded as the leading NOx aftertreatment technology to meet the 2010 NOx emission standards for on-highway vehicles running on heavy-duty diesel engines. However, issues such as low NOx conversion at low temperature conditions still exist due to various factors, including incomplete urea thermolysis, inhibition of SCR reactions by hydrocarbons and H2O. We have observed a noticeable reduction in the standard SCR reaction efficiency at low temperature with increasing water content. We observed a similar effect when hydrocarbons are present in the stream. This effect is absent under fast SCR conditions where NO ~ NO2 in the feed gas. As a first step in understanding the effects of such inhibition on SCR reaction steps, kinetic models that predict the inhibition behavior of H2O and hydrocarbons on NO oxidation are presented in the paper. A one-dimensional SCR model was developed based on conservation of species equations and was coded as a C-language S-function and implemented in Matlab/Simulink environment. NO oxidation and NO2 dissociation kinetics were defined as a function of the respective adsorbate’s storage in the SCR catalyst. The corresponding kinetic models were then validated on temperature ramp tests that showed good match with the test data.

  13. Effect of K loadings on nitrate formation/decomposition and on NOx storage performance of K-based NOx storage-reduction catalysts

    SciTech Connect

    Kim, Do Heui; Mudiyanselage, Kumudu K.; Szanyi, Janos; Kwak, Ja Hun; Zhu, Haiyang; Peden, Charles HF

    2013-10-25

    We have investigated nitrate formation and decomposition processes, and measured NOx storage performance on Pt-K2O/Al2O3 catalysts as a function of potassium loading. After NO2 adsorption at room temperature, ionic and bidentate nitrates were observed by fourier transform infra-red (FTIR) spectroscopy. The ratio of the former to the latter species increased with increasing potassium loading up to 10 wt%, and then stayed almost constant with additional K, demonstrating a clear dependence of loading on the morphology of the K species. Although both K2O(10)/Al2O3 and K2O(20)/Al2O3 samples have similar nitrate species after NO2 adsorption, the latter has more thermally stable nitrate species as evidenced by FTIR and NO2 temperature programmed desorption (TPD) results. With regard to NOx storage performance, the temperature of maximum NOx uptake (Tmax) is 573 K up to a potassium loading of 10 wt%. As the potassium loading increases from 10 wt% to 20 wt%, Tmax shifted from 573 K to 723 K. Moreover, the amount of NO uptake (38 cm3 NOx/g catal) at Tmax increased more than three times, indicating that efficiency of K in storing NOx is enhanced significantly at higher temperature, in good agreement with the NO2 TPD and FTIR results. Thus, a combination of characterization and NOx storage performance results demonstrates an unexpected effect of potassium loading on nitrate formation and decomposition processes; results important for developing Pt-K2O/Al2O3 for potential applications as high temperature NOx storage-reduction catalysts.

  14. Simultaneous Oxidization of NOx and SO2 by a New Non-thermal Plasma Reactor Enhanced by Catalyst and Additive

    NASA Astrophysics Data System (ADS)

    Kim, Heejoon; Jun, Han; Sakaguchi, Yuhei; Minami, Wataru

    2008-02-01

    The non-thermal plasma as one of the most promising technologies for removing NOx and SO2 has attracted much attention. In this study, a new plasma reactor combined with catalyst and additive was developed to effectively oxidize and remove NOx and SO2 in the flue gas. The experimental results showed that TiO2 could improve the oxidation efficiency of SO2 in the case of applying plasma while having a negative effect on the oxidation process of NO and NOx. With the addition of NH3, the oxidation rates of NOx, NO and SO2 were slightly increased. However, the effect of adding NH3 on NOx oxidation was negative when the temperature was above 200°C.

  15. Regeneration of field-spent activated carbon catalysts for low-temperature selective catalytic reduction of NOx with NH3

    SciTech Connect

    Jeon, Jong Ki; Kim, Hyeonjoo; Park, Young-Kwon; Peden, Charles HF; Kim, Do Heui

    2011-10-15

    In the process of producing liquid crystal displays (LCD), the emitted NOx is removed over an activated carbon catalyst by using selective catalytic reduction (SCR) with NH3 at low temperature. However, the catalyst rapidly deactivates primarily due to the deposition of boron discharged from the process onto the catalyst. Therefore, this study is aimed at developing an optimal regeneration process to remove boron from field-spent carbon catalysts. The spent carbon catalysts were regenerated by washing with a surfactant followed by drying and calcination. The physicochemical properties before and after the regeneration were investigated by using elemental analysis, TG/DTG (thermogravimetric/differential thermogravimetric) analysis, N2 adsorption-desorption and NH3 TPD (temperature programmed desorption). Spent carbon catalysts demonstrated a drastic decrease in DeNOx activity mainly due to heavy deposition of boron. Boron was accumulated to depths of about 50 {mu}m inside the granule surface of the activated carbons, as evidenced by cross-sectional SEM-EDX analysis. However, catalyst activity and surface area were significantly recovered by removing boron in the regeneration process, and the highest NOx conversions were obtained after washing with a non-ionic surfactant in H2O at 70 C, followed by treatment with N2 at 550 C.

  16. Development of Metal Substrate for Denox Catalysts and Particulate Trap

    SciTech Connect

    Pollard, Michael; Habeger, Craig; Frary, Megan; Haines, Scott; Fluharty, Amy; Dakhoul, Youssef; Carr, Michael; Park, Paul; Stefanick, Matthew; DaCosta, Herbert; Balmer-Millar, M Lou; Readey, Michael; McCluskey, Philip

    2005-12-31

    The objective of this project was to develop advanced metallic catalyst substrate materials and designs for use in off-highway applications. The new materials and designs will be used as catalyst substrates and diesel particulate traps. They will increase durability, reduce flow resistance, decrease time to light-off, and reduce cost relative to cordierite substrates. Metallic catalyst substrates are used extensively for diesel oxidation catalysts and have the potential to be used in other catalytic systems for diesel engines. Metallic substrates have many advantages over ceramic materials including improved durability and resistance to thermal shock and vibration. However, the cost is generally higher than cordierite. The most common foil material used for metallic substrates is FeCr Alloy, which is expensive and has temperature capabilities beyond what is necessary for diesel applications. The first task in the project was Identification and Testing of New Materials. In this task, several materials were analyzed to determine if a low cost substitute for FeCr Alloy was available or could be developed. Two materials were identified as having lower cost while showing no decrease in mechanical properties or oxidation resistance at the application temperatures. Also, the ability to fabricate these materials into a finished substrate was not compromised, and the ability to washcoat these materials was satisfactory. Therefore, both candidate materials were recommended for cost savings depending on which would be less expensive in production quantities. The second task dealt with the use of novel flow designs to improve the converter efficiency while possibly decreasing the size of the converter to reduce cost even more. A non-linear flow path was simulated to determine if there would be an increase in efficiency. From there, small samples were produced for bench testing. Bench tests showed that the use of non-linear channels significantly reduced the light

  17. Selective catalytic reduction system and process for treating NOx emissions using a palladium and rhodium or ruthenium catalyst

    DOEpatents

    Sobolevskiy, Anatoly; Rossin, Joseph A.; Knapke, Michael J.

    2011-07-12

    A process for the catalytic reduction of nitrogen oxides (NOx) in a gas stream (29) in the presence of H.sub.2 is provided. The process comprises contacting the gas stream with a catalyst system (38) comprising zirconia-silica washcoat particles (41), a pre-sulfated zirconia binder (44), and a catalyst combination (40) comprising palladium and at least one of rhodium, ruthenium, or a mixture of ruthenium and rhodium.

  18. Formation of NOx from N2 and O2 in catalyst-pellet filled dielectric barrier discharges at atmospheric pressure.

    PubMed

    Sun, Qi; Zhu, Aimin; Yang, Xuefeng; Niu, Jinhai; Xu, Yong

    2003-06-21

    At temperatures above 350 degrees C, significant amounts of NOx formed from N2 and O2 have been observed in Cu-ZSM-5 catalyst-pellet filled dielectric barrier discharges, indicating the necessity of using low-temperature performance in all plasma-catalytic processes for removal of air pollutants. PMID:12841270

  19. Bauxite-supported Transition Metal Oxides: Promising Low-temperature and SO2-tolerant Catalysts for Selective Catalytic Reduction of NOx

    PubMed Central

    Wang, Xiuyun; Wu, Wen; Chen, Zhilin; Wang, Ruihu

    2015-01-01

    In order to develop low-temperature (below 200 °C) and SO2-tolerant catalysts for selective catalytic reduction (SCR) of NOx, a series of cheap M/bauxite (M = Mn, Ni and Cu) catalysts were prepared using bauxite as a support. Their SCR performances are much superior to typical V2O5/TiO2, the addition of M into bauxite results in significant promotion of NOx removal efficiency, especially at low temperature. Among the catalysts, Cu/bauxite exhibits wide temperature window over 50–400 °C, strong resistance against SO2 and H2O as well as good regeneration ability in SCR of NOx. NOx conversion is more than 80% at 50–200 °C, and N2 selectivity is more than 98%. Cu/bauxite can serve as a promising catalyst in SCR of NOx. PMID:25988825

  20. Development of Optimal Catalyst Designs and Operating Strategies for Lean NOx Reduction in Coupled LNT-SCR Systems

    SciTech Connect

    Harold, Michael; Crocker, Mark; Balakotaiah, Vemuri; Luss, Dan; Choi, Jae-Soon; Dearth, Mark; McCabe, Bob; Theis, Joe

    2013-09-30

    Oxides of nitrogen in the form of nitric oxide (NO) and nitrogen dioxide (NO{sub 2}) commonly referred to as NO{sub x}, is one of the two chemical precursors that lead to ground-level ozone, a ubiquitous air pollutant in urban areas. A major source of NO{sub x} is generated by equipment and vehicles powered by diesel engines, which have a combustion exhaust that contains NO{sub x} in the presence of excess O{sub 2}. Catalytic abatement measures that are effective for gasoline-fueled engines such as the precious metal containing three-way catalytic converter (TWC) cannot be used to treat O2-laden exhaust containing NO{sub x}. Two catalytic technologies that have emerged as effective for NO{sub x} abatement are NO{sub x} storage and reduction (NSR) and selective catalytic reduction (SCR). NSR is similar to TWC but requires much larger quantities of expensive precious metals and sophisticated periodic switching operation, while SCR requires an on-board source of ammonia which serves as the chemical reductant of the NO{sub x}. The fact that NSR produces ammonia as a byproduct while SCR requires ammonia to work has led to interest in combining the two together to avoid the need for the cumbersome ammonia generation system. In this project a comprehensive study was carried out of the fundamental aspects and application feasibility of combined NSR/SCR. The project team, which included university, industry, and national lab researchers, investigated the kinetics and mechanistic features of the underlying chemistry in the lean NOx trap (LNT) wherein NSR was carried out, with particular focus on identifying the operating conditions such as temperature and catalytic properties which lead to the production of ammonia in the LNT. The performance features of SCR on both model and commercial catalysts focused on the synergy between the LNT and SCR converters in terms of utilizing the upstream-generated ammonia and alternative reductants such as propylene, representing the

  1. Dynamics of N2 and N2O peaks during and after the regeneration of lean NOx trap

    DOE PAGESBeta

    Mráček, David; Koci, Petr; Marek, Milos; Choi, Jae-Soon; Pihl, Josh A.; Partridge, Jr., William P.

    2014-12-04

    We study the dynamics and selectivity of N2 and N2O formation during and after the regeneration of a commercial NOx storage catalyst containing Pt, Pd, Rh, Ba on Ce/Zr, Mg/Al and Al oxides was studied with high-speed FTIR and SpaciMS analyzers. The lean/rich cycling experiments (60 s/5 s and 60 s/3 s) were performed in the temperature range 200–400°C, using H2, CO, and C3H6 individually for the reduction of adsorbed NOx. Isotopically labeled 15NO was employed in combination with Ar carrier gas in order to quantify the N2 product by mass spectrometry. N2 and N2O products were formed concurrently. Themore » primary peaks appeared immediately after the rich-phase inception, and tailed off with breakthrough of the reductant front (accompanied by NH3 product). Secondary N2 and N2O peaks appeared at the rich-to-lean transition as a result of reactions between surface-deposited reductants/intermediates (CO, HC, NH3, -NCO) and residual stored NOx. At 200–300 °C, up to 30% of N2 and 50% of N2O products originated from the secondary peaks. The N2O/N2 selectivity ratio as well as the magnitude of secondary peaks decreased with temperature and duration of the rich phase. Among the three reductants, propene generated secondary N2 peak up to the highest temperature. Lastly the primary N2 peak exhibited a broadened shoulder aligned with movement of reduction front from the zone where both NOx and oxygen were stored to the NOx-free zone where only oxygen storage capacity was saturated. N2 formed in the NOx-free zone originated from reaction of NH3 with stored oxygen, while N2O formation in this zone was very low.« less

  2. Reduction of NOx and SO2 in a non-thermal plasma reactor combined with catalyst and methanol

    NASA Astrophysics Data System (ADS)

    Jun, Han; Kim, Heejoon; Sakaguchi, Yuhei; Hong, Yao

    2008-10-01

    Non-thermal plasma technology has attracted considerable attention due to simultaneous removal of nitrogen oxide (NOx) and sulfur oxide (SO2) from flue gas. In this study, the synergistic effect of methanol and catalyst on NO, NOx and SO2 removal efficiency in a plasma reactor is investigated. The results show that the removal efficiency of NOx is dramatically enhanced by adding 0.4% methanol. Nevertheless, methanol has no significant beneficial effect on the oxidation of SO2. Based on the experimental results, the optimum content of methanol should be 0.4% and the preferable operating temperature is suggested to be 250 °C for removing NOx and SO2 in a non-thermal plasma-catalyst reactor. Moreover, V2O5/TiO2 is found to be more effective than TiO2 for oxidizing NO, whereas V2O5/TiO2 is not better than TiO2 for SO2 oxidization unless the discharge power is above 11 W.

  3. Thermally stable single-atom platinum-on-ceria catalysts via atom trapping.

    PubMed

    Jones, John; Xiong, Haifeng; DeLaRiva, Andrew T; Peterson, Eric J; Pham, Hien; Challa, Sivakumar R; Qi, Gongshin; Oh, Se; Wiebenga, Michelle H; Pereira Hernández, Xavier Isidro; Wang, Yong; Datye, Abhaya K

    2016-07-01

    Catalysts based on single atoms of scarce precious metals can lead to more efficient use through enhanced reactivity and selectivity. However, single atoms on catalyst supports can be mobile and aggregate into nanoparticles when heated at elevated temperatures. High temperatures are detrimental to catalyst performance unless these mobile atoms can be trapped. We used ceria powders having similar surface areas but different exposed surface facets. When mixed with a platinum/aluminum oxide catalyst and aged in air at 800°C, the platinum transferred to the ceria and was trapped. Polyhedral ceria and nanorods were more effective than ceria cubes at anchoring the platinum. Performing synthesis at high temperatures ensures that only the most stable binding sites are occupied, yielding a sinter-resistant, atomically dispersed catalyst. PMID:27387946

  4. Catalytic decomposition of H2O2 over Fe-based catalysts for simultaneous removal of NOX and SO2

    NASA Astrophysics Data System (ADS)

    Huang, Xianming; Ding, Jie; Zhong, Qin

    2015-01-01

    Simultaneous flue gas desulfurization and denitrification were achieved with rad OH radicals from the decomposition of H2O2 over hematite (Fe) as well as hematite supported on alumina (Fe-Al) and anatase (Fe-Ti). Under all conditions, SO2 achieved 100% removal, whereas NOX removal varies with the catalysts. The supporting of Fe over aluminum enhances the catalytic removal of NOX, whereas that of anatase presents negative effect. The NOX removal is determined by the decomposition rate of H2O2 into rad OH radicals over sbnd OH bonded with Fe (Fe-OH). The supporting of Fe over alumina enhances the content of Fe-OH and the points of zero charge (PZC) values, which are beneficial for the production of rad OH radicals. The supporting of Fe over anatase results in the formation of FeOTi, which cannot decompose H2O2 into rad OH radicals. Furthermore, H2O2 tends more to be reacted with TiOH to produce O2 over Fe-Ti. Finally, the enhancement mechanism of H2O2 decomposition over Fe-based catalysts is speculated. It has a contribution to the correct choice for supports and active ingredients of the catalyst in the future industrial applications.

  5. Simultaneous Removal of Particulates and NOx Using Catalyst Impregnated Fibrous Ceramic Filters

    SciTech Connect

    Choi, J.I.; Mun, S.H.; Kim, S.T.; Hong, M.S.; Lee, J.C.

    2002-09-19

    The research is focused on the development and commercialization of high efficiency, cost effective air pollution control system, which can replace in part air pollution control devices currently in use. In many industrial processes, hot exhaust gases are cooled down to recover heat and to remove air pollutants in exhaust gases. Conventional air pollution control devices such as bag filters, E.P. and adsorption towers withstand operating temperatures up to 300 C. Also, reheating is sometimes necessary to meet temperature windows for S.C.R. Since Oxidation reactions of acid gases such as SO{sub 2}, and HCl with lime are enhanced at high temperatures, catalyst impregnated ceramic filters can be candidate for efficient and cost effective air pollution control devices. As shown on Fig. 1., catalytic ceramic filters remove particulates on exterior surface of filters and acid gases are oxidized to salts reacting with limes injected in upstream ducts. Oxidation reactions are enhanced in the cake formed on exterior of filters. Finally, injected reducing gas such as NH{sub 3} react with NOx to form N{sub 2} and H{sub 2}O interior of filters in particulate-free environment. Operation and maintenance technology is similar to conventional bag filters except that systems are exposed to relatively high temperatures ranging 300-500 C.

  6. Simulation of lean NOx trap performance with microkinetic chemistry and without mass transfer.

    SciTech Connect

    Larson, Rich; Daw, C. Stuart; Pihl, Josh A.; Chakravarthy, V. Kalyana

    2011-08-01

    A microkinetic chemical reaction mechanism capable of describing both the storage and regeneration processes in a fully formulated lean NO{sub x} trap (LNT) is presented. The mechanism includes steps occurring on the precious metal, barium oxide (NO{sub x} storage), and cerium oxide (oxygen storage) sites of the catalyst. The complete reaction set is used in conjunction with a transient plug flow reactor code to simulate not only conventional storage/regeneration cycles with a CO/H{sub 2} reductant, but also steady flow temperature sweep experiments that were previously analyzed with just a precious metal mechanism and a steady state code. The results show that NO{sub x} storage is not negligible during some of the temperature ramps, necessitating a re-evaluation of the precious metal kinetic parameters. The parameters for the entire mechanism are inferred by finding the best overall fit to the complete set of experiments. Rigorous thermodynamic consistency is enforced for parallel reaction pathways and with respect to known data for all of the gas phase species involved. It is found that, with a few minor exceptions, all of the basic experimental observations can be reproduced with these purely kinetic simulations, i.e., without including mass-transfer limitations. In addition to accounting for normal cycling behavior, the final mechanism should provide a starting point for the description of further LNT phenomena such as desulfation and the role of alternative reductants.

  7. Simultaneous catalytic removal of NOx and diesel PM over La(0.9) K(0.1) CoO3 catalyst assisted by plasma.

    PubMed

    Pei, Mei-xiang; Lin, He; Shangguan, Wen-feng; Huang, Zhen

    2005-01-01

    The simultaneous removal of NOx and particulate matter (PM) from diesel exhaust is investigated over a mixed metal oxide catalyst of La(0.9) K(0.1) CoO3 loaded on gamma-Al2O3 spherules with the assistant of plasma. It was found that NOx was reduced by PM in oxygen rich atmosphere, the CO2 and N2 were produced in the same temperature window without considering the N2 formed by plasma decomposition. As a result, the temperature for the PM combustion decreases and the reduction efficiency of NOx to N2 increases during the plasma process, which indicated that the activity of the catalyst can be improved by plasma. The NOx is decomposed by plasma at both low temperature and high temperature. Therefore, the whole efficiency of NOx conversion is enhanced. PMID:16295893

  8. Diesel particulate abatement via wall-flow traps based on perovskite catalysts.

    PubMed

    Fino, Debora; Russo, Nunzio; Saracco, Guido; Specchia, Vito

    2003-01-01

    It is probably redundant to stress how extensive are nowadays the attempts to reduce the diesel particulate emissions from automotive and stationary sources. The present paper looks into a technology relied on a catalytic trap based on a SiC wall-flow monolith lined with suitable catalysts for the sake of promoting a more complete and faster regeneration after particulate capture. All the major steps of the catalytic filter preparation are dealt with, including: the synthesis and choice of the proper catalyst and trap materials, the development of an in situ catalyst deposition technique, the bench testing of the derived catalytic wall-flow. The best catalyst selected was the perovskite La0.9K0.1Cr0.9O3-delta. The filtration efficiency and the pressure drop of the catalytic and non-catalytic monoliths were evaluated on a diesel engine bench under various operating conditions. PMID:14672365

  9. Understanding NOx SCR Mechanism and Activity on Cu/Chabazite Structures throughout the Catalyst Life Cycle

    SciTech Connect

    Ribeiro, Fabio; Delgass, Nick; Gounder, Rajmani; Schneider, William F.; Miller, Jeff; Yezerets, Aleksey; McEwen, Jean-Sabin; Peden, Charles HF; Howden, Ken

    2014-12-09

    Oxides of nitrogen (NOx) compounds contribute to acid rain and photochemical smog and have been linked to respiratory ailments. NOx emissions regulations continue to tighten, driving the need for high performance, robust control strategies. The goal of this project is to develop a deep, molecular level understanding of the function of Cu-SSZ-13 and Cu-SAPO-34 materials that catalyze the SCR of NOx with NH3.

