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Sample records for nox storage 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. Effect of reductive treatments on Pt behavior and NOx storage in lean NOx trap catalysts

    SciTech Connect

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

    2011-10-01

    Lean NOx trap (LNT) catalysts represent a promising approach to meet increasingly stringent NOx emission regulations on diesel and other lean-burn engines. Pt material properties, including dispersion and particle size, are known to be important factors in determining NOx uptake performance, since Pt provides active sites for NO oxidation to NO2 necessary for storing NOx as nitrates, and for the reduction of nitrates to N2. In this work, the physicochemical properties of Pt in Pt-BaO/Al2O3 LNT catalysts, such as the Pt accessible surface area and particle size, were investigated by using various tools, such as irreversible volumetric H2 chemisorption, high resolution transmission electron microscopy (HRTEM), and X-ray diffraction (XRD), following successive reductive treatments at elevated temperatures. NOx uptake activities were also measured to establish a relationship between the properties of Pt and NOx storage following identical high-temperature reductive treatments. We find that the reductive treatments of Pt-BaO/Al2O3 lean NOx trap catalysts at temperatures up to 500 ºC promote a significant increase in NOx uptake explained, in part, by an induced close interaction between Pt and BaO phases in the catalyst, thus enabling facilitation of the NOx storage process.

  3. 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.

  4. Combining nonthermal plasma with perovskite-like catalyst for NOx storage and reduction.

    PubMed

    Peng, Han Hsuan; Pan, Kuan Lun; Yu, Sheng Jen; Yan, Shaw Yi; Chang, Moo Been

    2016-10-01

    A new NOx storage and reduction (NSR) system is developed for NOx removal by combining perovskite-like catalyst with nonthermal plasma technology. In this hybrid system, catalyst is mainly used for oxidizing NO to NO2 and storing them, while nonthermal plasma is applied as a desorption-reduction step for converting NOx into N2. An innovative catalyst with a high NOx storage capacity and good reduction performance is developed by successive impregnation. The catalysts prepared with various metal oxides were investigated for NOx storage capacity (NSC) and NOx conversion. Characterization of the catalysts prepared reveals that addition of cobalt (Co) and potassium (K) considerably increases the performance for NSC. Results also show that SrKMn0.8Co0.2O4 supported on BaO/Al2O3 has good NSC (209 μmol/gcatalyst) for the gas stream containing 500 ppm NO and 5 % O2 with N2 as carrier gas. For plasma reduction process, NOx conversion achieved with SrKMn0.8Co0.2O4/BaO/Al2O3 reaches 81 % with the applied voltage of 12 kV and frequency of 6 kHz in the absence of reducing agents. The results indicate that performance of plasma reduction process (81 %) is better than that of thermal reduction (64 %). Additionally, mixed gases including 1 % CO, 1 % H2 and 1 % CH4, and 2 % H2O(g) are simultaneously introduced into the system to investigate the effect on NSR with plasma system and results indicate that performance of NSR with plasma can be enhanced. Overall, the hybrid system is promising to be applied for removing NOx from gas streams. Graphical abstract ᅟ.

  5. 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.

  6. 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.

  7. 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.

  8. [NOx storage and decomposition behavior of Cu-Mg-Al catalyst].

    PubMed

    Kang, Shou-fang; Li, Jun-hua; Fu, Li-xin; Hao, Zheng-ping

    2007-05-01

    Cu-Mg-Al hydrotalcite mixed oxide was prepared by co-precipitation. The mixed oxide and its procurer were characterized by XRD. NO, storage performance and decomposition of the stored NO, over the catalyst were investigated by NO, storage experiment at constant temperature, temperature programmed desorption (TPD) and temperature programmed surface reaction (TPSR), respectively. The results indicate that Cu-Mg-Al hydrotalcite mixed oxide has a good performance of NO, storage. The formed nitrate can be decomposed to gaseous NOx rapidly in the investigated temperature range of 160-360 degrees C, and a small amount of gaseous NO, can be reduced by C3 H6 with increasing the concentration of C3 H6 in the inlet gas.

  9. Hydrotalcite-derived MnxMg3-xAlO catalysts used for soot combustion, NOx storage and simultaneous soot-NOx removal.

    PubMed

    Li, Qian; Meng, Ming; Xian, Hui; Tsubaki, Noritatsu; Li, Xingang; Xie, Yaning; Hu, Tiandou; Zhang, Jing

    2010-06-15

    The hydrotalcite-based Mn(x)Mg(3-x)AlO catalysts with different Mn:Mg atomic ratios were synthesized by coprecipitation, and employed for soot combustion, NOx storage and simultaneous soot-NO(x) removal. It is shown that with the increase of Mn content in the hydrotalcite-based Mn(x)Mg(3-x)AlO catalysts the major Mn-related species vary from MnAl(2)O(4) and Mg(2)MnO(4) to Mn(3)O(4) and Mn(2)O(3). The catalyst Mn(1.5)Mg(1.5)AlO displays the highest soot combustion activity with the temperature for maximal soot combustion rate decreased by 210 degrees C, as compared with the Mn-free catalyst. The highly reducible Mn(4+) ions in Mg(2)MnO(4) are identified as the most active species for soot combustion. For NO(x) storage, introduction of Mn greatly influences bulk NO(x) storage, with the adsorbed NO(x) species varying from linear nitrites to ionic and chelating bidentate nitrates gradually. The coexistence of highly oxidative Mn(4+) and highly reductive Mn(2+) in Mn(1.0)Mg(2.0)AlO is favorable to the simultaneous soot-NO(x) removal, giving a NO(x) reduction percentage of 24%. In situ DRIFTS reveals that the ionic nitrate species are more reactive with soot than nitrites and chelating bidentate nitrates, showing higher NO(x) reduction efficiency.

  10. 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

  11. 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.

  12. Sulfation and Desulfation Behavior of Pt-BaO/MgO-Al2O3 NOx Storage Reduction Catalyst.

    PubMed

    Jeong, Soyeon; Kim, Do Heui

    2016-05-01

    The comparative study between Pt-BaO/Al2O3 and Pt-BaO/MgO-Al2O3 gives the information about the effect of MgO addition to Al2O3 support on the sulfation and desulfation behavior of Pt-BaO/MgO-Al2O3 NOx storage reduction catalyst. The sulfated two samples were analyzed by using element analysis (EA), X-ray diffraction (XRD), H2 temperature programmed reaction (H2 TPRX) and NOx uptake measurement. The amount of sulfur uptake on 2 wt% Pt-20 wt% BaO/Al2O3 and 2 wt% Pt-20 wt% BaO/MgO-Al2O3 are almost identical as 0.45 and 0.40 of S/Ba, respectively, which yields the drastic decrease in NOx uptake for both sulfated samples. However, after desulfa- tion with H2 at 600 degrees C, the residual sulfur amount on MgO-Al2O3 supported catalyst is three times larger than that on Al2O3 supported one, indicating that sulfur species formed on the former are more stable than those on the latter. It is also well corresponding to the H2 TPRX results where the main H2S peak from MgO-Al2O3 supported sample is observed at higher temperature than Al2O3 supported one, resulting in the lower NOx uptake activity of former sample than the latter one. Meanwhile, after desulfation of MgO-Al2O3 supported sample at 700 degrees C and 800 degrees C, the activity is recovered more significantly due to the removal of the large amount of sulfur while Al2O3 supported one decreases monotonically due to the sintering of Pt crystallite and the formation of BaAl2O4 phase. It is summarized that MgO-Al2O3 supported catalyst enhances the thermal stability of the catalyst, however, forms the stable sulfate species, which needs to be improved to develop the more sulfur resistant NSR catalyst system.

  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. 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.

  15. Promotional Effects of H2O Treatment on NOx Storage over Fresh and Thermally Aged Pt-BaO/Al2O3 Lean NOx Trap Catalysts

    SciTech Connect

    Kim, Do Heui; Chin, Ya-Huei; Kwak, Ja Hun; Peden, Charles HF

    2008-08-01

    A simple liquid water treatment applied to fresh and thermally aged Pt(2wt%)-BaO(20wt%)/Al2O3 lean NOx trap catalysts at room temperature induces morphological and structural changes in the barium species as followed by XRD and TEM analysis. During the water treatment, liquid water sufficient to fill the catalyst pore volume is brought into contact with the samples. It was found that irrespective of the original barium chemical state (highly dispersed BaO or crystalline BaAl2O4), exposing the sample to this liquid water treatment promotes the formation of BaCO3 crystallites (about 15 – 25 nm of its size) without changing the Pt particle size. Such transformations of the barium species are found to significantly promote NOx uptake from 250 °C to 450 °C. The increase in the NOx uptake for the water-treated samples can be attributed to an enhanced Pt-Ba interaction through the redistribution of barium species. These results provide useful information for the regeneration of aged lean NOx trap catalysts since water is plentiful in the exhaust of diesel or lean-burn engines.

  16. 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

  17. Impact of Soot on NOx Adsorption over Cu-Modified Hydrotalcite-Derived Lean NOx Trap Catalyst.

    PubMed

    Li, Bo; Song, Chonglin; Lv, Gang; Chen, Ke; Cao, Xiaofeng

    2017-03-28

    The impact of soot on NOx adsorption was studied over a Cu-modified hydrotalcite-derived lean NOx trap catalyst in a NO + O2 atmosphere. Powder X-ray diffraction, scanning electron microscopy, Raman scattering spectroscopy, and X-ray photoelectron spectroscopy were used to characterize the surface properties of the pure catalyst and the soot/catalyst mixture. The adsorbed NOx species on the samples were evaluated by in situ diffuse reflectance Fourier transform spectroscopy. The soot coverage decreases the available adsorption sites on the surface of the catalyst, and a portion of active oxygen species are consumed by the soot oxidation during He pretreatment process. The NOx adsorption on two catalyst samples simultaneously undergoes two routes: the "nitrite route" and the "nitrate route". The "nitrite route" is more dominant than the "nitrate route". During NOx adsorption, the soot oxidation weakens the NO oxidation to NO2, and the released CO2 competes with NOx on the adsorption sites. Moreover, the temperature-programmed desorption tests indicate that the presence of soot reduces the NOx storage capacity of the catalyst and shifts the NO desorption peak to the lower temperature range by 50 °C.

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

    DOE PAGES

    Bartova, Sarka; Mracek, David; Koci, Petr; ...

    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

  19. 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.

  20. 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.

  1. 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

  2. NOx Uptake Mechanism on Pt/BaO/Al2O3 Catalysts

    SciTech Connect

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

    2006-11-01

    The NOx adsorption mechanism on Pt/BaO/Al2O3 catalysts was investigated by performing NOx storage/reduction cycles, NO2 adsorption and NO + O2 adsorption on 2%Pt/(x)BaO/Al2O3 (x = 2, 8 and 20 wt%) catalysts. NOx uptake profiles on 2%Pt/20%BaO/Al2O3 at 523 K show complete uptake behavior for almost 5 min, and then the NOx level starts gradually increasing with time and it reaches 75% of the inlet NOx concentration after 30 min time-on-stream. Although this catalyst shows fairly high NOx conversion at 523 K, only ~ 2.4 wt% out of 20 wt% BaO is converted to Ba(NO3)2. Adsorption studies by using NO2 and NO + O2 suggest two different NOx adsorption mechanisms. The NO2 uptake profile on 2%Pt/20%BaO/Al2O3 shows the absence of a complete NOx uptake period at the beginning of adsorption and the overall NOx uptake is controlled by the gas-solid equilibrium between NO2 and BaO/Ba(NO3)2 phase. When we use NO + O2, complete initial NOx uptake occurs and the time it takes to convert ~ 4 % of BaO to Ba(NO3)2 is independent of the NO concentration. These NOx uptake characteristics suggest that the NO + O2 reaction on the surface of Pt particles produces NO2 that is subsequently transferred to the neighboring BaO phase by spill over. At the beginning of the NOx uptake, this spill-over process is very fast and so it is able to provide complete NOx storage. However, the NOx uptake by this mechanism slows down as BaO in the vicinity of Pt particles are converted to Ba(NO3)2. The formation of Ba(NO3)2 around the Pt particles results in the development of a diffusion barrier for NO2, and increases the probability of NO2 desorption and consequently, the beginning of NOx slip. As NOx uptake by NO2 spill-over mechanism slows down due to the diffusion barrier formation, the rate and extent of NO2 uptake are determined by the diffusion rate of nitrate ions into the BaO bulk, which, in turn, is determined by the gas phase NO2 concentration.

  3. 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.

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

    DOE PAGES

    Brookshear, Daniel William; Nam, Jeong -Gil; Nguyen, Ke; ...

    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

  5. The capacity of modified nickel catalysts derived from discharged catalyst of fertilizer plants for NOx treatment

    NASA Astrophysics Data System (ADS)

    Ha, T. M. P.; Luong, N. T.; Le, P. N.

    2016-11-01

    In Vietnam for recent years, a large amount of hazardous waste containing nickel (Ni) derived from discharged catalyst of fertilizer plants has caused environmental problems in landfill overloading and the risk of soil or surface water sources pollution. Taking advantage of discharged catalyst, recycling Ni components and then synthesizing new catalysts apply for mono-nitrogen oxides (NOx) treatments is an approach to bring about both economic and environmental benefits. This study was carried out with the main objective: Evaluate the performance of modified catalysts (using recovered Ni from the discharged RKS-2-7H catalyst of Phu My Fertilizer Plant) on NOx treatment. The catalysts was synthesized and modified with active phases consist of recovered Ni and commercial Barium oxide (BaO), Manganese dioxide (MnO2) / Cerium (IV) oxide (CeO2) on the support Aluminium oxide (γ-Al2O3). The results show that the modified catalysts with Ni, Ba, Ce was not more beneficial for NOx removal than which with Ni, Ba, Mn. 98% NOx removal at 350°C with the start temperature at 115°C and the T60 value at 307°C can be obtained with 10Ni10Ba10Mn/Al catalyst.

  6. Congressionally Directed Project for Passive NOx Removal Catalysts Research

    SciTech Connect

    Schneider, William

    2014-12-29

    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.

  7. 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.

  8. 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.

  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. New Heterogeneous Catalysts for the Selective Reduction of NOx under Lean Conditions. Final Report

    SciTech Connect

    Amiridis, M. D.

    2004-05-31

    The original goal of this program was the identification and design of new noble-metal-based catalysts for the selective catalytic reduction of nitric oxide by hydrocarbons under excess oxygen (i.e., ''lean'') conditions (HC-SCR). Work conducted in the first funding cycle of this award (i.e., 1997-2000) was successful in allowing us to develop an understanding of the fundamental surface chemistry taking place during the adsorption and reaction of nitrogen oxides and propylene on the surface of supported noble metal catalysts. Both experimental results collected in our own group as well as molecular simulation results published by Professor Neurock suggested that in order to improve the performance of the Pt catalysts--in terms of the nitrogen selectivity and the temperature window of operation-- it was necessary to introduce a second metal. However, synthesizing such catalysts with the metals of interest (i.e., Pt-Au, Pt-Ru, Pt-Rh, etc.) with some degree of control of the structure and composition of the resulting supported metal particles is in itself a research challenge. Consequently, the bulk of our efforts during the second funding cycle of this award (covered by this report) was shifted to the use of organometallic cluster precursors for the synthesis on novel bimetallic catalysts. During this time we have also continued to maintain an interest in NOx abatement, but have redirected our efforts from the HC-SCR process to the more promising from a commercial standpoint NOx Storage Reduction (NSR) approach.

  11. 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.

  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. 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.

  14. 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.

  15. Nitrogen oxides storage catalysts containing cobalt

    DOEpatents

    Lauterbach, Jochen; Snively, Christopher M.; Vijay, Rohit; Hendershot, Reed; Feist, Ben

    2010-10-12

    Nitrogen oxides (NO.sub.x) storage catalysts comprising cobalt and barium with a lean NO.sub.x storage ratio of 1.3 or greater. The NO.sub.x storage catalysts can be used to reduce NO.sub.x emissions from diesel or gas combustion engines by contacting the catalysts with the exhaust gas from the engines. The NO.sub.x storage catalysts can be one of the active components of a catalytic converter, which is used to treat exhaust gas from such engines.

  16. Low-temperature NOx reduction processes using combined systems of pulsed corona discharge and catalysts

    NASA Astrophysics Data System (ADS)

    Kim, H. H.; Takashima, K.; Katsura, S.; Mizuno, A.

    2001-02-01

    In this paper, we will report NOx removal via reduction processes using two types of combined system of pulse corona discharge and catalysts: the single-stage plasma-driven catalyst (PDC) system, and the two-stage plasma-enhanced selective catalytic reduction (PE-SCR) system. Several catalysts, such as γ-alumina catalysts, mechanically mixed catalysts of γ-alumina with BaTiO3 or TiO2, and Co-ZSM-5 were tested. In the PDC system, which is directly activated by the discharge plasma, it was found that the use of additives was necessary to achieve NOx removal by reduction. Removal rates of NO and NOx were linearly increased as the molar ratio of additive to NOx increased. The dependence of NO and NOx removal on the gas hourly space velocity (GHSV) at a fixed specific input energy (SIE) indicates that plasma-induced surface reaction on the catalyst plays an important role in the PDC system. It was found that the optimal GHSV of the PDC system with the γ-alumina catalyst was smaller than 6000 h-1. Mechanical mixing of γ-alumina with BaTiO3 or TiO2 did not enhance NO and NOx removal and γ-alumina alone was found to be the most suitable catalyst. The dielectric constant of the catalyst only influenced the plasma intensity, not the NOx removal. In the PE-SCR system, plasma-treated NOx (mostly NO2) was reduced effectively with NH3 over the Co-ZSM-5 catalyst at a relatively low temperature of 150 °C. Under optimal conditions the energy cost and energy yield were 25 eV/molecule and 21 g-N (kWh)-1, respectively.

  17. 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.

  18. 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 PAGES

    Mráček, David; Koci, Petr; Choi, Jae -Soon; ...

    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

  19. Reduction of Stored NOx on Pt/Al₂O₃ and Pt/BaO/Al₂O₃ Catalysts with H₂ and CO

    SciTech Connect

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

    2006-04-01

    In situ FTIR spectroscopy coupled with mass spectrometry, and time resolved X-ray diffraction were used to study the efficiency of nitrate reduction with CO and H₂ on Pt/Al₂O₃ and Pt/BaO/Al₂O₃ NOx storage-reduction (NSR) catalysts. Surface nitrates were generated by NO₂ adsorption and their reduction efficiencies were examined on the catalysts together with the analysis of the gas phase composition in the presence of the two different reductants. H₂ was found to be a more effective reducing agent than CO. In particular, the reduction of surface nitrates proceeds very efficiently with H₂ even at low temperatures (~420 K). During reduction with CO, isocyanates were observed to form on every catalyst component. These surface isocyanates, however, readily react with water to form CO₂ and ammonia. The thus formed NH₃, in turn, reacts with stored NOx at higher temperatures (>473K) to produce N₂. In the absence of H₂O, the NCO species are stable to high temperatures, and removed only from the catalyst when they react with NOx thermal decomposition products to form N₂ and CO₂. The results of this study point to a complex reaction mechanism that involves the removal of surface oxygen atoms from the Pt particles by either H₂ or CO, the direct reduction of stored NOx with H₂ (low temperature NOx reduction), the formation and the subsequent hydrolysis of NCO species, as well as the direct reaction of NCO with decomposing NOx (high temperature NOx reduction).

  20. 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.

  1. 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.

  2. 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

  3. Synthesis of Pt/K2CO3/MgAlOx–reduced graphene oxide hybrids as promising NOx storage–reduction catalysts with superior catalytic performance

    PubMed Central

    Mei, Xueyi; Yan, Qinghua; Lu, Peng; Wang, Junya; Cui, Yuhan; Nie, Yu; Umar, Ahmad; Wang, Qiang

    2017-01-01

    Pt/K2CO3/MgAlOx–reduced graphene oxide (Pt/K/MgAlOx–rGO) hybrids were synthesized, characterized and tested as a promising NOx storage and reduction (NSR) catalyst. Mg–Al layered double hydroxides (LDHs) were grown on rGO via in situ hydrothermal crystallization. The structure and morphology of samples were thoroughly characterized using various techniques. Isothermal NOx adsorption tests indicated that MgAlOx–rGO hybrid exhibited better NOx trapping performance than MgAlOx, from 0.44 to 0.61 mmol · g−1, which can be attributed to the enhanced particle dispersion and stabilization. In addition, a series of MgAlOx–rGO loaded with 2 wt% Pt and different loadings (5, 10, 15, and 20 wt%) of K2CO3 (denoted as Pt/K/MgAlOx–rGO) were obtained by sequential impregnation. The influence of 5% H2O on the NOx storage capacity of MgAlOx–rGO loaded with 2 wt% Pt and 10% K2CO3 (2Pt/10 K/MgAlOx–rGO) catalyst was also evaluated. In all, the 2Pt/10 K/MgAlOx–rGO catalyst not only exhibited high thermal stability and NOx storage capacity of 1.12 mmol · g−1, but also possessed excellent H2O resistance and lean–rich cycling performance, with an overall 78.4% of NOx removal. This work provided a new scheme for the preparation of highly dispersed MgAlOx–rGO hybrid based NSR catalysts. PMID:28205630

  4. Synthesis of Pt/K2CO3/MgAlOx–reduced graphene oxide hybrids as promising NOx storage–reduction catalysts with superior catalytic performance

    NASA Astrophysics Data System (ADS)

    Mei, Xueyi; Yan, Qinghua; Lu, Peng; Wang, Junya; Cui, Yuhan; Nie, Yu; Umar, Ahmad; Wang, Qiang

    2017-02-01

    Pt/K2CO3/MgAlOx–reduced graphene oxide (Pt/K/MgAlOx–rGO) hybrids were synthesized, characterized and tested as a promising NOx storage and reduction (NSR) catalyst. Mg–Al layered double hydroxides (LDHs) were grown on rGO via in situ hydrothermal crystallization. The structure and morphology of samples were thoroughly characterized using various techniques. Isothermal NOx adsorption tests indicated that MgAlOx–rGO hybrid exhibited better NOx trapping performance than MgAlOx, from 0.44 to 0.61 mmol · g‑1, which can be attributed to the enhanced particle dispersion and stabilization. In addition, a series of MgAlOx–rGO loaded with 2 wt% Pt and different loadings (5, 10, 15, and 20 wt%) of K2CO3 (denoted as Pt/K/MgAlOx–rGO) were obtained by sequential impregnation. The influence of 5% H2O on the NOx storage capacity of MgAlOx–rGO loaded with 2 wt% Pt and 10% K2CO3 (2Pt/10 K/MgAlOx–rGO) catalyst was also evaluated. In all, the 2Pt/10 K/MgAlOx–rGO catalyst not only exhibited high thermal stability and NOx storage capacity of 1.12 mmol · g‑1, but also possessed excellent H2O resistance and lean–rich cycling performance, with an overall 78.4% of NOx removal. This work provided a new scheme for the preparation of highly dispersed MgAlOx–rGO hybrid based NSR catalysts.

  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.

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

    SciTech Connect

    Blint, Richard J.

    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.

  7. 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.