  10. SELECTIVE REDUCTION OF NOX IN OXYGEN RICH ENVIRONMENTS WITH PLASMA-ASSISTED CATALYSIS: CATALYST DEVELOPMENT AND MECHANISTIC STUDIES

    SciTech Connect

    Peden, C; Barlow, S; Hoard, J; Kwak, J; *Balmer-Millar, M; *Panov, A; Schmieg, S; Szanyi, J; Tonkyn, R

    2003-08-24

    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

  11. Understanding Automotive Exhaust Catalysts Using a Surface Science Approach: Model NOx Storage Materials

    SciTech Connect

    Szanyi, Janos; Yi, Cheol-Woo W.; Mudiyanselage, Kumudu K.; Kwak, Ja Hun

    2013-11-01

    The structure-reactivity relationships of model BaO-based NOx storage/reduction catalysts were investigated under well controlled experimental conditions using surface science analysis techniques. The reactivity of BaO toward NO2, CO2, and H2O was studied as a function of BaO layer thickness [0\\hBaO\\30 monolayer (ML)], sample temperature, reactant partial pressure, and the nature of the substrate the NOx storage material was deposited onto. Most of the efforts focused on understanding the mechanism of NO2 storage either on pure BaO, or on BaO exposed to CO2 or H2O prior to NO2 exposure. The interaction of NO2 with a pure BaO film results in the initial formation of nitrite/nitrate ion pairs by a cooperative adsorption mechanism predicted by prior theoretical calculations. The nitrites are then further oxidized to nitrates to produce a fully nitrated surface. The mechanism of NO2 uptake on thin BaO films (\\4 ML), BaO clusters (\\1 ML) and mixed BaO/Al2O3 layers are fundamentally different: in these systems initially nitrites are formed only, and then converted to nitrates at longer NO2 exposure times. These results clarify the contradicting mechanisms presented in prior studies in the literature. After the formation of a nitrate layer the further conversion of the underlying BaO is slow, and strongly depends on both the sample temperature and the NO2 partial pressure. At 300 K sample temperature amorphous Ba(NO3)2 forms that then can be converted to crystalline nitrates at elevated temperatures. The reaction between BaO and H2O is facile, a series of Ba(OH)2 phases form under the temperature and H2O partial pressure regimes studied. Both amorphous and crystalline Ba(OH)2 phases react with NO2, and initially form nitrites only that can be converted to nitrates. The NO2 adsorption capacities of BaO and Ba(OH)2 are identical, i.e., both of these phases can completely be converted to Ba(NO3)2. In contrast, the interaction of CO2 with pure BaO results in the formation

  12. Surface Tuning of La0.5Sr0.5CoO3 Perovskite Catalysts by Acetic Acid for NOx Storage and Reduction.

    PubMed

    Peng, Yue; Si, Wenzhe; Luo, Jinming; Su, Wenkang; Chang, Huazhen; Li, Junhua; Hao, Jiming; Crittenden, John

    2016-06-21

    Selective dissolution of perovskite A site (A of ABO3 structure) was performed on the La1 - xSrxCoO3 catalysts for the NOx storage and reduction (NSR) reaction. The surface area of the catalysts were enhanced using dilute HNO3 impregnation to dissolve Sr. Inactive SrCO3 was removed effectively within 6 h, and the catalyst preserved the perovskite framework after 24 h of treatment. The tuned catalysts exhibited higher NSR performance (both NOx storage and NO-to-NO2 oxidation) under lean-burn and fuel-rich cycles at 250 °C. Large amounts of NOx adsorption were due to the increase of nitrate/nitrite species bonding to the A site and the growth of newly formed monodentate nitrate species. Nitrate species were stored stably on the partial exposed Sr(2+) cations. These exposed Sr(2+) cations played an important role on the NOx reduction by C3H6. High NO-to-NO2 oxidation ability was due to the generation of oxygen defects and Co(2+)-Co(3+) redox couples, which resulted from B-site exsolution induced by A-site dissolution. Hence, our method is facile to modify the surface structures of perovskite catalysts and provides a new strategy to obtain highly active catalysts for the NSR reaction. PMID:27233105

  13. NOx abatement in the exhaust of lean-burn natural gas engines over Ag-supported γ-Al2O3 catalysts

    NASA Astrophysics Data System (ADS)

    Azizi, Y.; Kambolis, A.; Boréave, A.; Giroir-Fendler, A.; Retailleau-Mevel, L.; Guiot, B.; Marchand, O.; Walter, M.; Desse, M.-L.; Marchin, L.; Vernoux, P.

    2016-04-01

    A series of Ag catalysts supported on γ-Al2O3, including two different γ-Al2O3 supports and various Ag loadings (2-8 wt.%), was prepared, characterized (SEM, TEM, BET, physisorption, TPR, NH3-TPD) and tested for the selective catalytic reduction of NOx by CH4 for lean-burn natural gas engines exhausts. The catalysts containing 2 wt.% Ag supported on γ-Al2O3 were found to be most efficient for the NOx reduction into N2 with a maximal conversion of 23% at 650 °C. This activity was clearly linked with the ability of the catalyst to concomitantly produce CO, via the methane steam reforming, and NO2. The presence of small AgOx nanoparticles seems to be crucial for the methane activation and NOx reduction.

  14. Impacts of continuously regenerating trap and particle oxidation catalyst on the NO2 and particulate matter emissions emitted from diesel engine.

    PubMed

    Liu, Zhihua; Ge, Yunshan; Tan, Jianwei; He, Chao; Shah, Asad Naeem; Ding, Yan; Yu, Linxiao; Zhao, Wei

    2012-01-01

    Two continuously regenerating diesel particulate filter (CRDPF) with different configurations and one particles oxidation catalyst (POC) were employed to perform experiments in a controlled laboratory setting to evaluate their effects on NO2, smoke and particle number emissions. The results showed that the application of the after-treatments increased the emission ratios of NO2/NOx significantly. The results of smoke emissions and particle number (PN) emissions indicated that both CRDPFs had sufficient capacity to remove more than 90% of total particulate matter (PM) and more than 97% of solid particles. However, the POC was able to remove the organic components of total PM, and only partially to remove the carbonaceous particles with size less than 30 nm. The negligible effects of POC on larger particles were observed due to its honeycomb structure leads to an inadequate residence time to oxidize the solid particles or trap them. The particles removal efficiencies of CRDPFs had high degree of correlations with the emission ratio of NO2/NOx. The PN emission results from two CRDPFs indicated that more NO2 generating in diesel oxidation catalyst section could obtain the higher removal efficiency of solid particles. However this also increased the risk of NO2 exposure in atmosphere. PMID:22894096

  15. Supported, Alkali-Promoted Cobalt Oxide Catalysts for NOx Removal from Coal Combustion Flue Gases

    SciTech Connect

    Morris D. Argyle

    2005-12-31

    A series of cobalt oxide catalysts supported on alumina ({gamma}-Al{sub 2}O{sub 3}) were synthesized with varying contents of cobalt and of added alkali metals, including lithium, sodium, potassium, rubidium, and cesium. Unsupported cobalt oxide catalysts and several cobalt oxide catalysts supported ceria (CeO{sub 2}) with varying contents of cobalt with added potassium were also prepared. The catalysts were characterized with UV-visible spectroscopy and were examined for NO{sub x} decomposition activity. The CoO{sub x}/Al{sub 2}O{sub 3} catalysts and particularly the CoO{sub x}/CeO{sub 2} catalysts show N{sub 2}O decomposition activity, but none of the catalysts (unsupported Co{sub 3}O{sub 4} or those supported on ceria or alumina) displayed significant, sustained NO decomposition activity. For the Al{sub 2}O{sub 3}-supported catalysts, N{sub 2}O decomposition activity was observed over a range of reaction temperatures beginning about 723 K, but significant (>50%) conversions of N{sub 2}O were observed only for reaction temperatures >900 K, which are too high for practical commercial use. However, the CeO{sub 2}-supported catalysts display N{sub 2}O decomposition rates similar to the Al{sub 2}O{sub 3}-supported catalysts at much lower reaction temperatures, with activity beginning at {approx}573 K. Conversions of >90% were achieved at 773 K for the best catalysts. Catalytic rates per cobalt atom increased with decreasing cobalt content, which corresponds to increasing edge energies obtained from the UV-visible spectra. The decrease in edge energies suggests that the size and dimensionality of the cobalt oxide surface domains increase with increasing cobalt oxide content. The rate data normalized per mass of catalyst that shows the activity of the CeO{sub 2}-supported catalysts increases with increasing cobalt oxide content. The combination of these data suggest that supported cobalt oxide species similar to bulk Co{sub 3}O{sub 4} are inherently more active than

  16. Active sites in Cu-SSZ-13 deNOx catalyst under reaction conditions: a XAS/XES perspective

    NASA Astrophysics Data System (ADS)

    Lomachenko, Kirill A.; Borfecchia, Elisa; Bordiga, Silvia; Soldatov, Alexander V.; Beato, Pablo; Lamberti, Carlo

    2016-05-01

    Cu-SSZ-13 is a highly active catalyst for the NH3-assisted selective catalytic reduction (SCR) of the harmful nitrogen oxides (NOx, x=1, 2). Since the catalytically active sites for this reaction are mainly represented by isolated Cu ions incorporated into the zeolitic framework, element-selective studies of Cu local environment are crucial to fully understand the enhanced catalytic properties of this material. Herein, we highlight the recent advances in the characterization of the most abundant Cu-sites in Cu-SSZ-13 upon different reaction-relevant conditions made employing XAS and XES spectroscopies, complemented by computational analysis. A concise review of the most relevant literature is also presented.

  17. Catalysts, systems and methods to reduce NOX in an exhaust gas stream

    DOEpatents

    Castellano, Christopher R.; Moini, Ahmad; Koermer, Gerald S.; Furbeck, Howard

    2010-07-20

    Catalysts, systems and methods are described to reduce NO.sub.x emissions of an internal combustion engine. In one embodiment, an emissions treatment system for an exhaust stream is provided having an SCR catalyst comprising silver tungstate on an alumina support. The emissions treatment system may be used for the treatment of exhaust streams from diesel engines and lean burn gasoline engines. An emissions treatment system may further comprise an injection device operative to dispense a hydrocarbon reducing agent upstream of the catalyst.

  18. Current Understanding of Cu-Exchanged Chabazite Molecular Sieves for Use as Commercial Diesel Engine DeNOx Catalysts

    SciTech Connect

    Gao, Feng; Kwak, Ja Hun; Szanyi, Janos; Peden, Charles HF

    2013-11-03

    Selective catalytic reduction (SCR) of NOx with ammonia using metal-exchanged molecular sieves with a chabazite (CHA) structure has recently been commercialized on diesel vehicles. One of the commercialized catalysts, i.e., Cu-SSZ-13, has received much attention for both practical and fundamental studies. For the latter, the particularly well-defined structure of this zeolite is allowing long-standing issues of the catalytically active site for SCR in metal-exchanged zeolites to be addressed. In this review, recent progress is summarized with a focus on two areas. First, the technical significance of Cu-SSZ-13 as compared to other Cu-ion exchanged zeolites (e.g., Cu-ZSM-5 and Cu-beta) is highlighted. Specifically, the much enhanced hydrothermal stability for Cu-SSZ-13 compared to other zeolite catalysts is addressed via performance measurements and catalyst characterization using several techniques. The enhanced stability of Cu-SSZ-13 is rationalized in terms of the unique small pore structure of this zeolite catalyst. Second, the fundamentals of the catalytically active center; i.e., the chemical nature and locations within the SSZ-13 framework are presented with an emphasis on understanding structure-function relationships. For the SCR reaction, traditional kinetic studies are complicated by intra-particle diffusion limitations. However, a major side reaction, nonselective ammonia oxidation by oxygen, does not suffer from mass-transfer limitations at relatively low temperatures due to significantly lower reaction rates. This allows structure-function relationships that are rather well understood in terms of Cu ion locations and redox properties. Finally, some aspects of the SCR reaction mechanism are addressed on the basis of in-situ spectroscopic studies.

  19. Significant Promotion Effect of Mo Additive on a Novel Ce-Zr Mixed Oxide Catalyst for the Selective Catalytic Reduction of NO(x) with NH3.

    PubMed

    Ding, Shipeng; Liu, Fudong; Shi, Xiaoyan; Liu, Kuo; Lian, Zhihua; Xie, Lijuan; He, Hong

    2015-05-13

    A novel Mo-promoted Ce-Zr mixed oxide catalyst prepared by a homogeneous precipitation method was used for the selective catalytic reduction (SCR) of NO(x) with NH3. The optimal catalyst showed high NH3-SCR activity, SO2/H2O durability, and thermal stability under test conditions. The addition of Mo inhibited growth of the CeO2 particle size, improved the redox ability, and increased the amount of surface acidity, especially the Lewis acidity, all of which were favorable for the excellent NH3-SCR performance. It is believed that the catalyst is promising for the removal of NO(x) from diesel engine exhaust. PMID:25894854

  20. Excellent performance of one-pot synthesized Cu-SSZ-13 catalyst for the selective catalytic reduction of NOx with NH3.

    PubMed

    Xie, Lijuan; Liu, Fudong; Ren, Limin; Shi, Xiaoyan; Xiao, Feng-Shou; He, Hong

    2014-01-01

    Cu-SSZ-13 samples prepared by a novel one-pot synthesis method achieved excellent NH3-SCR performance and high N2 selectivity from 150 to 550 °C after ion exchange treatments. The selected Cu3.8-SSZ-13 catalyst was highly resistant to large space velocity (800 000 h(-1)) and also maintained high NOx conversion in the presence of CO2, H2O, and C3H6 in the simulated diesel exhaust. Isolated Cu(2+) ions located in three different sites were responsible for its excellent NH3-SCR activity. Primary results suggest that the one-pot synthesized Cu-SSZ-13 catalyst is a promising candidate as an NH3-SCR catalyst for the NOx abatement from diesel vehicles. PMID:24295053

  1. PARAMETRIC STUDIES OF CATALYSTS FOR NOX CONTROL FROM STATIONARY POWER PLANTS

    EPA Science Inventory

    The report gives results of a study of vanadia-alumina and iron oxide-chromium oxide-alumina catalysts for the reduction of NO with NH3 in simulated flue gas. Optimum catalyst compositions were 15% V2O5 on Al2O3 and 10% Fe-Cr oxides on Al2O3 with an Fe/Cr ratio of 1/9, respective...

  2. Platinum particle size and support effects in NO(x) mediated carbon oxidation over platinum catalysts.

    PubMed

    Villani, Kenneth; Vermandel, Walter; Smets, Koen; Liang, Duoduo; van Tendeloo, Gustaaf; Martens, Johan A

    2006-04-15

    Platinum metal was dispersed on microporous, mesoporous, and nonporous support materials including the zeolites Na-Y, Ba-Y, Ferrierite, ZSM-22, ETS-10, and AIPO-11, alumina, and titania. The oxidation of carbon black loosely mixed with catalyst powder was monitored gravimetrically in a gas stream containing nitric oxide, oxygen, and water. The carbon oxidation activity of the catalysts was found to be uniquely related to the Pt dispersion and little influenced by support type. The optimum dispersion is around 3-4% corresponding to relatively large Pt particle sizes of 20-40 nm. The carbon oxidation activity reflects the NO oxidation activity of the platinum catalyst, which reaches an optimum in the 20-40 nm Pt particle size range. The lowest carbon oxidation temperatures were achieved with platinum loaded ZSM-22 and AIPO-11 zeolite crystallites bearing platinum of optimum dispersion on their external surfaces. PMID:16683615

  3. Enhanced High- and Low-Temperature Performance of NOx Reduction Catalyst Materials

    SciTech Connect

    Gao, Feng; Muntean, George G.; Peden, Charles HF; Howden, Ken; Currier, Neal; Kamasamudram, Krishna; Kumar, Ashok; Li, Junhui; Luo, Jinyong; Stafford, Randy; Yezerets, Aleksey; Castagnola, Mario; Chen, Hai-Ying; Hess, Howard ..

    2014-12-09

    In this annual CRADA program report, we will briefly highlight results from our recent studies of the stability of candidate K-based high temperature NSR materials, and comparative studies of low temperature performance of SSZ-13 and SAPO-34 CHA catalysts; in particular, recent results comparing Fe- and Cu-based CHA materials.

  4. Effect of Unburned Methyl Esters on the NOx Conversion of Fe-Zeolite SCR Catalyst

    SciTech Connect

    Williams, A.; Ratcliff, M.; Pedersen, D.; McCormick, R.; Cavataio, G.; Ura, J.

    2010-03-01

    Engine and flow reactor experiments were conducted to determine the impact of biodiesel relative to ultra-low-sulfur diesel (ULSD) on inhibition of the selective catalytic reduction (SCR) reaction over an Fe-zeolite catalyst. Fe-zeolite SCR catalysts have the ability to adsorb and store unburned hydrocarbons (HC) at temperatures below 300 C. These stored HCs inhibit or block NO{sub x}-ammonia reaction sites at low temperatures. Although biodiesel is not a hydrocarbon, similar effects are anticipated for unburned biodiesel and its organic combustion products. Flow reactor experiments indicate that in the absence of exposure to HC or B100, NO{sub x} conversion begins at between 100 and 200 C. When exposure to unburned fuel occurs at higher temperatures (250-400 C), the catalyst is able to adsorb a greater mass of biodiesel than of ULSD. Experiments show that when the catalyst is masked with ULSD, NO{sub x} conversion is inhibited until it is heated to 400 C. However, when masked with biodiesel, NO{sub x} conversion is observed to begin at temperatures as low as 200 C. Engine test results also show low-temperature recovery from HC storage. Engine tests indicate that, overall, the SCR system has a faster recovery from HC masking with biodiesel. This is at least partially due to a reduction in exhaust HCs, and thus total HC exposure with biodiesel.

  5. EVALUATION OF SCR CATALYSTS FOR COMBINED CONTROL OF NOX AND MERCURY

    EPA Science Inventory

    The report documents two-task, bench- and pilot-scale research on the effect of selective catalytic reduction (SCR) catalysts on mercury speciation in Illinois and Powder River Basin (PRB) coal combustion flue gases. In task I, a bench-scale reactor was used to study the oxidatio...

  6. Simultaneous reduction of particulate matter and NO(x) emissions using 4-way catalyzed filtration systems.

    PubMed

    Swanson, Jacob J; Watts, Winthrop F; Newman, Robert A; Ziebarth, Robin R; Kittelson, David B

    2013-05-01

    The next generation of diesel emission control devices includes 4-way catalyzed filtration systems (4WCFS) consisting of both NOx and diesel particulate matter (DPM) control. A methodology was developed to simultaneously evaluate the NOx and DPM control performance of miniature 4WCFS made from acicular mullite, an advanced ceramic material (ACM), that were challenged with diesel exhaust. The impact of catalyst loading and substrate porosity on catalytic performance of the NOx trap was evaluated. Simultaneously with NOx measurements, the real-time solid particle filtration performance of catalyst-coated standard and high porosity filters was determined for steady-state and regenerative conditions. The use of high porosity ACM 4-way catalyzed filtration systems reduced NOx by 99% and solid and total particulate matter by 95% when averaged over 10 regeneration cycles. A "regeneration cycle" refers to an oxidizing ("lean") exhaust condition followed by a reducing ("rich") exhaust condition resulting in NOx storage and NOx reduction (i.e., trap "regeneration"), respectively. Standard porosity ACM 4-way catalyzed filtration systems reduced NOx by 60-75% and exhibited 99.9% filtration efficiency. The rich/lean cycling used to regenerate the filter had almost no impact on solid particle filtration efficiency but impacted NOx control. Cycling resulted in the formation of very low concentrations of semivolatile nucleation mode particles for some 4WCFS formulations. Overall, 4WCFS show promise for significantly reducing diesel emissions into the atmosphere in a single control device. PMID:23550802

  7. Roles of Promoters in V2O5/TiO2 Catalysts for Selective Catalytic Reduction of NOx with NH3: Effect of Order of Impregnation.

    PubMed

    Youn, Seunghee; Song, Inhak; Kim, Do Heui

    2016-05-01

    Recently, various promoters for commercial selective catalytic reduction (SCR) catalysts are used to improve DeNOx activity at low temperature. We aimed at finding the optimum condition to prepare V2O5/TiO2 catalyst by changing promoters (W, Ce, Zr and Mn), not only for improving SCR reactivity, but also for reducing N2O formation at high temperature. In addition, we changed the order of impregnation between promoter and vanadium precursors on TiO2 support and observed its effect on activity and N2O selectivity. We utilized various analytical techniques, such as N2 adsorption-desorption, X-ray Diffraction (XRD), Raman spectroscopy, UV-visible Diffuse Reflectance Spectroscopy (UV-vis DRS) and Temperature Programmed Reduction with hydrogen (H2-TPR) to investigate the physicochemical properties of V2O5/TiO2 catalysts. It was found that W and Ce added V2O5/TiO2 catalysts showed the most active DeNOx properties at low temperature. Additionally, the difference in impregnation order affected the SCR activity. The superiority of low temperature activity of the vanadium firstly added catalysts (W or Ce/V/TiO2) is attributed to the formation of more polymerized V2O5 on the sample. PMID:27483756

  8. Dosimeter-Type NOx Sensing Properties of KMnO4 and Its Electrical Conductivity during Temperature Programmed Desorption

    PubMed Central

    Groβ, Andrea; Kremling, Michael; Marr, Isabella; Kubinski, David J.; Visser, Jacobus H.; Tuller, Harry L.; Moos, Ralf

    2013-01-01

    An impedimetric NOx dosimeter based on the NOx sorption material KMnO4 is proposed. In addition to its application as a low level NOx dosimeter, KMnO4 shows potential as a precious metal free lean NOx trap material (LNT) for NOx storage catalysts (NSC) enabling electrical in-situ diagnostics. With this dosimeter, low levels of NO and NO2 exposure can be detected electrically as instantaneous values at 380 °C by progressive NOx accumulation in the KMnO4 based sensitive layer. The linear NOx sensing characteristics are recovered periodically by heating to 650 °C or switching to rich atmospheres. Further insight into the NOx sorption-dependent conductivity of the KMnO4-based material is obtained by the novel eTPD method that combines electrical characterization with classical temperature programmed desorption (TPD). The NOx loading amount increases proportionally to the NOx exposure time at sorption temperature. The cumulated NOx exposure, as well as the corresponding NOx loading state, can be detected linearly by electrical means in two modes: (1) time-continuously during the sorption interval including NOx concentration information from the signal derivative or (2) during the short-term thermal NOx release. PMID:23549366

  9. Dosimeter-type NOx sensing properties of KMnO4 and its electrical conductivity during temperature programmed desorption.

    PubMed

    Groß, Andrea; Kremling, Michael; Marr, Isabella; Kubinski, David J; Visser, Jacobus H; Tuller, Harry L; Moos, Ralf

    2013-01-01

    An impedimetric NOx dosimeter based on the NOx sorption material KMnO4 is proposed. In addition to its application as a low level NOx dosimeter, KMnO4 shows potential as a precious metal free lean NOx trap material (LNT) for NOx storage catalysts (NSC) enabling electrical in-situ diagnostics. With this dosimeter, low levels of NO and NO2 exposure can be detected electrically as instantaneous values at 380 °C by progressive NOx accumulation in the KMnO4 based sensitive layer. The linear NOx sensing characteristics are recovered periodically by heating to 650 °C or switching to rich atmospheres. Further insight into the NOx sorption-dependent conductivity of the KMnO4-based material is obtained by the novel eTPD method that combines electrical characterization with classical temperature programmed desorption (TPD). The NOx loading amount increases proportionally to the NOx exposure time at sorption temperature. The cumulated NOx exposure, as well as the corresponding NOx loading state, can be detected linearly by electrical means in two modes: (1) time-continuously during the sorption interval including NOx concentration information from the signal derivative or (2) during the short-term thermal NOx release. PMID:23549366

  10. Identification of the arsenic resistance on MoO3 doped CeO2/TiO2 catalyst for selective catalytic reduction of NOx with ammonia.

    PubMed

    Li, Xiang; Li, Xiansheng; Li, Junhua; Hao, Jiming

    2016-11-15

    Arsenic resistance on MoO3 doped CeO2/TiO2 catalysts for selective catalytic reduction of NOx with NH3 (NH3-SCR) is investigated. It is found that the activity loss of CeO2-MoO3/TiO2 caused by As oxide is obvious less than that of CeO2/TiO2 catalysts. The fresh and poisoned catalysts are compared and analyzed using XRD, Raman, XPS, H2-TPR and in situ DRIFTS. The results manifest that the introduction of arsenic oxide to CeO2/TiO2 catalyst not only weakens BET surface area, surface acid sites and adsorbed NOx species, but also destroy the redox circle of Ce(4+) to Ce(3+) because of interaction between Ce and As. When MoO3 is added into CeO2/TiO2 system, the main SCR reaction path are found to be changed from the reaction between coordinated NH3 and ad-NOx species to that between an amide and gaseous NO. Additionally, for CeO2-MoO3/TiO2 catalyst, As toxic effect on active sites CeO2 can be released because of stronger As-Mo interaction. Moreover, not only are the reactable Brønsted and Lewis acid sites partly restored, but the cycle of Ce(4+) to Ce(3+) can also be free to some extent. PMID:27474851

  11. Oxidation of elemental mercury by modified spent TiO2-based SCR-DeNOx catalysts in simulated coal-fired flue gas.

    PubMed

    Zhao, Lingkui; Li, Caiting; Zhang, Xunan; Zeng, Guangming; Zhang, Jie; Xie, Yin'e

    2016-01-01

    In order to reduce the costs, the recycle of spent TiO2-based SCR-DeNOx catalysts were employed as a potential catalytic support material for elemental mercury (Hg(0)) oxidation in simulated coal-fired flue gas. The catalytic mechanism for simultaneous removal of Hg(0) and NO was also investigated. The catalysts were characterized by Brunauer-Emmett-Teller (BET), scanning electron microscope (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) method. Results indicated that spent TiO2-based SCR-DeNOx catalyst supported Ce-Mn mixed oxides catalyst (CeMn/SCR1) was highly active for Hg(0) oxidation at low temperatures. The Ce1.00Mn/SCR1 performed the best catalytic activities, and approximately 92.80% mercury oxidation efficiency was obtained at 150 °C. The inhibition effect of NH3 on Hg(0) oxidation was confirmed in that NH3 consumed the surface oxygen. Moreover, H2O inhibited Hg(0) oxidation while SO2 had a promotional effect with the aid of O2. The XPS results illustrated that the surface oxygen was responsible for Hg(0) oxidation and NO conversion. Besides, the Hg(0) oxidation and NO conversion were thought to be aided by synergistic effect between the manganese and cerium oxides. PMID:26370819

  12. Large-scale growth of hierarchical transition-metal vanadate nanosheets on metal meshes as monolith catalysts for De-NOx reaction

    NASA Astrophysics Data System (ADS)

    Huang, Lei; Zhao, Xin; Zhang, Lei; Shi, Liyi; Zhang, Jianping; Zhang, Dengsong

    2015-01-01

    A facile method is developed for the large-scale growth of hierarchical transition-metal (Cu, Fe, and Ni) vanadate nanosheets on corresponding metal mesh as supports. The hierarchical transition-metal vanadate nanosheets were in situ grown on the metal meshes through an orientational etching process and simultaneous nucleation and growth process. Interestingly, the morphologies of the vanadate nanosheets are governed by the balance between dissolution rate and nucleation rate. Thus, the sizes and the thicknesses of the nanosheets could be facilely controlled by the reaction duration, the acidity of the solution and the concentration of vanadate precursor. Furthermore, the hierarchical transition-metal vanadate nanosheets supported on metal meshes are used as monolith catalysts for the selective catalytic reduction (SCR) of NO with NH3. The iron mesh based monolith catalyst shows excellent de-NOx performance with high efficiency and stability in the presence of SO2 and H2O, which provide a promising monolith de-NOx catalyst for stationary source at medium temperatures.A facile method is developed for the large-scale growth of hierarchical transition-metal (Cu, Fe, and Ni) vanadate nanosheets on corresponding metal mesh as supports. The hierarchical transition-metal vanadate nanosheets were in situ grown on the metal meshes through an orientational etching process and simultaneous nucleation and growth process. Interestingly, the morphologies of the vanadate nanosheets are governed by the balance between dissolution rate and nucleation rate. Thus, the sizes and the thicknesses of the nanosheets could be facilely controlled by the reaction duration, the acidity of the solution and the concentration of vanadate precursor. Furthermore, the hierarchical transition-metal vanadate nanosheets supported on metal meshes are used as monolith catalysts for the selective catalytic reduction (SCR) of NO with NH3. The iron mesh based monolith catalyst shows excellent de-NOx

  13. A Comparative Study of N2O Formation during the Selective Catalytic Reduction of NOx with NH3 on Zeolite Supported Cu Catalysts

    SciTech Connect

    Chen, Hai-Ying; Wei, Zhehao; Kollar, Marton; Gao, Feng; Wang, Yilin; Szanyi, Janos; Peden, Charles HF

    2015-09-01

    A comparative study was carried out on a small-pore CHA.Cu and a large-pore BEA.Cu zeolite catalyst to understand the lower N2O formation on small-pore zeolite supported Cu catalysts in the selective catalytic reduction (SCR) of NOx with NH3. On both catalysts, the N2O yield increases with an increase in the NO2/NOx ratios of the feed gas, suggesting N2O formation via the decomposition of NH4NO3. Temperature-programmed desorption experiments reveal that NH4NO3 is more stable on CHA.Cu than on BEA.Cu. In situ FTIR spectra following stepwise (NO2 + O2) and (15NO + NH3 + O2) adsorption and reaction, and product distribution analysis using isotope-labelled reactants, unambiguously prove that surface nitrate groups are essential for the formation of NH4NO3. Furthermore, CHA.Cu is shown to be considerably less active than BEA.Cu in catalyzing NO oxidation and the subsequent formation of surface nitrate groups. Both factors, i.e., (1) the higher thermal stability of NH4NO3 on CHA.Cu, and (2) the lower activity for this catalyst to catalyze NO oxidation and the subsequent formation of surface nitrates, likely contribute to the higher SCR selectivity with less N2O formation on this catalyst as compared to BEA.Cu. The latter is determined as the primary reason since surface nitrates are the source that leads to the formation of NH4NO3 on the catalysts.

  14. Highly-basic large-pore zeolite catalysts for NOx reduction at low temperatures

    DOEpatents

    Penetrante, Bernardino M.; Brusasco, Raymond M.; Merritt, Bernard T.; Vogtlin, George E.

    2004-02-03

    A high-surface-area (greater than 600 m2/g), large-pore (pore size diameter greater than 6.5 angstroms), basic zeolite having a structure such as an alkali metal cation-exchanged Y-zeolite is employed to convert NO.sub.x contained in an oxygen-rich engine exhaust to N.sub.2 and O.sub.2. Preferably, the invention relates to a two-stage method and apparatus for NO.sub.x reduction in an oxygen-rich engine exhaust such as diesel engine exhaust that includes a plasma oxidative stage and a selective reduction stage. The first stage employs a non-thermal plasma treatment of NO.sub.x gases in an oxygen-rich exhaust and is intended to convert NO to NO.sub.2 in the presence of O.sub.2 and added hydrocarbons. The second stage employs a lean-NO.sub.x catalyst including the basic zeolite at relatively low temperatures to convert such NO.sub.2 to environmentally benign gases that include N.sub.2, CO.sub.2, and H.sub.2 O.

  15. Sulfur Management of NOx Adsorber Technology for Diesel Light-Duty Vehicle and Truck Applications

    SciTech Connect

    Fang, Howard L.; Wang, Jerry C.; Yu, Robert C.; Wan, C. Z.; Howden, Ken

    2003-10-01

    Sulfur poisoning from engine fuel and lube is one of the most recognizable degradation mechanisms of a NOx adsorber catalyst system for diesel emission reduction. Even with the availability of 15 ppm sulfur diesel fuel, NOx adsorber will be deactivated without an effective sulfur management. Two general pathways are currently being explored for sulfur management: (1) the use of a disposable SOx trap that can be replaced or rejuvenated offline periodically, and (2) the use of diesel fuel injection in the exhaust and high temperature de-sulfation approach to remove the sulfur poisons to recover the NOx trapping efficiency. The major concern of the de-sulfation process is the many prolonged high temperature rich cycles that catalyst will encounter during its useful life. It is shown that NOx adsorber catalyst suffers some loss of its trapping capacity upon high temperature lean-rich exposure. With the use of a disposable SOx trap to remove large portion of the sulfur poisons from the exhaust, the NOx adsorber catalyst can be protected and the numbers of de-sulfation events can be greatly reduced. Spectroscopic techniques, such as DRIFTS and Raman, have been used to monitor the underlying chemical reactions during NOx trapping/ regeneration and de-sulfation periods, and provide a fundamental understanding of NOx storage capacity and catalyst degradation mechanism using model catalysts. This paper examines the sulfur effect on two model NOx adsorber catalysts. The chemistry of SOx/base metal oxides and the sulfation product pathways and their corresponding spectroscopic data are discussed. SAE Paper SAE-2003-01-3245 {copyright} 2003 SAE International. This paper is published on this website with permission from SAE International. As a user of this website, you are permitted to view this paper on-line, download this pdf file and print one copy of this paper at no cost for your use only. The downloaded pdf file and printout of this SAE paper may not be copied, distributed

  16. Catalysts as sensors--a promising novel approach in automotive exhaust gas aftertreatment.

    PubMed

    Moos, Ralf

    2010-01-01

    Sensors that detect directly and in situ the status of automotive exhaust gas catalysts by monitoring the electrical properties of the catalyst coating itself are overviewed. Examples included in this review are the in-situ determination of the electrical impedance of three-way catalysts based on ceria-zirconia solutions and of lean NO(x) traps of earth-alkaline based coatings, as well as approaches to determine the ammonia loading in Fe-SCR-zeolites with electrical ac measurements. Even more sophisticated approaches based on interactions with electromagnetic waves are also reviewed. For that purpose, metallic stick-like antennas are inserted into the exhaust pipe. The catalyst properties are measured in a contactless manner, directly indicating the catalyst status. The radio frequency probes gauge the oxygen loading degree of three-way catalysts, the NO(x)-loading of lean NO(x) traps, and the soot loading of Diesel particulate filters. PMID:22163575

  17. Enhanced catalytic activity over MIL-100(Fe) loaded ceria catalysts for the selective catalytic reduction of NOx with NH₃ at low temperature.

    PubMed

    Wang, Peng; Sun, Hong; Quan, Xie; Chen, Shuo

    2016-01-15

    The development of catalysts for selective catalytic reduction (SCR) reactions that are highly active at low temperatures and show good resistance to SO2 and H2O is still a challenge. In this study, we have designed and developed a high-performance SCR catalyst based on nano-sized ceria encapsulated inside the pores of MIL-100(Fe) that combines excellent catalytic power with a metal organic framework architecture synthesized by the impregnation method (IM). Transmission electron microscopy (TEM) revealed the encapsulation of ceria in the cavities of MIL-100(Fe). The prepared IM-CeO2/MIL-100(Fe) catalyst shows improved catalytic activity both at low temperatures and throughout a wide temperature window. The temperature window for 90% NOx conversion ranges from 196 to 300°C. X-ray photoelectron spectroscopy (XPS) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFT) analysis indicated that the nano-sized ceria encapsulated inside MIL-100(Fe) promotes the production of chemisorbed oxygen on the catalyst surface, which greatly enhances the formation of the NO2 species responsible for fast SCR reactions. PMID:26414927

  18. Photocatalytic oxidation of NOx over TiO2/HZSM-5 catalysts in the presence of water vapor: Effect of hydrophobicity of zeolites.

    PubMed

    Guo, Gaofei; Hu, Yun; Jiang, Shumei; Wei, Chaohai

    2012-07-15

    TiO(2) hybridized with HZSM-5 zeolites photocatalysts were prepared by a simple solid state dispersion method. The physicochemical properties of the catalysts were characterized by X-ray diffraction, UV-vis diffuse reflectance and FT-IR spectroscopy. The photocatalytic oxidation of NO(x) over TiO(2)/HZSM-5 having different Si/Al ratios was carried out under various levels of humidity and different pre-adsorption times in dark. The TiO(2)/HZSM-5 composite catalysts exhibited higher NO conversion and lower NO(2) formation than pure TiO(2). Pre-adsorption with water vapor and the high humidity during the photoreaction were harmful to the reactivity of TiO(2) hybridized with hydrophilic HZSM-5 zeolite. However, the photocatalytic reactivity of TiO(2) hybridized with hydrophobic zeolite varied little with increase in humidity. The results indicated that the high photocatalytic reactivity of TiO(2)/HZSM-5 catalysts is largely depended on the hydrophobicity of the zeolites. PMID:22579762

  19. DEVELOPMENT OF MULTI-TASK CATALYSTS FOR REMOVAL OF NOx AND TOXIC ORGANIC COMPOUNDS DURING COAL COMBUSTION

    SciTech Connect

    Panagiotis G. Smirniotis; Robert G. Jenkins

    2002-02-04

    The work performed during this project focused on the identification of materials capable of providing high activity and selectivity for the selective catalytic reduction of nitric oxide with ammonia. The material surface characteristics were correlated with the catalytic behavior of our catalysts to increase our understanding and to help improve the DeNO{sub x} efficiency. The catalysts employed in this study include mixed oxide composite powders (TiO{sub 2}-Cr{sub 2}O{sub 3}, TiO{sub 2}-ZrO{sub 2}, TiO{sub 2}-WO{sub 3}, TiO{sub 2}-SiO{sub 2}, and TiO{sub 2}-Al{sub 2}O{sub 3}) loaded with varying amounts of V{sub 2}O{sub 5}, along with 5 different commercial sources of TiO{sub 2}. V{sub 2}O{sub 5} was added to the commercial sources of TiO{sub 2} to achieve monolayer coverage. Since the valence state of vanadium in the precursor solution during the impregnation step significantly impacted catalytic performance, catalysts were synthesized from both V{sup +4} and V{sup +5} solutions explain this phenomenon. Specifically, the synthesis of catalysts from V{sup 5+} precursor solutions yields lower-performance catalysts compared to the case of V{sup 4+} under identical conditions. Aging the vanadium precursor solution, which is associated with the reduction of V{sup 5+} to V{sup 4+} (VO{sub 2}{sup +} {yields} VO{sup 2+}), prior to impregnation results in catalysts with excellent catalytic behavior under identical activation and operating conditions. This work also added vanadia to TiO{sub 2}-based supports with low crystallinity. These supports, which have traditionally performed poorly, are now able to function as effective SCR catalysts. Increasing the acidity of the support by incorporating oxides such as WO{sub 3} and Al{sub 2}O{sub 3} significantly improves the SCR activity and nitrogen selectivity. It was also found that the supports should be synthesized with the simultaneous precipitation of the corresponding precursors. The mixed oxide catalysts possess

  20. Mechanistic insight into aerobic alcohol oxidation using NOx-nitroxide catalysis based on catalyst structure-activity relationships.

    PubMed

    Shibuya, Masatoshi; Nagasawa, Shota; Osada, Yuji; Iwabuchi, Yoshiharu

    2014-11-01

    The mechanism of an NOx-assisted, nitroxide(nitroxyl radical)-catalyzed aerobic oxidation of alcohols was investigated using a set of sterically and electronically modified nitroxides (i.e., TEMPO, AZADO (1), 5-F-AZADO (2), 5,7-DiF-AZADO (3), 5-MeO-AZADO (4), 5,7-DiMeO-AZADO (5), oxa-AZADO (6), TsN-AZADO (7), and DiAZADO (8)). The motivation for the present study stemmed from our previous observation that the introduction of an F atom at a remote position from the nitroxyl radical moiety on the azaadamantane nucleus effectively enhanced the catalytic activity under typical NOx-mediated aerobic-oxidation conditions. The kinetic profiles of the azaadamantane-N-oxyl-[AZADO (1)-, 5-F-AZADO (2)-, and 5,7-DiF-AZADO (3)]-catalyzed aerobic oxidations were closely investigated, revealing that AZADO (1) showed a high initial reaction rate compared to 5-F-AZADO (2) and 5,7-DiF-AZADO (3); however, AZADO-catalyzed oxidation exhibited a marked slowdown, resulting in ∼90% conversion, whereas 5-F-AZADO-catalyzed oxidation smoothly reached completion without a marked slowdown. The reasons for the marked slowdown and the role of the fluoro group are discussed. Oxa-AZADO (6), TsN-AZADO (7), and DiAZADO (8) were designed and synthesized to confirm their comparable catalytic efficiency to that of 5-F-AZADO (2), providing supporting evidence for the electronic effect on the catalytic efficiency of the heteroatoms under NOx-assisted aerobic-oxidation conditions. PMID:25286356

  1. Selective catalytic reduction system and process for treating NOx emissions using a zinc or titanium promoted palladium-zirconium catalyst

    DOEpatents

    Sobolevskiy, Anatoly; Rossin, Joseph A.; Knapke, Michael J.

    2011-08-02

    A process and system (18) for reducing NO.sub.x in a gas using hydrogen as a reducing agent is provided. The process comprises contacting the gas stream (29) with a catalyst system (38) comprising sulfated zirconia washcoat particles (41), palladium, a pre-sulfated zirconia binder (44), and a promoter (45) comprising at least one of titanium, zinc, or a mixture thereof. The presence of zinc or titanium increases the resistance of the catalyst system to a sulfur and water-containing gas stream.

  2. Effects of Ba loading and calcination temperature on BaAl2O4 formation for BaO/Al2O3 NOx Storage and Reduction Catalysts

    SciTech Connect

    Szailer, Tamas; Kwak, Ja Hun; Kim, Do Heui; Szanyi, Janos; Wang, Chong M.; Peden, Charles HF

    2006-04-30

    The effect of thermal treatment on the structure and chemical properties of Ba-oxide-based NOx storage/reduction catalysts with different Ba loadings was investigated using BET, TEM, EDS, TPD and FTIR techniques. On the basis of the present and previously reported results, we propose that moderate (< ~873 K) temperature calcinations result in a single monolayer (ML) ‘coating’ of BaO on the alumina surface. At high Ba loading in excess of that required for a full monolayer ‘coating’ (> 8 wt.% BaO), small (~5 nm) particles of ‘bulk’ BaO are present on top of the 1 ML BaO/Al2O3 surface. We did not observe any detectable morphological changes upon higher temperature thermal treatment of 2 and 8 wt% BaO/Al2O3 samples, while dramatic changes occurred for the 20 wt% sample. In this latter case, the transformations included BaAl2O4 formation at the expense of the bulk BaO phase. In particular, we conclude that the surface (ML) BaO phase is quite stable against thermal treatment, while the bulk phase provides the source of Ba for BaAl2O4 formation.

  3. Ammonia reactions with the stored oxygen in a commercial lean NOx trap catalyst

    SciTech Connect

    Bartova, Sarka; Mracek, David; Koci, Petr; Marek, Milos; Choi, Jae -Soon

    2014-10-12

    Ammonia is an important intermediate of the NOx reduction in a NOx storage and reduction catalyst (aka lean NOx trap). NH3 formed under rich conditions in the reduced front part of the catalyst is transported by convection downstream to the unregenerated (still oxidized) zone of the catalyst, where it further reacts with the stored oxygen and NOx. In this paper, the kinetics and selectivity of NH3 reactions with the stored oxygen are studied in detail with a commercial Ba-based NOx storage catalyst containing platinum group metals (PGM), Ba and Ce oxides. Furthermore, steady-state NH3 decomposition, NH3 oxidation by O2 and NO, and N2O decomposition are examined in light-off experiments. Periodic lean/rich cycling is measured first with O2 and NH3, and then with NOx + O2 and NH3 to discriminate between the NH3 reactions with the stored oxygen and the stored NOx. The reaction of NH3 with the stored O2 is highly selective towards N2, however a certain amount of NOx and N2O is also formed. The formed NOx by-product is efficiently adsorbed on the NOx storage sites such that the NOx is not detected at the reactor outlet except at high temperatures. The stored NOx reacts with NH3 feed in the next rich phase, contributing to the N2O formation. Water inhibits the reactions of NH3 with the stored oxygen. On the contrary, the presence of CO2 increases the NH3 consumption. Furthermore, CO2 is able to provide additional oxygen for NH3 oxidation, forming –CO in analogy to the reverse water gas shift reaction.