  8. Self-Protection Mechanism of Hexagonal WO3-Based DeNOx Catalysts against Alkali Poisoning.

    PubMed

    Zheng, Li; Zhou, Meijuan; Huang, Zhiwei; Chen, Yaxin; Gao, Jiayi; Ma, Zhen; Chen, Jianmin; Tang, Xingfu

    2016-11-01

    A good catalyst for efficiently controlling NOx emissions often demands strong resistance against alkali poisoning. Although the traditional ion-exchange model, based on acid-base reactions of alkalis with Brønsted acid sites, has been established over the past two decades, it is difficult to be used as a guideline to develop such an alkali-resistant catalyst. Here we establish a self-protection mechanism of deNOx catalysts against alkali poisoning by systematically studying the intrinsic nature of alkali resistance of V2O5/HWO (HWO = hexagonal WO3) that shows excellent resistance to alkali poisoning in selective catalytic reduction of NOx with NH3 (SCR). Synchrotron X-ray diffraction and absorption spectroscopies demonstrate that V2O5/HWO has spatially separated catalytically active sites (CASs) and alkali-trapping sites (ATSs). During the SCR process, ATSs spontaneously trap alkali ions such as K(+), even if alkali ions initially block CASs, thus releasing CASs to realize the self-protection against alkali poisoning. X-ray photoelectron spectra coupled with theoretical calculations indicate that the electronic interaction between the alkali ions and ATSs with an energy saving is the driving force of the self-protection. This work provides a strategy to design alkali-resistant deNOx catalysts.

  9. 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.

  10. Combined fast selective reduction using Mn-based catalysts and nonthermal plasma for NOx removal.

    PubMed

    Chen, Jun Xiang; Pan, Kuan Lun; Yu, Sheng Jen; Yen, Shaw Yi; Chang, Moo Been

    2017-07-26

    In this study, the concept of fast SCR for NO reduction with NH3 as reducing agent is realized via the combination of nonthermal plasma (NTP) with Mn-based catalyst. Experimental results indicate that 10% wt. Mn-Ce-Ni/TiO2 possesses better physical and chemical properties of surface, resulting in higher NO removal efficiency if compared with 10% wt. Mn-Ce/TiO2 and 10% wt. Mn-Ce-Cu/TiO2. Mn-Ce-Ni/TiO2 of 10% wt. achieves 100% NOx conversion at 150 °C, while 10% wt. Mn-Ce/TiO2 and 10% wt. Mn-Ce-Cu/TiO2 need to be operated at a temperature above 200 °C for 100% NOx conversion. However, NO conversion achieved with 10% wt. Mn-Ce-Ni/TiO2 is significantly reduced as H2O(g) and SO2 are introduced into the SCR system simultaneously. Further, two-stage system (SCR with DBD) is compared with the catalyst-alone for NOx conversion and N2 selectivity. The results indicate that 100% NOx conversion can be achieved with two-stage system at 100 °C, while N2 selectivity reaches 80%. Importantly, NOx conversion achieved with two-stage system could maintain >95% in the presence of C2H4, CO, SO2, and H2O(g), indicating that two-stage system has better tolerance for complicated gas composition. Overall, this study demonstrates that combining NTP with Mn-based catalyst is effective in reducing NOx emission at a low temperature (≤200 °C) and has good potential for industrial application.

  11. 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

    2015-06-02

    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.

  12. 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.

  13. 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.

  14. 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.

  15. Lean NOx reduction over Ag/alumina catalysts via ethanol-SCR using ethanol/gasoline blends

    DOE PAGES

    Gunnarsson, Fredrik; Pihl, Josh A.; Toops, Todd J.; ...

    2016-09-04

    This paper focuses on the activity for lean NOx reduction over sol-gel synthesized silver alumina (Ag/Al2O3) catalysts, with and without platinum doping, using ethanol (EtOH), EtOH/C3H6 and EtOH/gasoline blends as reducing agents. The effect of ethanol concentration, both by varying the hydrocarbon-to-NOx ratio and by alternating the gasoline concentration in the EtOH/gasoline mixture, is investigated. High activity for NOx reduction is demonstrated for powder catalysts for EtOH and EtOH/C3H6 as well as for monolith coated catalysts (EtOH and EtOH/gasoline). The results show that pure Ag/Al2O3 catalysts display higher NOx reduction and lower light-off temperature as compared to the platinum dopedmore » samples. The 4 wt.% Ag/Al2O3 catalyst displays 100% reduction in the range 340–425 °C, with up to 37% selectivity towards NH3. These results are also supported by DRIFTS (Diffuse reflection infrared Fourier transform spectroscopy) experiments. Finally, the high ammonia formation could, in combination with an NH3-SCR catalyst, be utilized to construct a NOx reduction system with lower fuel penalty cf. stand alone HC-SCR. In addition, it would result in an overall decrease in CO2 emissions.« less

  16. Removal of NO(x) at low temperature over mesoporous alpha-Mn2O3 catalyst.

    PubMed

    Jeon, Mi-Jin; Park, Sung Hoon; Kim, Ji Man; Jeon, Jong-Ki; Kim, Sang Chai; Kim, Do Heui; Park, Young-Kwon

    2014-03-01

    Low-temperature selective catalytic reduction was carried out over various kinds of manganese oxide (MnOx) catalysts. Mesoporous alpha-Mn2O3, commercial bulk Mn2O3, and Mn/SBA-15 were used as the catalyst. The NOx removal performances of the catalysts were compared. Three different amounts of Mn (5, 10, and 15 wt%) were impregnated on SBA-15 to synthesize Mn/SBA-15. The physical and chemical properties of the catalysts were examined by Brunauer-Emmett-Teller, X-ray diffraction, X-ray photoelectron spectroscopy, and H2-temperature programmed reduction analyses. Of all catalysts examined, mesoporous alpha-Mn2O3 exhibited the highest low-temperature SCR de-NOx efficiency, reaching about 90% at 175 degrees C. This is attributed to strong reducing ability and high oxygen mobility of mesoporous alpha-Mn2O3 and well dispersed Mn2O3 in its mesoporous framework.

  17. Effects of Rapid High Temperature Cyclic Aging on a Fully-Formulated Lean NOx Trap Catalyst

    SciTech Connect

    Ottinger, Nathan; Nguyen, Ke; Bunting, Bruce G; Toops, Todd J; Howe, Janet E

    2009-01-01

    In this study, high-temperature deactivation of a fully-formulated lean NOx trap (LNT) is investigated with an accelerated aging protocol where accelerated aging is accomplished by rapid temperature cycling and by higher temperatures. Thermal aging is carried out in a bench-flow reactor at nominal temperatures of 700, 800, 900, and 1000 C using an aging cycle consisting of a 130s lean-phase and a 50s rich-phase. After a prescribed number of lean/rich aging cycles, the NOx conversion of the aged LNT is evaluated at 200, 300, and 400 C. The NOx performance is obtained at a GHSV of 30,000 h-1 using an evaluation cycle consisting of a 60s lean-phase and 5s rich-phase. The effects of aging on the LNT washcoat are determined with EPMA, XRD, STEM/EDS, and BET. Aging at 700 and 800 C has a minimal effect on LNT performance and material properties. However, at aging temperatures of 900 and 1000 C reduction in surface area and sintering of PGM particles are observed and result in a drastic reduction in NOx conversion. Additionally, after aging at 900 C and 1000 C the NOx storage medium, BaCO3, is no longer visible in the XRD patterns, even though a Ba-phase identified by EPMA still exists in all aged samples. BaAl2O4 is not identified at any aging temperatures; possibly due to stabilization effects provided by washcoat additives present in this particular LNT.

  18. 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.

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

    DOEpatents

    Sobolevskiy, Anatoly [Orlando, FL; Rossin, Joseph A [Columbus, OH; Knapke, Michael J [Columbus, OH

    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.

  20. Combination of photocatalysis and HC/SCR for improved activity and durability of DeNOx catalysts.

    PubMed

    Heo, Iljeong; Kim, Mun Kyu; Sung, Samkyung; Nam, In-Sik; Cho, Byong K; Olson, Keith L; Li, Wei

    2013-04-16

    A photocatalytic HC/SCR system has been developed and its high deNOx performance (54.0-98.6% NOx conversion) at low temperatures (150-250 °C) demonstrated by using a representative diesel fuel hydrocarbon (dodecane) as the reductant over a hybrid SCR system of a photocatalytic reactor (PCR) and a dual-bed HC/SCR reactor. The PCR generates highly active oxidants such as O3 and NO2 from O2 and NO in the feed stream, followed by the subsequent formation of highly efficient reductants such as oxygenated hydrocarbon (OHC), NH3, and organo-nitrogen compounds. These reductants are the key components for enhancing the low temperature deNOx performance of the dual-bed HC/SCR system containing Ag/Al2O3 and CuCoY in the front and rear bed of the reactor, respectively. The OHCs are particularly effective for both NOx reduction and NH3 formation over the Ag/Al2O3 catalyst, while NH3 and organo-nitrogen compounds are effective for NOx reduction over the CuCoY catalyst. The hybrid HC/SCR system assisted by photocatalysis has shown an overall deNOx performance comparable to that of the NH3/SCR, demonstrating its potential as a promising alternative to the current urea/SCR and LNT technologies. Superior durability of HC/SCR catalysts against coking by HCs has also been demonstrated by a PCR-assisted regeneration scheme for deactivating catalysts.

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

    PubMed

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

    2015-05-19

    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.

  2. 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

  3. Modification of CeO2-ZrO2 catalyst by potassium for NOx-assisted soot oxidation.

    PubMed

    Weng, Duan; Li, Jia; Wu, Xiaodong; Si, Zhichun

    2011-01-01

    Potassium-modified ceria-zirconia catalyst was synthesized by wetness impregnation method. The ageing treatment was performed in static air at 800degrees C for 20 hr to evaluate the thermal stability of the catalyst. The catalysts were characterized by X-ray diffraction, BET surface area, oxygen storage capacity, NO(x)-temperature programmed desorption and soot-temperature programmed oxidation measurements. By introduction of potassium, the maximum soot oxidation rate temperature (T(m)) of the ceria-zirconia based catalyst decreased from 525 to 428 degrees C in the presence of NO under a loose contact mode. The shift of T(m) of the K-modified catalyst after ageing is only 15 degrees C. The enhanced activity of the aged catalyst mainly lies in the promotional effect of potassium on the NO(x)/oxygen storage capacity as well as the soot-catalyst contact.

  4. Regeneration and sulfur poisoning behavior of In/H-BEA catalyst for NOx reduction by CH4

    NASA Astrophysics Data System (ADS)

    Pan, Hua; Jian, Yanfei; Yu, Yanke; He, Chi; Shen, Zhenxing; Liu, Hongxia

    2017-04-01

    Sulfur poisoning and regeneration behavior of In/H-BEA catalyst were carried out in NOx reduction by CH4. In/H-BEA catalyst exhibited a poor resistance to sulfur dioxide after addition of 200 ppm SO2 and 10 vol.% H2O into NO reduction with CH4 at 450 °C for 45 h. Sulfur poisoning of In/H-BEA was attributed to the inhibition of NOx adsorption on Brønsted acid sites, suppression of reaction intermediates generation on the active sites, and the formation of surface sulfate species. The formation of surface sulfate reduced the availability of surface active sites, blocked the pore structure and decreased the surface area of catalyst. These changes in chemical and textural properties resulted in a severe loss in the activity of sulfated In/H-BEA catalyst for NO reduction with CH4. H2 reduction is a promising technology for regeneration of In/H-BEA deactivated by SO2 for removing NOx from lean-burn and diesel exhausts. Indium sulfate could be reduced by H2 to InO+ with In2O3 and In(OH)2+ as the intermediates. The optimal parameters of H2 reduction was regeneration temperature of 400 °C and regeneration time of 60 min which completely recovered the catalytic activity of In/H-BEA.

  5. 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.

  6. 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

  7. Novel Ce-W-Sb mixed oxide catalyst for selective catalytic reduction of NOx with NH3

    NASA Astrophysics Data System (ADS)

    Liu, Jun; Li, Guo-qiang; Zhang, Yong-fa; Liu, Xiao-qing; Wang, Ying; Li, Yuan

    2017-04-01

    A novel Ce3W2SbOx catalyst prepared by the co-precipitation method have been investigated for the selective catalysis reduction (SCR) of NOx with NH3. It was found that the Ce-W-Sb oxide catalyst exhibited an excellent conversion ratio of NOx and a high tolerance to H2O and SO2 in a wide operation temperature window. The catalysts were characterized by N2-adsorption, XRD, Raman, H2-TPR, NH3-TPD, XPS and DRIFTS. The results suggest that the strong interaction between Sb, W and Ce species not only enhances the redox property of the catalyst but also increases the surface acidity, thus promoting the adsorption and activation of NH3 species, which is favorable for high NH3-SCR performance. Based on in situ DRIFTS results, it was concluded that the Langmuir-Hinshelwood (L-H) mechanism existed at the temperature of below 300 °C, while at above 300 °C the Eley-Rideal (E-R) mechanism dominate the NH3-SCR reaction over the Ce3W2SbOx catalyst. Overall, these findings indicate that Ce3W2SbOx is promising for industrial applications.

  8. [Deactivation by SO2 of transition metal oxides modified low-temperature SCR catalyst for NOx reduction with NH3].

    PubMed

    Shen, Bo-xiong; Liu, Ting; Yang, Ting-ting; Xiong, Li-xian; Wang, Jing

    2009-08-15

    MnOx-CeOx/ACF catalyst was prepared by impregnation method, which exhibited high activity for low-temperature selective catalytic reduction of NOx over the temperature range 110-230 degrees C. Experiments results indicated that the catalyst yielded 80% NO conversion at 150 degrees C and 90% at 230 degrees C. The Oxides of Fe,Cu and V were added to the catalysts based on MnOx-CeOx/ACF. The additions of these transition metal oxides had a negative effect on the activity of the catalysts. Compared with MnOx-CeOx/ACF and Cu and V modified catalysts, NO conversion for Fe-MnOx-CeOx/ACF catalyst leveled off at nearly 75% in the first 6 h in the presence of SO2. Two mechanisms of catalyst deactivation by SO2 were discovered by the methods of X-ray photoelectron spectrum (XPS) and Fourier transform infrared spectra (FTIR), indicating that the catalysts were covered by ammonium sulfates and the metal oxides, acting as active components, were also sulfated by SO2 to form metal sulfates.

  9. 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.

  10. 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.

  11. 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.

  12. 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

  13. A Curtin-Hammett mechanism for the copolymerization of ethylene and methyl acrylate monomer using a PymNox nickel catalyst as revealed by DFT computational studies.

    PubMed

    Ramos, Javier; Martínez, Sonia; Cruz, Víctor L; Martínez-Salazar, Javier

    2012-02-01

    In this work, the copolymerization of ethylene and methyl acrylate (MA) as catalyzed by a new Ni-based PymNox organometallic compound was studied computationally. We recently tested the behavior of this type of catalyst in ethylene homopolymerization. Experimental results show that the unsubstituted catalyst Ni2 (aldimino PymNox catalyst) is unable to incorporate the MA monomer, whereas methyl-substituted Ni1 (acetaldimino PymNox catalyst) is able to achieve copolymerization. The reactivities of both catalysts were examined using density functional theory (DFT) models. Based on energy profiles calculated at the BP86 level, a Curtin-Hammett mechanism was proposed to explain the different reactivities of the catalysts in ethylene/MA copolymerization. Our results indicate that the methyl substituent Ni1 introduces additional steric hindrance that results in a catalyst conformation that is better suited to polar monomer incorporation. This model provides insights into the design of new catalysts to produce polar functionalized copolymers based on ethylene.

  14. 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.

  15. Selective catalytic reduction of NOx with NH3 over iron-cerium-tungsten mixed oxide catalyst prepared by different methods

    NASA Astrophysics Data System (ADS)

    Xiong, Zhi-bo; Liu, Jing; Zhou, Fei; Liu, Dun-yu; Lu, Wei; Jin, Jing; Ding, Shi-fa

    2017-06-01

    A series of magnetic Fe0.85Ce0.10W0.05Oz catalysts were synthesized by three different methods(Co-precipitation(Fe0.85Ce0.10W0.05Oz-CP), Hydrothermal treatment assistant critic acid sol-gel method(Fe0.85Ce0.10W0.05Oz-HT) and Microwave irradiation assistant critic acid sol-gel method(Fe0.85Ce0.10W0.05Oz-MW)), and the catalytic activity was evaluated for selective catalytic reduction of NO with NH3. The catalyst was characterized by XRD, N2 adsorption-desorption, XPS, H2-TPR and NH3-TPD. Among the tested catalysts, Fe0.85Ce0.10W0.05Oz-MW shows the highest NOx conversion over per gram in unit time with NOx conversion of 60.8% at 350 °C under a high gas hourly space velocity of 1,200,000 ml/(g h). Different from Fe0.85Ce0.10W0.05Oz-CP catalyst, there exists a large of iron oxide crystallite(γ-Fe2O3 and α-Fe2O3) scattered in Fe0.85Ce0.10W0.05Oz catalysts prepared through hydrothermal treatment or microwave irradiation assistant critic acid sol-gel method, and higher iron atomic concentration on their surface. And Fe0.85Ce0.10W0.05Oz-MW shows higher surface absorbed oxygen concentration and better dispersion compared with Fe0.85Ce0.10W0.05Oz-HT catalyst. These features were favorable for the high catalytic performance of NO reduction with NH3 over Fe0.85Ce0.10W0.05Oz-MW catalyst.

  16. DRIFT study on cerium-tungsten/titania catalyst for selective catalytic reduction of NOx with NH3.

    PubMed

    Chen, Liang; Li, Junhua; Ge, Maofa

    2010-12-15

    CeO(2)/TiO(2) and CeO(2)-WO(3)/TiO(2) catalysts prepared by impregnation method assisted with ultrasonic energy were investigated on the selective catalytic reduction (SCR) of NO(x) (NO and NO(2)) by NH(3). The catalytic activity of 10% CeO(2)/TiO(2) (CeTi) was greatly enhanced by the addition of 6% WO(3) in the broad temperature range of 200-500 °C, the promotion mechanism was proposed on basis of the results of in situ diffuse reflectance infrared transform spectroscopy (DRIFT). When NH(3) was introduced into both catalysts preadsorbed with NO + O(2), SCR would not proceed except for the reaction between NO(2) and ammonia. For CeO(2)/TiO(2) catalysts, coordinated NH(3) linked to Lewis acid sites were the main adsorbed ammonia species. When NO + O(2) was introduced, all the ammonia species consumed rapidly, indicating that these species could react with NO(x) effectively. Two different reaction routes, L-H mechanism at low temperature (<200 °C) and E-R mechanism at high temperatures (>200 °C), were presented for SCR reaction over CeO(2)/TiO(2) catalyst. For CeO(2)-WO(3)/TiO(2) catalysts, the Lewis acid sites on Ce(4+) state could be converted to Brønsted acid sites due to the unsaturated coordination of Ce(n+) and W(n+) ions. When NO + O(2) was introduced, the reaction proceeded more quickly than that on CeO(2)/TiO(2). The reaction route mainly followed E-R mechanism in the temperature range investigated (150-350 °C) over CeO(2)-WO(3)/TiO(2) catalysts. Tungstation was beneficial for the formation of Ce(3+), which would influence the active sites of the catalyst and further change the mechanisms of SCR reaction. In this way, the cooperation of tungstation and the presence of Ce(3+) state resulted in the better activity of CeO(2)-WO(3)/TiO(2) compared to that of CeO(2)/TiO(2).

  17. Oxidation of SO[sub 2] to SO[sub 3] over honeycomb DeNoxing catalysts

    SciTech Connect

    Svachula, J.; Alemany, L.J.; Ferlazzo, N.; Forzatti, P.; Tronconi, E. ); Bregani, F. )

    1993-05-01

    A systematic study addressing the effects of the operating conditions (contact time, temperature), of feed composition (O[sub 2], SO[sub 2], H[sub 2]O, NH[sub 3], NO[sub x], NH[sub 3] + NO[sub x] concentrations), and of catalyst design parameters (wall thickness, V content) in the oxidation of SO[sub 2] to SO[sub 3] over honeycomb commercial-type DeNoxing catalysts is described. Data are presented which refer to transient behavior of the catalysts, indicating that long conditioning times are required associated with the buildup of surface sulfate species. The steady-state reaction rate is of variable order in SO[sub 2], the order increasing with SO[sub 2] concentration as long as this is below 200 ppm and then decreasing; it is asymptotically independent of oxygen, depressed by water, strongly inhibited by ammonia, and slightly enhanced by NO[sub x]. The apparent activation energy changes from [approximately]50 to [approximately]20 kcal/mol on increasing the reaction temperature. A redox steady-state kinetic model is presented which accommodates qualitatively all of the observed effects. Once properly modified the same model has the potential to explain also transient effects during conditioning of the catalyst.

  18. MOF-74 as an Efficient Catalyst for the Low-Temperature Selective Catalytic Reduction of NOx with NH3.

    PubMed

    Jiang, Haoxi; Wang, Qianyun; Wang, Huiqin; Chen, Yifei; Zhang, Minhua

    2016-10-12

    In this work, Mn-MOF-74 with hollow spherical structure and Co-MOF-74 with petal-like shape have been prepared successfully via the hydrothermal method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), thermogravimetry-mass spectrum analysis (TG-MS), N2 adsorption/desorption, scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). It is found that MOF-74(Mn, Co) exhibits the capability for selective catalytic reduction (SCR) of NOx at low temperatures. Both experimental (temperature-programmed desorption, TPD) and computational methods have shown that Co-MOF-74 and Mn-MOF-74 owned high adsorption and activation abilities for NO and NH3. The catalytic activities of Mn-MOF-74 and Co-MOF-74 for low-temperature denitrification (deNOx) in the presence of NH3 were 99% at 220 °C and 70% at 210 °C, respectively. It is found that the coordinatively unsaturated metal sites (CUSs) in M-MOF-74 (M = Mn and Co) played important roles in SCR reaction. M-MOF-74 (M = Mn and Co), especially Mn-MOF-74, showed excellent catalytic performance for low-temperature SCR. In addition, in the reaction process, NO conversion on Mn-MOF-74 decreased with the introduction of H2O and SO2 and almost recovered when gas was cut off. However, for Co-MOF-74, SO2 almost has no effect on the catalytic activity. This work showed that MOF-74 could be used prospectively as deNOx catalyst.

  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. Evaluation of Cu-PPHs as active catalysts for the SCR process to control NOx emissions from heavy duty diesel vehicles.

    PubMed

    Moreno-Tost, Ramón; Oliveira, Mona Lisa; Eliche-Quesada, Dolores; Jiménez-Jiménez, José; Jiménez-López, Antonio; Rodríguez-Castellón, Enrique

    2008-06-01

    Copper based catalysts supported on mesoporous materials, which were in turn based on a surfactant expanded zirconium phosphate for the formation of silica galleries in the interlayer space, were prepared by the impregnation method. They were then characterised and tested in the selective catalytic reduction of NO with ammonia as active catalysts for the control of the NOx emissions from heavy duty vehicles. Copper catalysts displayed a high catalytic performance, even in the presence of 14% (v/v) of H2O and 100 ppm of SO2. They also displayed improved catalytic behaviour when compared to a CuZSM5 catalyst.