  4. NOx Reduction on a Transition Metal-free γ-Al2O3 Catalyst Using Dimethylether (DME)

    SciTech Connect

    Ozensoy, Emrah; Herling, Darrell R.; Szanyi, Janos

    2008-07-15

    NO2 and dimethylether (DME) adsorption as well as DME and NO2 coadsorption on a transition metal-free γ-alumina catalyst were investigated via in-situ transmission Fourier transform infrared spectroscopy (in-situ FTIR), residual gas analysis (RGA) and temperature programmed desorption (TPD) techniques. NO2 adsorption at room temperature leads to the formation of surface nitrates and nitrites. DME adsorption on the alumina surface at 300 K leads to molecularly adsorbed DME, molecularly adsorbed methanol and surface methoxides. Upon heating the DME-exposed alumina to 500-600 K the surface is dominated by methoxide groups. At higher temperatures methoxide groups are converted into formates. At T > 510 K formate decomposition takes place to form H2O(g) and CO(g). DME and NO2 coadsorption at 423 K do not indicate a significant reaction between DME and NO2. However, in similar experiments at 573 K, fast reaction occurs and the methoxides present at 573 K before the NO2 adsorption are converted into formates, simultaneously with the formation of isocyanates. Under these conditions, NCO can further be hydrolyzed into isocyanic acid or ammonia with the help of water which is generated during the formate formation, decomposition and/or NCO formation steps.

  5. Physico-Chemical Property and Catalytic Activity of a CeO2-Doped MnO(x)-TiO2 Catalyst with SO2 Resistance for Low-Temperature NH3-SCR of NO(x).

    PubMed

    Shin, Byeongkil; Chun, Ho Hwan; Cha, Jin-Sun; Shin, Min-Chul; Lee, Heesoo

    2016-05-01

    The effects of CeO2 addition on the catalytic activity and the SO2 resistance of CeO2-doped MnO(x)-TiO2 catalysts were investigated for the low-temperature selective catalytic reduction (SCR) with NH3 of NO(x) emissions in marine applications. The most active catalyst was obtained from 30 wt% CeO2-MnO(x)-TiO2 catalyst in the whole temperature range of 100-300 degrees C at a low gas hourly space velocity (GHSV) of 10,000 h(-)1, and its de-NO(x) efficiency was higher than 90% over 250 degrees C. The enhanced catalytic activity may contribute to the dispersion state and catalytic acidity on the catalyst surface, and the highly dispersed Mn and Ce on the nano-scaled TiO2 catalyst affects the increase of Lewis and Brønsted acid sites. A CeO2-rich additive on MnO(x)-TiO2 could provide stronger catalytic acid sites, associated with NH3 adsorption and the SCR performance. As the results of sulfur resistance in flue gas that contains SO2, the de-NO(x) efficiency of MnO(x)-TiO2 decreased by 15% over 200 degrees C, whereas that of 30 wt% ceria-doped catalyst increased by 14-21% over 150 degrees C. The high SO2 resistance of CeO2-MnO(x)-TiO2 catalysts that resulted from the addition of ceria suppressed the formation of Mn sulfate species, which led to deactivation on the surface of nano-catalyst. PMID:27483759

  6. Ultrafine PM emissions from natural gas, oxidation-catalyst diesel, and particle-trap diesel heavy-duty transit buses.

    PubMed

    Holmén, Britt A; Ayala, Alberto

    2002-12-01

    This paper addresses how current technologies effective for reducing PM emissions of heavy-duty engines may affect the physical characteristics of the particles emitted. Three in-use transit bus configurations were compared in terms of submicron particle size distributions using simultaneous SMPS measurements under two dilution conditions, a minidiluter and the legislated constant volume sampler (CVS). The compressed natural gas (CNG)-fueled and diesel particulate filter (DPF)-equipped diesel configurations are two "green" alternatives to conventional diesel engines. The CNG bus in this study did not have an oxidation catalyst whereas the diesel configurations (with and without particulate filter) employed catalysts. The DPF was a continuously regenerating trap (CRT). Particle size distributions were collected between 6 and 237 nm using 2-minute SMPS scans during idle and 55 mph steady-state cruise operation. Average particle size distributions collected during idle operation of the diesel baseline bus operating on ultralow sulfur fuel showed evidence for nanoparticle growth under CVS dilution conditions relative to the minidiluter. The CRT effectively reduced both accumulation and nuclei mode concentrations by factors of 10-100 except under CVS dilution conditions where nuclei mode concentrations were measured during 55 mph steady-state cruise that exceeded baseline diesel concentrations. The CVS data suggest some variability in trap performance. The CNG bus had accumulation mode concentrations 10-100x lower than the diesel baseline but often displayed large nuclei modes, especially under CVS dilution conditions. Partly this may be explained by the lack of an oxidation catalyst on the CNG, but differences between the minidiluter and CVS size distributions suggest that dilution ratio, temperature-related wall interactions, and differences in tunnel background between the diluters contributed to creating nanoparticle concentrations that sometimes exceeded diesel

  7. Design Strategies for CeO2-MoO3 Catalysts for DeNOx and Hg(0) Oxidation in the Presence of HCl: The Significance of the Surface Acid-Base Properties.

    PubMed

    Chang, Huazhen; Wu, Qingru; Zhang, Tao; Li, Mingguan; Sun, Xiaoxu; Li, Junhua; Duan, Lei; Hao, Jiming

    2015-10-20

    A series of CeMoOx catalysts with different surface Ce/Mo ratios was synthesized by a coprecipitation method via changing precipitation pH value. The surface basicity on selective catalytic reduction (SCR) catalysts (CeMoOx and VMo/Ti) was characterized and correlated to the durability and activity of catalyst for simultaneous elimination of NOx and Hg(0). The pH value in the preparation process affected the surface concentrations of Ce and Mo, the Brunauer-Emmett-Teller (BET) specific surface area, and the acid-base properties over the CeMoOx catalysts. The O 1s X-ray photoelectron spectroscopy (XPS) spectra and CO2-temperature programmed desorption (TPD) suggested that the surface basicity increased as the pH value increased. The existence of strong basic sites contributed to the deactivation effect of HCl over the VMo/Ti and CeMoOx catalysts prepared at pH = 12. For the CeMoOx catalysts prepared at pH = 9 and 6, the appearance of surface molybdena species replaced the surface -OH, and the existence of appropriate medium-strength basic sites contributed to their resistance to HCl poisoning in the SCR reaction. Moreover, these sites facilitated the adsorption and activation of HCl and enhanced Hg(0) oxidation. On the other hand, the inhibitory effect of NH3 on Hg(0) oxidation was correlated with the competitive adsorption of NH3 and Hg(0) on acidic surface sites. Therefore, acidic surface sites may play an important role in Hg(0) adsorption. The characterization and balance of basicity and acidity of an SCR catalyst is believed to be helpful in preventing deactivation by acid gas in the SCR reaction and simultaneous Hg(0) oxidation. PMID:26421943

  8. Influence of the addition of transition metals (Cr, Zr, Mo) on the properties of MnOx-FeOx catalysts for low-temperature selective catalytic reduction of NOx by Ammonia.

    PubMed

    Zhou, Changcheng; Zhang, Yaping; Wang, Xiaolei; Xu, Haitao; Sun, Keqin; Shen, Kai

    2013-02-15

    The co-precipitation and citric acid methods were employed to prepare MnO(x)-FeO(x) catalysts for the low-temperature selective catalytic reduction (SCR) of NO(x) by ammonia. It was found that the Mn-Fe (CP) sample obtained from the co-precipitation method, which exhibited low crystalline of manganese oxides on the surface, high specific surface area and abundant acid sites at the surface, had better catalytic activity. The effects of doping different transition metals (Mo, Zr, Cr) in the Mn-Fe (CP) catalysts were further investigated. The study suggested that the addition of Cr can obviously reduce the take-off temperature of Mn-Fe catalyst to 90°C, while the impregnation of Zr and Mo raised that remarkably. The texture and micro-structure analysis revealed that for the Cr-doped Mn-Fe catalysts, the active components had better dispersion with less agglomeration and sintering and the largest BET surface specific area. In situ FTIR study indicated that the addition of Cr can increase significantly the surface acidity, especially, the Lewis acid sites, and promote the formation of the intermediate -NH(3)(+). H(2)-TPR results confirmed the better low-temperature redox properties of Mn-Fe-Cr. PMID:23142012

  9. Redox properties and metal-support interaction of Pd/Ce0.67Zr0.33O2-Al2O3 catalyst for CO, HC and NOx elimination

    NASA Astrophysics Data System (ADS)

    Lin, Siyu; Yang, Linyan; Yang, Xue; Zhou, Renxian

    2014-06-01

    Ce0.67Zr0.33O2, Ce0.67Zr0.33O2-Al2O3 and γ-Al2O3 supported Pd catalysts (designated as Pd/CZ, Pd/CZA and Pd/Al2O3) have been characterized by XRD, CO chemisorption, in situ DRIFTS, XPS, HRTEM, H2-TPR, O2-TPSR and catalytic performance test. The results show that the small PdOx particles dispersed in CZ would promote the conversion of HC, CO and NO2, while the PdOx particles dispersed in Al2O3 promote the conversion of NO in the light-off process. PdOx species mainly disperse on Al2O3-rich grains surface for fresh Pd/CZA catalyst, but easily migrate onto CZ-rich grains surface due to the strong interaction between Pd and ceria-based oxide under high temperature reaction conditions. And it promotes the thermal stability of PdO species and resilience of Pd0 to PdO, therefore enhances the catalytic performance for HC, CO and NOx elimination. Meanwhile, the interaction between CZ and Al2O3 can be enhanced after aging treatment, resulting in increasing the thermal stability of Pd/CZA catalyst.

  10. HERFD-XANES and XES as complementary operando tools for monitoring the structure of Cu-based zeolite catalysts during NOx-removal by ammonia SCR

    NASA Astrophysics Data System (ADS)

    Günter, T.; Doronkin, D. E.; Carvalho, H. W. P.; Casapu, M.; Grunwaldt, J.-D.

    2016-05-01

    In this article, we demonstrate the potential of hard X-ray techniques to characterize catalysts under working conditions. Operando high energy resolution fluorescence detected (HERFD) XANES and valence to core (vtc) X-ray emission spectroscopy (XES) have been used in a spatially-resolved manner to study Cu-zeolite catalysts during the standard-SCR reaction and related model conditions. The results show a gradient in Cu oxidation state and coordination along the catalyst bed as the reactants are consumed. Vtc-XES gives complementary information on the direct adsorption of ammonia at the Cu sites. The structural information on the catalyst shows the suitability of X-ray techniques to understand catalytic reactions and to facilitate catalyst optimization.

  11. NOx analyser interefence from alkenes

    NASA Astrophysics Data System (ADS)

    Bloss, W. J.; Alam, M. S.; Lee, J. D.; Vazquez, M.; Munoz, A.; Rodenas, M.

    2012-04-01

    Nitrogen oxides (NO and NO2, collectively NOx) are critical intermediates in atmospheric chemistry. NOx abundance controls the levels of the primary atmospheric oxidants OH, NO3 and O3, and regulates the ozone production which results from the degradation of volatile organic compounds. NOx are also atmospheric pollutants in their own right, and NO2 is commonly included in air quality objectives and regulations. In addition to their role in controlling ozone formation, NOx levels affect the production of other pollutants such as the lachrymator PAN, and the nitrate component of secondary aerosol particles. Consequently, accurate measurement of nitrogen oxides in the atmosphere is of major importance for understanding our atmosphere. The most widely employed approach for the measurement of NOx is chemiluminescent detection of NO2* from the NO + O3 reaction, combined with NO2 reduction by either a heated catalyst or photoconvertor. The reaction between alkenes and ozone is also chemiluminescent; therefore alkenes may contribute to the measured NOx signal, depending upon the instrumental background subtraction cycle employed. This interference has been noted previously, and indeed the effect has been used to measure both alkenes and ozone in the atmosphere. Here we report the results of a systematic investigation of the response of a selection of NOx analysers, ranging from systems used for routine air quality monitoring to atmospheric research instrumentation, to a series of alkenes ranging from ethene to the biogenic monoterpenes, as a function of conditions (co-reactants, humidity). Experiments were performed in the European Photoreactor (EUPHORE) to ensure common calibration, a common sample for the monitors, and to unequivocally confirm the alkene (via FTIR) and NO2 (via DOAS) levels present. The instrument responses ranged from negligible levels up to 10 % depending upon the alkene present and conditions used. Such interferences may be of substantial importance

  12. Effect of water and ammonia on surface species formed during NO(x) storage-reduction cycles over Pt-K/Al2O3 and Pt-Ba/Al2O3 catalysts.

    PubMed

    Morandi, Sara; Prinetto, Federica; Castoldi, Lidia; Lietti, Luca; Forzatti, Pio; Ghiotti, Giovanna

    2013-08-28

    The effect of water, in the temperature range 25-350 °C, and ammonia at RT on two different surface species formed on Pt-K/Al2O3 and Pt-Ba/Al2O3 NSR catalysts during NO(x) storage-reduction cycles was investigated. The surface species involved are nitrates, formed during the NO(x) storage step, and isocyanates, which are found to be intermediates in N2 production during reduction by CO. FT-IR experiments demonstrate that the dissociative chemisorption of water and ammonia causes the transformation of the bidentate nitrates and linearly bonded NCO(-) species into more symmetric species that we call ionic species. In the case of water, the effect on nitrates is observable at all the temperatures studied; however, the extent of the transformation decreases upon increasing temperature, consistent with the decreased extent of dissociatively adsorbed water. It was possible to hypothesize that the dissociative chemisorption of water and ammonia takes place in a competitive way on surface sites able to give bidentate nitrates and linearly bonded NCO(-) that are dislocated, remaining on the surface as ionic species. PMID:23860492

  13. Promotion effect of H2 on ethanol oxidation and NOx reduction with ethanol over Ag/Al2O3 catalyst.

    PubMed

    Yu, Yunbo; Li, Yi; Zhang, Xiuli; Deng, Hua; He, Hong; Li, Yuyang

    2015-01-01

    The catalytic partial oxidation of ethanol and selective catalytic reduction of NOx with ethanol (ethanol-SCR) over Ag/Al2O3 were studied using synchrotron vacuum ultraviolet (VUV) photoionization mass spectrometry (PIMS). The intermediates were identified by PIMS and their photoionization efficiency (PIE) spectra. The results indicate that H2 promotes the partial oxidation of ethanol to acetaldehyde over Ag/Al2O3, while the simultaneously occurring processes of dehydration and dehydrogenation were inhibited. H2 addition favors the formation of ammonia during ethanol-SCR over Ag/Al2O3, the occurrence of which creates an effective pathway for NOx reduction by direct reaction with NH3. Simultaneously, the enhancement of the formation of ammonia benefits its reaction with surface enolic species, resulting in producing -NCO species again, leading to enhancement of ethanol-SCR over Ag/Al2O3 by H2. Using VUV-PIMS, the reactive vinyloxy radical was observed in the gas phase during the NOx reduction by ethanol for the first time, particularly in the presence of H2. Identification of such a reaction occurring in the gas phase may be crucial for understanding the reaction pathway of HC-SCR over Ag/Al2O3. PMID:25485626

  14. Diesel Fuel Sulfur Effects on the Performance of Diesel Oxidation Catalysts

    SciTech Connect

    Whitacre, Shawn D.

    2000-08-20

    Research focus: - Impact of sulfur on: Catalyst performance; Short term catalyst durability. This presentation summarizes results from fresh catalyst performance evaluations - WVU contracted to conduct DOC and Lean NOx catalyst testing for DECSE DECSE program. (experimental details discussed previously)

  15. A Fundamental Consideration on NOx Adsorber Technology for DI Diesel Application

    SciTech Connect

    Fang, Howard L.; Huang, Shyan C.; Yu, Robert C.; Wan, C. Z.; Howden, Ken

    2002-10-01

    Diesel engines are far more efficient than gasoline engines of comparable size, and emit less greenhouse gases that have been implicated in global warming. In 2000, the US EPA proposed very stringent emissions standards to be introduced in 2007 along with low sulfur (< 15 ppm) diesel fuel. The California Air Resource Board (CARB) has also established the principle that future diesel fueled vehicles should meet the same low emissions standards as gasoline fueled vehicles and the EPA followed suit with its Tier II emissions regulation. Achieving such low emissions cannot be done through engine development and fuel reformulation alone, and requires application of NOx and particulate matter (PM) aftertreatment control devices. There is a widespread consensus that NOx adsorbers and particulate filter are required in order for diesel engines to meet the 2007 emissions regulations for NOx and PM. In this paper, the key exhaust characteristics from an advanced diesel engine are reviewed. Development of the NOx adsorber technology is discussed. Spectroscopic techniques are applied to understand the underlying chemical reactions over the catalyst surface during NOx trapping and regeneration periods. In-situ surface probes are useful in providing not only thermodynamic and kinetics information required for model development but also a fundamental understanding of storage capacity and degradation mechanisms. The distribution of various nitration/sulfation species is related to surface basicity. Surface displacement reactions of carbonates also play roles in affecting the trapping capability of NOx adsorbers. When ultralow-S fuel is used as a reductant during the regeneration, sulfur induced performance degradation is still observed in an aged catalyst. Other possible sources related to catalyst deactivation include incomplete reduction of surface nitration, coke formation derived from incomplete hydrocarbon burning, and lubricant formulations. Sulfur management and the

  16. Cold-Start Emissions Control in Hybrid Vehicles Equipped with a Passive Hydrocarbon and NOx Adsorber

    SciTech Connect

    Gao, Zhiming; Kim, Miyoung; Choi, Jae-Soon; Daw, C Stuart; Parks, II, James E; Smith, David E

    2012-01-01

    We presents a study of the potential for using low-cost sorbent materials (i.e. Ag-Beta-zeolite and Fe-Mn-Zr transition metal oxides) to temporally trap hydrocarbons (HCs) and nitrogen oxides (NOx) emissions during cold-start periods in HEVs and PHEVs over transient driving cycles. The adsorption behavior of the candidate sorbent materials was characterized in our laboratory flow reactor experiments. The parameters were then used to develop a one-dimensional, transient device model which has been implemented in the Powertrain Systems Analysis Toolkit (PSAT) to simulate a passive HC and NOx absorber device. The results show that such an absorber can substantially reduce HC and NOx emissions by storing them when the 3-way catalyst is too cool to function and re-releasing them when the exhaust temperature rises. These improved emission controls do not involve any penalty in fuel consumption or require any change in engine operation. The cost of these sorbent materials is also much less than conventional 3-way catalysts.

  17. NOx technology for power plant emissions selection of catalysts and type of SCR for process for gas and coal fired power stations

    SciTech Connect

    Ghoreski, D.F.; Negrea, S.

    1993-12-31

    The paper will discuss the basic principle under which SCR system suppliers select the catalyst type and system appropriate for their project. A discussion of temperature, materials, contamination risks and activation properties will be covered for various types of catalysts. The presentation for the selection of type of SCR in the High Dust, Low Dust and Tail gas positions will also be discussed. Further covered is the decision making process to ascertain if an in-duct or conventional SCR system is to be considered. The paper uses examples of pricing for various arrangements in 2,500 MW of gas fired boilers in Southern California a 420 MW coal fired boiler in Florida.

  18. Selective catalytic reduction of NOx with NH3 over a Cu-SSZ-13 catalyst prepared by a solid state ion exchange method

    SciTech Connect

    Wang, Di; Gao, Feng; Peden, Charles HF; Li, Junhui; Kamasamudram, Krishna; Epling, William S.

    2014-06-01

    A novel solid state method was developed to synthesize Cu-SSZ-13 catalysts with excellent NH3-SCR performance and durable hydrothermal stability. After the solid state ion exchange (SSIE) process, the SSZ framework structure and surface area was maintained. In-situ DRIFTS and NH3-TPD experiments provide evidence that isolated Cu ions were successfully exchanged into the pores, which are the active centers for the NH3-SCR reaction.

  19. NOx reduction by electron beam-produced nitrogen atom injection

    DOEpatents

    Penetrante, Bernardino M.

    2002-01-01

    Deactivated atomic nitrogen generated by an electron beam from a gas stream containing more than 99% N.sub.2 is injected at low temperatures into an engine exhaust to reduce NOx emissions. High NOx reduction efficiency is achieved with compact electron beam devices without use of a catalyst.

  20. PLASMA-ASSISTED CATALYTIC REDUCTION OF NOX

    EPA Science Inventory

    Many studies suggest that lean-NOx SCR proceeds via oxidation of NO to NO2 by oxygen, followed by the reaction of the NO2 with hydrocarbons. On catalysts that are not very effective in catalyzing the equilibration of NO+O2 and NO2, the rate of N2 formation is substantially higher...

  1. AMMONIA-FREE NOx CONTROL SYSTEM

    SciTech Connect

    Song Wu; Zhen Fan; Andrew H. Seltzer; Richard G. Herman

    2006-06-01

    This report describes a novel NOx control system that has the potential to drastically reduce cost, and enhance performance, operation and safety of power plant NOx control. The new system optimizes the burner and the furnace to achieve very low NOx levels and to provide an adequate amount of CO, and uses the CO for reducing NO both in-furnace and over a downstream AFSCR (ammonia-free selective catalytic reduction) reactor. The AF-SCR combines the advantages of the highly successful SCR technology for power plants and the TWC (three-way catalytic converter) widely used on automobiles. Like the SCR, it works in oxidizing environment of combustion flue gas and uses only base metal catalysts. Like the TWC, the AF-SCR removes NO and excess CO simultaneously without using any external reagent, such as ammonia. This new process has been studied in a development program jointed funded by the US Department of Energy and Foster Wheeler. The report outlines the experimental catalyst work performed on a bench-scale reactor, including test procedure, operating conditions, and results of various catalyst formulations. Several candidate catalysts, prepared with readily available transition metal oxides and common substrate materials, have shown over 80-90% removal for both NO and CO in oxidizing gas mixtures and at elevated temperatures. A detailed combustion study of a 400 MWe coal-fired boiler, applying computational fluid dynamics techniques to model boiler and burner design, has been carried out to investigate ways to optimize the combustion process for the lowest NOx formation and optimum CO/NO ratios. Results of this boiler and burner optimization work are reported. The paper further discusses catalyst scale-up considerations and the conceptual design of a 400 MWe size AF-SCR reactor, as well as economics analysis indicating large cost savings of the ammonia-free NOx control process over the current SCR technology.

  2. NOX2-dependent regulation of inflammation.

    PubMed

    Singel, Kelly L; Segal, Brahm H

    2016-04-01

    NADPH oxidase (NOX) isoforms together have multiple functions that are important for normal physiology and have been implicated in the pathogenesis of a broad range of diseases, including atherosclerosis, cancer and neurodegenerative diseases. The phagocyte NADPH oxidase (NOX2) is critical for antimicrobial host defence. Chronic granulomatous disease (CGD) is an inherited disorder of NOX2 characterized by severe life-threatening bacterial and fungal infections and by excessive inflammation, including Crohn's-like inflammatory bowel disease (IBD). NOX2 defends against microbes through the direct antimicrobial activity of reactive oxidants and through activation of granular proteases and generation of neutrophil extracellular traps (NETs). NETosis involves the breakdown of cell membranes and extracellular release of chromatin and neutrophil granular constituents that target extracellular pathogens. Although the immediate effects of oxidant generation and NETosis are predicted to be injurious, NOX2, in several contexts, limits inflammation and injury by modulation of key signalling pathways that affect neutrophil accumulation and clearance. NOX2 also plays a role in antigen presentation and regulation of adaptive immunity. Specific NOX2-activated pathways such as nuclear factor erythroid 2-related factor 2 (Nrf2), a transcriptional factor that induces antioxidative and cytoprotective responses, may be important therapeutic targets for CGD and, more broadly, diseases associated with excessive inflammation and injury. PMID:26888560

  3. NOx production in lightning

    NASA Technical Reports Server (NTRS)

    Chameides, W. L.; Stedman, D. H.; Dickerson, R. R.; Rusch, D. W.; Cicerone, R. J.

    1977-01-01

    The rate of odd nitrogen (NOx) production by electrical discharge through air was theoretically and experimentally estimated to be about 60,000 trillion NOx molecules per joule. The theoretical treatment employed a cylindrical shock-wave solution to calculate the rate of NOx production in high temperature reactions. The limits obtained were experimentally verified by subjecting a regulated air flow to electrical discharges followed by a measurement of NOx production using chemiluminescence. These measurements also indicated that water vapor content has no detectable effect on the NOx production rate. The results imply that lightning is a significant source of NOx, producing about 30-40 megatons NOx-N per year and possibly accounting for as much as 50% of the total atmospheric NOx source.

  4. Research Approach for Aging and Evaluating Diesel Exhaust catalysts

    SciTech Connect

    Wayne, Scott

    2000-08-20

    To determine the impact of diesel fuel sulfur levels on emissions control devices that could lower emissions of oxides of nitrogen (NOX) and particulate matter (PM) from on-highway trucks and buses in the 2002-2004 model years. West Virginia University is evaluating: - Diesel Oxidation Catalysts - Lean NOX Catalysts

  5. An examination of the role of plasma treatment for lean NOx reduction over sodium zeolite Y and gamma alumina: Part 1. Plasma assisted NOx reduction over NaY and Al2O3

    SciTech Connect

    Yoon, Ilsop S.; Panov, Alexander G.; Tonkyn, Russell G.; Ebeling, Ana C.; Barlow, Stephan E.; Balmer, Mari Lou

    2002-03-15

    The role of plasma processing on NOx reduction over gammma-alumina and a basic zeolite, NaY was examined. During the plasma treatment NO is oxidized to NO2 and propylene is partially oxidized to CO, CO2, acetaldehyde, and formaldehyde. With plasma treatment, NO as the NOx gas, and a NaY catalyst, the maximum NOx conversion was 70% between 180 and 230?C. The activity decreased at higher and lower temperatures. As high as 80% NOx removal over gamma alumina was measured by a chemiluminescent NOx meter with plasma treatment and NO as the NOx gas. For both catalysts a simultaneous decrease in NOx and aldehydes concentrations was observed, which suggests that aldehyde may be important components for NOx reduction in plasma-treated exhaust.

  6. NOX REMOVAL WITH COMBINED SELECTIVE CATALYTIC REDUCTION AND SELECTIVE NONCATALYTIC REDUCTION: PILOT- SCALE TEST RESULTS

    EPA Science Inventory

    Pilot-scale tests were conducted to develop a combined nitrogen oxide (NOx) reduction technology using both selective catalytic reduction (SCR) and selective noncatalytic reduction (SNCR). A commercially available vanadium-and titatnium-based composite honeycomb catalyst and enh...

  7. HITACHI ZOSEN NOX FLUE GAS TREATMENT PROCESS. VOLUME 1. PILOT PLANT EVALUATION

    EPA Science Inventory

    The report gives results of a pilot plant evaluation of the Hitachi Zosen NOx flue gas treatment process. The project--evaluating selective catalytic reduction (SCR) of NOx on a coal-fired source--operated for 1-1/2 years. A newly developed catalyst, NOXNON 600, was successfully ...

  8. Investigation of NO(x) Removal from Small Engine Exhaust

    NASA Technical Reports Server (NTRS)

    Akyurtlu, Ates; Akyurtlu, Jale F.

    1999-01-01

    Contribution of emissions from small engines to the air pollution is significant. Due to differences in operating conditions and economics, the pollution control systems designed for automobiles will be neither suitable nor economically feasible for use on small engines. The objective of this project was to find a catalyst for the removal of NOx from the exhaust of small engines which use a rich air to fuel ratio. The desired catalyst should be inexpensive so that the cost of the pollution control unit will be only a small fraction of the total equipment cost. The high cost of noble metals makes them too expensive for use as NOx catalyst for small engines. Catalytic reduction of NO can also be accomplished by base-metal oxide catalysts. The main disadvantage of base-metal catalysts is their deactivation by poisons and high temperatures. Requirements for the length of the life of the small engine exhaust catalysts are much less than those for automobile exhaust catalysts. Since there is no oxygen in the exhaust gases, reduction selectivity is not a problem. Also, the reducing exhaust gases might help prevent the harmful interactions of the catalyst with the support. For these reasons only the supported metal oxide catalysts were investigated in this project.

  9. Investigation of NOx Removal from Small Engine Exhaust

    NASA Technical Reports Server (NTRS)

    Akyurtlu, Ates; Akyurtlu, Jale F.

    1999-01-01

    Contribution of emissions from small engines to the air pollution is significant. Due to differences in operating conditions and economics, the pollution control systems designed for automobiles will be neither suitable nor economically feasible for use on small engines. The objective of this project was to find a catalyst for the removal of NOx from the exhaust of small engines which use a rich air to fuel ratio. The desired catalyst should be inexpensive so that the cost of the pollution control unit will be only a small fraction of the total equipment cost. The high cost of noble metals makes them too expensive for use as NOx catalyst for small engines. Catalytic reduction of Nitrogen Oxide (NO) can also be accomplished by base-metal oxide catalysts. The main disadvantage of base-metal catalysts is their deactivation by poisons and high temperatures. Requirements for the length of the life of the small engine exhaust catalysts are much less than those for automobile exhaust catalysts. Since there is no oxygen in the exhaust gases, reduction selectivity is not a problem. Also, the reducing exhaust gases might help prevent the harmful interactions of the catalyst with the support. For these reasons only the supported metal oxide catalysts were investigated in this project.

  10. SELECTIVE CATALYTIC REDUCTION OF DIESEL ENGINE NOX EMISSIONS USING ETHANOL AS A REDUCTANT

    SciTech Connect

    Kass, M; Thomas, J; Lewis, S; Storey, J; Domingo, N; Graves, R Panov, A

    2003-08-24

    NOx emissions from a heavy-duty diesel engine were reduced by more than 90% and 80% utilizing a full-scale ethanol-SCR system for space velocities of 21000/h and 57000/h respectively. These results were achieved for catalyst temperatures between 360 and 400 C and for C1:NOx ratios of 4-6. The SCR process appears to rapidly convert ethanol to acetaldehyde, which subsequently slipped past the catalyst at appreciable levels at a space velocity of 57000/h. Ammonia and N2O were produced during conversion; the concentrations of each were higher for the low space velocity condition. However, the concentration of N2O did not exceed 10 ppm. In contrast to other catalyst technologies, NOx reduction appeared to be enhanced by initial catalyst aging, with the presumed mechanism being sulfate accumulation within the catalyst. A concept for utilizing ethanol (distilled from an E-diesel fuel) as the SCR reductant was demonstrated.

  11. Respiratory alkalosis does not alter NOx concentrations in human plasma and erythrocytes.

    PubMed

    Ishibashi, T; Kubota, K; Himeno, M; Matsubara, T; Hori, T; Ozaki, K; Yamozoe, M; Aizawa, Y; Yoshida, J; Nishio, M

    2001-12-01

    To test the hypothesis that NOx (NO and NO, metabolites of NO) accumulates in red blood cells (RBC) in response to changes in PCO(2) and bicarbonate (HCO) concentration in blood, we examined the effect of changes in PCO(2) and HCO induced by hyperventilation in healthy adults on partitioning of NOx in whole blood. NOx in hemolysate was measured by a high-performance liquid chromatography-Griess system equipped with a C(18) reverse phase column to trap hemoglobin, which enables determination of whole blood NOx concentration and calculation of NOx concentration in RBC with high accuracy and reproducibility. NOx concentration in RBC was lower than that in plasma, and equilibrium between plasma and RBC was achieved rapidly after addition of NO. Changes in PCO(2) and HCO by hyperventilation failed to influence NOx concentrations in both plasma and RBC. Plasma NOx concentrations correlated with whole blood NOx and RBC NOx concentrations. Our results indicate that changes in PCO(2) or HCO induced by hyperventilation do not influence NOx compartmentalization in plasma and RBC. PMID:11709445

  12. Reactions of NO2 with BaO/Pt(111) Model Catalysts: The Effects of BaO Film Thickness and NO2 Pressure on the Formation of Ba(NOx)2 Species

    SciTech Connect

    Mudiyanselage, Kumudu; Yi, Cheol-Woo; Szanyi, Janos

    2011-05-31

    The adsorption and reaction of NO2 on BaO (<1, ~3, and >20 monolayer equivalent (MLE))/Pt(111) model systems were studied with temperature programmed desorption (TPD), X-ray photoelectron spectroscopy (XPS), and infrared reflection absorption spectroscopy (IRAS) under ultra-high vacuum (UHV) as well as elevated pressure conditions. NO2 reacts with sub-monolayer BaO (<1 MLE) to form nitrites only, whereas the reaction of NO2 with BaO (~3 MLE)/Pt(111) produces mainly nitrites and a small amount of nitrates under UHV conditions (PNO2 ~ 1.0 × 10-9 Torr) at 300 K. In contrast, a thick BaO(>20 MLE) layer on Pt(111) reacts with NO2 to form nitrite-nitrate ion pairs under the same conditions. At elevated NO2 pressures (≥ 1.0 × 10-5 Torr), however, BaO layers at all these three coverages convert to amorphous barium nitrates at 300 K. Upon annealing to 500 K, these amorphous barium nitrate layers transform into crystalline phases. The thermal decomposition of the thus-formed Ba(NOx)2 species is also influenced by the coverage of BaO on the Pt(111) substrate: at low BaO coverages, these species decompose at significantly lower temperatures in comparison with those formed on thick BaO films due to the presence of Ba(NOx)2/Pt interface where the decomposition can proceed at lower temperatures. However, the thermal decomposition of the thick Ba(NO3)2 films follows that of bulk nitrates. Results obtained from these BaO/Pt(111) model systems under UHV and elevated pressure conditions clearly demonstrate that both the BaO film thickness and the applied NO2 pressure are critical in the Ba(NOx)2 formation and subsequent thermal decomposition processes.

  13. Comprehensive catalyst management

    SciTech Connect

    Pritchard, S.

    2007-05-15

    From January 2009, as SCR season expands from five months to year-round to meet new US Clean Air Interstate Rule standards, new catalyst strategies are increasingly important. Power plants will need a comprehensive management strategy that accounts for a wide range of old and new issues to achieve peak performance. An optimum plan is necessary for catalyst replacement or addition. SCR systems should be inspected and evaluated at least once a year. Levels of deactivation agents, most often arsenic and calcium oxide, need to match the particular coals used. Tools such as Cormetech's FIELD Guide are available to quantify the effect on catalyst life under various fuel-firing scenarios. Tests should be conducted to evaluate the NH{sub 3}/NOx distribution over time to maximise catalyst performance. The article gives a case study of catalyst management at the Tennessee Valley Authority Allen plant. Recent changes have created new variables to be considered in a catalyst management process, notably the expansion of the operating temperature range, mercury oxidation and SO{sub 3} emission limits. Cormetech has researched these areas. 5 figs., 2 photos.

  14. Advanced Petroleum-Based Fuels - Diesel Emissions Project (APBF-DEC): 2,000-Hour Performance of a NOx Adsorber Catalyst and Diesel Particle Filter System for a Medium-Duty, Pick-Up Diesel Engine Platform; Final Report

    SciTech Connect

    Not Available

    2007-03-01

    Presents the results of a 2,000-hour test of an emissions control system consisting of a nitrogen oxides adsorber catalyst in combination with a diesel particle filter, advanced fuels, and advanced engine controls in an SUV/pick-up truck vehicle platform.

  15. Continuous reduction of cyclic adsorbed and desorbed NO(x) in diesel emission using nonthermal plasma.

    PubMed

    Kuwahara, Takuya; Nakaguchi, Harunobu; Kuroki, Tomoyuki; Okubo, Masaaki

    2016-05-01

    Considering the recent stringent regulations governing diesel NO(x) emission, an aftertreatment system for the reduction of NO(x) in the exhaust gas has been proposed and studied. The proposed system is a hybrid method combining nonthermal plasma and NOx adsorbent. The system does not require precious metal catalysts or harmful chemicals such as urea and ammonia. In the present system, NO(x) in diesel emission is treated by adsorption and desorption by adsorbent as well as nonthermal plasma reduction. In addition, the remaining NO(x) in the adsorbent is desorbed again in the supplied air by residual heat. The desorbed NO(x) in air recirculates into the intake of the engine, and this process, i.e., exhaust gas components' recirculation (EGCR) achieves NO(x) reduction. Alternate utilization of two adsorption chambers in the system can achieve high-efficiency NO(x) removal continuously. An experiment with a stationary diesel engine for electric power generation demonstrates an energy efficiency of 154 g(NO2)/kWh for NO(x) removal and continuous NO(x) reduction of 70.3%. Considering the regulation against diesel emission in Japan, i.e., the new regulation to be imposed on vehicles of 3.5-7.5 ton since 2016, the present aftertreatment system fulfills the requirement with only 1.0% of engine power. PMID:26844402

  16. Reactivity of Pt/BaO/Al₂O₃ for NOx Storage/Reduction: Effects of Pt and Ba Loading

    SciTech Connect

    Kwak, Ja Hun; Kim, Do Heui; Szanyi, Janos; Szailer, Tamas; Peden, Charles HF

    2005-02-01

    The control of NOx (NO and NO₂) emissions from combustion processes, including vehicle engines, remains a challenge particularly for systems operating at high air-to-fuel ratios (so-called ‘lean’ combustion). The current “3-way”, precious metal-based catalytic converters are unable to selectively reduce NOx with reductants (e.g., CO and residual unburned hydrocarbon) in the presence of excess O₂. In the last few years, worldwide environmental regulations regarding NOx emissions from diesel engines (inherently operated ‘lean’) have become significantly more stringent resulting in considerable research efforts to reduce NOx under the highly oxidizing engine operation conditions. Urea selective catalytic reduction (SCR) and non-thermal plasma assisted NOx reduction have been explored as possible technologies. In recent years, alkaline and alkaline earth oxide-based NOx storage/reduction catalysts (especially BaO/Al₂O₃) have been developed, and have shown promising activities for lean-NOx reduction [1,2].

  17. Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials.

    PubMed

    Beale, A M; Gao, F; Lezcano-Gonzalez, I; Peden, C H F; Szanyi, J

    2015-10-21

    The ever increasing demand to develop highly fuel efficient engines coincides with the need to minimize air pollution originating from the exhaust gases of internal combustion engines. Dramatically improved fuel efficiency can be achieved at air-to-fuel ratios much higher than stoichiometric. In the presence of oxygen in large excess, however, traditional three-way catalysts are unable to reduce NOx. Among the number of lean-NOx reduction technologies, selective catalytic reduction (SCR) of NOx by NH3 over Cu- and Fe-ion exchanged zeolite catalysts has been extensively studied over the past 30+ years. Despite the significant advances in developing a viable practical zeolite-based catalyst for lean NOx reduction, the insufficient hydrothermal stabilities of the zeolite structures considered cast doubts about their real-world applicability. During the past decade renewed interest in zeolite-based lean NOx reduction was spurred by the discovery of the very high activity of Cu-SSZ-13 (and the isostructural Cu-SAPO-34) in the NH3-SCR of NOx. These new, small-pore zeolite-based catalysts not only exhibited very high NOx conversion and N2 selectivity, but also exhibited exceptionally high hydrothermal stability at high temperatures. In this review we summarize the key discoveries of the past ∼5 years that led to the introduction of these catalysts into practical applications. This review first briefly discusses the structure and preparation of the CHA structure-based zeolite catalysts, and then summarizes the key learnings of the rather extensive (but not complete) characterisation work. Then we summarize the key findings of reaction kinetic studies, and provide some mechanistic details emerging from these investigations. At the end of the review we highlight some of the issues that still need to be addressed in automotive exhaust control catalysis. PMID:25913215

  18. DIESEL NOX CONTROL APPLICATION

    EPA Science Inventory

    The paper gives results of a project to design, develop, and demonstrate a diesel engine nitrogen oxide (NOx) and particulate matter (PM) control package that will meet the U.S. Navy's emission control requirements. (NOTE: In 1994, EPA issued a Notice for Proposed Rule Making (NP...

  19. The Simplest Amino-borane H2 B=NH2 Trapped on a Rhodium Dimer: Pre-Catalysts for Amine-Borane Dehydropolymerization.

    PubMed

    Kumar, Amit; Beattie, Nicholas A; Pike, Sebastian D; Macgregor, Stuart A; Weller, Andrew S

    2016-06-01

    The μ-amino-borane complexes [Rh2 (L(R) )2 (μ-H)(μ-H2 B=NHR')][BAr(F) 4 ] (L(R) =R2 P(CH2 )3 PR2 ; R=Ph, (i) Pr; R'=H, Me) form by addition of H3 B⋅NMeR'H2 to [Rh(L(R) )(η(6) -C6 H5 F)][BAr(F) 4 ]. DFT calculations demonstrate that the amino-borane interacts with the Rh centers through strong Rh-H and Rh-B interactions. Mechanistic investigations show that these dimers can form by a boronium-mediated route, and are pre-catalysts for amine-borane dehydropolymerization, suggesting a possible role for bimetallic motifs in catalysis. PMID:27100775

  20. Oxidation catalyst

    DOEpatents

    Ceyer, Sylvia T.; Lahr, David L.

    2010-11-09

    The present invention generally relates to catalyst systems and methods for oxidation of carbon monoxide. The invention involves catalyst compositions which may be advantageously altered by, for example, modification of the catalyst surface to enhance catalyst performance. Catalyst systems of the present invention may be capable of performing the oxidation of carbon monoxide at relatively lower temperatures (e.g., 200 K and below) and at relatively higher reaction rates than known catalysts. Additionally, catalyst systems disclosed herein may be substantially lower in cost than current commercial catalysts. Such catalyst systems may be useful in, for example, catalytic converters, fuel cells, sensors, and the like.

  1. Trapped Surfaces

    NASA Astrophysics Data System (ADS)

    Senovilla, José M. M.

    I review the definition and types of (closed) trapped surfaces. Surprising global properties are shown, such as their "clairvoyance" and the possibility that they enter into flat portions of the spacetime. Several results on the interplay of trapped surfaces with vector fields and with spatial hypersurfaces are presented. Applications to the quasi-local definition of Black Holes are discussed, with particular emphasis set onto marginally trapped tubes, trapping horizons and the boundary of the region with closed trapped surfaces. Finally, the core of a trapped region is introduced, and its importance discussed.

  2. Trapped Surfaces

    NASA Astrophysics Data System (ADS)

    Senovilla, José M. M.

    2013-03-01

    I review the definition and types of (closed) trapped surfaces. Surprising global properties are pointed out, such as their "clairvoyance" and the possibility that they enter into flat portions of the spacetime. Several results on the interplay of trapped surfaces with vector fields and with spatial hypersurfaces are presented. Applications to the quasi-local definition of Black Holes are analyzed, with particular emphasis set onto marginally trapped tubes, trapping horizons and the boundary of the region with closed trapped surfaces. Finally, the core of a trapped region is introduced, and its importance briefly discussed.

  3. Fischer-Tropsch-Type Production of Organic Materials in the Solar Nebula: Studies Using Graphite Catalysts and Measuring the Trapping of Noble Gases

    NASA Technical Reports Server (NTRS)

    Nuth, Joseph A., III; Ferguson, Frank T.; Lucas, Christopher; Kimura, Yuki; Hohenberg, Charles

    2009-01-01

    The formation of abundant carbonaceous material in meteorites is a long standing problem and an important factor in the debate on the potential for the origin of life in other stellar systems. The Fischer-Tropsch-type (FTT) catalytic reduction of CO by hydrogen was once the preferred model for production of organic materials in the primitive solar nebula. We have demonstrated that many grain surfaces can catalyze both FTT and HB-type reactions, including amorphous iron and magnesium silicates, pure silica smokes as well as several minerals. Graphite is not a particularly good FTT catalyst, especially compared to iron powder or to amorphous iron silicate. However, like other silicates that we have studied, it gets better with exposure to CO. N2 and H2 over time: e.g., after formation of a macromolecular carbonaceous layer on the surfaces of the underlying gains. While amorphous iron silicates required only 1 or 2 experimental runs to achieve steady state reaction rates, graphite only achieved steady state after 6 or more experiments. We will present results showing the catalytic action of graphite grains increasing with increasing number of experiments and will also discuss the nature of the final "graphite" grains aster completion of our experiments.

  4. ULTRA LOW NOx CATALYTIC COMBUSTION FOR IGCC POWER PLANTS

    SciTech Connect

    Lance L. Smith

    2004-03-01

    Tests were performed in PCI's sub-scale high-pressure (10 atm) test rig, using PCI's two-stage (catalytic / gas-phase) combustion process for syngas fuel. In this process, the first stage is a Rich-Catalytic Lean-burn (RCL{trademark}) catalytic reactor, wherein a fuel-rich mixture contacts the catalyst and reacts while final and excess combustion air cool the catalyst. The second stage is a gas-phase combustor, wherein the catalyst cooling air mixes with the catalytic reactor effluent to provide for final gas-phase burnout and dilution to fuel-lean combustion products. During the reporting period, PCI successfully achieved NOx = 0.011 lbs/MMBtu at 10 atm pressure (corresponding to 2.0 ppm NOx corrected to 15% O{sub 2} dry) with near-zero CO emissions, surpassing the project goal of < 0.03 lbs/MMBtu NOx. These emissions levels were achieved at scaled (10 atm, sub-scale) baseload conditions corresponding to Tampa Electric's Polk Power Station operation on 100% syngas (no co-firing of natural gas).