  1. Pilot-scale evaluation of a novel TiO2-supported V2O5 catalyst for DeNOx at low temperatures at a waste incinerator.

    PubMed

    Jung, Hyounduk; Park, Eunseuk; Kim, Minsu; Jurng, Jongsoo

    2017-03-01

    The removal of NOx by catalytic technology at low temperatures is significant for treatment of flue gas in waste incineration plants, especially at temperatures below 200°C. A novel highly active TiO2-supported vanadium oxide catalyst at low temperatures (200-250°C) has been developed for the selective catalytic reduction (SCR) de-NOx process with ammonia. The catalyst was evaluated in a pilot-scale equipment, and the results were compared with those obtained in our previous work using laboratory scale (small volume test) equipment as well as bench-scale laboratory equipment. In the present work, we have performed our experiments in pilot scale equipment using a part of effluent flue gas that was obtained from flue gas cleaning equipment in a full-scale waste incineration plant in South Korea. Based on our previous work, we have prepared a TiO2-supported V2O5 catalyst coated (with a loading of 7wt% of impregnated V2O5) on a honeycomb cordierite monolith to remove NOx from a waste incinerator flue gas at low temperatures. The NOx (nitrogen oxides) removal efficiency of the SCR catalyst bed was measured in a catalyst fixed-bed reactor (flow rate: 100m(3)h(-1)) using real exhaust gas from the waste incinerator. The experimental results showed that the V2O5/TiO2 SCR catalyst exhibited good DeNOx performance (over 98% conversion at an operating temperature of 300°C, 95% at 250°C, and 70% at 200°C), and was much better than the performance of commercial SCR catalysts (as low as 55% conversion at 250°C) under the same operating conditions. Copyright © 2016 Elsevier Ltd. All rights reserved.

  2. [Selective catalytic reduction of NOx over Pd/CeZr/TiO2/Al2O3 wire-mesh honeycomb catalysts].

    PubMed

    Sun, Hong; Quan, Xie; Zhang, Yao-bin; Zhao, Ya-zhi

    2008-06-01

    Pd/CeZr/TiO2/Al2O3 wire-mesh honeycomb catalyst was prepared by sol-gel and impregnation. Furthermore, selective catalytic reduction of NOx over Pd/CeZr/TiO2/Al2O3 wire-mesh honeycomb catalyst with propylene under lean burn condition was studied. The effects of the concentration of tetra-n-butyl titanate and dipcoat cycles on TiO2 washcoat were studied by SEM, and the effects of Pd concentration, O2 concentration and gas velocity on catalytic activity were investigated. The experimental results showed that the TiO2 washcoat on wire-mesh support is even and crack-free when the support is impregnated in 20.0% tetra- n-butyl titanate sol for 2 cycles. The NOx conversion decreases with Pd concentration increase. When Pd concentration is 0.23%, NOx conversion is highest. NOx conversion increases with oxygen concentration increase in the range of 1.5%-6.0%. However, when oxygen concentration is higher than 6.0%, NOx conversion decreases with increasing oxygen concentration. The NOx conversion decreases with gas velocity increase and its effect is severer at high temperature than low temperature.

  3. 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

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. Environmentally-benign catalysts for the selective catalytic reduction of NO(x) from diesel engines: structure-activity relationship and reaction mechanism aspects.

    PubMed

    Liu, Fudong; Yu, Yunbo; He, Hong

    2014-08-11

    Selective catalytic reduction of NOx using NH3 or hydrocarbons (NH3-SCR or HC-SCR) in oxygen-rich exhaust from diesel engines remains a major challenge in environmental catalysis. The development of highly efficient, stable and environmentally-benign catalysts for SCR processes is very important for practical use. In this feature article, the structure-activity relationship of vanadium-free catalysts in the NH3-SCR reaction is discussed in detail, including Fe-, Ce-based oxide catalysts and Fe-, Cu-based zeolite catalysts, which is beneficial for catalyst redesign and activity improvement. Based on our research, a comprehensive mechanism contributing to the performance of Ag/Al2O3 in HC-SCR is provided, giving a clue to the design of a catalytic system with high efficiency.

  10. 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.

  11. 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...

  12. Mono- and bimetallic Rh and Pt NSR-catalysts prepared by controlled deposition of noble metals on support or storage component

    PubMed Central

    Büchel, Robert; Pratsinis, Sotiris E.; Baiker, Alfons

    2013-01-01

    Mono- and bimetallic Rh and Pt based NOx storage-reduction (NSR) catalysts, where the noble metals were deposited on the Al2O3 support or BaCO3 storage component, have been prepared using a twin flame spray pyrolysis setup. The catalysts were characterized by nitrogen adsorption, CO chemisorption combined with diffuse reflectance infrared Fourier transform spectroscopy, X-ray diffraction, and scanning transmission electron microscopy combined with energy dispersive X-ray spectroscopy. The NSR performance of the catalysts was investigated by fuel lean/rich cycling in the absence and presence of SO2 (25 ppm) as well as after H2 desulfation at 750 °C. The performance increased when Rh was located on BaCO3 enabling good catalyst regeneration during the fuel rich phase. Best performance was observed for bimetallic catalysts where the noble metals were separated, with Pt on Al2O3 and Rh on BaCO3. The Rh-containing catalysts generally showed much higher tolerance to SO2 during fuel rich conditions and lost only little activity during thermal aging at 750 °C. PMID:23741085

  13. Mono- and bimetallic Rh and Pt NSR-catalysts prepared by controlled deposition of noble metals on support or storage component.

    PubMed

    Büchel, Robert; Pratsinis, Sotiris E; Baiker, Alfons

    2012-02-22

    Mono- and bimetallic Rh and Pt based NOx storage-reduction (NSR) catalysts, where the noble metals were deposited on the Al2O3 support or BaCO3 storage component, have been prepared using a twin flame spray pyrolysis setup. The catalysts were characterized by nitrogen adsorption, CO chemisorption combined with diffuse reflectance infrared Fourier transform spectroscopy, X-ray diffraction, and scanning transmission electron microscopy combined with energy dispersive X-ray spectroscopy. The NSR performance of the catalysts was investigated by fuel lean/rich cycling in the absence and presence of SO2 (25 ppm) as well as after H2 desulfation at 750 °C. The performance increased when Rh was located on BaCO3 enabling good catalyst regeneration during the fuel rich phase. Best performance was observed for bimetallic catalysts where the noble metals were separated, with Pt on Al2O3 and Rh on BaCO3. The Rh-containing catalysts generally showed much higher tolerance to SO2 during fuel rich conditions and lost only little activity during thermal aging at 750 °C.

  14. Deactivation mechanism of potassium on the V₂O₅/CeO₂ catalysts for SCR reaction: acidity, reducibility and adsorbed-NOx.

    PubMed

    Peng, Yue; Li, Junhua; Huang, Xu; Li, Xiang; Su, Wenkang; Sun, Xiaoxu; Wang, Dezhi; Hao, Jiming

    2014-04-15

    A series of V2O5/CeO2 catalysts with different potassium loadings were prepared to investigate alkali deactivations for selective catalytic reduction of NOx with NH3. An alkali poisoning mechanism could be attributed to surface acidity, reducibility, and NOx adsorption/desorption behaviors. The detailed factors are as follows: (1) decrease of surface acidity suppresses NH3 adsorption by strong bonding of alkali to vanadia (major factor); (2) low reducibility prohibits NH3 activation and NO oxidation by formation bonding of alkali to vanadia and ceria (important factor); (3) active NOx(-) species at low temperature diminish because of coverage of alkali on the surfaces (minor factor); and (4) stable, inactive nitrate species at high temperature increase by generating new basic sites (important factor).

  15. Effect of MoO3 on vanadium based catalysts for the selective catalytic reduction of NOx with NH3 at low temperature.

    PubMed

    Zhu, Lin; Zhong, Zhaoping; Yang, Han; Wang, Chunhua

    2017-06-01

    The selective catalytic reduction (SCR) activities of the MoO3 doped V/WTi catalysts prepared by the incipient wetness impregnation method at low temperature were investigated. The results showed that the addition of MoO3 could enhance the NOx conversion at low temperature and the best SCR activity was obtained when the dosage of MoO3 reached 5wt.%. The NH3-TPD and DRIFTS experiments indicated that the addition of MoO3 changed the type and number of acid sites on the surface of catalysts and reaction activities of acid sites were altered at the same time. The redox capacity and amount of active oxygen species got improved for V3Mo5/WTi catalyst, which could be confirmed by the H2-TPR and transient response experiments. Water vapor inhibited the NOx conversion at low temperature. Deposition of ammonium sulfate or bisulfate might be main reason for the loss of catalytic activity in the presence of SO2 at low temperature. Choosing the suitable NH3/NO ratio and elevation of reaction temperature both could weaken the influence of SO2 on the SCR activity of the V3Mo5/WTi catalyst. Thermal treatment of the deactivated catalyst at 350°C could get the low temperature activity recovered. The decrease of GHSV improved the deNOx efficiency at low temperature and we speculated that the rational technological process and operation parameters could contribute to the application of this kind of catalysts in real industrial environment. Copyright © 2016. Published by Elsevier B.V.

  16. 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.

  17. Investigation on the structure-activity relationship of BaO promoting Pd/CeO2-ZrO2 catalysts for CO, HC and NOx conversions.

    PubMed

    Lin, Jiansong; Yang, Linyan; Wang, Ting; Zhou, Renxian

    2017-03-15

    Four different synthetic routes (co-precipitation, oxidation-precipitation, citric acid sol-gel and reversed microemulsion) are adopted to prepare barium modified Pd/CeO2-ZrO2 catalysts and their catalytic activity towards CO, HC and NOx conversions is studied. The surface and bulk properties of these catalysts are characterized via XRD, N2 adsorption, XPS, UV-Raman, H2-TPR, and in situ DRIFTS. The catalyst prepared via the co-precipitation method exhibits the optimum three-way catalytic behavior, which is mainly due to its superior redox ability, whereas the oxidation-precipitation synthesis renders the catalyst with the best homogeneity and thermal resistance. However, for the catalyst prepared via the sol-gel route, its worst NOx reduction capacity is verified by the scarce appearance of negatively charged Pd(0)-N[double bond, length as m-dash]O(δ-) species, which is related to the faster dissociation of NO based on in situ DRIFTS, and the abundance of surface CO-Pd(+) species reveals its unsatisfactory deep oxidizability of the HC reactant.

  18. Alkali metal poisoning of a CeO2-WO3 catalyst used in the selective catalytic reduction of NOx with NH3: an experimental and theoretical study.

    PubMed

    Peng, Yue; Li, Junhua; Chen, Liang; Chen, Jinghuan; Han, Jian; Zhang, He; Han, Wei

    2012-03-06

    The alkali metal-induced deactivation of a novel CeO(2)-WO(3) (CeW) catalyst used for selective catalytic reduction (SCR) was investigated. The CeW catalyst could resist greater amounts of alkali metals than V(2)O(5)-WO(3)/TiO(2). At the same molar concentration, the K-poisoned catalyst exhibited a greater loss in activity compared with the Na-poisoned catalyst below 200 °C. A combination of experimental and theoretical methods, including NH(3)-TPD, DRIFTS, H(2)-TPR, and density functional theory (DFT) calculations, were used to elucidate the mechanism of the alkali metal deactivation of the CeW catalyst in SCR reaction. Experiments results indicated that decreases in the reduction activity and the quantity of Brønsted acid sites rather than the acid strength were responsible for the catalyst deactivation. The DFT calculations revealed that Na and K could easily adsorb on the CeW (110) surface and that the surface oxygen could migrate to cover the active tungsten, and then inhibit the SCR of NO(x) with ammonia. Hot water washing is a convenient and effective method to regenerate alkali metal-poisoned CeW catalysts, and the catalytic activity could be recovered 90% of the fresh catalyst.

  19. Co-firing coal and straw in PF boilers -- Performance impact of straw with emphasis on SCR catalyst for deNOx catalysts

    SciTech Connect

    Wieck-Hansen, K.

    1999-07-01

    A two year co-firing coal/straw program was carried out on a 150 MWel pulverized fired boiler at Studstrupvaerket in Denmark from January 1996 to January 1998. The reason for burning straw is based on a political decision where the Power utilities have accepted to burn 1 mill ton straw/year and 0.4-mill tons wood. This amount is about 5 % of the total fuel consumption for energy production in Denmark. Straw is found to be CO{sub 2} neutral and therefore an important factor in CO{sub 2} reduction. This full-scale long-term test was based on many years' experience with straw firing. Late 1980 tests with coal and straw co-combustion on a test CFB plant were carried out with such successful results, that a full scale plant of 80 MWth was built and commissioned in January 1992. In 1992 the first tests were performed on a grate fired boiler, where up to 30 % straw on energy basis, were co-fired with coal. The growing optimism lead to a short-term test with coal and straw on a pulverized fuel-fired 330th MW boiler in 1993. Limited corrosion was found and a long-term test was accepted on another full-scale boiler. To minimize the overall risk, the authors chose an old boiler, but with the intention of using the technique on new and modern plants equipped with desulfurization and DeNOx catalyst. A comprehensive test program was carried out in order to evaluate and quantify the impact of straw on corrosion, slagging and fouling, emissions and on SCR catalysts deactivation.

  20. The Active Sites of a Rod-Shaped Hollandite DeNOx Catalyst.

    PubMed

    Hu, Pingping; Schuster, Manfred Erwin; Huang, Zhiwei; Xu, Fei; Jin, Shifeng; Chen, Yaxin; Hua, Weiming; Su, Dang Sheng; Tang, Xingfu

    2015-06-26

    The identification of catalytically active sites (CASs) in heterogeneous catalysis is of vital importance to design and develop improved catalysts, but remains a great challenge. The CASs have been identified in the low-temperature selective catalytic reduction of nitrogen oxides by ammonia (SCR) over a hollandite manganese oxide (HMO) catalyst with a rod-shaped morphology and one-dimensional tunnels. Electron microscopy and synchrotron X-ray diffraction determine the surface and crystal structures of the one-dimensional HMO rods closed by {100} side facets and {001} top facets. A combination of X-ray absorption spectra, molecular probes with potassium and nitric oxide, and catalytic tests reveals that the CASs are located on the {100} side facets of the HMO rods rather than on the top facets or in the tunnels, and hence semi-tunnel structural motifs on the {100} facets are evidenced to be the CASs of the SCR reaction. This work paves the way to further investigate the intrinsic mechanisms of SCR reactions.

  1. 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.

  2. Mechanistic Investigation into the Effect of Sulfuration on the FeW Catalysts for the Selective Catalytic Reduction of NOx with NH3.

    PubMed

    Wang, Hui; Qu, Zhenping; Dong, Shicheng; Tang, Chen

    2017-03-01

    Iron tungsten (FeW) catalyst is a potential candidate for the selective catalytic reduction (SCR) of NOx with ammonia because of its excellent performance in a wide operating window. Sulfur poisoning effects in SCR catalysts have long been recognized as a challenge in development of efficient catalysts for applications. In this paper, the impact of sulfuration on catalyst structure, NH3-SCR reaction performance and mechanism was systematically investigated through spectroscopic and temperature-programmed approaches. The sulfuration inhibited the SCR activity at low temperatures (<300 °C), while no evident effect was observed at high temperatures (≥300 °C). After sulfuration for FeW oxides catalyst, the organic-like with covalent S═O bonds sulfate species were mainly formed over the FeW catalysts. Combining TPD with in situ DRIFTS results, it was found that the Lewis and the Brønsted acidity were enhanced by the interaction between metal species and sulfate species due to the strong electron withdrawing effect of the S═O double bonds. The in situ DRIFTS study showed that the formation of NO2 was hindered, leading to the "fast-SCR" pathway was partly cut off by the sulfuration process and thereby the loss of SCR activity at low temperatures. However, the Langmuir-Hinshelwood reaction pathway between adsorbed NH3/NH4(+) species and nitrate species was facilitated and dominated at high temperatures, making the as-synthesized FeW catalysts resistant to SO2 poisoning.

  3. 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.

  4. 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.

  5. 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.

  6. 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

  7. WO3/CeO2/TiO2 Catalysts for Selective Catalytic Reduction of NO(x) by NH3: Effect of the Synthesis Method.

    PubMed

    Michalow-Mauke, Katarzyna A; Lu, Ye; Ferri, Davide; Graule, Thomas; Kowalski, Kazimierz; Elsener, Martin; Kröcher, Oliver

    2015-01-01

    WO3/CeO2/TiO2, CeO2/TiO2 and WO3/TiO2 catalysts were prepared by wet impregnation. CeO2/TiO2 and WO3/TiO2 showed activity towards the selective catalytic reduction (SCR) of NO(x) by NH3, which was significantly improved by subsequent impregnation of CeO/TiO2 with WO3. Catalytic performance, NH3 oxidation and NH3 temperature programmed desorption of wet-impregnated WO3/CeO2/TiO2 were compared to those of a flame-made counterpart. The flame-made catalyst exhibits a peculiar arrangement of W-Ce-Ti-oxides that makes it very active for NH3-SCR. Catalysts prepared by wet impregnation with the aim to mimic the structure of the flame-made catalyst were not able to fully reproduce its activity. The differences in the catalytic performance between the investigated catalysts were related to their structural properties and the different interaction of the catalyst components.

  8. The deactivation mechanism of Pb on the Ce/TiO2 catalyst for the selective catalytic reduction of NOx with NH3: TPD and DRIFT studies.

    PubMed

    Wang, Shu-Xian; Guo, Rui-Tang; Pan, Wei-Guo; Li, Ming-Yuan; Sun, Peng; Liu, Shu-Ming; Liu, Shuai-Wei; Sun, Xiao; Liu, Jian

    2017-02-15

    It was well recognized that Pb had a poisoning effect on a SCR catalyst. In this study, the deactivation mechanism of Pb on the Ce/TiO2 catalyst was investigated based on the characterization results of TPD and in situ DRIFT studies. It was found that the addition of Pb on the Ce/TiO2 catalyst not only inhibited the adsorption and activation of NH3 species, but also led to the decrease of the activity of adsorbed NH3 species in the SCR reaction. The adsorption of NOx species and the oxidation of NO by O2 over the Ce/TiO2 catalyst were also suppressed by the addition of Pb, while the reactivity of adsorbed NO2 species did not decrease. Moreover, the results revealed that the NH3-SCR reaction over the Ce/TiO2 catalyst followed both the E-R and L-H mechanisms, while the NH3-SCR reaction over Ce/TiO2-Pb was mainly controlled by the L-H mechanism. The contributions of the L-H mechanism to the SCR reactions over Ce/TiO2 and Ce/TiO2-Pb decreased with increasing reaction temperature. The deactivation of Ce/TiO2-Pb was mainly attributed to the suppressed NH3 adsorption and activation, accompanied by the inhibited NO oxidation and the decrease of Brønsted acid sites.

  9. Hybrid selective noncatalytic reduction (SNCR)/selective catalytic reduction (SCR) for NOx removal using low-temperature SCR with Mn-V2O5/TiO2 catalyst.

    PubMed

    Choi, Sung-Woo; Choi, Sang-Ki; Bae, Hun-Kyun

    2015-04-01

    A hybrid selective noncatalytic reduction/selective catalytic reduction (SNCR/SCR) system that uses two types of technology, low-temperature SCR process and SNCR process, was designed to develop nitrogen oxide (NOx) reduction technology. SCR was conducted with space velocity (SV)=2400 hr(-1) and hybrid SNCR/SCR with SV=6000 hr(-1), since the study focused on reducing the amount of catalyst and both achieved 98% NOx reduction efficiency. Characteristics of NOx reduction by NH3 were studied for low-temperature SCR system at 150 °C using Mn-V2O5/TiO2 catalyst. Mn-added V2O5/TiO2 catalyst was produced, and selective catalyst reduction of NOx by NH3 was experimented. NOx reduction rate according to added Mn content in Mn-V2O5/TiO2 catalyst was studied with varying conditions of reaction temperature, normalized stoichiometric ratio (NSR), SV, and O2 concentration. In the catalyst experiment according to V2O5 concentration, 1 wt.% V2O5 catalyst showed the highest NOx reduction rate: 98% reduction at temperature window of 200~250 °C. As a promoter of the V2O5 catalyst, 5 wt.% Mn was added, and the catalyst showed 47~90% higher efficiency even with low temperatures, 100~200 °C. Mn-V2O5/TiO2 catalyst, prepared by adding 5 wt.% Mn in V2O5/TiO2 catalyst, showed increments of catalyst activation at 150 °C as well as NOx reduction. Mn-V2O5/TiO2 catalyst showed 8% higher rate for NOx reduction compared with V2O5/TiO2 catalyst in 150 °C SCR. Thus, (5 wt.%)Mn-(1 wt.%)V2O5/TiO2 catalyst was applied in SCR of hybrid SNCR/SCR system of low temperature at 150 °C. Low-temperature SCR hybrid SNCR/SCR (150 °C) system and hybrid SNCR/SCR (350 °C) showed 91~95% total reduction rate with conditions of SV=2400~6000 hr(-1) SCR and 850~1050 °C SNCR, NSR=1.5~2.0, and 5% O2. Hybrid SNCR/SCR (150 °C) system proved to be more effective than the hybrid SNCR/SCR (350 °C) system at low temperature. NOx control is very important, since they are the part of greenhouse gases as well as the

  10. Density functional calculations in the automotive industry: Catalyst supports and hydrogen storage materials

    NASA Astrophysics Data System (ADS)

    Wolverton, Christopher

    2006-03-01

    In my talk, I will describe some uses of density functional theory (DFT) calculations in the research laboratory at Ford, and particularly highlight work that was inspired by, or performed in collaboration with Ken Hass. I begin with a discussion of past work on γ-Al2O3 catalyst support materials, but also discuss the current main focus of our group's activities: hydrogen storage materials. Catalyst Supports: In current three-way automotive catalysts, precious metals are often supported by the phase of aluminum oxide known as γ-Al2O3. Despite the ubiquitous nature of this oxide in current automobile catalysts, and a considerable amount of effort expended to understand this material, many questions about the phase stability and even crystal structure of γ-Al2O3 remain. DFT calculations have made significant progress in unraveling these unanswered questions, allowing one to construct realistic models of the supported catalysts materials. Hydrogen Storage Materials: One of the major bottlenecks to the widespread use of hydrogen-fueled vehicles is the ability to store sufficient energy on-board to enable vehicle attributes acceptable to customers. I will give a general introduction to the topic of hydrogen storage, and a broad survey of the various classes of hydrogen storage technologies, and point out some pros and cons associated with each class. Currently known technologies have insufficient usable energy densities, and I will describe how DFT calculations are aiding the search for improved high density storage materials.

  11. 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.

  12. 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

    2013-05-07

    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.

  13. 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.

  14. 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. Copyright © 2012 Elsevier B.V. All rights reserved.

  15. 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

  16. SSZ-52, a zeolite with an 18-layer aluminosilicate framework structure related to that of the DeNOx catalyst Cu-SSZ-13.