  5. LOW NOX BURNER DEVELOPMENT

    SciTech Connect

    KRISHNA,C.R.; BUTCHER,T.

    2004-09-30

    The objective of the task is to develop concepts for ultra low NOx burners. One approach that has been tested previously uses internal recirculation of hot gases and the objective was to how to implement variable recirculation rates during burner operation. The second approach was to use fuel oil aerosolization (vaporization) and combustion in a porous medium in a manner similar to gas-fired radiant burners. This task is trying the second approach with the use of a somewhat novel, prototype system for aerosolization of the liquid fuel.

  6. Kinetic and spectroscopic study of catalysts for water-gas shift and nitrogen oxide removal

    NASA Astrophysics Data System (ADS)

    Kispersky, Vincent Frederick

    Nitrogen oxides (NOx) are formed in high temperature combustion processes such as in power generation and motor vehicles. Increasingly stringent regulation of these harmful emissions continues to drive interest in developing, understanding and studying new catalytic formulations for exhaust aftertreatment. For mobile sources, predominantly heavy duty diesel engines, selective catalytic reduction (SCR) with NH3 has become the principal means of NO x abatement. An alternative technology developed, but now surpassed by SCR, is NOx Storage Reduction (NSR) catalysis. Both technologies have been studied in our laboratory and are the basis for this dissertation. We studied seven different lean NOx trap (LNT) monolith formulations for NSR ranging from 0.6 to 6.2 wt.% Pt and 4 to 20 wt.% Ba loadings on γ-Al 2O3. The noble metal component of a LNT oxidizes NO to NO 2 aiding in the storage of NO2 on the alkaline earth component. Before the storage component saturates, a reductant such as H2 is introduced into the vehicular exhaust and the stored NOx is released and reduced to N2. Once the storage component is free of NOx, reductant flow is ceased and storage is begun anew. Our research focused on understanding the effects that CO2 and H2O have on the storage capacity of the LNT over short as well as extended periods of time. We found that for high Ba loadings, CO 2 had a consistently detrimental effect on the fast NOx storage capacity (NSC), defined as the amount of NOx the catalyst can store before 1% of the inlet NOx is measured in the reactor outlet. Over long NOx storage periods, CO2 continued to inhibit storage compared to the same catalyst in CO2 free conditions. On low loadings of Ba, however, the inhibition of CO2 was significantly reduced. We found that the loading dependent characteristics of the Ba phase affected the way in which CO2 adsorbed on the storage component, which greatly affected the stability of the species on lower Ba loadings. The less stable

  7. Novel fluidized bed reactor for integrated NOx adsorption-reduction with hydrocarbons

    SciTech Connect

    Terris T. Yang; Hsiaotao T. Bi

    2009-07-01

    In order to avoid the negative impact of excessive oxygen in the combustion flue gases on the selectivity of most hydrocarbon selective catalytic reduction (HC-SCR) catalysts, an integrated NOx adsorption-reduction process has been proposed in this study for the treatment of flue gases under lean burn conditions by decoupling the adsorption and reduction into two different zones. The hypothesis has been validated in a novel internal circulating fluidized bed (ICFB) reactor using Fe/ZSM-5 as the catalyst and propylene as the reducing agent. Effects of propylene to the NOx molar ratio, flue gas oxygen concentration, and gas velocity on NOx conversion were studied using simulated flue gases. The results showed that increasing the ratio of HC:NO improved the reduction performance of Fe/ZSM-5 in the ICFB reactor. NOx conversion decreased with an increasing flue gas flow velocity in the annulus U{sub A} but increased with an increasing reductant gas flow velocity in the draft tube U{sub D}. The NOx adsorption ratio decreased with increasing U{sub A}. In most cases, NOx conversion was higher than the adsorption ratio due to the relatively poor adsorption performance of the catalyst. Fe/ZSM-5 showed a promising reduction performance and a strong inhibiting ability on the negative impact of excessive O{sub 2} in the ICFB reactor, proving that such an ICFB reactor possessed the ability to overcome the negative impact of excessive O{sub 2} in the flue gas using Fe/ZSM-5 as the deNOx catalyst. 22 refs., 10 figs.

  8. Process of activation of a palladium catalyst system

    DOEpatents

    Sobolevskiy, Anatoly; Rossin, Joseph A.; Knapke, Michael J.

    2011-08-02

    Improved processes for activating a catalyst system used for the reduction of nitrogen oxides are provided. In one embodiment, the catalyst system is activated by passing an activation gas stream having an amount of each of oxygen, water vapor, nitrogen oxides, and hydrogen over the catalyst system and increasing a temperature of the catalyst system to a temperature of at least 180.degree. C. at a heating rate of from 1-20.degree./min. Use of activation processes described herein leads to a catalyst system with superior NOx reduction capabilities.

  9. NOx Control Options and Integration for US Coal Fired Boilers

    SciTech Connect

    Mike Bockelie; Marc Cremer; Kevin Davis; Martin Denison; Adel Sarofim; Connie Senior; Hong-Shig Shim; Dave Swenson; Bob Hurt; Eric Suuberg; Eric Eddings; Kevin Whitty; Larry Baxter; Calvin Bartholomew; William Hecker

    2006-06-30

    This is the Final Report for DOE Cooperative Agreement No: DE-FC26-00NT40753. The goal of the project was to develop cost-effective analysis tools and techniques for demonstrating and evaluating low-NOx control strategies and their possible impact on boiler performance for boilers firing US coals. The Electric Power Research Institute (EPRI) provided co-funding for this program. This project included research on: (1) In furnace NOx control; (2) Impacts of combustion modifications on boiler operation; (3) Selective Catalytic Reduction (SCR) catalyst testing and (4) Ammonia adsorption/removal on fly ash. Important accomplishments were achieved in all aspects of the project. Rich Reagent Injection (RRI), an in-furnace NOx reduction strategy based on injecting urea or anhydrous ammonia into fuel rich regions in the lower furnace, was evaluated for cyclone-barrel and PC fired utility boilers. Field tests successfully demonstrated the ability of the RRI process to significantly reduce NOx emissions from a staged cyclone-fired furnace operating with overfire air. The field tests also verified the accuracy of the Computational Fluid Dynamic (CFD) modeling used to develop the RRI design and highlighted the importance of using CFD modeling to properly locate and configure the reagent injectors within the furnace. Low NOx firing conditions can adversely impact boiler operation due to increased waterwall wastage (corrosion) and increased soot production. A corrosion monitoring system that uses electrochemical noise (ECN) corrosion probes to monitor, on a real-time basis, high temperature corrosion events within the boiler was evaluated. Field tests were successfully conducted at two plants. The Ohio Coal Development Office provided financial assistance to perform the field tests. To investigate soot behavior, an advanced model to predict soot production and destruction was implemented into an existing reacting CFD modeling tool. Comparisons between experimental data collected

  10. Method and apparatus for reducing NOx emissions

    SciTech Connect

    Spokoyny, F.E.; Krigmont, H.V.

    1993-08-24

    A method is described of reducing NOx from a flue gas stream produced from a burner, which flue gas stream passes from the burner through a rotary regenerative heat exchanger which rotates in a direction generally transverse to the direction of the flow of the flue gas stream and wherein at least a portion of the heat transfer elements of the heat exchanger carry a catalyst which, in the presence of a nitrogeneous compound, promote the reduction of NOx from the flue gas stream passing thereby, comprising the steps of: injecting a quantity of a nitrogeneous compound onto the catalyzed heat transfer elements, such injecting being at a plurality of fixed locations along the arcuate path of travel of the catalyzed elements with respect to the flue gas stream; determining the temperature of the portion of the heat transfer elements as such elements travel in an arcuate path with respect to the flow of the flue gas stream; and in response to said step of determining, selectively varying the quantity of nitrogeneous compound injected at each of such fixed locations.

  11. THE ACID RAIN NOX PROGRAM

    EPA Science Inventory

    Between 350,000 and 400,000 tons of annual NOx emissions have been eliminated as a result of Phase I of the Acid Rain NOx Program. As expected. the utilities have chosen emissions averaging as the primary compliance option. This reflects that, in general, NO x reductions have ...

  12. Don't NOx Texas

    SciTech Connect

    Mathis, J.D.; Lachowicz, Y.

    2005-07-01

    Modifications to boiler combustion systems allow Fayette Power Projects units 1 and 2 to meet new NOx emissions limits east of La Grange in Eastern Texas. The article describes modifications executed by Alstom in 2004 which attained an overall reduction in NOx emissions of almost 69%. 4 figs., 1 tab., 1 photo.

  13. Two-stage Catalytic Reduction of NOx with Hydrocarbons

    SciTech Connect

    Umit S. Ozkan; Erik M. Holmgreen; Matthew M. Yung; Jonathan Halter; Joel Hiltner

    2005-12-21

    A two-stage system for the catalytic reduction of NO from lean-burn natural gas reciprocating engine exhaust is investigated. Each of the two stages uses a distinct catalyst. The first stage is oxidation of NO to NO{sub 2} and the second stage is reduction of NO{sub 2} to N{sub 2} with a hydrocarbon. The central idea is that since NO{sub 2} is a more easily reduced species than NO, it should be better able to compete with oxygen for the combustion reaction of hydrocarbon, which is a challenge in lean conditions. Early work focused on demonstrating that the N{sub 2} yield obtained when NO{sub 2} was reduced was greater than when NO was reduced. NO{sub 2} reduction catalysts were designed and silver supported on alumina (Ag/Al{sub 2}O{sub 3}) was found to be quite active, able to achieve 95% N{sub 2} yield in 10% O{sub 2} using propane as the reducing agent. The design of a catalyst for NO oxidation was also investigated, and a Co/TiO{sub 2} catalyst prepared by sol-gel was shown to have high activity for the reaction, able to reach equilibrium conversion of 80% at 300 C at GHSV of 50,000h{sup -1}. After it was shown that NO{sub 2} could be more easily reduced to N{sub 2} than NO, the focus shifted on developing a catalyst that could use methane as the reducing agent. The Ag/Al{sub 2}O{sub 3} catalyst was tested and found to be inactive for NOx reduction with methane. Through iterative catalyst design, a palladium-based catalyst on a sulfated-zirconia support (Pd/SZ) was synthesized and shown to be able to selectively reduce NO{sub 2} in lean conditions using methane. Development of catalysts for the oxidation reaction also continued and higher activity, as well as stability in 10% water, was observed on a Co/ZrO{sub 2} catalyst, which reached equilibrium conversion of 94% at 250 C at the same GHSV. The Co/ZrO{sub 2} catalyst was also found to be extremely active for oxidation of CO, ethane, and propane, which could potential eliminate the need for any separate

  14. Optical trapping

    PubMed Central

    Neuman, Keir C.; Block, Steven M.

    2006-01-01

    Since their invention just over 20 years ago, optical traps have emerged as a powerful tool with broad-reaching applications in biology and physics. Capabilities have evolved from simple manipulation to the application of calibrated forces on—and the measurement of nanometer-level displacements of—optically trapped objects. We review progress in the development of optical trapping apparatus, including instrument design considerations, position detection schemes and calibration techniques, with an emphasis on recent advances. We conclude with a brief summary of innovative optical trapping configurations and applications. PMID:16878180

  15. COLD TRAPS

    DOEpatents

    Thompson, W.I.

    1958-09-30

    A cold trap is presented for removing a condensable component from a gas mixture by cooling. It consists of a shell, the exterior surface of which is chilled by a refrigerant, and conductive fins welded inside the shell to condense the gas, and distribute the condensate evenly throughout the length of the trap, so that the trap may function until it becomes completely filled with the condensed solid. The contents may then be removed as either a gas or as a liquid by heating the trap. This device has particuinr use as a means for removing uranium hexafluoride from the gaseous diffusion separation process during equipment breakdown and repair periods.

  16. New vanadium trap proven in commercial trials

    SciTech Connect

    Dougan, T.J. ); Alkemade, U.; Lakhanpal, B. ); Boock, L.T. )

    1994-09-26

    A vanadium trap technology called RV4+ has demonstrated in a variety of commercial fluid catalytic cracking (FCC) units its ability to reduce vanadium on equilibrium catalyst by more than 20%. Reducing vanadium loading increases microactivity and zeolite surface area retention, confirming that RV4+ protects zeolites from vanadium deactivation. Sulfur competition had prevented some previous traps from working commercially, but was not a factor with the new trap. The technology can save refiners millions of dollars per year in catalyst costs, or allow them to process feeds containing higher vanadium concentrations. The paper discusses vanadium traps, deactivation mechanism, history of traps, vanadium mobility, intraparticle mobility, interparticle mobility, measuring performance, commercial results, sulfur competition, and economic value.

  17. Noble metal ionic catalysts.

    PubMed

    Hegde, M S; Madras, Giridhar; Patil, K C

    2009-06-16

    Because of growing environmental concerns and increasingly stringent regulations governing auto emissions, new more efficient exhaust catalysts are needed to reduce the amount of pollutants released from internal combustion engines. To accomplish this goal, the major pollutants in exhaust-CO, NO(x), and unburned hydrocarbons-need to be fully converted to CO(2), N(2), and H(2)O. Most exhaust catalysts contain nanocrystalline noble metals (Pt, Pd, Rh) dispersed on oxide supports such as Al(2)O(3) or SiO(2) promoted by CeO(2). However, in conventional catalysts, only the surface atoms of the noble metal particles serve as adsorption sites, and even in 4-6 nm metal particles, only 1/4 to 1/5 of the total noble metal atoms are utilized for catalytic conversion. The complete dispersion of noble metals can be achieved only as ions within an oxide support. In this Account, we describe a novel solution to this dispersion problem: a new solution combustion method for synthesizing dispersed noble metal ionic catalysts. We have synthesized nanocrystalline, single-phase Ce(1-x)M(x)O(2-delta) and Ce(1-x-y)Ti(y)M(x)O(2-delta) (M = Pt, Pd, Rh; x = 0.01-0.02, delta approximately x, y = 0.15-0.25) oxides in fluorite structure. In these oxide catalysts, Pt(2+), Pd(2+), or Rh(3+) ions are substituted only to the extent of 1-2% of Ce(4+) ion. Lower-valent noble metal ion substitution in CeO(2) creates oxygen vacancies. Reducing molecules (CO, H(2), NH(3)) are adsorbed onto electron-deficient noble metal ions, while oxidizing (O(2), NO) molecules are absorbed onto electron-rich oxide ion vacancy sites. The rates of CO and hydrocarbon oxidation and NO(x) reduction (with >80% N(2) selectivity) are 15-30 times higher in the presence of these ionic catalysts than when the same amount of noble metal loaded on an oxide support is used. Catalysts with palladium ion dispersed in CeO(2) or Ce(1-x)Ti(x)O(2) were far superior to Pt or Rh ionic catalysts. Therefore, we have demonstrated that the

  18. HWVP Iodine Trap Evaluation

    SciTech Connect

    Burger, Leland L.; Scheele, Randall D.

    2004-09-24

    This report details our assessment of the chemistry of the planned Hanford Waste Vitrification Plant (HWVP) off-gas system and its impact on the applicability of known iodine removal and control methods. To predict the gaseous species in the off-gas system, we completed thermodynamic calculations to determine theoretical equilibrium concentrations of the various potential chemical species. In addition, we found that HWVP pilot-plant experiments were generally consistent with the known chemistry of the individual elements present in the off gas. Of the known trapping techniques for radioiodine, caustic scrubbing and silver-containing sorbents are, in our opinion, the most attractive methods to reduce the iodine concentration in the HWVP melter off gas (MOG) after it has passed through the high-efficiency particulate air (HEPA) filter. These two methods were selected because they (1) have demonstrated retention factors (RFs), ratio of amount in and amount out, of 10 to 1000, which would be sufficient to reduce the iodine concentration in the MOG to below regulatory limits; (2) are simple to apply; (3) are resistant to oxidizing gases such as NOx; (4) do not employ highly hazardous or highly corrosive agents; (5) require containment vessels constructed or common materials; (6) have received extensive laboratory development; (7) and the radioactive wastes produced should be easy to handle. On the basis of iodine trapping efficiency, simplicity of operation, and waste management, silver sorbents are superior to caustic scrubbing, and, or these sorbents, we prefer the silver zeolites. No method has been fully demonstrated, from laboratory-scale through pilot-plant testing, to be an effective iodine trap at the low iodine concentration (2 x 10-11 mol I/L) expected in the MOG of the HWVP in the presence of the other gaseous off gas components. In terms of compatibility of the trapping technology with the components in the MOG, there is some question about the resistance of

  19. NOx Binding and Dissociation: Enhanced Ferroelectric Surface Chemistry by Catalytic Monolayers

    NASA Astrophysics Data System (ADS)

    Kakekhani, Arvin; Ismail-Beigi, Sohrab

    2013-03-01

    NOx molecules are regulated air pollutants produced during automotive combustion. As part of an effort to design viable catalysts for NOx decomposition operating at higher temperatures that would allow for improved fuel efficiency, we examine NOx chemistry on ferroelectric perovskite surfaces. Changing the direction of ferroelectric polarization can modify surface electronic properties and may lead to switchable surface chemistry. Here, we describe our recent work on potentially enhanced surface chemistry using catalytic RuO2 monolayers on perovskite ferroelectric substrates. In addition to thermodynamic stabilization of the RuO2 layer, we present results on the polarization-dependent binding of NO, O2, N2, and atomic O and N. We present results showing that one key problem with current catalysts, involving the difficulty of releasing dissociation products (especially oxygen), can be ameliorated by this method. Primary support from Toyota Motor Engineering and Manufacturing, North America, Inc.

  20. Method for reducing NOx during combustion of coal in a burner

    DOEpatents

    Zhou, Bing; Parasher, Sukesh; Hare, Jeffrey J.; Harding, N. Stanley; Black, Stephanie E.; Johnson, Kenneth R.

    2008-04-15

    An organically complexed nanocatalyst composition is applied to or mixed with coal prior to or upon introducing the coal into a coal burner in order to catalyze the removal of coal nitrogen from the coal and its conversion into nitrogen gas prior to combustion of the coal. This process leads to reduced NOx production during coal combustion. The nanocatalyst compositions include a nanoparticle catalyst that is made using a dispersing agent that can bond with the catalyst atoms. The dispersing agent forms stable, dispersed, nano-sized catalyst particles. The catalyst composition can be formed as a stable suspension to facilitate storage, transportation and application of the catalyst nanoparticles to a coal material. The catalyst composition can be applied before or after pulverizing the coal material or it may be injected directly into the coal burner together with pulverized coal.

  1. 40 CFR 97.12 - Changing NOX authorized account representative and alternate NOX authorized account...

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Changing NOX authorized account representative and alternate NOX authorized account representative; changes in owners and operators. 97.12... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Authorized...

  2. 40 CFR 97.12 - Changing NOX authorized account representative and alternate NOX authorized account...

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Changing NOX authorized account representative and alternate NOX authorized account representative; changes in owners and operators. 97.12... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Authorized...

  3. Copper catalysts for soot oxidation: alumina versus perovskite supports.

    PubMed

    López-Suárez, F E; Bueno-López, A; Illán-Gómez, M J; Adamski, A; Ura, B; Trawczynski, J

    2008-10-15

    Copper catalysts prepared using four supports (Mg- and Sr-modified Al2O3 and MgTiO3 and SrTiO3 perovskites) have been tested for soot oxidation by 02 and NOx/O2. Among the catalysts studied, Cu/SrTiO3 is the most active for soot oxidation by NOx/O2 and the support affects positively copper activity. With this catalyst, and under the experimental conditions used, the soot combustion by NOx/O2 presents a considerable rate from 500 degrees C (100 degrees C below the uncatalysed reaction). The Cu/ SrTiO3 catalyst is also the most effective for NOx chemisorption around 425 degrees C. The best activity of Cu/SrTiO3 can be attributed to the improved redox properties of copper originated by Cu-support interactions. This seems to be related to the presence of weakly bound oxygen on this sample. The copper species present in the catalyst Cu/SrTiO3 can be reduced more easily than those in other supports, and for this reason, this catalyst seems to be the most effective to convert NO into NO2, which explains its highest activity for soot oxidation. PMID:18983091

  4. Novel fluidized bed reactor for integrated NO(x) adsorption-reduction with hydrocarbons.

    PubMed

    Yang, Terris T; Bi, Hsiaotao T

    2009-07-01

    In order to avoid the negative impact of excessive oxygen in the combustion flue gases on the selectivity of most hydrocarbon selective catalytic reduction (HC-SCR) catalysts, an integrated NO(x) adsorption-reduction process has been proposed in this study for the treatment of flue gases under lean burn conditions by decoupling the adsorption and reduction into two different zones. The hypothesis has been validated in a novel internal circulating fluidized bed (ICFB) reactor using Fe/ZSM-5 as the catalyst and propylene as the reducing agent. Effects of propylene to the NO(x) molar ratio, flue gas oxygen concentration, and gas velocity on NO(x) conversion were studied using simulated flue gases. The results showed that increasing the ratio of HC:NO improved the reduction performance of Fe/ZSM-5 in the ICFB reactor. NO(x) conversion decreased with an increasing flue gas flow velocity in the annulus U(A) but increased with an increasing reductant gas flow velocity in the draft tube U(D). The NO(x) adsorption ratio decreased with increasing U(A). In most cases, NO(x) conversion was higher than the adsorption ratio due to the relatively poor adsorption performance of the catalyst. Fe/ZSM-5 showed a promising reduction performance and a strong inhibiting ability on the negative impact of excessive O2 in the ICFB reactor, proving that such an ICFB reactor possessed the ability to overcome the negative impact of excessive O2 in the flue gas using Fe/ZSM-5 as the deNO(x) catalyst. PMID:19673305

  5. SOURCEBOOK: NOX CONTROL TECHNOLOGY DATA

    EPA Science Inventory

    The report, a compilation of available information on the control of nitrogen oxide (NOx) emissions from stationary sources, is provided to assist new source permitting activities by regulatory agencies. he sources covered are combustion turbines, internal combustion engines, non...