    PubMed

    Xie, Dan; McCusker, Lynne B; Baerlocher, Christian; Zones, Stacey I; Wan, Wei; Zou, Xiaodong

    2013-07-17

    A new zeolite (SSZ-52, |(C14H28N)6Na6(H2O)18|[Al12Si96O216]), related to the DeNOx catalyst Cu-SSZ-13 (CHA framework type), has been synthesized using an unusual polycyclic quaternary ammonium cation as the structure-directing agent. By combining X-ray powder diffraction (XPD), high-resolution transmission electron microscopy (HRTEM) and molecular modeling techniques, its porous aluminosilicate framework structure (R3m, a = 13.6373(1) Å, c = 44.7311(4) Å), which can be viewed as an 18-layer stacking sequence of hexagonally arranged (Si,Al)6O6 rings (6-rings), has been elucidated. The structure has a three-dimensional 8-ring channel system and is a member of the ABC-6 family of zeolites (those that can be described in terms of 6-ring stacking sequences) like SSZ-13, but it has cavities that are twice as large. The code SFW has been assigned to this new framework type. The large cavities contain pairs of the bulky organic cations. HRTEM and XPD simulations show that stacking faults do occur, but only at the 5-10% level. SSZ-52 has considerable potential as a catalyst in the areas of gas conversion and sequestration.

  17. Task 2.6 - Catalyst for Utilization of Methane in Selective Catalytic Reduction of NOx: Topical report, July 1, 1995

    SciTech Connect

    1997-12-31

    Selective catalytic reduction (SCR) of nitrogen oxides (NO{sub x}) in flue gas or engine exhaust gas with hydrocarbons as the reductant has great potential for less expense, less pollution, and easier operation than SCR with ammonia. Methane is the preferred reducing gas because of its low cost and low toxicity. Stable, low-cost catalysts for SCR with methane are required to demonstrate this technology for controlling NO{sub x} emissions. Several cobalt and nickel catalysts on synthetic clay and uranium oxide supports were investigated for their activities in reducing NO{sub x} with methane in the presence of air. The efficiency of the synthetic clay-supported nickel and cobalt catalysts for nitric oxide (NO) reduction with methane as the reducing gas was poor. The nickel oxide-uranium oxide catalyst, which was chosen for its high stability, was also ineffective. Results from the two-step experiments conducted at two temperatures produced some interesting information on the reactions of methane with the catalysts and the reactivity of the carbonaceous intermediate. The carbonaceous material formed from methane dissociation at 450{degrees}C not only reduces NO to N{sub 2}O at lower temperatures, but also prevents oxidation of NO to NO{sub 2}. Unfortunately, the carbonaceous forms that reduce the NO are not available for reactions at 400{degrees}C in the presence of oxygen. A two-step process employing this chemistry would be difficult because the catalyst would have to be cycled between the two temperatures. Also the desired reduction to nitrogen is not very efficient.

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

    DOEpatents

    Sobolevskiy, Anatoly [Orlando, FL; Rossin, Joseph A [Columbus, OH; Knapke, Michael J [Columbus, OH

    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.

  19. CRADA Final Report: Mechanisms of Sulfur Poisoning of NOx Adsorber Materials

    SciTech Connect

    Kim, Do Heui; Muntean, George G.; Peden, Charles H. F.; Howden, Ken; Stafford, Randy; Stang, John; Yezerets, Aleksey; Currier, Neal; Chen, H. -Y.; Hess, H.

    2009-03-01

    The control of NOx (NO and NO2) emissions from so-called ‘lean-burn’ vehicle engines remains a challenge. The now commercial NOx adsorber (also known as lean-NOx trap (LNT) and NOx storage reduction (NSR) catalyst) technology is based upon the concept of storing NOx as nitrates over storage components, typically alkali or alkaline-earth species such as barium, during a lean-burn operation cycle and then reducing the stored nitrates to N2 during fuel-rich conditions over a precious metal catalyst. In part via this successful five-year CRADA project between PNNL and Cummins Inc. (CRADA PNNL/213), Cummins and the Johnson/Matthey Company commercialized this technology on the 2007 Dodge Ram pickup truck. In particular, this CRADA has focused on problems arising from either or both thermal and SO2 deactivation which were impeding the ability of the technology to meet durability standards. The results obtained in this CRADA have provided an essential understanding of these deactivation processes thereby leading to materials and process improvements that enabled the commercialization effort. The objective of this project has been to identify a clear pathway to robust NOx after-treatment solutions for light-duty diesel engines. The project focussed on understanding and characterizing the NOx storage, release and conversion of existing NOx adsorber materials. The impact of sulfur on these processes was studied, with special attention given to methods of regenerating the catalyst in the presence of sulfur and the effects of these regeneration treatments on long-term catalyst durability. Model catalysts and more fully formulated catalysts were both studied. The goal of this project has been to identify and understand the deactivation mechanisms of LNT materials in order to provide more robust systems for diesel after-treatment systems that will meet the key emission standards for NOx. Furthermore, the project aimed to provide information critical to

  20. Response improvement of a mover device using hydrogen storage alloy powder by addition of catalyst

    NASA Astrophysics Data System (ADS)

    Sato, Akira; Akazawa, Kaoru; Ogasawara, Takashi; Uchida, Haru-Hisa; Nishi, Yoshitake

    2007-01-01

    Recently we proposed a mechanical mover device in a unimorph structure with powder hydrogen storage alloy dispersed. A silicone rubber sheet with the alloy was piled up on another pure silicone rubber sheet, then mechanical movement was generated by hydrogen gas absorption and desorption. Because the response of the movement was slow, therefore, in this research we tested the additive effect of catalyst of Pd-Al IIO 3 powder into the hydrogen storage alloy powder before mixing with rubber. The mover device with the catalyst indicated drastically modified responses, such as higher initial moving rate and also larger displacement. The results suggested the possibility of the device for medical purpose such as catheter because of a powerful but tender characteristic of the device.

  1. 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.

  2. Nano-structured gold catalysts supported on CeO2 and CeO2-Al2O3 for NOx reduction by CO: effect of catalyst pretreatment and feed composition.

    PubMed

    Ilieva-Gencheva, L; Pantaleo, G; Mintcheva, N; Ivanov, I; Venezia, A M; Andreeva, D

    2008-02-01

    Gold catalysts supported on ceria and ceria-alumina were studied in NOx reduction by CO. Gold was loaded using deposition-precipitation method. The ceria-alumina (20 wt% alumina) support was synthesized by co-precipitation. The average size of gold and ceria nano-particles was bellow 10 nm. It was established that the type of pretreatment do not have a substantial effect on the catalytic activity. The presence of O2 in the feed leads to a high conversion of CO to CO2 but no NO conversion was registered. Both NO and CO conversion was increased adding H2 to the feed. The catalytic activity became higher upon adding higher amount of H2. Supplementary to the main reaction parallel reactions took place. Bellow 200 degrees C N2O formation and at 250 degrees C and above the NH3 formation was detected. At around 200 degrees C it was established 100% selectivity to N2. The addition of water to the feed influenced positively the CO conversion and did not influence negatively the conversion of NO. The selectivity to N2 at around 200 degrees C remained 100% independent of the presence of moisture. Alumina in the mixed support prevents the sintering of both gold and ceria nano-particles. The results obtained make the catalysts containing gold supported on ceria-alumina promising for practical application.

  3. System and method for controlling an engine based on ammonia storage in multiple selective catalytic reduction catalysts

    DOEpatents

    Sun, MIn; Perry, Kevin L.

    2015-11-20

    A system according to the principles of the present disclosure includes a storage estimation module and an air/fuel ratio control module. The storage estimation module estimates a first amount of ammonia stored in a first selective catalytic reduction (SCR) catalyst and estimates a second amount of ammonia stored in a second SCR catalyst. The air/fuel ratio control module controls an air/fuel ratio of an engine based on the first amount, the second amount, and a temperature of a substrate disposed in the second SCR catalyst.

  4. 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.

  5. Novel Co-Mg-Al-Ti-O catalyst derived from hydrotalcite-like compound for NO storage/decomposition.

    PubMed

    Cheng, Jie; Wang, Xiaoping; Ma, Chunyan; Hao, Zhengping

    2012-01-01

    Catalysts of Co1.5Mg1.5/Al0.9Ti0.1O and Co1.5Mg1.5/A1O were successfully prepared by calcinations of corresponding hydrotalcite-like compounds at 800 degrees C for 4 hr. The derived oxides were of spinel phase and a small quantity of Ti substitution did not change the crystal purity. Their catalytic performance for the NO storage/decomposition was investigated. Ti incorporation enhanced the NO decomposition activity while has an opposite effect on the storage capacity of catalyst. In situ FT-IR spectra of the catalysts showed that the final adsorption species on the catalysts was coordinated nitrates/nitrites. In addition, NO storage/decomposition mechanism has been discussed on the basis of these observations.

  6. 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.

  7. 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.

  8. Single-catalyst high-weight% hydrogen storage in an N-heterocycle synthesized from lignin hydrogenolysis products and ammonia

    NASA Astrophysics Data System (ADS)

    Forberg, Daniel; Schwob, Tobias; Zaheer, Muhammad; Friedrich, Martin; Miyajima, Nobuyoshi; Kempe, Rhett

    2016-10-01

    Large-scale energy storage and the utilization of biomass as a sustainable carbon source are global challenges of this century. The reversible storage of hydrogen covalently bound in chemical compounds is a particularly promising energy storage technology. For this, compounds that can be sustainably synthesized and that permit high-weight% hydrogen storage would be highly desirable. Herein, we report that catalytically modified lignin, an indigestible, abundantly available and hitherto barely used biomass, can be harnessed to reversibly store hydrogen. A novel reusable bimetallic catalyst has been developed, which is able to hydrogenate and dehydrogenate N-heterocycles most efficiently. Furthermore, a particular N-heterocycle has been identified that can be synthesized catalytically in one step from the main lignin hydrogenolysis product and ammonia, and in which the new bimetallic catalyst allows multiple cycles of high-weight% hydrogen storage.

  9. Single-catalyst high-weight% hydrogen storage in an N-heterocycle synthesized from lignin hydrogenolysis products and ammonia.

    PubMed

    Forberg, Daniel; Schwob, Tobias; Zaheer, Muhammad; Friedrich, Martin; Miyajima, Nobuyoshi; Kempe, Rhett

    2016-10-20

    Large-scale energy storage and the utilization of biomass as a sustainable carbon source are global challenges of this century. The reversible storage of hydrogen covalently bound in chemical compounds is a particularly promising energy storage technology. For this, compounds that can be sustainably synthesized and that permit high-weight% hydrogen storage would be highly desirable. Herein, we report that catalytically modified lignin, an indigestible, abundantly available and hitherto barely used biomass, can be harnessed to reversibly store hydrogen. A novel reusable bimetallic catalyst has been developed, which is able to hydrogenate and dehydrogenate N-heterocycles most efficiently. Furthermore, a particular N-heterocycle has been identified that can be synthesized catalytically in one step from the main lignin hydrogenolysis product and ammonia, and in which the new bimetallic catalyst allows multiple cycles of high-weight% hydrogen storage.

  10. Single-catalyst high-weight% hydrogen storage in an N-heterocycle synthesized from lignin hydrogenolysis products and ammonia

    PubMed Central

    Forberg, Daniel; Schwob, Tobias; Zaheer, Muhammad; Friedrich, Martin; Miyajima, Nobuyoshi; Kempe, Rhett

    2016-01-01

    Large-scale energy storage and the utilization of biomass as a sustainable carbon source are global challenges of this century. The reversible storage of hydrogen covalently bound in chemical compounds is a particularly promising energy storage technology. For this, compounds that can be sustainably synthesized and that permit high-weight% hydrogen storage would be highly desirable. Herein, we report that catalytically modified lignin, an indigestible, abundantly available and hitherto barely used biomass, can be harnessed to reversibly store hydrogen. A novel reusable bimetallic catalyst has been developed, which is able to hydrogenate and dehydrogenate N-heterocycles most efficiently. Furthermore, a particular N-heterocycle has been identified that can be synthesized catalytically in one step from the main lignin hydrogenolysis product and ammonia, and in which the new bimetallic catalyst allows multiple cycles of high-weight% hydrogen storage. PMID:27762267

  11. 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

  12. 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.

  13. UREA INFRASTRUCTURE FOR UREA SCR NOX REDUCTION

    SciTech Connect

    Bunting, Bruce G.

    2000-08-20

    Urea SCR is currently the only proven NOX aftertreatment for diesel engines - high NOX reduction possible - some SCR catalyst systems are robust against fuel sulfur - durability has been demonstrated - many systems in the field - long history in other markets - Major limitations to acceptance - distribution of urea solution to end user - ensuring that urea solution is added to vehicle.

  14. 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.

  15. Promotional effects of Titanium additive on the surface properties, active sites and catalytic activity of W/CeZrOx monolithic catalyst for the selective catalytic reduction of NOx with NH3

    NASA Astrophysics Data System (ADS)

    Xu, Haidi; Feng, Xi; Liu, Shuang; Wang, Yun; Sun, Mengmeng; Wang, Jianli; Chen, Yaoqiang

    2017-10-01

    CeZrTixO2 mixed oxides were prepared by a co-precipitation method, and serial WO3/CeZrTixO2 catalysts were prepared to investigate the influence of doping TiO2 into CeZrO2 on the catalytic performance of selective catalytic reduction of NOx with NH3. The activity results showed that the introduction of appropriate amount of TiO2 could effectively improve the catalytic performance. WO3/CeZrTi20O2 with 20 wt.% TiO2 showed better deNOx activity and sulfur/water vapor tolerance than W/CeZrO2. Several techniques, including N2 physisorption, XRD, XPS, H2-TPR, NH3-TPD and in situ DRIFTS, were employed to characterize catalysts. The results indicated that doping TiO2 led to the formation of cerium-zirconium-titanium solid solution with larger surface area. The interactions among metal oxides could enhance the redox properties of the catalyst, which was helpful to the improvement of the low-temperature NH3-SCR activity. Moreover, the addition of TiO2 promoted the adsorption and activation of NH3 and increased the reactivity of adsorbed nitrate species with NH3 species, which significantly affected the NH3-SCR performance. Finally, the results of in situ DRIFTS demonstrated that the NH3-SCR reaction mainly followed the Langmuir-Hinshelwood mechanism over W/CeZrO2 and W/CeZrTi20O2 catalysts at 200 °C.

  16. 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.

  17. 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

  18. 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).

  19. Sulfur impact on NOx storage, oxygen storage and ammonia breakthrough during cyclic lean/rich operation of a commercial lean NOx trap

    SciTech Connect

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

    2007-01-01

    The objective of the present study was to develop an improved understanding of how sulfur affects the spatiotemporal distribution of reactions and temperature inside a monolithic lean NO{sub x} trap (LNT). These spatiotemporal distributions are believed to be major factors in LNT function, and thus, we expect that a better understanding of these phenomena can benefit the design and operation of commercial LNTs. In our study, we experimentally evaluated a commercial LNT monolith installed in a bench-flow reactor with simulated engine exhaust. The reactor feed gas composition was cycled to simulate fast lean/rich LNT operation at 325 C, and spatiotemporal species and temperature profiles were monitored along the LNT axis at different sulfur loadings. Reactor outlet NO{sub x}, NO, N{sub 2}O, and NH{sub 3} were also measured. Sulfur tended to accumulate in a plug-like fashion in the reactor and progressively inhibited NO{sub x} storage capacity along the axis. The NO{sub x} storage/reduction (NSR) reactions occurred over a relatively short portion of the reactor (NSR zone) under the conditions used in this study, and thus, net NO{sub x} conversion was only significantly reduced at high sulfur loading. Oxygen storage capacity (OSC) was poisoned by sulfur also in a progressive manner but to a lesser extent than the NO{sub x} storage capacity. Global selectivity for N{sub 2}O remained low at all sulfur loadings, but NH{sub 3} selectivity increased significantly with sulfur loading. We conjecture that NH{sub 3} breakthrough increased because of decreasing oxidation of NH{sub 3}, slipping from the NSR zone, by downstream stored oxygen. The NSR and oxygen storage/reduction (OSR) generated distinctive exotherms during the rich phase and at the rich/lean transition. Exotherm locations shifted downstream with sulfur accumulation in a manner that was consistent with the progressive poisoning of NSR and OSR sites.

  20. 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.

  1. Palladium on Nitrogen-Doped Mesoporous Carbon: A Bifunctional Catalyst for Formate-Based, Carbon-Neutral Hydrogen Storage.

    PubMed

    Wang, Fanan; Xu, Jinming; Shao, Xianzhao; Su, Xiong; Huang, Yanqiang; Zhang, Tao

    2016-02-08

    The lack of safe, efficient, and economical hydrogen storage technologies is a hindrance to the realization of the hydrogen economy. Reported herein is a reversible formate-based carbon-neutral hydrogen storage system that is established over a novel catalyst comprising palladium nanoparticles supported on nitrogen-doped mesoporous carbon. The support was fabricated by a hard template method and nitridated under a flow of ammonia. Detailed analyses demonstrate that this bicarbonate/formate redox equilibrium is promoted by the cooperative role of the doped nitrogen functionalities and the well-dispersed, electron-enriched palladium nanoparticles.

  2. Phenylamine-functionalized mesoporous silica supported PdAg nanoparticles: a dual heterogeneous catalyst for formic acid/CO2-mediated chemical hydrogen delivery/storage.

    PubMed

    Mori, Kohsuke; Masuda, Shinya; Tanaka, Hiromasa; Yoshizawa, Kazunari; Che, Michel; Yamashita, Hiromi

    2017-04-25

    A PdAg-based nanoparticle catalyst supported on the mesoporous silica material, SBA-15, modified with a weakly basic phenylamine functional group has been developed as a dual heterogeneous catalyst for the H2 delivery and H2 storage reactions mediated by formic acid and carbon dioxide.

  3. Toward improved catalytic low-temperature NOx removal in diesel-powered vehicles.

    PubMed

    Klingstedt, Fredrik; Arve, Kalle; Eränen, Kari; Murzin, Dmitry Yu

    2006-04-01

    The potential of different catalytic after treatment techniques to meet future diesel emission standards, which are strongly shifted toward urban driving conditions including cold start, are critically discussed in this Account and evaluated for their suitability for commercial applications. The dominating techniques in this field are NO(x) storage, urea-selective catalytic reduction (SCR), and HC-SCR. Each of these techniques have significant disadvantages such as sulfur sensitiveness and regeneration requirements of NO(x)-storage materials, infrastructure issues and formation of ammonium nitrate (at low temperatures) for urea-SCR, and low-temperature activity of HC-SCR catalysts. Ways to overcome these disadvantages in commercial applications may involve optimized regeneration strategies, reactor modifications, flow reversal, closed-loop NO(x) feedback systems, nonthermal plasma, and/or hydrogen-assisted catalyses, etc.

  4. 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

    2015-01-06

    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.

  5. Lean NOx Trap Modeling in Vehicle Systems Simulations

    SciTech Connect

    Gao, Zhiming; Chakravarthy, Veerathu K; Daw, C Stuart; Conklin, Jim

    2010-09-01

    A one-dimensional model for simulating lean NOx trap (LNT) performance is developed and validated using both steady state cycling data and transient data from FTP testing cycles. The model consists of the conservation equations for chemical species and energy in the bulk flow, energy of the solid walls, O2 storage and NOx storage (in the form of nitrites and nitrates). Nitrites and nitrates are formed by diffusion of NO and NO2, respectively, into sorbent particles (assumed to be hemi-spherical in shape) along with O2 and their formation rates are controlled by chemical kinetics as well as solid-phase diffusion rates of NOx species. The model also accounts for thermal aging and sulfation of LNTs. Empirical correlations are developed on the basis of published experimental data to capture these effects. These empirical correlations depend on total mileage for which the LNT has been in use, the mileage accumulated since the last desulfation event in addition to the freshly degreened catalyst characteristics. The model has been used in studies of vehicle systems (integration, performance etc.) including hybrid powertrain configurations. Since the engines in hybrid vehicles turn on and off multiple number of times during single drive cycles, the exhaust systems may encounter multiple cold start transients. Accurate modeling of catalyst warm-up and cooling is, therefore, very important to simulate LNT performance in such vehicles. For this purpose, the convective heat loss from the LNT to the ambient is modeled using a Nusselt number correlation that includes effects of both forced convection and natural convection (with later being important when vehicle is stationary). Using the model, the fuel penalty associated with operating LNTs on small diesel engine powered car during FTP drive cycles is estimated.

  6. Down Select Report of Chemical Hydrogen Storage Materials, Catalysts, and Spent Fuel Regeneration Processes - May 2008

    SciTech Connect

    Ott, Kevin C.; Linehan, Sue; Lipiecki, Frank; Christopher, Aardahl L.

    2008-05-12

    Chemical Hydrogen Storage Center of Excellence FY2008 Second Quarter Milestone Report: Technical report describing assessment of hydrogen storage materials and progress towards meeting DOE’s hydrogen storage targets.

  7. Highly efficient bimetal synergetic catalysis by a multi-wall carbon nanotube supported palladium and nickel catalyst for the hydrogen storage of magnesium hydride.

    PubMed

    Yuan, Jianguang; Zhu, Yunfeng; Li, Liquan

    2014-06-25

    A multi-wall carbon nanotube supported Pd and Ni catalyst efficiently catalyzes the hydrogen storage of magnesium hydride prepared by HCS + MM. Excellent hydrogen storage properties were obtained: hydrogen absorption - 6.44 wt% within 100 s at 373 K, hydrogen desorption - 6.41 wt% within 1800 s at 523 K and 6.70 wt% within 400 s at 573 K.

  8. EFFECT OF ENGINE-BASED THERMAL AGING ON SURFACE MORPHOLOGY AND PERFORMANCE OF LEAN NOX TRAPS

    SciTech Connect

    Toops, Todd J; Bunting, Bruce G; Nguyen, Ke; Gopinath, Ajit

    2007-01-01

    A small single-cylinder diesel engine is used to thermally age model (Pt + Rh/Ba/{gamma}-Al{sub 2}O{sub 3}) lean NOx traps (LNTs) under lean/rich cycling at target temperatures of 600 C, 700 C, and 800 C. During an aging cycle, fuel is injected into the exhaust to achieve reproducible exotherms under lean and rich conditions with the average temperature approximating the target temperature. Aging is performed until the cycle-average NOx conversion measured at 400 C is approximately constant. Engine-based NOx conversion decreased by 42% after 60 cycles at 600 C, 36% after 76 cycles at 700 C and 57% after 46 cycles at 800 C. The catalyst samples were removed and characterized by XRD and using a microreactor that allowed controlled measurements of surface area, precious metal size, NOx storage, and reaction rates. Three aging mechanisms responsible for the deactivation of LNTs have been identified: (i) loss of dispersion of the precious metals, (ii) phase transitions in the washcoat materials, and (iii) loss of surface area of the storage component and support. These three mechanisms are accelerated when the aging temperature exceeds 850 C--the {gamma} to {delta} transition temperature of Al{sub 2}O{sub 3}. Normalization of rates of NO reacted at 400 C to total surface area demonstrates the biggest impact on performance stems from surface area losses rather than from precious metal sintering.

  9. Local ammonia storage and ammonia inhibition in a monolithic copper-beta zeolite SCR catalyst

    SciTech Connect

    Auvray, Xavier P; Partridge Jr, William P; Choi, Jae-Soon; Pihl, Josh A; Yezerets, Alex; Kamasamudram, Krishna; Currier, Neal; Olsson, Louise

    2012-01-01

    Selective catalytic reduction of NO with NH{sub 3} was studied on a Cu-beta zeolite catalyst, with specific focus on the distributed NH{sub 3} capacity utilization and inhibition. In addition, several other relevant catalyst parameter distributions were quantified including the SCR zone, or catalyst region where SCR occurs, and NO and NH{sub 3} oxidation. We show that the full NH{sub 3} capacity (100% coverage) is used within the SCR zone for a range of temperatures. By corollary, unused NH{sub 3} capacity exists downstream of the SCR zone. Consequently, the unused capacity relative to the total capacity is indicative of the portion of the catalyst unused for SCR. Dynamic NH{sub 3} inhibition distributions, which create local transient conversion inflections, are measured. Dynamic inhibition is observed where the gas phase NH{sub 3} and NO concentrations are high, driving rapid NH{sub 3} coverage buildup and SCR. Accordingly, we observe dynamic inhibition at low temperatures and in hydrothermally aged states, but predict its existence very near the catalyst front in higher conversion conditions where we did not specifically monitor its impact. While this paper addresses some general distributed SCR performance parameters including Oxidation and SCR zone, our major new contributions are associated with the NH{sub 3} capacity saturation within the SCR zone and dynamic inhibition distributions and the associated observations. These new insights are relevant to developing accurate models, designs and control strategies for automotive SCR catalyst applications.

  10. 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.

  11. 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.

  12. 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)

  13. The impact of CO2 impurities (SO2, NOx, O2) on mineral dissolution/precipitation processes in a CO2 storage reservoir - Field-based results from the CO2CRC Otway Project site

    NASA Astrophysics Data System (ADS)

    Vu, H. P.; Black, J. R.; Haese, R. R.

    2015-12-01

    CO2 storage with impurities such as O2, NOx and SO2 is increasingly considered, because the complete removal of impurities is costly. Theoretical and laboratory-based studies have mostly focused on the formation of sulfuric and nitric acid from SO2 and NOx, respectively, while redox reactions induced by the co-injection of O2 have received little attention. Here we present results from the first field-based experiment pointing to an important role of O2. At the CO2CRC Otway Project site, CO2 and CO2 enriched with impurities (54 ppm SO2, 9 ppm NOx and 6150 ppm O2) were mixed at depth with water leading to CO2 saturated water. The CO2 saturated water was then allowed to react with the reservoir at a depth of 1400 m (Paaratte Formation, Otway Basin) over a total of 23 days. Reservoir water at in situ pressure conditions was taken for analyses using the U-tube sampling system. Back-produced water showed no evidence of silica or carbonate mineral dissolution, which can be explained by the level of alkalinity effectively buffering the additional acidity (as the result of the co-injection of SO2 and NOx). Independently, co-injected O2 caused oxidation of pyrite, resulting in rapid increase in SO42- concentration during the first three days of the subsurface incubation. Subsequently, the SO42- concentration dropped in the back-produced water, which may be explained by SO42- adsorption on the surface of minerals like iron (oxyhydr)oxides and kaolinite or by reduced pyrite oxidation at distance from the well bore. Reactive transport modeling is currently underway to better understand the observations.

  14. Formation of Multiple-Phase Catalysts for the Hydrogen Storage of Mg Nanoparticles by Adding Flowerlike NiS.

    PubMed

    Xie, Xiubo; Ma, Xiujuan; Liu, Peng; Shang, Jiaxiang; Li, Xingguo; Liu, Tong

    2017-02-22

    In order to enhance the hydrogen storage properties of Mg, flowerlike NiS particles have been successfully prepared by solvothermal reaction method, and are subsequently ball milled with Mg nanoparticles (NPs) to fabricate Mg-5 wt % NiS nanocomposite. The nanocomposite displays Mg/NiS core/shell structure. The NiS shell decomposes into Ni, MgS and Mg2Ni multiple-phases, decorating on the surface of the Mg NPs after the first hydrogen absorption and desorption cycle at 673 K. The Mg-MgS-Mg2Ni-Ni nanocomposite shows enhanced hydrogenation and dehydrogenation rates: it can quickly uptake 3.5 wt % H2 within 10 min at 423 K and release 3.1 wt % H2 within 10 min at 573 K. The apparent hydrogen absorption and desorption activation energies are decreased to 45.45 and 64.71 kJ mol(-1). The enhanced sorption kinetics of the nanocomposite is attributed to the synergistic catalytic effects of the in situ formed MgS, Ni and Mg2Ni multiple-phase catalysts during the hydrogenation/dehydrogenation process, the porthole effects for the volume expansion and microstrain of the phase transformation of Mg2Ni and Mg2NiH4 and the reduced hydrogen diffusion distance caused by nanosized Mg. This novel method of in situ producing multiple-phase catalysts gives a new horizon for designing high performance hydrogen storage material.

  15. Down Select Report of Chemical Hydrogen Storage Materials, Catalysts, and Spent Fuel Regeneration Processes

    SciTech Connect

    Ott, Kevin; Linehan, Sue; Lipiecki, Frank; Aardahl, Christopher L.

    2008-08-24

    The DOE Hydrogen Storage Program is focused on identifying and developing viable hydrogen storage systems for onboard vehicular applications. The program funds exploratory research directed at identifying new materials and concepts for storage of hydrogen having high gravimetric and volumetric capacities that have the potential to meet long term technical targets for onboard storage. Approaches currently being examined are reversible metal hydride storage materials, reversible hydrogen sorption systems, and chemical hydrogen storage systems. The latter approach concerns materials that release hydrogen in endothermic or exothermic chemical bond-breaking processes. To regenerate the spent fuels arising from hydrogen release from such materials, chemical processes must be employed. These chemical regeneration processes are envisioned to occur offboard the vehicle.

  16. Isothermal desulfation of pre-sulfated Pt-BaO/γ-Al2O3 lean NOx trap catalysts with H2: the effect of H2 concentration and the roles of CO2 and H2O

    SciTech Connect

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

    2012-01-12

    The desulfation mechanisms of pre-sulfated Pt-BaO/{gamma}-Al{sub 2}O{sub 3} lean NOx trap catalysts were investigated under isothermal conditions (600 C) using H{sub 2} as the reductant. Sulfates were found to be reduced first with H{sub 2} to produce SO{sub 2}, followed by a reaction between SO{sub 2} and H{sub 2} to produce H{sub 2}S. Gas analysis during the rich pulse reveals that the sulfur removal efficiency is initially proportional to the H{sub 2} concentration. At constant H{sub 2} concentration the overall desulfation efficiency decreases in the order of H{sub 2}/CO{sub 2}/H{sub 2}O > H{sub 2}/CO{sub 2} > H{sub 2}/H{sub 2}O > H{sub 2}, as confirmed by XPS analysis of residual sulfur in the desulfated samples. H{sub 2}O limits the evolution of SO{sub 2} at an early stage of the rich pulse and enhances the production of H{sub 2}S in later stages of reduction. CO{sub 2} is involved in both the formation of COS and the production of H{sub 2}O (via the reverse water-gas shift reaction), therefore, resulting in an increased overall efficiency.

  17. 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.

  18. Synthetic Catalysts for CO2 Storage: Catalytic Improvement of Solvent Capture Systems

    SciTech Connect

    2010-08-15

    IMPACCT Project: LLNL is designing a process to pull CO2 out of the exhaust gas of coal-fired power plants so it can be transported, stored, or utilized elsewhere. Human lungs rely on an enzyme known as carbonic anhydrase to help separate CO2 from our blood and tissue as part of the normal breathing process. LLNL is designing a synthetic catalyst with the same function as this enzyme. The catalyst can be used to quickly capture CO2 from coal exhaust, just as the natural enzyme does in our lungs. LLNL is also developing a method of encapsulating chemical solvents in permeable microspheres that will greatly increase the speed of binding of CO2. The goal of the project is an industry-ready chemical vehicle that can withstand the harsh environments found in exhaust gas and enable new, simple process designs requiring less capital investment.

  19. Understanding the nature of surface nitrates in BaO/gamma-Al2O3 NOx storage materials: A combined experimental and theoretical study

    SciTech Connect

    Kwak, Ja Hun; Mei, Donghai; Yi, Cheol-Woo W.; Kim, Do Heui; Peden, Charles HF; Allard, Larry; Szanyi, Janos

    2009-01-01

    The special role of the interface between the active catalytic phase (metal or metal oxide) and the oxide support in determining the properties of practical catalysts has long been recognized; however, it is still very poorly understood in most systems

  20. The Cu-CHA deNOx Catalyst in Action: Temperature-Dependent NH3-Assisted Selective Catalytic Reduction Monitored by Operando XAS and XES.

    PubMed

    Lomachenko, Kirill A; Borfecchia, Elisa; Negri, Chiara; Berlier, Gloria; Lamberti, Carlo; Beato, Pablo; Falsig, Hanne; Bordiga, Silvia

    2016-09-21

    The small-pore Cu-CHA zeolite is today the object of intensive research efforts to rationalize its outstanding performance in the NH3-assisted selective catalytic reduction (SCR) of harmful nitrogen oxides and to unveil the SCR mechanism. Herein we exploit operando X-ray spectroscopies to monitor the Cu-CHA catalyst in action during NH3-SCR in the 150-400 °C range, targeting Cu oxidation state, mobility, and preferential N or O ligation as a function of reaction temperature. By combining operando XANES, EXAFS, and vtc-XES, we unambiguously identify two distinct regimes for the atomic-scale behavior of Cu active-sites. Low-temperature SCR, up to ∼200 °C, is characterized by balanced populations of Cu(I)/Cu(II) sites and dominated by mobile NH3-solvated Cu-species. From 250 °C upward, in correspondence to the steep increase in catalytic activity, the largely dominant Cu-species are framework-coordinated Cu(II) sites, likely representing the active sites for high-temperature SCR.

  1. Electron beam treatment of exhaust gas with high NOx concentration

    NASA Astrophysics Data System (ADS)

    Licki, Janusz; Chmielewski, Andrzej G.; Pawelec, Andrzej; Zimek, Zbigniew; Witman, Sylwia

    2014-05-01

    Simulated exhaust gases with a high NOx concentration, ranging from 200 to 1700 ppmv, were irradiated by an electron beam from an accelerator. In the first part of this study, only exhaust gases were treated. Low NOx removal efficiencies were obtained for high NOx concentrations, even with high irradiation doses applied. In the second part of study, gaseous ammonia or/and vapor ethanol were added to the exhaust gas before its inlet to the plasma reactor. These additions significantly enhanced the NOx removal efficiency. The synergistic effect of high SO2 concentration on NOx removal was observed. The combination of electron beam treatment with the introduction of the above additions and with the performance of irradiation under optimal parameters ensured high NOx removal efficiency without the application of a solid-state catalyst.

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

    DOE PAGES

    Mráček, David; Koci, Petr; Marek, Milos; ...

    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

  3. 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

  4. Modeling Species Inhibition and Competitive Adsorption in Urea-SCR Catalysts

    SciTech Connect

    Devarakonda, Maruthi N.; Tonkyn, Russell G.; Lee, Jong H.

    2012-04-16

    Although the urea-SCR technology exhibits high NOx reduction efficiency over a wide 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. Urea-SCR catalysts exhibit poor NOx reduction performance at low temperature operating conditions (T < 150 C). We postulate that the poor performance is either due to NH3 storage inhibition by species like hydrocarbons or due to competitive adsorption between NH3 and other adsorbates such as H2O and hydrocarbons in the exhaust stream. In this paper we attempt to develop one-dimensional models to characterize inhibition and competitive adsorption in Fe-zeolite based urea-SCR catalysts based on bench reactor experiments. We further use the competitive adsorption (CA) model to develop a standard SCR model based on previously identified kinetics. Simulation results indicate that the CA model predicts catalyst outlet NO and NH3 concentrations with minimal root mean square error.

  5. A review of catalyst-enhanced magnesium hydride as a hydrogen storage material

    NASA Astrophysics Data System (ADS)

    Webb, C. J.

    2015-09-01

    Magnesium hydride remains an attractive hydrogen storage material due to the high hydrogen capacity and low cost of production. A high activation energy and poor kinetics at practical temperatures for the pure material have driven research into different additives to improve the sorption properties. This review details the development of catalytic additives and their effect on the activation energy, kinetics and thermodynamic properties of magnesium hydride.

  6. Impact of initial catalyst form on the 3D structure and performance of ball-milled Ni-catalyzed MgH2 for hydrogen storage

    DOE PAGES

    House, Stephen D.; Vajo, John J.; Ren, Chai; ...

    2017-02-24

    Although it has been shown that the hydrogen storage kinetics of metal hydrides can be significantly improved by the addition of transition metal-based catalysts, relatively little attention has been paid to the impact that the form in which these catalysts are introduced during synthesis has on the resulting structure and how this alters performance. Two mixtures of MgH2 doped with Ni were prepared via high-energy ball-milling under identical conditions, one using a pure Ni nanopowder catalyst and the other using anhydrous NiCl2. The resulting Ni catalyst particles of the NiCl2-doped material were 10-100 times smaller, as well as more uniformmore » in size and shape. Electron tomography revealed that the additive form also altered its incorporation and 3D spatial distribution, with Ni particles limited to the outer surface in the NiCl2-doped case. The significantly lower desorption performance measured in the NiCl2-doped material is attributed to regions of MgCl2 acting as barriers between the MgH2 and Ni, hindering the ability of the latter to effectively catalyze the reactions. Finally, this work demonstrates the hazards in assuming different catalyst forms produce similar final structures and highlights the potential of catalyst form as a synthesis tool for optimizing the material structure and performance.« less

  7. Effects of carbon nanotubes and metal catalysts on hydrogen storage in magnesium nanocomposites.

    PubMed

    Yao, X; Wu, C Z; Wang, H; Cheng, H M; Lu, G Q

    2006-02-01

    This paper reports a study on nanostructured magnesium composites with carbon nanotubes (CNTs) and catalytic transition metals with high H2 adsorption capacity and fast adsorption kinetics at reduced hydrogenation temperatures. Nanostructures in such a composite are shown to be responsible for improvements in both adsorption capacity and kinetics. It is found that the carbon nanotubes significantly increase the hydrogen storage capacity, and the catalytic transition metals (Fe and Ti) greatly improve the kinetics. This could be understood from the enhancement of diffusion by CNTs and decrease in energy barrier of hydrogen dissociation at the magnesium surface.

  8. Effect of H2O on the morphological changes of KNO3 formed on K2O/Al2O3 NOx storage materials: Fourier transform infra-red (FTIR) and time-resolved x-ray diffraction (TR-XRD) studies

    SciTech Connect

    Kim, Do Heui; Mudiyanselage, Kumudu K.; Szanyi, Janos; Hanson, Jonathan C.; Peden, Charles HF

    2014-02-27

    Based on combined FTIR and XRD studies, we report here that H2O induces a morphological change of KNO3 species formed on model K2O/Al2O3 NOx storage-reduction catalysts. Specifically as evidenced by FTIR, the contact of H2O with NO2 pre-adsorbed on K2O/Al2O3 promotes the transformation from bidentate (surface-like) KNO3 species to ionic (bulk-like) ones irrespective of K loadings. Once H2O is removed from the sample, a reversible transformation into bidentate KNO3 is observed, demonstrating a significant dependence of H2O on such morphological changes. TR-XRD results show the formation of two different types of bulk KNO3 phases (orthorhomobic and rhombohedral) in an as-impregnated sample. Once H2O begins to desorb above 400 K, the former is transformed into the latter, resulting in the existence of only the rhombohedral KNO3 phase. On the basis of consistent FTIR and TR-XRD results, we propose a model for the morphological changes of KNO3 species with respect to NO2 adsorption/desorption, H2O and/or heat treatments. Compared with the BaO/Al2O3 system, K2O/Al2O3 shows some similarities with respect to the formation of bulk nitrates upon H2O contact. However, there are significant differences that originate from the lower melting temperature of KNO3 relative to Ba(NO3)2.

  9. Air-stable magnesium nanocomposites provide rapid and high-capacity hydrogen storage without using heavy-metal catalysts

    NASA Astrophysics Data System (ADS)

    Jeon, Ki-Joon; Moon, Hoi Ri; Ruminski, Anne M.; Jiang, Bin; Kisielowski, Christian; Bardhan, Rizia; Urban, Jeffrey J.

    2011-04-01

    Hydrogen is a promising alternative energy carrier that can potentially facilitate the transition from fossil fuels to sources of clean energy because of its prominent advantages such as high energy density (142 MJ kg-1 ref. 1), great variety of potential sources (for example water, biomass, organic matter), light weight, and low environmental impact (water is the sole combustion product). However, there remains a challenge to produce a material capable of simultaneously optimizing two conflicting criteria—absorbing hydrogen strongly enough to form a stable thermodynamic state, but weakly enough to release it on-demand with a small temperature rise. Many materials under development, including metal-organic frameworks, nanoporous polymers, and other carbon-based materials, physisorb only a small amount of hydrogen (typically 1-2 wt%) at room temperature. Metal hydrides were traditionally thought to be unsuitable materials because of their high bond formation enthalpies (for example MgH2 has a ΔHf˜75 kJ mol-1), thus requiring unacceptably high release temperatures resulting in low energy efficiency. However, recent theoretical calculations and metal-catalysed thin-film studies have shown that microstructuring of these materials can enhance the kinetics by decreasing diffusion path lengths for hydrogen and decreasing the required thickness of the poorly permeable hydride layer that forms during absorption. Here, we report the synthesis of an air-stable composite material that consists of metallic Mg nanocrystals (NCs) in a gas-barrier polymer matrix that enables both the storage of a high density of hydrogen (up to 6 wt% of Mg, 4 wt% for the composite) and rapid kinetics (loading in <30 min at 200 °C). Moreover, nanostructuring of the Mg provides rapid storage kinetics without using expensive heavy-metal catalysts.

  10. Air-stable magnesium nanocomposites provide rapid and high-capacity hydrogen storage without using heavy-metal catalysts.

    PubMed

    Jeon, Ki-Joon; Moon, Hoi Ri; Ruminski, Anne M; Jiang, Bin; Kisielowski, Christian; Bardhan, Rizia; Urban, Jeffrey J

    2011-04-01

    Hydrogen is a promising alternative energy carrier that can potentially facilitate the transition from fossil fuels to sources of clean energy because of its prominent advantages such as high energy density (142 MJ kg(-1); ref. 1), great variety of potential sources (for example water, biomass, organic matter), light weight, and low environmental impact (water is the sole combustion product). However, there remains a challenge to produce a material capable of simultaneously optimizing two conflicting criteria--absorbing hydrogen strongly enough to form a stable thermodynamic state, but weakly enough to release it on-demand with a small temperature rise. Many materials under development, including metal-organic frameworks, nanoporous polymers, and other carbon-based materials, physisorb only a small amount of hydrogen (typically 1-2 wt%) at room temperature. Metal hydrides were traditionally thought to be unsuitable materials because of their high bond formation enthalpies (for example MgH(2) has a ΔHf~75 kJ mol(-1)), thus requiring unacceptably high release temperatures resulting in low energy efficiency. However, recent theoretical calculations and metal-catalysed thin-film studies have shown that microstructuring of these materials can enhance the kinetics by decreasing diffusion path lengths for hydrogen and decreasing the required thickness of the poorly permeable hydride layer that forms during absorption. Here, we report the synthesis of an air-stable composite material that consists of metallic Mg nanocrystals (NCs) in a gas-barrier polymer matrix that enables both the storage of a high density of hydrogen (up to 6 wt% of Mg, 4 wt% for the composite) and rapid kinetics (loading in <30 min at 200 °C). Moreover, nanostructuring of the Mg provides rapid storage kinetics without using expensive heavy-metal catalysts.

  11. Characteristics of hydrogen storage by spillover on Pt-doped carbon and catalyst-bridged metal organic framework.

    PubMed

    Stuckert, Nicholas R; Wang, Lifeng; Yang, Ralph T

    2010-07-20

    Metal dispersion is a crucially important factor for hydrogen spillover storage on metal/carbon materials. For Pt on carbon (Pt/C), dispersion into nearly 2 nm clusters or nanoparticles is necessary to facilitate spillover. On an effective Pt/C spillover sorbent, temperature-programmed desorption (TPD) results reveal the highest hydrogen signal is from the high-energy Pt edges, steps or (110) surfaces, even though the (111) faces are more abundant. Previous theoretical studies showed the high-energy sites (including the 110 face) are by far the most preferred for effective splitting of hydrogen. These are in significantly smaller fractions for larger particles, and thus the larger particles are less efficient. In addition, the rate-limiting step for spillover on effective Pt/C is identified by the susceptibility to isotopic differences, first-order behavior and isolation from catalyzed H(2)/HD/D(2) equilibrium measurements; we conclude it is the spillover step or surface diffusion. We extended our analysis to a review of our previous work, spillover on metal organic frameworks (MOFs). This has been achieved by bridging a commercial H(2) dissociation catalyst (Pt/C) to MOFs, large enhancement factors (up to 8) were observed. Unlike Pt/C sorbents, sample-to-sample consistency in storage capacity on the bridged MOF samples is difficult to achieve. Inconsistency in the enhancements by spillover is shown; however, significant enhancement factors are still observed when samples are prepared and activated properly. Common pitfalls (and their consequences) in sample preparation for both Pt/C and bridged MOFs are discussed in detail.

  12. Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures.

    PubMed

    Hull, Jonathan F; Himeda, Yuichiro; Wang, Wan-Hui; Hashiguchi, Brian; Periana, Roy; Szalda, David J; Muckerman, James T; Fujita, Etsuko

    2012-03-18

    Green plants convert CO(2) to sugar for energy storage via photosynthesis. We report a novel catalyst that uses CO(2) and hydrogen to store energy in formic acid. Using a homogeneous iridium catalyst with a proton-responsive ligand, we show the first reversible and recyclable hydrogen storage system that operates under mild conditions using CO(2), formate and formic acid. This system is energy-efficient and green because it operates near ambient conditions, uses water as a solvent, produces high-pressure CO-free hydrogen, and uses pH to control hydrogen production or consumption. The extraordinary and switchable catalytic activity is attributed to the multifunctional ligand, which acts as a proton-relay and strong π-donor, and is rationalized by theoretical and experimental studies.

  13. Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures

    NASA Astrophysics Data System (ADS)

    Hull, Jonathan F.; Himeda, Yuichiro; Wang, Wan-Hui; Hashiguchi, Brian; Periana, Roy; Szalda, David J.; Muckerman, James T.; Fujita, Etsuko

    2012-05-01

    Green plants convert CO2 to sugar for energy storage via photosynthesis. We report a novel catalyst that uses CO2 and hydrogen to store energy in formic acid. Using a homogeneous iridium catalyst with a proton-responsive ligand, we show the first reversible and recyclable hydrogen storage system that operates under mild conditions using CO2, formate and formic acid. This system is energy-efficient and green because it operates near ambient conditions, uses water as a solvent, produces high-pressure CO-free hydrogen, and uses pH to control hydrogen production or consumption. The extraordinary and switchable catalytic activity is attributed to the multifunctional ligand, which acts as a proton-relay and strong π-donor, and is rationalized by theoretical and experimental studies.