  6. Kinetic and spectroscopic study of catalysts for water-gas shift and nitrogen oxide removal

    NASA Astrophysics Data System (ADS)

    Kispersky, Vincent Frederick

    Nitrogen oxides (NOx) are formed in high temperature combustion processes such as in power generation and motor vehicles. Increasingly stringent regulation of these harmful emissions continues to drive interest in developing, understanding and studying new catalytic formulations for exhaust aftertreatment. For mobile sources, predominantly heavy duty diesel engines, selective catalytic reduction (SCR) with NH3 has become the principal means of NO x abatement. An alternative technology developed, but now surpassed by SCR, is NOx Storage Reduction (NSR) catalysis. Both technologies have been studied in our laboratory and are the basis for this dissertation. We studied seven different lean NOx trap (LNT) monolith formulations for NSR ranging from 0.6 to 6.2 wt.% Pt and 4 to 20 wt.% Ba loadings on γ-Al 2O3. The noble metal component of a LNT oxidizes NO to NO 2 aiding in the storage of NO2 on the alkaline earth component. Before the storage component saturates, a reductant such as H2 is introduced into the vehicular exhaust and the stored NOx is released and reduced to N2. Once the storage component is free of NOx, reductant flow is ceased and storage is begun anew. Our research focused on understanding the effects that CO2 and H2O have on the storage capacity of the LNT over short as well as extended periods of time. We found that for high Ba loadings, CO 2 had a consistently detrimental effect on the fast NOx storage capacity (NSC), defined as the amount of NOx the catalyst can store before 1% of the inlet NOx is measured in the reactor outlet. Over long NOx storage periods, CO2 continued to inhibit storage compared to the same catalyst in CO2 free conditions. On low loadings of Ba, however, the inhibition of CO2 was significantly reduced. We found that the loading dependent characteristics of the Ba phase affected the way in which CO2 adsorbed on the storage component, which greatly affected the stability of the species on lower Ba loadings. The less stable

  7. Engine NOx reduction system

    SciTech Connect

    Berriman, L.P.; Zabsky, J.M.; Davis, J.W.; Hylton, W.H.

    1993-07-06

    Apparatus for use with an engine having a power-generating portion that burns a hydrocarbon fuel and air and produces hot exhaust gases is described, having a catalytic converter device that includes a catalyst for enhancing reactions of components of said exhaust gases, and having a conduit that couples said power-generating portion to said catalytic converter device, for reducing pollution in the exhaust, wherein said power-generating portion comprises a plurality of cylinders in which said fuel and air are burned, a mechanism for applying fuel and air to said cylinders, and a plurality of exhaust valves through which burned fuel and air is exhausted and which are connected to said upstream end of said conduit, said conduit including a manifold which is connected to a plurality of said exhaust valves and a downstream conduit portion which connects said manifold to said catalytic converter device, comprising: a device coupled to said conduit, which stores ammonia and injects it into said conduit at a location where the exhaust gases have a substantially maximum temperature, but which is devoid of open flames, to mix with said hot exhaust gases and pass with them along said conduit and then through said catalyst, said location being closer to said power-generating portion than to said catalytic converter and lying in said manifold.

  8. Ultra Low NOx Catalytic Combustion for IGCC Power Plants

    SciTech Connect

    Shahrokh Etemad; Benjamin Baird; Sandeep Alavandi; William Pfefferle

    2008-03-31

    In order to meet DOE's goals of developing low-emissions coal-based power systems, PCI has further developed and adapted it's Rich-Catalytic Lean-burn (RCL{reg_sign}) catalytic reactor to a combustion system operating on syngas as a fuel. The technology offers ultra-low emissions without the cost of exhaust after-treatment, with high efficiency (avoidance of after-treatment losses and reduced diluent requirements), and with catalytically stabilized combustion which extends the lower Btu limit for syngas operation. Tests were performed in PCI's sub-scale high-pressure (10 atm) test rig, using a two-stage (catalytic then gas-phase) combustion process for syngas fuel. In this process, the first stage consists of a fuel-rich mixture reacting on a catalyst with final and excess combustion air used to cool the catalyst. The second stage is a gas-phase combustor, where the air used for cooling the catalyst mixes with the catalytic reactor effluent to provide for final gas-phase burnout and dilution to fuel-lean combustion products. During testing, operating with a simulated Tampa Electric's Polk Power Station syngas, the NOx emissions program goal of less than 0.03 lbs/MMBtu (6 ppm at 15% O{sub 2}) was met. NOx emissions were generally near 0.01 lbs/MMBtu (2 ppm at 15% O{sub 2}) (PCI's target) over a range on engine firing temperatures. In addition, low emissions were shown for alternative fuels including high hydrogen content refinery fuel gas and low BTU content Blast Furnace Gas (BFG). For the refinery fuel gas increased resistance to combustor flashback was achieved through preferential consumption of hydrogen in the catalytic bed. In the case of BFG, stable combustion for fuels as low as 88 BTU/ft{sup 3} was established and maintained without the need for using co-firing. This was achieved based on the upstream catalytic reaction delivering a hotter (and thus more reactive) product to the flame zone. The PCI catalytic reactor was also shown to be active in ammonia

  9. Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials

    SciTech Connect

    Beale, Andrew M.; Gao, Feng; Lezcano-Gonzalez, Ines; Peden, Charles HF; Szanyi, Janos

    2015-10-05

    The ever increasing demand to develop highly fuel efficient engines coincides with the need to minimize air pollution originating from the exhaust gases of internal combustion engines. Dramatically improved fuel efficiency can be achieved at air-to-fuel ratios much higher than stoichiometric. In the presence of oxygen in large excess, however, traditional three-way catalysts are unable to reduce NOx. Among the number of lean-NOx reduction technologies, selective catalytic reduction (SCR) of NOx by NH3 over Cu- and Fe-ion exchanged zeolite catalysts has been extensively studied over the past 30+ years. Despite the significant advances in developing a viable practical zeolite-based catalyst for lean NOx reduction, the insufficient hydrothermal stabilities of the zeolite structures considered cast doubts about their real-world applicability. During the past decade a renewed interest in zeolite-based lean NOx reduction was spurred by the discovery of the very high activity of Cu-SSZ-13 (and the isostructural Cu-SAPO-34) in the NH3 SCR of NOx. These new, small-pore zeolite-based catalysts not only exhibited very high NOx conversion and N2 selectivity, but also exhibited exceptional high hydrothermal stability at high temperatures. In this review we summarize the key discoveries of the past ~5 years that lead to the introduction of these catalysts into practical application. The review first briefly discusses the structure and preparation of the CHA structure-based zeolite catalysts, and then summarizes the key learnings of the rather extensive (but not complete) characterisation work. Then we summarize the key findings of reaction kinetics studies, and provide some mechanistic details emerging from these investigations. At the end of the review we highlight some of the issues that are still need to be addressed in automotive exhaust control catalysis. Funding A.M.B. and I.L.G. would like to thank EPSRC for funding. F.G., C.H.F.P. and J.Sz. gratefully acknowledge

  10. Nox NADPH Oxidases and the Endoplasmic Reticulum

    PubMed Central

    Araujo, Thaís L.S.; Abrahão, Thalita B.

    2014-01-01

    Abstract Significance: Understanding isoform- and context-specific subcellular Nox reduced nicotinamide adenine dinucleotide phosphate (NADPH) oxidase compartmentalization allows relevant functional inferences. This review addresses the interplay between Nox NADPH oxidases and the endoplasmic reticulum (ER), an increasingly evident player in redox pathophysiology given its role in redox protein folding and stress responses. Recent Advances: Catalytic/regulatory transmembrane subunits are synthesized in the ER and their processing includes folding, N-glycosylation, heme insertion, p22phox heterodimerization, as shown for phagocyte Nox2. Dual oxidase (Duox) maturation also involves the regulation by ER-resident Duoxa2. The ER is the activation site for some isoforms, typically Nox4, but potentially other isoforms. Such location influences redox/Nox-mediated calcium signaling regulation via ER targets, such as sarcoendoplasmic reticulum calcium ATPase (SERCA). Growing evidence suggests that Noxes are integral signaling elements of the unfolded protein response during ER stress, with Nox4 playing a dual prosurvival/proapoptotic role in this setting, whereas Nox2 enhances proapoptotic signaling. ER chaperones such as protein disulfide isomerase (PDI) closely interact with Noxes. PDI supports growth factor-dependent Nox1 activation and mRNA expression, as well as migration in smooth muscle cells, and PDI overexpression induces acute spontaneous Nox activation. Critical Issues: Mechanisms of PDI effects include possible support of complex formation and RhoGTPase activation. In phagocytes, PDI supports phagocytosis, Nox activation, and redox-dependent interactions with p47phox. Together, the results implicate PDI as possible Nox organizer. Future Directions: We propose that convergence between Noxes and ER may have evolutive roots given ER-related functional contexts, which paved Nox evolution, namely calcium signaling and pathogen killing. Overall, the interplay between

  11. The SCONOx catalytic absorption system: Combined CO, NOx, and SOx control for power generation

    SciTech Connect

    MacDonald, R.J.; Girdlestone, T.

    1998-07-01

    Goal Line Environmental Technologies has revolutionized the pollution control industry with its SCONOx{trademark} Catalytic Absorption System for Power Generation. The system has been installed at Sunlaw Energy Corporation's Federal Cogeneration Plant since December 20, 1996, with average NOx readings of less than 2 ppm and average CO readings of less than 1 ppm in base load operation. This plant is a 30 MW facility that fires a GE LM2500 gas turbine. The SCONOx{trademark} system uses a single catalyst for both CO and NOx control. It oxidizes CO to CO{sub 2} and NO to NO{sub 2}, and the NO{sub 2} is then absorbed onto the surface of the catalyst. Just as a sponge absorbs water and must be wrung out periodically, the SCONOx{trademark} catalyst must be periodically regenerated. This is accomplished by passing a dilute hydrogen gas across the surface of the catalyst in the absence of oxygen. Nitrogen oxides are broken down into nitrogen and water vapor, and this is exhausted up the stack instead of NOx. No ammonia or other hazardous materials are required in the process. Goal Line's SCOCOx{trademark} Sulfur Removal System works in a similar manner, sub favors the absorption of sulfur compounds instead of NOx. The SCONOx{trademark}/SCOSOx{trademark} system is a breakthrough in CO, NOx, and SOx control technology that makes it possible to have clean air without the use of ammonia or other hazardous materials. This paper will describe the development of the system and full-scale operational results, as well as focusing on the implications that SCONOx{trademark} as an ultra-clean pollution control technology has on the power generation industry.

  12. Lean NOx Reduction in Two Stages: Non-thermal Plasma Followed by Heterogeneous Catalysis

    SciTech Connect

    Tonkyn, Russell G.; Yoon, Ilsop S.; Barlow, Stephan E.; Panov, Alexander G.; Kolwaite, A; Balmer, Mari LOU.

    2000-10-16

    We present data in this paper showing that non-thermal plasma in combination with heterogeneous catalysis is a promising technique for the treatment of NOx in diesel exhaust. Using a commonly available zeolite catalyst, sodium Y, to treat synthetic diesel exhaust we report approximately 50% chemical reduction of NOx over a broad, representative temperature range. We have measured the overall efficiency as a function of the temperature and hydrocarbon concentration. The direct detection of N2 and N2O when the background gas is replaced by helium confirms that true chemical reduction is occurring.

  13. NOx adsorber and method of regenerating same

    SciTech Connect

    Endicott, Dennis L.; Verkiel, Maarten; Driscoll, James J.

    2007-01-30

    New technologies, such as NOx adsorber catalytic converters, are being used to meet increasingly stringent regulations on undesirable emissions, including NOx emissions. NOx adsorbers must be periodically regenerated, which requires an increased fuel consumption. The present disclosure includes a method of regenerating a NOx adsorber within a NOx adsorber catalytic converter. At least one sensor positioned downstream from the NOx adsorber senses, in the downstream exhaust, at least one of NOx, nitrous oxide and ammonia concentrations a plurality of times during a regeneration phase. The sensor is in communication with an electronic control module that includes a regeneration monitoring algorithm operable to end the regeneration phase when a time rate of change of the at least one of NOx, nitrous oxide and ammonia concentrations is after an expected plateau region begins.

  14. 40 CFR 52.2237 - NOX RACT and NOX conformity exemption.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 4 2011-07-01 2011-07-01 false NOX RACT and NOX conformity exemption... PROGRAMS (CONTINUED) APPROVAL AND PROMULGATION OF IMPLEMENTATION PLANS (CONTINUED) Tennessee § 52.2237 NOX RACT and NOX conformity exemption. Approval. EPA is approving the section 182(f) oxides of...

  15. 40 CFR 96.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false CAIR NOX allowance allocations to CAIR NOX opt-in units. 96.188 Section 96.188 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS...

  16. 40 CFR 97.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false CAIR NOX allowance allocations to CAIR NOX opt-in units. 97.188 Section 97.188 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING...

  17. 40 CFR 96.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Allowance Tracking System responsibilities of NOX authorized account representative. 96.52 Section 96.52 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX...

  18. 40 CFR 96.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Allowance Tracking System responsibilities of NOX authorized account representative. 96.52 Section 96.52 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX...

  19. 40 CFR 96.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false CAIR NOX allowance allocations to CAIR NOX opt-in units. 96.188 Section 96.188 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS...

  20. 40 CFR 52.2237 - NOX RACT and NOX conformity exemption.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 4 2010-07-01 2010-07-01 false NOX RACT and NOX conformity exemption... PROGRAMS (CONTINUED) APPROVAL AND PROMULGATION OF IMPLEMENTATION PLANS (CONTINUED) Tennessee § 52.2237 NOX RACT and NOX conformity exemption. Approval. EPA is approving the section 182(f) oxides of...

  1. 40 CFR 97.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false CAIR NOX allowance allocations to CAIR NOX opt-in units. 97.188 Section 97.188 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING...

  2. 40 CFR 96.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false NOX Allowance Tracking System... SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.52 NOX Allowance Tracking System responsibilities of NOX authorized account representative. (a) Following...

  3. 40 CFR 96.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false NOX Allowance Tracking System... SO 2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.52 NOX Allowance Tracking System responsibilities of NOX authorized account representative. (a) Following...

  4. 40 CFR 97.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false NOX Allowance Tracking System... NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.52 NOX Allowance Tracking System... Tracking System account, all submissions to the Administrator pertaining to the account, including, but...

  5. 40 CFR 97.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false NOX Allowance Tracking System... NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.52 NOX Allowance Tracking System... Tracking System account, all submissions to the Administrator pertaining to the account, including, but...

  6. 40 CFR 97.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false NOX Allowance Tracking System... NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.52 NOX Allowance Tracking System... Tracking System account, all submissions to the Administrator pertaining to the account, including, but...

  7. 40 CFR 96.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false NOX Allowance Tracking System... SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.52 NOX Allowance Tracking System responsibilities of NOX authorized account representative. (a) Following...

  8. 40 CFR 97.60 - Submission of NOX allowance transfers.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Submission of NOX allowance transfers... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Transfers § 97.60 Submission of NOX allowance transfers. The NOX authorized account representatives...

  9. 40 CFR 97.11 - Alternate NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Alternate NOX authorized account... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Authorized Account Representative for NOX Budget Sources § 97.11 Alternate NOX authorized...

  10. 40 CFR 97.11 - Alternate NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Alternate NOX authorized account... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Authorized Account Representative for NOX Budget Sources § 97.11 Alternate NOX authorized...

  11. 40 CFR 96.60 - Submission of NOX allowance transfers.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Submission of NOX allowance transfers... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Transfers § 96.60 Submission of NOX allowance transfers. The NOX...

  12. 40 CFR 96.60 - Submission of NOX allowance transfers.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Submission of NOX allowance transfers... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Transfers § 96.60 Submission of NOX allowance transfers. The NOX...

  13. 40 CFR 97.60 - Submission of NOX allowance transfers.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Submission of NOX allowance transfers... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Transfers § 97.60 Submission of NOX allowance transfers. The NOX authorized account representatives...

  14. Bimetallic Catalysts.

    ERIC Educational Resources Information Center

    Sinfelt, John H.

    1985-01-01

    Chemical reaction rates can be controlled by varying composition of miniscule clusters of metal atoms. These bimetallic catalysts have had major impact on petroleum refining, where work has involved heterogeneous catalysis (reacting molecules in a phase separate from catalyst.) Experimentation involving hydrocarbon reactions, catalytic…

  15. Investigation of Mixed Oxide Catalysts for NO Oxidation

    SciTech Connect

    Szanyi, Janos; Karim, Ayman M.; Pederson, Larry R.; Kwak, Ja Hun; Mei, Donghai; Tran, Diana N.; Herling, Darrell R.; Muntean, George G.; Peden, Charles HF; Howden, Ken; Qi, Gongshin; Li, Wei

    2014-12-09

    The oxidation of engine-generated NO to NO2 is an important step in the reduction of NOx in lean engine exhaust because NO2 is required for the performance of the LNT technology [2], and it enhances the activities of ammonia selective catalytic reduction (SCR) catalysts [1]. In particular, for SCR catalysts an NO:NO2 ratio of 1:1 is most effective for NOx reduction, whereas for LNT catalysts, NO must be oxidized to NO2 before adsorption on the storage components. However, NO2 typically constitutes less than 10% of NOx in lean exhaust, so catalytic oxidation of NO is essential. Platinum has been found to be especially active for NO oxidation, and is widely used in DOC and LNT catalysts. However, because of the high cost and poor thermal durability of Pt-based catalysts, there is substantial interest in the development of alternatives. The objective of this project, in collaboration with partner General Motors, is to develop mixed metal oxide catalysts for NO oxidation, enabling lower precious metal usage in emission control systems. [1] M. Koebel, G. Madia, and M. Elsener, Catalysis Today 73, 239 (2002). [2] C. H. Kim, G. S. Qi, K. Dahlberg, and W. Li, Science 327, 1624 (2010).

  16. Oxyhydrochlorination catalyst

    DOEpatents

    Taylor, Charles E.; Noceti, Richard P.

    1992-01-01

    An improved catalyst and method for the oxyhydrochlorination of methane is disclosed. The catalyst includes a pyrogenic porous support on which is layered as active material, cobalt chloride in major proportion, and minor proportions of an alkali metal chloride and of a rare earth chloride. On contact of the catalyst with a gas flow of methane, HCl and oxygen, more than 60% of the methane is converted and of that converted more than 40% occurs as monochloromethane. Advantageously, the monochloromethane can be used to produce gasoline boiling range hydrocarbons with the recycle of HCl for further reaction. This catalyst is also of value for the production of formic acid as are analogous catalysts with lead, silver or nickel chlorides substituted for the cobalt chloride.

  17. NOx Control Options and Integration for US Coal Fired Boilers

    SciTech Connect

    Mike Bockelie; Kevin Davis; Temi Linjewile; Connie Senior; Eric Eddings; Kevin Whitty; Larry Baxter; Calvin Bartholomew; William Hecker; Stan Harding

    2003-06-30

    This is the twelfth Quarterly Technical Report for DOE Cooperative Agreement No: DE-FC26-00NT40753. The goal of the project is to develop cost effective analysis tools and techniques for demonstrating and evaluating low NOx control strategies and their possible impact on boiler performance for boilers firing US coals. The Electric Power Research Institute (EPRI) is providing co-funding for this program. This program contains multiple tasks and good progress is being made on all fronts. During this quarter, a new effort was begun on the development of a corrosion management system for minimizing the impacts of low NOx combustion systems on waterwalls; a kickoff meeting was held at the host site, AEP's Gavin Plant, and work commenced on fabrication of the probes. FTIR experiments for SCR catalyst sulfation were finished at BYU and indicated no vanadium/vanadyl sulfate formation at reactor conditions. Improvements on the mass-spectrometer system at BYU have been made and work on the steady state reactor system shakedown neared completion. The slipstream reactor continued to operate at AEP's Rockport plant; at the end of the quarter, the catalysts had been exposed to flue gas for about 1000 hours. Some operational problems were addressed that enable the reactor to run without excessive downtime by the end of the quarter.

  18. Ripple Trap

    NASA Technical Reports Server (NTRS)

    2006-01-01

    3 April 2006 This Mars Global Surveyor (MGS) Mars Orbiter Camera (MOC) image shows the margin of a lava flow on a cratered plain in the Athabasca Vallis region of Mars. Remarkably, the cratered plain in this scene is essentially free of bright, windblown ripples. Conversely, the lava flow apparently acted as a trap for windblown materials, illustrated by the presence of the light-toned, wave-like texture over much of the flow. That the lava flow surface trapped windblown sand and granules better than the cratered plain indicates that the flow surface has a rougher texture at a scale too small to resolve in this image.

    Location near: 10.7oN, 204.5oW Image width: 3 km (1.9 mi) Illumination from: lower left Season: Northern Winter

  19. Three-Dimensional Composite Nanostructures for Lean NOx Emission Control

    SciTech Connect

    Gao, Pu-Xian

    2013-07-31

    This final report to the Department of Energy (DOE) and National Energy Technology Laboratory (NETL) for DE-EE0000210 covers the period from October 1, 2009 to July 31, 2013. Under this project, DOE awarded UConn about $1,248,242 to conduct the research and development on a new class of 3D composite nanostructure based catalysts for lean NOx emission control. Much of the material presented here has already been submitted to DOE/NETL in quarterly technical reports. In this project, through a scalable solution process, we have successfully fabricated a new class of catalytic reactors, i.e., the composite nanostructure array (nano-array) based catalytic converters. These nanocatalysts, distinct from traditional powder washcoat based catalytic converters, directly integrate monolithic substrates together with nanostructures with well-defined size and shape during the scalable hydrothermal process. The new monolithic nanocatalysts are demonstrated to be able to save raw materials including Pt-group metals and support metal oxides by an order of magnitude, while perform well at various oxidation (e.g., CO oxidation and NO oxidation) and reduction reactions (H{sub 2} reduction of NOx) involved in the lean NOx emissions. The size, shape and arrangement of the composite nanostructures within the monolithic substrates are found to be the key in enabling the drastically reduced materials usage while maintaining the good catalytic reactivity in the enabled devices. The further understanding of the reaction kinetics associated with the unique mass transport and surface chemistry behind is needed for further optimizing the design and fabrication of good nanostructure array based catalytic converters. On the other hand, the high temperature stability, hydrothermal aging stability, as well as S-poisoning resistance have been investigated in this project on the nanocatalysts, which revealed promising results toward good chemical and mechanical robustness, as well as S

  20. Method And Apparatus For Regenerating Nox Adsorbers

    DOEpatents

    Driscoll, J. Joshua; Endicott, Dennis L.; Faulkner, Stephen A.; Verkiel, Maarten

    2006-03-28

    Methods and apparatuses for regenerating a NOx adsorber coupled with an exhaust of an engine. An actuator drives a throttle valve to a first position when regeneration of the NOx adsorber is desired. The first position is a position that causes the regeneration of the NOx adsorber. An actuator drives the throttle valve to a second position while regeneration of the NOx adsorber is still desired. The second position being a position that is more open than the first position and operable to regenerate a NOx adsorber.