  14. Reversible Hydrogen Storage using CO2 and a Proton-Switchable Iridium Catalyst in Aqueous Media under Mild Temperatures and Pressures

    SciTech Connect

    Hull J. F.; Himeda, Y.; Wang, W.-H.; Hashiguchi, B.; Szalda, D.J.; Muckerman, J.T.; Fujita, E.

    2012-05-01

    Green plants convert CO{sub 2} to sugar for energy storage via photosynthesis. We report a novel catalyst that uses CO{sub 2} and hydrogen to store energy in formic acid. Using a homogeneous iridium catalyst with a proton-responsive ligand, we show the first reversible and recyclable hydrogen storage system that operates under mild conditions using CO{sub 2}, formate and formic acid. This system is energy-efficient and green because it operates near ambient conditions, uses water as a solvent, produces high-pressure CO-free hydrogen, and uses pH to control hydrogen production or consumption. The extraordinary and switchable catalytic activity is attributed to the multifunctional ligand, which acts as a proton-relay and strong {pi}-donor, and is rationalized by theoretical and experimental studies.

  15. Efficient hydrogen storage and production using a catalyst with an imidazoline-based, proton-responsive ligand

    DOE PAGES

    Wang, Lin; Onishi, Naoya; Murata, Kazuhisa; ...

    2016-12-28

    A series of new imidazoline-based iridium complexes has been developed for hydrogenation of CO2 and dehydrogenation of formic acid. One of the proton-responsive complexes bearing two –OH groups at ortho and para positions on a coordinating pyridine ring (3 b) can catalyze efficiently the chemical fixation of CO2 and release H2 under mild conditions in aqueous media without using organic additives/solvents. Notably, hydrogenation of CO2 can be efficiently carried out under CO2 and H2 at atmospheric pressure in basic water by 3 b, achieving a turnover frequency of 106 h–1 and a turnover number of 7280 at 25 °C, whichmore » are higher than ever reported. Furthermore, highly efficient CO-free hydrogen production from formic acid in aqueous solution employing the same catalyst under mild conditions has been achieved, thus providing a promising potential H2-storage system in water.« less

  16. Efficient hydrogen storage and production using a catalyst with an imidazoline-based, proton-responsive ligand

    SciTech Connect

    Wang, Lin; Onishi, Naoya; Murata, Kazuhisa; Hirose, Takuji; Muckerman, James T.; Fujita, Etsuko; Himeda, Yuichiro

    2016-12-28

    A series of new imidazoline-based iridium complexes has been developed for hydrogenation of CO2 and dehydrogenation of formic acid. One of the proton-responsive complexes bearing two –OH groups at ortho and para positions on a coordinating pyridine ring (3 b) can catalyze efficiently the chemical fixation of CO2 and release H2 under mild conditions in aqueous media without using organic additives/solvents. Notably, hydrogenation of CO2 can be efficiently carried out under CO2 and H2 at atmospheric pressure in basic water by 3 b, achieving a turnover frequency of 106 h–1 and a turnover number of 7280 at 25 °C, which are higher than ever reported. Furthermore, highly efficient CO-free hydrogen production from formic acid in aqueous solution employing the same catalyst under mild conditions has been achieved, thus providing a promising potential H2-storage system in water.

  17. Efficient Hydrogen Storage and Production Using a Catalyst with an Imidazoline-Based, Proton-Responsive Ligand.

    PubMed

    Wang, Lin; Onishi, Naoya; Murata, Kazuhisa; Hirose, Takuji; Muckerman, James T; Fujita, Etsuko; Himeda, Yuichiro

    2017-03-22

    A series of new imidazoline-based iridium complexes has been developed for hydrogenation of CO2 and dehydrogenation of formic acid. One of the proton-responsive complexes bearing two -OH groups at ortho and para positions on a coordinating pyridine ring (3 b) can catalyze efficiently the chemical fixation of CO2 and release H2 under mild conditions in aqueous media without using organic additives/solvents. Notably, hydrogenation of CO2 can be efficiently carried out under CO2 and H2 at atmospheric pressure in basic water by 3 b, achieving a turnover frequency of 106 h(-1) and a turnover number of 7280 at 25 °C, which are higher than ever reported. Moreover, highly efficient CO-free hydrogen production from formic acid in aqueous solution employing the same catalyst under mild conditions has been achieved, thus providing a promising potential H2 -storage system in water. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. 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.

  19. Water-Induced Morphology Changes in BaO/gamma-Al2O3 NOx Storage Materials: an FTIR, TPD, and Time-Resolved Synchrotron XRD Study

    SciTech Connect

    Szanyi,J.; Kwak, J.; Kim, D.; Wang, X.; Chimentao, R.; Hanson, J.; Epling, W.; Peden, C.

    2007-01-01

    The effect of water on the morphology of BaO/Al{sub 2}O{sub 3}-based NO{sub x} storage materials was investigated using Fourier transform infrared spectroscopy, temperature programmed desorption, and time-resolved synchrotron X-ray diffraction techniques. The results of this multispectroscopy study reveal that in the presence of water surface Ba-nitrates convert to bulk nitrates and water facilitates the formation of large Ba(NO{sub 3}){sub 2} particles. The conversion of surface to bulk Ba-nitrates is completely reversible (i.e., after the removal of water from the storage material a significant fraction of the bulk nitrates reconverts to surface nitrates). NO{sub 2} exposure of a H{sub 2}O-containing (wet) BaO/Al{sub 2}O{sub 3} sample results in the formation of nitrites and bulk nitrates exclusively (i.e., no surface nitrates form). After further exposure to NO{sub 2}, the nitrites completely convert to bulk nitrates. The amount of NO{sub x} taken up by the storage material, however, is essentially unaffected by the presence of water regardless of whether the water was dosed prior to or after NO{sub 2} exposure. On the basis of the results of this study, we are now able to explain most of the observations reported in the literature on the effect of water on NO{sub x} uptake on similar storage materials.

  20. Lean NOx catalysis for gasoline fueled European cars

    SciTech Connect

    1997-02-01

    There is increasing interest in operating gasoline fueled passenger cars lean of the stoichiometric air/fuel (A/F) ratio to improve fuel economy. These types of engines will operate at lean A/F ratios while cruising at partial load, and return to stoichiometric or even rich conditions when more power is required. The challenge for the engine and catalyst manufacturer is to develop a system which will combine the high activity rates of a state-of-the-art three-way catalyst (TWC) with the ability to reduce nitrogen oxides (NOx) in the presence of excess oxygen. The objective is to achieve the future legislative limits (EURO III/IV) in the European Union. Recent developments in automotive pollution control catalysis show that the use of NOx adsorption materials is a suitable way to reduce NOx emissions of gasoline-fueled lean-burn engines. However, the primary task for the implementation of this technology in the European market will be to improve the catalyst`s high-temperature stability and to decrease its susceptibility to sulfur poisoning. Outlined here are results of a recent R and D program to achieve NOx reduction under lean-burn gasoline engine conditions. Model gas test results as well as engine bench data are used for discussion of the parameters which control NOx adsorption efficiency under various conditions.

  1. Study of Lean NOx Technology for Diesel Emission Control

    SciTech Connect

    Mital, R.

    2000-08-20

    Diesel engines because of their reliability and efficiency are a popular mobile source. The diesel engine operates at higher compression ratios and with leaner fuel mixtures and produces lower carbon monoxide and hydrocarbon emissions. The oxygen-rich environment leads to higher nitrogen oxides in the form of NO. Catalysts selectively promoting the reduction of NOx by HCs in a lean environment have been termed lean NOx catalyst ''LNC''. The two groups that have shown most promise are, Copper exchanged zeolite Cu/ZSM5, and Platinum on alumina Pt/Al2O3.

  2. Aluminium doped ceria–zirconia supported palladium-alumina catalyst with high oxygen storage capacity and CO oxidation activity

    SciTech Connect

    Dong, Qiang; Yin, Shu Guo, Chongshen; Wu, Xiaoyong; Kimura, Takeshi; Sato, Tsugio

    2013-12-15

    Graphical abstract: Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} possessed high OSC and CO oxidation activity at low temperature. - Highlights: • A new OSC material of Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} is prepared via a mechanochemical method. • Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} showed high OSC even after calcination at 1000 °C for 20 h. • Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd/γ-Al{sub 2}O{sub 3} exhibited the highest CO oxidation activity at low temperature correlates with enhanced OSC. - Abstract: The Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd-γ-Al{sub 2}O{sub 3} catalyst prepared by a mechanochemical route and calcined at 1000 °C for 20 h in air atmosphere to evaluate the thermal stability. The prepared Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd-γ-Al{sub 2}O{sub 3} catalyst was characterized for the oxygen storage capacity (OSC) and CO oxidation activity in automotive catalysis. For the characterization, X-ray diffraction, transmission electron microscopy and the Brunauer–Emmet–Teller (BET) technique were employed. The OSC values of all samples were measured at 600 °C using thermogravimetric-differential thermal analysis. Ce{sub 0.5}Zr{sub 0.3}Al{sub 0.2}O{sub 1.9}/Pd-γ-Al{sub 2}O{sub 3} catalyst calcined at 1000 °C for 20 h with a BET surface area of 41 m{sup 2} g{sup −1} exhibited the considerably high OSC of 583 μmol-O g{sup −1} and good OSC performance stability. The same synthesis route was employed for the preparation of the CeO{sub 2}/Pd-γ-Al{sub 2}O{sub 3} and Ce{sub 0.5}Zr{sub 0.5}O{sub 2}/Pd-γ-Al{sub 2}O{sub 3} for comparison.

  3. Effect of Na3FeF6 catalyst on the hydrogen storage properties of MgH2.

    PubMed

    Sulaiman, N N; Mustafa, N S; Ismail, M

    2016-04-28

    The effects of Na3FeF6 catalyst on the hydrogen storage properties of MgH2 have been studied for the first time. The results showed that for the MgH2 sample doped with 10 wt% Na3FeF6, the onset dehydrogenation temperature decreased to 255 °C, which was 100 °C and 162 °C lower than those of the as-milled and as-received MgH2 sample, respectively. The re/dehydrogenation kinetics were also significantly enhanced compared to the un-doped MgH2. The absorption kinetics showed that the as-milled MgH2 only absorbed 3.0 wt% of hydrogen at 320 °C in 2 min of rehydrogenation, but about 3.6 wt% of hydrogen was absorbed within the same period of time after 10 wt% Na3FeF6 was added to MgH2. The desorption kinetics showed that the MgH2 + 10 wt% Na3FeF6 sample could desorb about 3.8 wt% of hydrogen in 10 min at 320 °C. In contrast, the un-doped MgH2 sample desorbed only 0.2 wt% of hydrogen in the same period of time. The activation energy for the decomposition of the as-milled MgH2 was 167.0 kJ mol(-1), and this value decreased to 75.0 kJ mol(-1) after the addition of 10 wt% Na3FeF6 (a reduction by about 92.0 kJ mol(-1)). It is believed that the in situ formation of the active species of NaMgF3, NaF and Fe during the heating process could enhance the hydrogen storage properties of MgH2, due to the catalytic effects of these new species.

  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. Towards the design of novel boron- and nitrogen-substituted ammonia-borane and bifunctional arene ruthenium catalysts for hydrogen storage.

    PubMed

    Bandaru, Sateesh; English, Niall J; Phillips, Andrew D; MacElroy, J M D

    2014-05-05

    Electronic-structure density functional theory calculations have been performed to construct the potential energy surface for H2 release from ammonia-borane, with a novel bifunctional cationic ruthenium catalyst based on the sterically bulky β-diketiminato ligand (Schreiber et al., ACS Catal. 2012, 2, 2505). The focus is on identifying both a suitable substitution pattern for ammonia-borane optimized for chemical hydrogen storage and allowing for low-energy dehydrogenation. The interaction of ammonia-borane, and related substituted ammonia-boranes, with a bifunctional η(6)-arene ruthenium catalyst and associated variants is investigated for dehydrogenation. Interestingly, in a number of cases, hydride-proton transfer from the substituted ammonia-borane to the catalyst undergoes a barrier-less process in the gas phase, with rapid formation of hydrogenated catalyst in the gas phase. Amongst the catalysts considered, N,N-difluoro ammonia-borane and N-phenyl ammonia-borane systems resulted in negative activation energy barriers. However, these types of ammonia-boranes are inherently thermodynamically unstable and undergo barrierless decay in the gas phase. Apart from N,N-difluoro ammonia-borane, the interaction between different types of catalyst and ammonia borane was modeled in the solvent phase, revealing free-energy barriers slightly higher than those in the gas phase. Amongst the various potential candidate Ru-complexes screened, few are found to differ in terms of efficiency for the dehydrogenation (rate-limiting) step. To model dehydrogenation more accurately, a selection of explicit protic solvent molecules was considered, with the goal of lowering energy barriers for H-H recombination. It was found that primary (1°), 2°, and 3° alcohols are the most suitable to enhance reaction rate.

  6. Radio-Frequency-Based NH3-Selective Catalytic Reduction Catalyst Control: Studies on Temperature Dependency and Humidity Influences

    PubMed Central

    Dietrich, Markus; Hagen, Gunter; Reitmeier, Willibald; Burger, Katharina; Hien, Markus; Grass, Philippe; Kubinski, David; Visser, Jaco; Moos, Ralf

    2017-01-01

    The upcoming more stringent automotive emission legislations and current developments have promoted new technologies for more precise and reliable catalyst control. For this purpose, radio-frequency-based (RF) catalyst state determination offers the only approach for directly measuring the NH3 loading on selective catalytic reduction (SCR) catalysts and the state of other catalysts and filter systems. Recently, the ability of this technique to directly control the urea dosing on a current NH3 storing zeolite catalyst has been demonstrated on an engine dynamometer for the first time and this paper continues that work. Therefore, a well-known serial-type and zeolite-based SCR catalyst (Cu-SSZ-13) was investigated under deliberately chosen high space velocities. At first, the full functionality of the RF system with Cu-SSZ-13 as sample was tested successfully. By direct RF-based NH3 storage control, the influence of the storage degree on the catalyst performance, i.e., on NOx conversion and NH3 slip, was investigated in a temperature range between 250 and 400 °C. For each operation point, an ideal and a critical NH3 storage degree was found and analyzed in the whole temperature range. Based on the data of all experimental runs, temperature dependent calibration functions were developed as a basis for upcoming tests under transient conditions. Additionally, the influence of exhaust humidity was observed with special focus on cold start water and its effects to the RF signals. PMID:28704929

  7. 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...

  8. 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...

  9. The role of nano-Ni catalyst in MgH2 obtained by reactive mechanical milling method for solid hydrogen storage application

    NASA Astrophysics Data System (ADS)

    Jalil, Zulkarnain; Rahwanto, Adi; Handoko, Erfan; Mustanir

    2017-03-01

    Magnesium (Mg) is regarded as one of the candidate material for absorbing hydrogen, because theoretically, has the ability to absorb hydrogen in the large quantities (7.6 wt%). However, Mg has shortage, namely its kinetic reaction is very slow, it takes time to absorb hydrogen at least 60 minutes with very high operating temperatures (300-400°C). The aim of this study is to improve the hydrogen desorption temperature of Mg-based hydrogen storage material. In this work, we used nano-nickel (Ni) as catalyst in MgH2 and obtained by reactive mechanical milling method. The duration of milling was done in 2 hours (soft milling) with the 2 mol% Ni catalyst and milled under hydrogen atmosphere (10 bar). As the results, small amount of 2 mol% Ni in nanometer scale acts as a suitable catalyst for improvement the kinetics of MgH2 which could absorp 5.5 wt% of hydrogen within 10 minutes at 300°C. It is obvious that small amount has much better as catalyst in nanoparticle size and at the same time allowed to reduce the milling process in short time.

  10. 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.

  11. 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.

  12. 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.

  13. NOX REDUCTION FOR LEAN EXHAUST USING PLASMA ASSISTED CATALYSIS

    SciTech Connect

    Bhatt, B.

    2000-08-20

    Currently CARB estimates on road diesel vehicles contribute 50% of the NOX and 78% of the particulates being discharged from mobile sources. Diesel emissions obviously must be reduced if future air quality targets are to be met. A critical technological barrier exists because there are no commercial technologies available, which can reduce NOX from diesel (lean), exhaust containing 5-15% O2 concentration. One promising approach to reducing NOX and particulates from diesel exhaust is to use a combination of plasma with catalyst. Plasma can be generated thermally or non-thermally. Thermal plasma is formed by heating the system to an exceedingly high temperature (>2000 C). High temperature requirements for plasma makes thermal plasma inefficient and requires skillful thermal management and hence is considered impractical for mobile applications. Non-thermal plasma directs electrical energy into the creation of free electrons, which in turn react with gaseous species thus creating plasma. A combination of non-thermal plasma with catalysts can be referred to Plasma Assisted Catalysts or PAC. PAC technology has been demonstrated in stationary sources where non-thermal plasma catalysis is carried out in presence of NH3 as a reductant. In stationary applications NO is oxidized to HNO3 and then into ammonium nitrate where it is condensed and removed. This approach is impractical for mobile application because of the ammonia requirement and the ultimate mechanism by which NOX is removed. However, if a suitable catalyst can be found which can use onboard fuel as reductant then the technology holds a considerable promise. NOX REDUCTION FOR LEAN EXHAUST USING PLASMA ASSISTED CATALYSIS Ralph Slone, B. Bhatt and Victor Puchkarev NOXTECH INC. In addition to the development of an effective catalyst, a non-thermal plasma reactor needs be scaled and demonstrated along with a reliable and cost effective plasma power source and onboard HC source needs to be proven. Under the work

  14. 40 CFR 96.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Opt-in Units § 96.188 CAIR NOX allowance allocations to CAIR NOX...

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

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Opt-in Units § 96.188 CAIR NOX allowance allocations to CAIR NOX...

  16. Chemiluminescence analyzer of NOx as a high-throughput screening tool in selective catalytic reduction of NO

    PubMed Central

    Oh, Kwang Seok; Woo, Seong Ihl

    2011-01-01

    A chemiluminescence-based analyzer of NOx gas species has been applied for high-throughput screening of a library of catalytic materials. The applicability of the commercial NOx analyzer as a rapid screening tool was evaluated using selective catalytic reduction of NO gas. A library of 60 binary alloys composed of Pt and Co, Zr, La, Ce, Fe or W on Al2O3 substrate was tested for the efficiency of NOx removal using a home-built 64-channel parallel and sequential tubular reactor. The NOx concentrations measured by the NOx analyzer agreed well with the results obtained using micro gas chromatography for a reference catalyst consisting of 1 wt% Pt on γ-Al2O3. Most alloys showed high efficiency at 275 °C, which is typical of Pt-based catalysts for selective catalytic reduction of NO. The screening with NOx analyzer allowed to select Pt-Ce(X) (X=1–3) and Pt–Fe(2) as the optimal catalysts for NOx removal: 73% NOx conversion was achieved with the Pt–Fe(2) alloy, which was much better than the results for the reference catalyst and the other library alloys. This study demonstrates a sequential high-throughput method of practical evaluation of catalysts for the selective reduction of NO. PMID:27877438

  17. Microkinetic Modeling of Lean NOx Trap Storage and Regeneration

    SciTech Connect

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

    2011-12-01

    A microkinetic chemical reaction mechanism capable of describing both the storage and regeneration processes in a fully formulated lean NOx trap (LNT) is presented. The mechanism includes steps occurring on the precious metal, barium oxide (NOx 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 (including boundary layer mass transfer) to simulate not only a set of long storage/regeneration cycles with a CO/H2 reductant, but also a series of steady flow temperature sweep experiments that were previously analyzed with just a precious metal mechanism and a steady state code neglecting mass transfer. The results show that, while mass transfer effects are generally minor, NOx 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 the transient simulations. 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.

  18. Argus NOx/SCR report

    SciTech Connect

    2005-05-15

    This document reports on NOx units at more than 350 coal and gas-fired power plants in the USA. Formerly known as the Argus SCR Report, the data are now expanded to include other forms of NOx control, including selective non-catalytic reduction (SNCR), low NOx burners and overfire air.

  19. 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...

  20. 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...

  1. 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

  2. Zeolites as nanoporous, gas-sensitive materials for in situ monitoring of DeNOx-SCR

    PubMed Central

    Simons, Thomas

    2012-01-01

    Summary In a proof-of-concept study we demonstrate in situ reaction monitoring of DeNOx-SCR on proton-conducting zeolites serving as catalyst and gas sensor at the same time. By means of temperature-dependent impedance spectroscopy we found that the thermally induced NH3 desorption in H-form and in Fe-loaded zeolite H-ZSM-5 follow the same process, while a remarkable difference under DeNOx-SCR reaction conditions was found. The Fe-loaded catalyst shows a significantly lower onset temperature, and time-dependent measurements suggest different SCR reaction mechanisms for the two catalysts tested. These results may help in the development of catalysts for the reduction of NOx emissions and ammonia consumption, and provide insight into the elementary catalytic process promoting a full description of the NH3-SCR reaction system. PMID:23213630

  3. NOx reduction aftertreatment system using nitrogen nonthermal plasma desorption

    SciTech Connect

    Okubo, M.; Inoue, M.; Kuroki, T.; Yamamoto, T.

    2005-08-01

    In the flue emission from an internal combustion system using diffusing combustion such as coal or oil fuel boiler, incinerator, or diesel engine, around 10% oxygen is usually included. It is difficult to reduce the NOx in the emission completely using catalysts or plasma alone because part of the NO is oxidized under an O{sub 2}-rich environment. In order to overcome these difficulties, we propose a new aftertreatment system of NOx included in the exhaust gas of the combustion system using nonthermal plasma (NTP) desorption and reduction. In this system, exchangeable adsorbent columns are equipped. As an initial step to realize such kind of aftertreatment system, the basic characteristics of the N{sub 2} NTP desorption and NOx reduction were examined experimentally using a pulse corona NTP reactor. After several adsorption/desorption processes, the amount of NOx adsorbed becomes equal to that of the NOx desorbed, that is, all the NO, was desorbed in a single desorption process. It is confirmed that the NOx complete reduction using N{sub 2} NTP desorption is possible not only for a simulated exhaust gas but for a real diesel engine gas. The effective specific energy density can be decreased down to 22 Wh/m{sup 3}.

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

    PubMed

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

    2016-05-05

    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. Copyright © 2016. Published by Elsevier B.V.

  5. 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.

  6. 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.

  7. Passive SCR for lean gasoline NOX control: Engine-based strategies to minimize fuel penalty associated with catalytic NH3 generation

    DOE PAGES

    Prikhodko, Vitaly Y.; Parks, James E.; Pihl, Josh A.; ...