  1. Controlling NOx emission from industrial sources

    SciTech Connect

    Srivastava, R.K.; Nueffer, W.; Grano, D.; Khan, S.; Staudt, J.E.; Jozewicz, W.

    2005-07-01

    A number of regulatory actions focused on reducing NOx emissions from stationary combustion sources have been taken in the United States in the last decade. These actions include the Acid Rain NOx regulations, the Ozone Transport Commission's NOx Budget Program, and the NOx SIP Call rulemakings. In addition to these regulations, the recent Interstate Air Quality Rulemaking proposal and other bills in the Congress are focusing on additional reductions of NOx. Industrial combustion sources accounted for about 18016 of NOx emissions in the United States in 2000 and constituted the second largest emitting source category within stationary sources, only behind electric utility sources. Based on these data, reduction of NOx emissions from industrial combustion sources is an important consideration in efforts undertaken to address the environmental concerns associated with NOx. This paper discusses primary and secondary NOx control technologies applicable to various major categories of industrial sources. The sources considered in this paper include large boilers, furnaces and fired heaters, combustion turbines, large IC engines, and cement kilns. For each source category considered in this paper, primary NOx controls are discussed first, followed by a discussion of secondary NOx controls.

  2. Polymerization catalyst

    SciTech Connect

    Graves, V.

    1987-05-12

    A process is described for polymerizing at least one alpha olefin under conditions characteristic of Ziegler polymerization wherein the polymerization is conducted in the presence of a catalyst system which comprises: a supported catalyst prepared under anhydrous conditions by the sequential steps of: preparing a slurry of inert particulate support material; adding to the slurry a solution of an organomagnesium compound; adding to the slurry and reacting a solution of a zirconium halide compound, hafnium compound or mixtures thereof; adding to the slurry and reacting a halogenator; adding to the slurry and reacting a tetravalent titanium halide compound; and recovering solid catalyst.

  3. Polymerization catalyst

    SciTech Connect

    Graves, V.

    1986-10-21

    A process is described for polymerizing at least one alpha-olefin under conditions characteristic of Ziegler polymerization wherein the polymerization is conducted in the presence of a catalyst comprising: a supported catalyst prepared under anhydrous conditions by the steps of: (1) sequentially; (a) preparing a slurry of inert particulate support material; (b) adding to the slurry a solution of an organomagnesium compound; (c) adding to the slurry and reacting a solution of zirconium compound; and (2) thereafter; (d) adding to the slurry and reacting a halogenator; (e) adding to the slurry and reacting a tetravalent titanium compound; (f) recovering solid catalyst; and an organoaluminum compound.

  4. PHOTOCATALYTIC OXIDATION FOR NOx ABATEMENT: DEVELOPMENT OF A KINETIC EXPRESSION AND DESIGN TOOLS

    SciTech Connect

    Rajiv Srivastava; M. A. Ebadian

    2000-09-15

    The ''Nitrogen Oxides Emission Reduction Program'' and ''Ozone Non-Attainment Program'' in the 1990 Clean Air Act provide guidelines for controlling NOx (NO and NO{sub 2}) emissions in new and existing stationary sources. NOx emissions have local (air quality), regional (acid rain), and global (ozone production) consequences. This study aids in developing the photocatalyst technology that has potential for use in abatement of NOx. The objective of the proposed project is to apply the principles of chemical engineering fundamentals--reaction kinetics, transport phenomena and thermodynamics--in the process design for a system that will utilize a photocatalytic reactor to oxidize NOx to nitric acid (HNO{sub 3}). HNO{sub 3} can be more easily trapped than NOx on adsorbent surfaces or in water. The project dealt with the engineering aspect of the gas-solid heterogeneous oxidation of NOx. The experiments were conducted in a photocatalyst wash-coated glass flow tube reactor. A mathematical model was developed based on a rigorous description of the physical and chemical processes occurring in the reactor. The mathematical model took into account (1) intrinsic reaction kinetics (i.e., true reaction rates), (2) transport phenomena that deal with the mass transfer effects in the reactor, and (3) the geometry of the reactor. The experimental results were used for validation of the mathematical model that provides the basis for a versatile and reliable method for the purpose of design, scale-up and process control. The NOx abatement was successfully carried out in a flow tube reactor surrounded by black lights under the exploratory grant. Due to lack of funds, a comprehensive kinetic analysis for the photocatalytic reaction scheme could not be carried out. The initial experiments look very promising for use of photocatalysis for NOx abatement.

  5. Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3

    SciTech Connect

    Kwak, Ja Hun; Tonkyn, Russell G.; Kim, Do Heui; Szanyi, Janos; Peden, Charles HF

    2010-10-21

    Superior activity and selectivity of a Cu ion-exchanged SSZ-13 zeolite in the selective catalytic reduction (SCR) of NOx with NH3 were observed, in comparison to Cu-beta and Cu-ZSM-5 zeolites. Cu-SSZ-13 was not only more active in the NOx SCR reaction over the entire temperature range studied (up to 550 °C), but also more selective toward nitrogen formation, resulting in significantly lower amounts of NOx by-products (i.e., NO2 and N2O) than the other two zeolites. In addition, Cu-SSZ-13 demonstrated the highest activity and N2 formation selectivity in the oxidation of NH3. The results of this study strongly suggest that Cu-SSZ-13 is a promising candidate as a catalyst for NOx SCR with great potential in after-treatment systems for either mobile or stationary sources.

  6. Trapped antihydrogen.

    PubMed

    Andresen, G B; Ashkezari, M D; Baquero-Ruiz, M; Bertsche, W; Bowe, P D; Butler, E; Cesar, C L; Chapman, S; Charlton, M; Deller, A; Eriksson, S; Fajans, J; Friesen, T; Fujiwara, M C; Gill, D R; Gutierrez, A; Hangst, J S; Hardy, W N; Hayden, M E; Humphries, A J; Hydomako, R; Jenkins, M J; Jonsell, S; Jørgensen, L V; Kurchaninov, L; Madsen, N; Menary, S; Nolan, P; Olchanski, K; Olin, A; Povilus, A; Pusa, P; Robicheaux, F; Sarid, E; el Nasr, S Seif; Silveira, D M; So, C; Storey, J W; Thompson, R I; van der Werf, D P; Wurtele, J S; Yamazaki, Y

    2010-12-01

    Antimatter was first predicted in 1931, by Dirac. Work with high-energy antiparticles is now commonplace, and anti-electrons are used regularly in the medical technique of positron emission tomography scanning. Antihydrogen, the bound state of an antiproton and a positron, has been produced at low energies at CERN (the European Organization for Nuclear Research) since 2002. Antihydrogen is of interest for use in a precision test of nature's fundamental symmetries. The charge conjugation/parity/time reversal (CPT) theorem, a crucial part of the foundation of the standard model of elementary particles and interactions, demands that hydrogen and antihydrogen have the same spectrum. Given the current experimental precision of measurements on the hydrogen atom (about two parts in 10(14) for the frequency of the 1s-to-2s transition), subjecting antihydrogen to rigorous spectroscopic examination would constitute a compelling, model-independent test of CPT. Antihydrogen could also be used to study the gravitational behaviour of antimatter. However, so far experiments have produced antihydrogen that is not confined, precluding detailed study of its structure. Here we demonstrate trapping of antihydrogen atoms. From the interaction of about 10(7) antiprotons and 7 × 10(8) positrons, we observed 38 annihilation events consistent with the controlled release of trapped antihydrogen from our magnetic trap; the measured background is 1.4 ± 1.4 events. This result opens the door to precision measurements on anti-atoms, which can soon be subjected to the same techniques as developed for hydrogen. PMID:21085118

  7. Recent Developments of Electrochemical Promotion of Catalysis in the Techniques of DeNOx

    PubMed Central

    Tang, Xiaolong; Yi, Honghong; Chen, Chen; Wang, Chuan

    2013-01-01

    Electrochemical promotion of catalysis reactions (EPOC) is one of the most significant discoveries in the field of catalytic and environmental protection. The work presented in this paper focuses on the aspects of reaction mechanism, influencing factors, and recent positive results. It has been shown with more than 80 different catalytic systems that the catalytic activity and selectivity of conductive catalysts deposited on solid electrolytes can be altered in the last 30 years. The active ingredient of catalyst can be activated by applying constant voltage or constant current to the catalysts/electrolyte interface. The effect of EPOC can improve greatly the conversion rate of NOx. And it can also improve the lifetime of catalyst by inhibiting its poisoning. PMID:23970835

  8. COLD TRAP

    DOEpatents

    Milleron, N.

    1963-03-12

    An improved linear-flow cold trap is designed for highvacuum applications such as mitigating back migration of diffusion pump oil moiecules. A central pot of liquid nitrogen is nested within and supported by a surrounding, vertical, helical coil of metai sheet, all enveloped by a larger, upright, cylindrical, vacuum vessel. The vertical interstices between successive turns of the coil afford lineal, axial, high-vacuum passages between open mouths at top and bottom of said vessel, while the coil, being cold by virtue of thermal contact of its innermost turn with the nitrogen pot, affords expansive proximate condensation surfaces. (AEC)

  9. VACUUM TRAP

    DOEpatents

    Gordon, H.S.

    1959-09-15

    An improved adsorption vacuum trap for use in vacuum systems was designed. The distinguishing feature is the placement of a plurality of torsionally deformed metallic fins within a vacuum jacket extending from the walls to the central axis so that substantially all gas molecules pass through the jacket will impinge upon the fin surfaces. T fins are heated by direct metallic conduction, thereby ol taining a uniform temperature at the adeorbing surfaces so that essentially all of the condensible impurities from the evacuating gas are removed from the vacuum system.

  10. NOx Control Options and Integration for US Coal Fired Boilers

    SciTech Connect

    Mike Bockelie; Kevin Davis; Temi Linjewile; Connie Senior; Eric Eddings; Kevin Whitty; Larry Baxter; Calvin Bartholomew; William Hecker; Stan Harding; Robert Hurt

    2003-12-31

    This is the fourteenth Quarterly Technical Report for DOE Cooperative Agreement No: DEFC26-00NT40753. The goal of the project is to develop cost effective analysis tools and techniques for demonstrating and evaluating low NOx control strategies and their possible impact on boiler performance for boilers firing US coals. The Electric Power Research Institute (EPRI) is providing co-funding for this program. Using the initial CFD baseline modeling of the Gavin Station and the plant corrosion maps, six boiler locations for the corrosion probes were identified and access ports have been installed. Preliminary corrosion data obtained appear consistent and believable. In situ, spectroscopic experiments at BYU reported in part last quarter were completed. New reactor tubes have been made for BYU's CCR that allow for testing smaller amounts of catalyst and thus increasing space velocity; monolith catalysts have been cut and a small reactor that can accommodate these pieces for testing is in its final stages of construction. A poisoning study on Ca-poisoned catalysts was begun this quarter. A possible site for a biomass co-firing test of the slipstream reactor was visited this quarter. The slipstream reactor at Rockport required repair and refurbishment, and will be re-started in the next quarter. This report describes the final results of an experimental project at Brown University on the fundamentals of ammonia / fly ash interactions with relevance to the operation of advanced NOx control technologies such as selective catalytic reduction. The Brown task focused on the measurement of ammonia adsorption isotherms on commercial fly ash samples subjected to a variety of treatments and on the chemistry of dry and semi-dry ammonia removal processes.

  11. Photo-oxidation catalysts

    DOEpatents

    Pitts, J. Roland; Liu, Ping; Smith, R. Davis

    2009-07-14

    Photo-oxidation catalysts and methods for cleaning a metal-based catalyst are disclosed. An exemplary catalyst system implementing a photo-oxidation catalyst may comprise a metal-based catalyst, and a photo-oxidation catalyst for cleaning the metal-based catalyst in the presence of light. The exposure to light enables the photo-oxidation catalyst to substantially oxidize absorbed contaminants and reduce accumulation of the contaminants on the metal-based catalyst. Applications are also disclosed.

  12. Nox regulation of smooth muscle contraction

    PubMed Central

    Ritsick, Darren R.; Edens, William A.; Finnerty, Victoria; Lambeth, J. David

    2007-01-01

    The catalytic subunit, gp91phox (a.k.a., Nox2) of the NADPH-oxidase of mammalian phagocytes is activated by microbes and immune mediators to produce large amounts of reactive oxygen species (ROS) which participate in microbial killing. Homologs of gp91phox, the Nox and Duox enzymes, were recently described in a range of organisms, including plants, vertebrates, and invertebrates such as Drosophila melanogaster. While their enzymology and cell biology is being extensively studied in many laboratories, little is known about in vivo functions of Noxes. Here, we establish and use an inducible system for RNAi to discover functions of dNox, an ortholog of human Nox5 in Drosophila. We report here that depletion of dNox in musculature causes retention of mature eggs within ovaries, leading to female sterility. In dNox-depleted ovaries and ovaries treated with a Nox inhibitor, muscular contractions induced by the neuropeptide proctolin are markedly inhibited. This functional defect results from a requirement for dNox for the proctolin-induced calcium flux in Drosophila ovaries. Thus, these studies demonstrate a novel biological role for Nox-generated ROS in mediating agonist-induced calcium flux and smooth muscle contraction. PMID:17561091

  13. Ammonia Generation over TWC for Passive SCR NOX Control for Lean Gasoline Engines

    SciTech Connect

    Prikhodko, Vitaly Y; Parks, II, James E; Pihl, Josh A; Toops, Todd J

    2014-01-01

    A commercial three-way catalyst (TWC) was evaluated for ammonia (NH3) generation on a 2.0-liter BMW lean burn gasoline direct injection engine as a component in a passive ammonia selective catalytic reduction (SCR) system. The passive NH3 SCR system is a potential low cost approach for controlling nitrogen oxides (NOX) emissions from lean burn gasoline engines. In this system, NH3 is generated over a close-coupled TWC during periodic slightly rich engine operation and subsequently stored on an underfloor SCR catalyst. Upon switching to lean, NOX passes through the TWC and is reduced by the stored NH3 on the SCR catalyst. NH3 generation was evaluated at different air-fuel equivalence ratios at multiple engine speed and load conditions. Near complete conversion of NOX to NH3 was achieved at =0.96 for nearly all conditions studied. At the =0.96 condition, HC emissions were relatively minimal, but CO emissions were significant. Operation at AFRs richer than =0.96 did not provide more NH3 yield and led to higher HC and CO emissions. Results of the reductant conversion and consumption processes were used to calculate a representative fuel consumption of the engine operating with an ideal passive SCR system. The results show a 1-7% fuel economy benefit at various steady-state engine speed and load points relative to a stoichiometric engine operation.

  14. New operation strategy for driving the selectivity of NOx reduction to N2, NH3 or N2O during lean/rich cycling of a lean NOx trap catalyst

    SciTech Connect

    Mráček, David; Koci, Petr; Choi, Jae -Soon; Partridge, Jr., William P.

    2015-09-08

    Periodical regeneration of NOx storage catalyst (also known as lean NOx trap) by short rich pulses of CO, H2 and hydrocarbons is necessary for the reduction of nitrogen oxides adsorbed on the catalyst surface. Ideally, the stored NOx is converted into N2, but N2O and NH3 by-products can be formed as well, particularly at low-intermediate temperatures. The N2 and N2O products are formed concurrently in two peaks. The primary peaks appear immediately after the rich-phase inception, and tail off with the breakthrough of the reductant front accompanied by NH3 product. In addition, the secondary N2 and N2O peaks then appear at the rich-to-lean transition as a result of reactions between surface-deposited reductants/intermediates (CO, HC, NH3, — NCO) and residual stored NOx under increasingly lean conditions.

  15. 40 CFR 97.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false NOX Budget permit contents. 97.23... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.23 NOX Budget permit contents. (a) Each NOX Budget permit will contain, in a format prescribed by the...

  16. 40 CFR 97.24 - NOX Budget permit revisions.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false NOX Budget permit revisions. 97.24... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.24 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating permit, except as...

  17. 40 CFR 97.24 - NOX Budget permit revisions.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false NOX Budget permit revisions. 97.24... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.24 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating permit, except as...

  18. 40 CFR 96.25 - NOX Budget permit revisions.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false NOX Budget permit revisions. 96.25... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO 2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.25 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating...

  19. 40 CFR 97.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false NOX Budget permit contents. 97.23... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.23 NOX Budget permit contents. (a) Each NOX Budget permit will contain, in a format prescribed by the...

  20. 40 CFR 96.25 - NOX Budget permit revisions.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false NOX Budget permit revisions. 96.25... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.25 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating...

  1. 40 CFR 96.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false NOX Budget permit contents. 96.23... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO 2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents. (a) Each NOX Budget permit (including any draft or...

  2. 40 CFR 96.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false NOX Budget permit contents. 96.23... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents. (a) Each NOX Budget permit (including any draft or...

  3. 40 CFR 96.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false NOX Budget permit contents. 96.23... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents. (a) Each NOX Budget permit (including any draft or...

  4. 40 CFR 97.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false NOX Budget permit contents. 97.23... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.23 NOX Budget permit contents. (a) Each NOX Budget permit will contain, in a format prescribed by the...

  5. 40 CFR 97.24 - NOX Budget permit revisions.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false NOX Budget permit revisions. 97.24... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.24 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating permit, except as...

  6. 40 CFR 96.25 - NOX Budget permit revisions.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false NOX Budget permit revisions. 96.25... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.25 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating...

  7. 40 CFR 96.11 - Alternate NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Alternate NOX authorized account... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Authorized Account Representative for NOX Budget Sources § 96.11 Alternate...

  8. 40 CFR 96.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Budget permit contents. 96.23... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents. (a) Each NOX Budget permit (including any draft or...

  9. 40 CFR 96.42 - NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX allowance allocations. 96.42... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Allocations § 96.42 NOX allowance allocations. (a)(1) The heat input (in mmBtu) used...

  10. 40 CFR 96.50 - NOX Allowance Tracking System accounts.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Allowance Tracking System accounts... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.50 NOX Allowance Tracking System accounts. (a) Nature...

  11. 40 CFR 96.42 - NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX allowance allocations. 96.42... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Allocations § 96.42 NOX allowance allocations. (a)(1) The heat input (in mmBtu) used...

  12. 40 CFR 96.53 - Recordation of NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Recordation of NOX allowance... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.53 Recordation of NOX allowance allocations. (a)...

  13. 40 CFR 96.25 - NOX Budget permit revisions.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Budget permit revisions. 96.25... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.25 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating...

  14. 40 CFR 97.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Budget permit contents. 97.23... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.23 NOX Budget permit contents. (a) Each NOX Budget permit will contain, in a format prescribed by the...

  15. 40 CFR 96.25 - NOX Budget permit revisions.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Budget permit revisions. 96.25... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.25 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating...

  16. 40 CFR 96.142 - CAIR NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false CAIR NOX allowance allocations. 96.142... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Allocations § 96.142 CAIR NOX allowance allocations. (a)(1) The baseline heat...

  17. 40 CFR 97.50 - NOX Allowance Tracking System accounts.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Allowance Tracking System accounts... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.50 NOX Allowance Tracking System accounts. (a) Nature and function of...

  18. 40 CFR 96.50 - NOX Allowance Tracking System accounts.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Allowance Tracking System accounts... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.50 NOX Allowance Tracking System accounts. (a) Nature...

  19. 40 CFR 97.50 - NOX Allowance Tracking System accounts.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Allowance Tracking System accounts... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.50 NOX Allowance Tracking System accounts. (a) Nature and function of...

  20. 40 CFR 97.24 - NOX Budget permit revisions.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Budget permit revisions. 97.24... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.24 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating permit, except as...

  1. 40 CFR 96.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Budget permit contents. 96.23... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents. (a) Each NOX Budget permit (including any draft or...

  2. 40 CFR 96.53 - Recordation of NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Recordation of NOX allowance... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.53 Recordation of NOX allowance allocations. (a)...

  3. 40 CFR 97.53 - Recordation of NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Recordation of NOX allowance... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.53 Recordation of NOX allowance allocations. (a) The Administrator will record the...

  4. 40 CFR 97.42 - NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX allowance allocations. 97.42... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Allocations § 97.42 NOX allowance allocations. (a)(1) The heat input (in mmBtu) used for calculating...

  5. 40 CFR 97.42 - NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX allowance allocations. 97.42... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Allocations § 97.42 NOX allowance allocations. (a)(1) The heat input (in mmBtu) used for calculating...

  6. 40 CFR 97.23 - NOX Budget permit contents.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Budget permit contents. 97.23... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.23 NOX Budget permit contents. (a) Each NOX Budget permit will contain, in a format prescribed by the...

  7. 40 CFR 96.11 - Alternate NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Alternate NOX authorized account... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Authorized Account Representative for NOX Budget Sources § 96.11 Alternate...

  8. 40 CFR 97.53 - Recordation of NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Recordation of NOX allowance... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS NOX Allowance Tracking System § 97.53 Recordation of NOX allowance allocations. (a) The Administrator will record the...

  9. 40 CFR 97.142 - CAIR NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false CAIR NOX allowance allocations. 97.142... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS CAIR NOX Allowance Allocations § 97.142 CAIR NOX allowance allocations. (a)(1) The baseline heat input (in mmBtu) used...

  10. 40 CFR 97.24 - NOX Budget permit revisions.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false NOX Budget permit revisions. 97.24... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.24 NOX Budget permit revisions. (a) For a NOX Budget source with a title V operating permit, except as...