    2016-02-18

    Lean gasoline engines offer greater fuel economy than common stoichiometric gasoline engines. However, excess oxygen prevents the use of the current three-way catalyst (TWC) to control nitrogen oxide (NOX) emissions in lean exhaust. A passive SCR concept, introduced by General Motors Global R&D, makes use of a TWC that is already onboard to generate NH3 under slightly rich conditions, which is stored on the downstream SCR. The stored NH3 is then used to reduce NOX emissions when the engine switches to lean operation. In this work, the effect of engine parameters, such as air-fuel equivalence ratio and spark timing, onmore » NH3 generation over a commercial Pd-only TWC with no dedicated oxygen storage component was evaluated on a 2.0-liter BMW lean burn gasoline direct injection engine. NOX reduction, NH3 formation, and reductant utilization processes were evaluated, and fuel efficiency was assessed and compared to the stoichiometric engine operation case. We found air-fuel equivalence ratio to be one of the most important parameters in controlling the NH3 production; however, the rich operation necessary for NH3 production results in a fuel consumption penalty. The fuel penalty can be minimized by adjusting spark timing to increase rich-phase engine out NOX emissions and, thereby, NH3 levels. Additionally, higher engine out NOX during engine load increase to simulate acceleration resulted in additional fuel savings. Ultimately, a 10% fuel consumption benefit was achieved with the passive SCR approach by optimizing rich air-fuel equivalence ratio and spark timing while also utilizing acceleration load conditions.« less

  8. Catalytic NOx reduction with simultaneous dioxin and furan oxidation.

    PubMed

    Goemans, Marcel; Clarysse, Patrick; Joannès, Joseph; De Clercq, Petra; Lenaerts, Silvia; Matthys, Karel; Boels, Kris

    2004-03-01

    The engineering, construction, performance and running costs of a catalytic flue gas cleaning component in the low dust area of a municipal waste incinerator is discussed. For this purpose, the case study of a Flemish incineration plant is presented, covering the history, the design procedure of the catalyst, relevant process data and the financial aspects. A reliable PCDD/F-destruction by means of oxidation by the catalyst to typical values of 0.001 ng TEQ/Nm3 has been demonstrated. At the same time, NOx- and CO-emissions are reduced by 90% and 20% to about 50 mg/Nm3 and below 10 mg/Nm3, respectively.

  9. 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).

  10. 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 ...

  11. Proceedings: 2000 NOx Controls Workshop

    SciTech Connect

    2001-04-01

    The 2000 EPRI workshop on nitrogen oxide (NOx) controls for utility boilers provided a medium for member utilities to augment their knowledge of recent operating experience and developments on NOx control technologies. The event focused on improving methods of compliance with emission regulations mandated by the Clean Air Act Amendments (CAAA) of 1990 without jeopardizing efficiency and plant performance.

  12. 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 ...

  13. 40 CFR 96.60 - Submission of NOX allowance transfers.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 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...

  14. 40 CFR 96.60 - Submission of NOX allowance transfers.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 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...

  15. DOE Hydrogen Sorption Center of Excellence: Synthesis and Processing of Single-Walled Carbon Nanohorns for Hydrogen Storage and Catalyst Supports

    SciTech Connect

    David B. Geohegan; Hui Hu; Mina Yoon; Alex A. Puretzky; Christopher M. Rouleau; Norbert Thonnard; Gerd Duscher; Karren More

    2011-05-24

    The objective of the project was to exploit the unique morphology, tunable porosity and excellent metal supportability of single-walled carbon nanohorns (SWNHs) to optimize hydrogen uptake and binding energy through an understanding of metal-carbon interactions and nanoscale confinement. SWNHs provided a unique material to understand these effects because they are carbon nanomaterials which are synthesized from the 'bottom-up' with well-defined, sub-nm pores and consist of single-layer graphene, rolled up into closed, conical, horn-shaped units which form ball-shaped aggregates of {approx}100-nm diameter. SWNHs were synthesized without metal catalysts by the high-temperature vaporization of solid carbon, so they can be used to explore metal-free hydrogen storage. However, SWNHs can also be decorated with metal nanoparticles or coatings in post-processing treatments to understand how metals augment hydrogen storage. The project first explored how the synthesis and processing of SWNHs could be modified to tailor pore sizes to optimal size ranges. Nanohorns were rapidly synthesized at 20g/hr rates by high-power laser vaporization enabling studies such as neutron scattering with gram quantities. Diagnostics of the synthesis process including high-speed videography, fast pyrometry of the graphite target, and differential mobility analysis monitoring of particle size distributions were applied in this project to provide in situ process control of SWNH morphology, and to understand the conditions for different pore sizes. We conclude that the high-temperature carbon-vaporization process to synthesize SWNHs is scalable, and can be performed by electric arc or other similar techniques as economically as carbon can be vaporized. However, the laser vaporization approach was utilized in this project to permit the precise tuning of the synthesis process through adjustment of the laser pulse width and repetition rate. A result of this processing control in the project was to

  16. 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

  17. NOX5 in Human Spermatozoa

    PubMed Central

    Musset, Boris; Clark, Robert A.; DeCoursey, Thomas E.; Petheo, Gabor L.; Geiszt, Miklos; Chen, Yumin; Cornell, John E.; Eddy, Carlton A.; Brzyski, Robert G.; El Jamali, Amina

    2012-01-01

    Physiological and pathological processes in spermatozoa involve the production of reactive oxygen species (ROS), but the identity of the ROS-producing enzyme system(s) remains a matter of speculation. We provide the first evidence that NOX5 NADPH oxidase is expressed and functions in human spermatozoa. Immunofluorescence microscopy detected NOX5 protein in both the flagella/neck region and the acrosome. Functionally, spermatozoa exposed to calcium ionophore, phorbol ester, or H2O2 exhibited superoxide anion production, which was blocked by addition of superoxide dismutase, a Ca2+ chelator, or inhibitors of either flavoprotein oxidases (diphenylene iododonium) or NOX enzymes (GKT136901). Consistent with our previous overexpression studies, we found that H2O2-induced superoxide production by primary sperm cells was mediated by the non-receptor tyrosine kinase c-Abl. Moreover, the HV1 proton channel, which was recently implicated in spermatozoa motility, was required for optimal superoxide production by spermatozoa. Immunoprecipitation experiments suggested an interaction among NOX5, c-Abl, and HV1. H2O2 treatment increased the proportion of motile sperm in a NOX5-dependent manner. Statistical analyses showed a pH-dependent correlation between superoxide production and enhanced sperm motility. Collectively, our findings show that NOX5 is a major source of ROS in human spermatozoa and indicate a role for NOX5-dependent ROS generation in human spermatozoa motility. PMID:22291013

  18. Bimetallic NiCo functional graphene: an efficient catalyst for hydrogen-storage properties of MgH₂.

    PubMed

    Wang, Ying; Liu, Guang; An, Cuihua; Li, Li; Qiu, Fangyuan; Wang, Yijing; Jiao, Lifang; Yuan, Huatang

    2014-09-01

    Bimetallic NiCo functional graphene (NiCo/rGO) was synthesized by a facile one-pot method. During the coreduction process, the as-synthesized ultrafine NiCo nanoparticles (NPs), with a typical size of 4-6 nm, were uniformly anchored onto the surface of reduced graphene oxide (rGO). The NiCo bimetal-supported graphene was found to be more efficient than their single metals. Synergetic catalysis of NiCo NPs and rGO was confirmed, which can significantly improve the hydrogen-storage properties of MgH2. The apparent activation energy (E(a)) of the MgH2-NiCo/rGO sample decreases to 105 kJ mol(-1), which is 40.7% lower than that of pure MgH2. More importantly, the as-prepared MgH2-NiCo/rGO sample can absorb 5.5 and 6.1 wt% hydrogen within 100 and 350 s, respectively, at 300 °C under 0.9 MPa H2 pressure. Further cyclic kinetics investigation indicates that MgH2-NiCo/rGO nanocomposites have excellent cycle stability. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  19. Supported Pd nanoclusters with enhanced hydrogen spillover for NOx removal via H2-SCR: the elimination of "volcano-type" behaviour.

    PubMed

    Peng, Zhezhe; Li, Zongyuan; Liu, Yun-Quan; Yan, Shuai; Tong, Jianing; Wang, Duo; Ye, Yueyuan; Li, Shuirong

    2017-05-30

    A rational design of a Pd catalyst with highly dispersed Pd nanoclusters on an Al doped ceria-based oxide for low temperature selective catalytic reduction of NOx by hydrogen with excess O2 was achieved. The supported Pd nanocluster shows a high hydrogen spillover ability and a NOx conversion of >84% within 100-300 °C.

  20. 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

  1. 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... RACT and NOX conformity exemption. Approval. EPA is approving the section 182(f) oxides of nitrogen (NOX) reasonably available control technology (RACT) and NOX conformity exemption request submitted...

  2. 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... RACT and NOX conformity exemption. Approval. EPA is approving the section 182(f) oxides of nitrogen (NOX) reasonably available control technology (RACT) and NOX conformity exemption request submitted...

  3. Hydrocarbon Effect on a Fe-zeolite Urea-SCR Catalyst: An Experimental and Modeling Study

    SciTech Connect

    Devarakonda, Maruthi N.; Tonkyn, Russell G.; Herling, Darrell R.

    2010-04-14

    Synergies between various catalytic converters such as SCR and DPF are vital to the success of an integrated aftertreatment system for simultaneous NOx and particulate matter control in diesel engines. Several issues such as hydrocarbon poisoning, thermal aging and other coupled aftertreatment dynamics need to be addressed to develop an effective emission control system. This paper reports an experimental and modeling study to understand the effect of hydrocarbons on a Fe-zeolite urea-SCR bench reactor. Several bench-reactor tests to understand the inhibition of NOx oxidation, to characterize hydrocarbon storage and to investigate the impact of hydrocarbons on SCR reactions were conducted. Toluene was chosen as a representative hydrocarbon in diesel exhaust and various tests using toluene reveal its inhibition of NO oxidation at low temperatures and its oxidation to CO and CO2 at high temperatures. Surface isotherm tests were conducted to characterize the adsorption-desorption equilibrium of toluene through Langmuir isotherms. Using the rate parameters, a toluene storage model was developed and validated in simulation. With toluene in the stream, controlled SCR tests were run on the reactor and performance metrics such as NOx conversion and NH3 slip were compared to a set of previously run tests with no toluene in the stream. Tests indicate a significant effect of toluene on NOx and NH3 conversion efficiencies even at temperatures greater than 300oC. A kinetic model to address the toluene inhibition during NO oxidation reaction was developed and is reported in the paper. This work is significant especially in an integrated DPF-SCR aftertreatment scenario where the SCR catalyst on the filter substrate is exposed to un-burnt diesel hydrocarbons during active regeneration of the particulate filter.

  4. 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.

  5. 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.

  6. 40 CFR 96.52 - NOX Allowance Tracking System responsibilities of NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.52...

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

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Tracking System § 96.52...

  8. 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.

  9. Study on Reaction Products in Plasma-Assisted Selective Catalytic Reduction of NOx

    NASA Astrophysics Data System (ADS)

    Yoshizawa, Hayato; Tochikubo, Fumiyoshi; Uchida, Satoshi; Watanabe, Tsuneo

    Since the gas discharge plasma easily converts NO to NO2, which can be reduced more actively in selective catalytic reduction with hydrocarbons (HC-SCR), the plasma-assisted HC-SCR is an effective method for NOx reduction from diesel engine exhaust gases. In this work, the relation between NOx removal and reaction products is investigated in plasma-assisted HC-SCR in simulated flue gas as parameters of gas composition, plasma specific energy and catalyst temperature. C2H4 is used as a hydrocarbon and commercially available Al2O3 is used as a catalyst. After the plasma treatment of simulated flue gas, HCHO and HCOOH were generated as by-products, while NO was effectively converted to NO2. These by-products were confirmed to be reactive at lower catalyst temperature than C2H4 in HC-SCR. The relation between NOx removal and reaction products suggests that HCHO and HCOOH contribute the effective NOx reduction at low catalyst temperature in plasma-assisted HC-SCR.

  10. 40 CFR 96.12 - Changing the NOX authorized account representative and the alternate NOX authorized account...

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Authorized Account Representative for NOX Budget Sources § 96.12 Changing the NOX authorized... on the new NOX authorized account representative and the owners and operators of the NOX...

  11. 40 CFR 96.12 - Changing the NOX authorized account representative and the alternate NOX authorized account...

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Authorized Account Representative for NOX Budget Sources § 96.12 Changing the NOX authorized... on the new NOX authorized account representative and the owners and operators of the NOX...

  12. 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

  13. Process of activation of a palladium catalyst system

    SciTech Connect

    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.

  14. 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

  15. Nox NADPH oxidases and the endoplasmic reticulum.

    PubMed

    Laurindo, Francisco R M; Araujo, Thaís L S; Abrahão, Thalita B

    2014-06-10

    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. 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. 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. 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 Noxes and the ER may provide relevant insights in Nox-related (patho)physiology.

  16. Involvement of Nox2 and Nox4 NADPH oxidases in early brain injury after subarachnoid hemorrhage.

    PubMed

    Zhang, Li; Li, Zhen; Feng, Dongxia; Shen, Haitao; Tian, Xiaodi; Li, Haiying; Wang, Zhong; Chen, Gang

    2017-04-09

    Oxidative stress is responsible for a poor prognosis of subarachnoid hemorrhage (SAH) patients. Nox2 has been shown to participate in SAH-induced early brain injury (EBI). Nox4 is another major subtype of Nox family widely expressed in central nervous system (CNS). Here, we investigated the role of Nox4 and whether there was a synergistic effect of Nox2 and Nox4 in SAH-induced EBI. Clinical brain biopsies of four patients with traumatic brain injury (TBI) and perihematomal brain tissue from six subjects with SAH were examined. Gp91ds-tat (a specific inhibitor of Nox2), GKT137831 (a specific inhibitor of Nox4), and apocynin (a non-specific Nox inhibitor) were used to test the role of Nox2 and Nox4. The protein levels of Nox2 and Nox4 were elevated in rat neurons and astrocytes at 12 h after SAH, and in cultured brain microvascular endothelial cells at 24 h after exposure to OxyHb. Similarly, there were higher Nox2 and Nox4 protein levels in perihematomal neurons and astrocytes in SAH patients than that in brain tissue from subjects with TBI. In SAH rat model, gp91ds-tat and GKT137831 could reduce SAH-induced neuronal death and degeneration, whereas apocynin did not induce a more intense neuroprotection. Consistently, in in vitro SAH model, siRNA-mediated silencing of Nox2 and Nox4 suppressed the OxyHb-induced neuronal apoptosis, whereas Nox2 and Nox4 co-knockdown also did not show a remarkable overlay effect. In conclusion, Nox4 should contribute to the pathological processes in SAH-induced EBI, and there was not an overlay effect of Nox2 inhibition and Nox4 inhibition on preventing SAH-induced EBI.

  17. Catalysts as Sensors—A Promising Novel Approach in Automotive Exhaust Gas Aftertreatment

    PubMed Central

    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 NOx 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 NOx-loading of lean NOx traps, and the soot loading of Diesel particulate filters. PMID:22163575

  18. 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

  19. 40 CFR 96.11 - Alternate NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 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...

  20. 40 CFR 96.11 - Alternate NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 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...

  1. NOx adsorber and method of regenerating same

    DOEpatents

    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.

  2. 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

  3. Microkinetic modeling of lean NOx trap chemistry

    SciTech Connect

    Larson, Rich; Chakravathy, Kalyana; Pihl, Josh A; Daw, C Stuart

    2012-01-01

    A microkinetic chemical reaction mechanism capable of describing both the storage and regeneration processes in a fully formulated lean NO{sub x} trap is presented. The mechanism includes steps occurring on the precious metal, NO{sub x} storage, and oxygen storage sites of the catalyst. The complete reaction set is used with a transient plug flow reactor code (including boundary layer mass transfer) to simulate not only 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 simpler steady state code. The results imply that NO{sub x} storage was 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 gas phase species. It is found that nearly all of the basic experimental observations can be reproduced with the transient simulations.

  4. Plasma Catalysis for NOx Reduction from Light-Duty Diesel Vehicles

    SciTech Connect

    Barlow, Stephan E.; Kwak, Ja Hun; Peden, Charles HF; Szanyi, Janos; Tonkyn, Russell G.; Singh, Gurpreet; Stork, Kevin; Hoard, John W.; Cho, Byong; Brooks, David J.; Nunn, Steven

    2004-10-01

    This annual report reviews FY 2003 progress of a program aimed at the development of a novel plasma/catalyst technology for the remediation of NOx under lean (excess oxygen) conditions, specifically for compression ignition direct injection (CIDI) diesel engines that have significant fuel economy benefits over conventional stoichiometric gasoline engines. Our previous work has shown that a non-thermal plasma in combination with an appropriate catalyst can provide NOx emission reduction efficiency of 60-80% using a simulated diesel exhaust. Based on these levels of NOx reduction obtained in the lab, a simple model was developed in this program that allows for the estimation of the fuel economy penalty that would be incurred by operating a plasma/catalyst system. Results obtained from this model suggest that a 5% fuel economy penalty is achievable with the then current (FY2000) state-of-the-art catalyst materials and plasma reactor designs. In this last year, we have continued to focus on (1) improving the catalyst and plasma reactor efficiencies for NOx reduction, (2) studies to reveal important details of the reaction mechanism(s) that can then guide our catalyst and reactor development efforts (focus 1), and (3) evaluating the performance of prototype systems on real engine exhaust. While studies of the effects of the plasma on PM in real diesel engine exhaust is meant to be part of the program, this year we did not conduct any experiments along these lines due to the major effort required to carry out the engine testing (focus 3).

  5. 40 CFR 96.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false CAIR NOX allowance allocations to CAIR NOX opt-in units. 96.188 Section 96.188 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY... period in 2009 through 2014 for which the CAIR NOX opt-in unit is to be allocated CAIR NOX allowances, (i...

  6. 40 CFR 97.188 - CAIR NOX allowance allocations to CAIR NOX opt-in units.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false CAIR NOX allowance allocations to CAIR NOX opt-in units. 97.188 Section 97.188 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY... control period in 2009 through 2014 for which the CAIR NOX opt-in unit is to be allocated CAIR NOX...

  7. 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

  8. 40 CFR 96.53 - Recordation of NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 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) The Administrator will record the NOX allowances for 2003 in the NOX Budget units' compliance accounts and...

  9. 40 CFR 96.42 - NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS... calculating NOX allowance allocations for each NOX Budget unit under § 96.4 will be: (i) For a NOX allowance... the NOX Budget unit was otherwise subject to the requirements of part 75 of this chapter for the...

  10. 40 CFR 96.53 - Recordation of NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 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) The Administrator will record the NOX allowances for 2003 in the NOX Budget units' compliance accounts and...

  11. 40 CFR 96.42 - NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS... calculating NOX allowance allocations for each NOX Budget unit under § 96.4 will be: (i) For a NOX allowance... the NOX Budget unit was otherwise subject to the requirements of part 75 of this chapter for the...

  12. Low-temperature SCR of NOx by NH3 over MnOx/SAPO-34 prepared by two different methods: a comparative study.

    PubMed

    Yu, Chenglong; Dong, Lifu; Chen, Feng; Liu, Xiaoqing; Huang, Bichun

    2017-04-01

    The low-temperature selective catalytic reduction (SCR) of NOx is a promising technology for removing NOx from flue gases. However, the vulnerability of Mn-based catalysts to SO2 and H2O poisoning makes them unsuitable for industrial application. Herein, catalysts based on the MnOx/SAPO-34 catalysts were prepared by conventional impregnation and an improved molecularly designed dispersion method for use in the low-temperature SCR. The improved molecularly designed catalyst containing 20 wt% of MnOx exhibited high low-temperature NH3-SCR activity. Nearly 90% of the NOx was converted exclusively to N2 at 160°C using this catalyst. The structure and morphological analyses of the catalyst showed that the amorphous MnOx was well dispersed on the surface of the support. The reasons for the high performance of the catalysts were ascertained using surface N2 adsorption, XPS, H2-TPR and NH3-TPD. The results of these analyses indicated that high specific surface area and the redox capability, of the abundant Mn(4+) and Mn(3+) species, coupled with the surface chemisorbed oxygen and strong acid sites had a significant effect on the SCR reaction. In addition, the effects of SO2 and H2O on activity of the catalysts were also investigated and it was found that the highly dispersed 20 wt% MnOx/SAPO-34 catalyst exhibited better SO2 poisoning resistance than the other impregnated catalysts.

  13. 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.

  14. USE OF A DIESEL FUEL PROCESSOR FOR RAPID AND EFFICIENT REGENERATION OF SINGLE LEG NOX ADSORBER SYSTEMS

    SciTech Connect

    Betta, R; Cizeron, J; Sheridan, D; Davis, T

    2003-08-24

    Lean NOx adsorber systems are one of the primary candidate technologies for the control of NOx from diesel engines to meet the 2007-2010 US emissions regulations, which require a 90% reduction of NOx from the 2004 regulations. Several of the technical challenges facing this technology are regeneration at low exhaust temperatures and the efficient use of diesel fuel to minimize fuel penalty. A diesel processor system has been developed and tested in a single leg NOx adsorber configuration on a diesel engine test stand. During NOx adsorber regeneration, this fuel processor system performs reduces the exhaust O2 level to zero and efficiently processes the diesel fuel to H2 and CO. Combined with a Nox adsorber catalyst, this system has demonstrated NOx reduction above 90%, regeneration of the NOx adsorber H2/CO pulses as short as 1 second and fuel penalties in the 3 to 4% range at 50% load. This fuel processor system can also be used to provide the desulfation cycle required with sulfur containing fuels as well as providing thermal management for PM filter regeneration.

  15. 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.

  16. 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.

  17. 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.

  18. Nitrate storage behavior of Ba/MnOx-CeO2 catalyst and its activity for soot oxidation with heat transfer limitations.

    PubMed

    Wu, Xiaodong; Liu, Shuang; Lin, Fan; Weng, Duan

    2010-09-15

    A BaMnCe ternary catalyst was prepared by impregnating barium acetate on MnO(x)-CeO(2) mixed oxides, with the monoxide supported catalysts and the solid solution support as references. The activities of the catalysts for soot oxidation were evaluated in the presence of NO under an energy transference controlled regime. BaMnCe presented the lowest maximal soot oxidation rate temperature at 393 degrees C among the catalysts investigated. Although BaMnCe experienced a loss in the specific surface area and low-temperature redox property due to blocking of the support pores by barium carbonate, its superior soot oxidation activity highlighted the importance of relatively stable bidentate/monodentate nitrates coordinated to Mn(x+) and Ce(x+) sites and more stable ionic barium nitrate. About half of the nitrates stored on this catalyst decomposed within the temperature interval of 350-450 degrees C, and the ignition temperature of soot decreased significantly with involvement of the nitrates or NO(2) released.

  19. 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.

  20. Surfactant free RGO/Pd nanocomposites as highly active heterogeneous catalysts for the hydrolytic dehydrogenation of ammonia borane for chemical hydrogen storage.

    PubMed

    Xi, Pinxian; Chen, Fengjuan; Xie, Guoqiang; Ma, Cai; Liu, Hongyan; Shao, Changwei; Wang, Jun; Xu, Zhihong; Xu, Ximing; Zeng, Zhengzhi

    2012-09-21

    In this study, monodisperse palladium (Pd) nanoparticles on reduced graphene oxide (RGO) surfaces were successfully prepared by a "wet" and "clean" method in aqueous solution. Without any surface treatment, Pd nanoparticles are firmly attached to the RGO sheets. These RGO/Pd nanocomposites exhibited catalytic activity in hydrogen generation from the hydrolysis of ammonia borane (AB). Their hydrolysis completion time and activation energy were 12.5 min and 51 ± 1 kJ mol(-1), respectively, which were comparable to the best Pd-based catalyst reported. The TOF values (mol of H(2)× (mol of catalyst × min)(-1)) of RGO/Pd is 6.25, which appears to be one of the best catalysts reported so far. We also obtained a (11)B NMR spectrum to investigate the mechanism of this catalytic hydrolysis process. This simple and straightforward method is of significance for the facile preparation of metal nanocatalysts with high catalytic activity on proper supporting materials.

  1. 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

  2. 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.

  3. Surfactant free RGO/Pd nanocomposites as highly active heterogeneous catalysts for the hydrolytic dehydrogenation of ammonia borane for chemical hydrogen storage

    NASA Astrophysics Data System (ADS)

    Xi, Pinxian; Chen, Fengjuan; Xie, Guoqiang; Ma, Cai; Liu, Hongyan; Shao, Changwei; Wang, Jun; Xu, Zhihong; Xu, Ximing; Zeng, Zhengzhi

    2012-08-01

    In this study, monodisperse palladium (Pd) nanoparticles on reduced graphene oxide (RGO) surfaces were successfully prepared by a ``wet'' and ``clean'' method in aqueous solution. Without any surface treatment, Pd nanoparticles are firmly attached to the RGO sheets. These RGO/Pd nanocomposites exhibited catalytic activity in hydrogen generation from the hydrolysis of ammonia borane (AB). Their hydrolysis completion time and activation energy were 12.5 min and 51 +/- 1 kJ mol-1, respectively, which were comparable to the best Pd-based catalyst reported. The TOF values (mol of H2 × (mol of catalyst × min)-1) of RGO/Pd is 6.25, which appears to be one of the best catalysts reported so far. We also obtained a 11B NMR spectrum to investigate the mechanism of this catalytic hydrolysis process. This simple and straightforward method is of significance for the facile preparation of metal nanocatalysts with high catalytic activity on proper supporting materials.In this study, monodisperse palladium (Pd) nanoparticles on reduced graphene oxide (RGO) surfaces were successfully prepared by a ``wet'' and ``clean'' method in aqueous solution. Without any surface treatment, Pd nanoparticles are firmly attached to the RGO sheets. These RGO/Pd nanocomposites exhibited catalytic activity in hydrogen generation from the hydrolysis of ammonia borane (AB). Their hydrolysis completion time and activation energy were 12.5 min and 51 +/- 1 kJ mol-1, respectively, which were comparable to the best Pd-based catalyst reported. The TOF values (mol of H2 × (mol of catalyst × min)-1) of RGO/Pd is 6.25, which appears to be one of the best catalysts reported so far. We also obtained a 11B NMR spectrum to investigate the mechanism of this catalytic hydrolysis process. This simple and straightforward method is of significance for the facile preparation of metal nanocatalysts with high catalytic activity on proper supporting materials. Electronic supplementary information (ESI) available. See

  4. 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 Section 97.23 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (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...

  5. 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 Section 97.23 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.23 NOX Budget permit contents. (a) Each NOX Budget...

  6. 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 permit...

  7. 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 provided...

  8. 40 CFR 96.82 - NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Individual Unit Opt-ins § 96.82 NOX authorized account representative. A unit for which an application for a NOX Budget opt-in permit is submitted and not denied or withdrawn, or a NOX Budget...

  9. 40 CFR 96.50 - NOX Allowance Tracking System accounts.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 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 and... establish one compliance account for each NOX Budget unit and one overdraft account for each source with...

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

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 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 and... establish one compliance account for each NOX Budget unit and one overdraft account for each source with...

  11. 40 CFR 96.25 - NOX Budget permit revisions.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... (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 permit... 40 Protection of Environment 21 2011-07-01 2011-07-01 false NOX Budget permit revisions....

  12. 40 CFR 96.82 - NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Individual Unit Opt-ins § 96.82 NOX authorized account representative. A unit for which an application for a NOX Budget opt-in permit is submitted and not denied or withdrawn, or a NOX Budget...

  13. Ammonia-Free NOx Control System

    SciTech Connect

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

    2005-03-31

    Research is being conducted under United States Department of Energy (DOE) Contract DE-FC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia.

  14. NOx control buys to peak in `98

    SciTech Connect

    McIlvaine, R.W.

    1995-10-01

    Titles I and IV of the Clean Air Act provide the legislative framework for a huge NOx reduction program now in operation. This reduction will have a substantial effect in reducing ground-level ozone. A new McIlvaine report concludes that US utilities and industrial companies during the next 10 years will spend more than $800 million annually to meet CAA`s NOx-control regulations. Much of that investment will be for low-NOx burners, which minimize NOx formation. Many utilities and industrial boilers can be retrofitted with a new generation of burners; however, this technology achieves less than 50% NOx reduction. Post-combustion technologies, such as selective catalytic reduction and selective noncatalytic reduction, can reduce NOx as much as 90%. Therefore, plants needing greater NOx reduction will use post-combustion technologies, often in combination with low-NOx burners. The peak order year for NOx-control equipment will be 1998, primarily because Title IV of CAA requires utilities to comply by 2000. Many industrial sources also will be ordering equipment in 1998.

  15. Ammonia-Free NOx Control System

    SciTech Connect

    Song Wu; Zhen Fan; Andrew H. Seltzer

    2005-06-30

    Research is being conducted under United States Department of Energy (DOE) Contract DEFC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia.

  16. Energy Storage

    SciTech Connect

    Mukundan, Rangachary

    2014-09-30

    Energy storage technology is critical if the U.S. is to achieve more than 25% penetration of renewable electrical energy, given the intermittency of wind and solar. Energy density is a critical parameter in the economic viability of any energy storage system with liquid fuels being 10 to 100 times better than batteries. However, the economical conversion of electricity to fuel still presents significant technical challenges. This project addressed these challenges by focusing on a specific approach: efficient processes to convert electricity, water and nitrogen to ammonia. Ammonia has many attributes that make it the ideal energy storage compound. The feed stocks are plentiful, ammonia is easily liquefied and routinely stored in large volumes in cheap containers, and it has exceptional energy density for grid scale electrical energy storage. Ammonia can be oxidized efficiently in fuel cells or advanced Carnot cycle engines yielding water and nitrogen as end products. Because of the high energy density and low reactivity of ammonia, the capital cost for grid storage will be lower than any other storage application. This project developed the theoretical foundations of N2 catalysis on specific catalysts and provided for the first time experimental evidence for activation of Mo 2N based catalysts. Theory also revealed that the N atom adsorbed in the bridging position between two metal atoms is the critical step for catalysis. Simple electrochemical ammonia production reactors were designed and built in this project using two novel electrolyte systems. The first one demonstrated the use of ionic liquid electrolytes at room temperature and the second the use of pyrophosphate based electrolytes at intermediate temperatures (200 – 300 ºC). The mechanism of high proton conduction in the pyrophosphate materials was found to be associated with a polyphosphate second phase contrary to literature claims and ammonia production rates as high as 5X 10

  17. 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

  18. Recent developments of electrochemical promotion of catalysis in the techniques of DeNOx.

    PubMed

    Tang, Xiaolong; Xu, Xianmang; 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.

  19. Wildfire and soil emissions of NOx and their consequences for ozone observed at a remote mountaintop site in Central California

    NASA Astrophysics Data System (ADS)

    Asher, E. C. C.; Caputi, D.; Conley, S. A.; Faloona, I. C.

    2016-12-01

    Nitric oxide (NOx) emissions contribute to the production of tropospheric ozone and the nutrient supply fueling primary production. Current global estimates indicate that biomass burning, including wildfires, and soil emissions represent 15 - 25 % of the total emissions. Yet estimates suggest that in North America during the summer, natural sources, including biomass burning, soil emissions and lightning, are responsible for nearly half of total emissions. Thus, as domestic air quality standards grow stricter and anthropogenic sources more regulated, constraining natural sources of NOx becomes critical. NOx concentrations in wildfire smoke differ based on the age of the plume, fire intensity and vegetation type. NOx soil emissions depend on soil moisture, soil temperature, soil porosity, and nitrogen storage. We present two years of NOx and ozone (O3) measurements from a remote mountaintop monitoring site located on Chews Ridge in the coastal mountains of Central California, airborne observations, and remotely sensed NO2 tropospheric columns retrieved using the Ozone Monitoring Instrument (OMI). We explore controls on NOx concentrations at Chews Ridge, in Monterey County, such as the age of wildfire smoke plumes and wildfire intensity (i.e. burning vs. smoldering), as well as soil moisture and precipitation, which can lead to pulsed NOx fluxes. Most recently our in situ observations fortuitously captured differing amounts of the active plume of the Soberanes wildfire, which to date has burned >45,000 acres and is expected to continue partially contained through August 2016. Implications of these episodic sources of NOx on the regional ozone budget will be discussed.

  20. Catalyzed borohydrides for hydrogen storage

    DOEpatents

    Au, Ming [Augusta, GA

    2012-02-28

    A hydrogen storage material and process is provided in which alkali borohydride materials are created which contain effective amounts of catalyst(s) which include transition metal oxides, halides, and chlorides of titanium, zirconium, tin, and combinations of the various catalysts. When the catalysts are added to an alkali borodydride such as a lithium borohydride, the initial hydrogen release point of the resulting mixture is substantially lowered. Additionally, the hydrogen storage material may be rehydrided with weight percent values of hydrogen at least about 9 percent.

  1. 40 CFR 97.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season 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 Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 97.388 Section 97.388 Protection of Environment... NOX AND SO2 TRADING PROGRAMS CAIR NOX Ozone Season Opt-in Units § 97.388 CAIR NOX Ozone...

  2. 40 CFR 97.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season 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 Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 97.388 Section 97.388 Protection of Environment... NOX AND SO2 TRADING PROGRAMS CAIR NOX Ozone Season Opt-in Units § 97.388 CAIR NOX Ozone...

  3. 40 CFR 97.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 97.388 Section 97.388 Protection of Environment... NOX AND SO2 TRADING PROGRAMS CAIR NOX Ozone Season Opt-in Units § 97.388 CAIR NOX Ozone...

  4. 40 CFR 97.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 97.388 Section 97.388 Protection of Environment... NOX AND SO2 TRADING PROGRAMS CAIR NOX Ozone Season Opt-in Units § 97.388 CAIR NOX Ozone...

  5. 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.

  6. NOx Chemical Sinks in the Upper Troposphere

    NASA Astrophysics Data System (ADS)

    Henderson, B. H.; Pinder, R. W.; Crooks, J.; Cohen, R. C.; Hutzell, W. T.; Sarwar, G.; Goliff, W. S.; Stockwell, W. R.; Fahr, A.; Mathur, R.; Carlton, A. G.; Vizuete, W.

    2010-12-01

    Chemical transport model evaluations in the upper troposphere (UT) have shown a NOx low-bias (Singh et al., 2007; Napelenok et al., 2008) and HOx high-bias (Bertram et al., 2007, Ren et al., 2008). The combined biases suggest an over-prediction of simulated chemical sinks of NOx. We developed a model framework that isolates gas-phase chemistry for evaluation against in situ INTEX-NA aircraft measurements. We evaluated seven chemical mechanisms (CB05, RACM2, SAPRC99, SAPRC07, GEOS-Chem, MOZART4, and MCM) whose designs range from near-explicit to condensed, and whose intended scales range from point to global simulation. Our evaluation finds that chemical sinks of NOx cause a 30% under-prediction of NOx. Inter-mechanism comparison identified inconsistencies and recommendations, but did not meaningfully improve over-estimation of simulated NOx chemical sinks. We designed experiments to test the model sensitivity to initial conditions, heterogeneous processing, and gas-phase reaction rate uncertainty. Initial results suggest that the over-prediction of chemical sinks is robust to uncertainty in initial conditions, but can be improved by adjusting reaction rate constants. Adding heterogeneous processing exacerbated the loss of NOx via N2O5 conversion to HNO3. We then tested sensitivity to reaction coefficients by re-evaluating the GEOS-Chem mechanism with each of its 293 reactions adjusted by 10%. We find that the chemical lifetime of NOx is most sensitive to OH + NO2 and HO2 + NO, which both have high JPL reported uncertainty at low temperatures. The rapid chemical loss of NOx suggests over estimation of total oxidation, which influences ozone in the upper troposphere where it most efficiently absorbs outgoing radiation. The oxidation bias will also influence the results of NOx sink attribution and O3 source attributions. To reduce the uncertainty in chemical sinks of NOx, we need further kinetic studies of HOx + NOx reactions under UT relevant conditions.

  7. Reforming catalysts

    SciTech Connect

    Givens, E.N.; Plank, C.J.; Rosinski, E.J.

    1980-03-04

    Crystalline aluminosilicate zeolites are mixed with conventional reforming catalysts to produce new catalytic compositions with high catalytic activity and selectivity and excellent aging characteristics. These new catalytic compositions may be utilized alone or in conjunction with conventional reforming catalysts. The acidic activity of the total catalyst system is controlled within defined limits. When so controlled the utility of these catalyst systems in reforming hydrocarbon mixtures is to reduce the C1 and C2 concentrations in reformer gas product, while increasing the C3 and C4 concentrations and maintaining high liquid yield at high octane numbers.

  8. Low NOx Advanced Vortex Combustor

    SciTech Connect

    Edmonds, Ryan G; Williams, Joseph T; Steele, Robert C; Straub, Douglas L; Casleton, Kent H; Bining, Avtar

    2008-05-01

    A lean-premixed advanced vortex combustor (AVC) has been developed and tested. The natural gas fueled AVC was tested at the U.S. Department of Energy’s National Energy Technology Laboratory in Morgantown, WV. All testing was performed at elevated pressures and inlet temperatures and at lean fuel-air ratios representative of industrial gas turbines. The improved AVC design exhibited simultaneous NOx /CO/unburned hydrocarbon (UHC) emissions of 4/4/0 ppmv (all emissions corrected to 15% O2 dry). The design also achieved less than 3 ppmv NOx with combustion efficiencies in excess of 99.5%. The design demonstrated marked acoustic dynamic stability over a wide range of operating conditions, which potentially makes this approach significantly more attractive than other lean-premixed combustion approaches. In addition, the measured 1.75% pressure drop is significantly lower than conventional gas turbine combustors, which could translate into an overall gas turbine cycle efficiency improvement. The relatively high velocities and low pressure drop achievable with this technology make the AVC approach an attractive alternative for syngas fuel applications.

  9. Low NOx Advanced Vortex Combustor

    SciTech Connect

    Edmonds, R.G.; Williams, J.T.; Steele, R.C.; Straub, D.L.; Casleton, K.H.; Bining, Avtar

    2008-05-01

    A lean-premixed advanced vortex combustor (AVC) has been developed and tested. The natural gas fueled AVC was tested at the U.S. Department of Energy’s National Energy Technology Laboratory in Morgantown, WV. All testing was performed at elevated pressures and inlet temperatures and at lean fuel-air ratios representative of industrial gas turbines. The improved AVC design exhibited simultaneous NOx /CO/unburned hydrocarbon (UHC) emissions of 4/4/0 ppmv (all emissions corrected to 15% O2 dry). The design also achieved less than 3 ppmv NOx with combustion efficiencies in excess of 99.5%. The design demonstrated marked acoustic dynamic stability over a wide range of operating conditions, which potentially makes this approach significantly more attractive than other lean-premixed combustion approaches. In addition, the measured 1.75% pressure drop is significantly lower than conventional gas turbine combustors, which could translate into an overall gas turbine cycle efficiency improvement. The relatively high velocities and low pressure drop achievable with this technology make the AVC approach an attractive alternative for syngas fuel applications.

  10. Systems and methods for solar energy storage, transportation, and conversion utilizing photochemically active organometallic isomeric compounds and solid-state catalysts

    DOEpatents

    Vollhardt, K. Peter C.; Segalman, Rachel A; Majumdar, Arunava; Meier, Steven

    2015-02-10

    A system for converting solar energy to chemical energy, and, subsequently, to thermal energy includes a light-harvesting station, a storage station, and a thermal energy release station. The system may include additional stations for converting the released thermal energy to other energy forms, e.g., to electrical energy and mechanical work. At the light-harvesting station, a photochemically active first organometallic compound, e.g., a fulvalenyl diruthenium complex, is exposed to light and is photochemically converted to a second, higher-energy organometallic compound, which is then transported to a storage station. At the storage station, the high-energy organometallic compound is stored for a desired time and/or is transported to a desired location for thermal energy release. At the thermal energy release station, the high-energy organometallic compound is catalytically converted back to the photochemically active organometallic compound by an exothermic process, while the released thermal energy is captured for subsequent use.

  11. LOW-CONCENTRATION NOX EMISSIONS MEASUREMENT

    EPA Science Inventory

    The paper gives results of a recent series of low-concentration nitrogen oxides (NOx) emission measurements, made by Midwest Research Institute (MRI) during U.S. EPA-sponsored Environmental Technology Verification (ETV) test of a NOx control system called Xonon (TM) Cool Combust...

  12. NOX4 regulates autophagy during energy deprivation

    PubMed Central

    Sciarretta, Sebastiano; Volpe, Massimo; Sadoshima, Junichi

    2014-01-01

    NADPH oxidase is a cellular enzyme devoted to the production of reactive oxygen species (ROS). NOX4 and NOX2 are the main isoforms of NADPH oxidase in the cardiovascular system. In our recent study, we demonstrated that NOX4, but not NOX2, is a critical mediator of the cardiomyocyte adaptive response to energy stress. NOX4 activity and protein levels are increased in the endoplasmic reticulum (ER) but not in mitochondria of cardiomyocytes during the early phase of energy deprivation. NOX4-derived production of ROS in the ER is a critical event that activates autophagy through stimulation of the EIF2AK3/PERK-EIF2S1/eIF-2α-ATF4 pathway. NOX4-dependent autophagy is an important mechanism to preserve cellular energy and limit cell death in energy-deprived cardiomyocytes. Aside from elucidating a crucial physiological function of NOX4 during cellular energy stress, our study dissects a novel signaling mechanism that regulates autophagy under this condition. PMID:24492492

  13. NOX4 regulates autophagy during energy deprivation.

    PubMed

    Sciarretta, Sebastiano; Volpe, Massimo; Sadoshima, Junichi

    2014-04-01

    NADPH oxidase is a cellular enzyme devoted to the production of reactive oxygen species (ROS). NOX4 and NOX2 are the main isoforms of NADPH oxidase in the cardiovascular system. In our recent study, we demonstrated that NOX4, but not NOX2, is a critical mediator of the cardiomyocyte adaptive response to energy stress. NOX4 activity and protein levels are increased in the endoplasmic reticulum (ER) but not in mitochondria of cardiomyocytes during the early phase of energy deprivation. NOX4-derived production of ROS in the ER is a critical event that activates autophagy through stimulation of the EIF2AK3/PERK-EIF2S1/eIF-2α-ATF4 pathway. NOX4-dependent autophagy is an important mechanism to preserve cellular energy and limit cell death in energy-deprived cardiomyocytes. Aside from elucidating a crucial physiological function of NOX4 during cellular energy stress, our study dissects a novel signaling mechanism that regulates autophagy under this condition.

  14. LOW-CONCENTRATION NOX EMISSIONS MEASUREMENT

    EPA Science Inventory

    The paper gives results of a recent series of low-concentration nitrogen oxides (NOx) emission measurements, made by Midwest Research Institute (MRI) during U.S. EPA-sponsored Environmental Technology Verification (ETV) test of a NOx control system called Xonon (TM) Cool Combust...

  15. Minimize NOx using only combustion control

    SciTech Connect

    Penterson, C.A.; Hules, K.R.

    2005-10-01

    The retrofit of a 600 MW opposed wall-fired utility boiler with low-NOx, dual air zone burners and overfire air cut the Wyoming PRB coal burner's NOx output by nearly half. The key to the project's success from the design stage through final testing and boiler tuning was CFD modeling. 7 figs., 2 tabs.

  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.

  17. NOx reduction in a lignite cyclone furnace

    SciTech Connect

    Melland, C.; O`Connor, D.

    1998-12-31

    Reburning, selective catalytic reduction, and selective noncatalytic reduction techniques have demonstrated some potential for NOx reduction in cyclone boilers. These techniques are costly in terms of both capital and operating costs. Lignite cyclone combustion modeling studies indicated that modifying combustion inside the cyclone barrel could reduce cyclone NOx emissions. The modeling showed that air staging, secondary air basing, flue gas injection and variations in coal moisture content could affect NOx emissions. Short term lignite boiler tests and now longer term boiler operation have confirmed that significant NOx reductions can be accomplished merely by modifying cyclone combustion. The low NOx operation does not appear to significantly impact maintenance, reliability or capacity of the cyclone burner or furnace.

  18. [NADPH oxidases, Nox: new isoenzymes family].

    PubMed

    Chuong Nguyen, Minh Vu; Lardy, Bernard; Paclet, Marie-Hélène; Rousset, Francis; Berthier, Sylvie; Baillet, Athan; Grange, Laurent; Gaudin, Philippe; Morel, Françoise

    2015-01-01

    NADPH oxidases, Nox, are a family of isoenzymes, composed of seven members, whose sole function is to produce reactive oxygen species (ROS). Although Nox catalyze the same enzymatic reaction, they acquired from a common ancestor during evolution, specificities related to their tissue expression, subcellular localization, activation mechanisms and regulation. Their functions could vary depending on the pathophysiological state of the tissues. Indeed, ROS are not only bactericidal weapons in phagocytes but also essential cellular signaling molecules and their overproduction is involved in chronic diseases and diseases of aging. The understanding of the mechanisms involved in the function of Nox and the emergence of Nox inhibitors, require a thorough knowledge of their nature and structure. The objectives of this review are to highlight, in a structure/function approach, the main similar and differentiated properties shared by the human Nox isoenzymes.

  19. High-Potential Electrocatalytic O2 Reduction with Nitroxyl/NOx Mediators: Implications for Fuel Cells and Aerobic Oxidation Catalysis

    PubMed Central

    2015-01-01

    Efficient reduction of O2 to water is a central challenge in energy conversion and many aerobic oxidation reactions. Here, we show that the electrochemical oxygen reduction reaction (ORR) can be achieved at high potentials by using soluble organic nitroxyl and nitrogen oxide (NOx) mediators. When used alone, neither organic nitroxyls, such as 2,2,6,6-tetramethyl-1-piperidinyl-N-oxyl (TEMPO), nor NOx species, such as sodium nitrite, are effective ORR mediators. The combination of nitroxyl/NOx species, however, mediates sustained O2 reduction with overpotentials as low as 300 mV in acetonitrile containing trifluoroacetic acid. Mechanistic analysis of the coupled redox reactions supports a process in which the nitrogen oxide catalyst drives aerobic oxidation of a nitroxyl mediator to an oxoammonium species, which then is reduced back to the nitroxyl at the cathode. The electrolysis potential is dictated by the oxoammonium/nitroxyl reduction potential. The overpotentials accessible with this ORR system are significantly lower than widely studied molecular metal-macrocycle ORR catalysts and benefit from the mechanism-based specificity for four-electron reduction of oxygen to water mediated by NOx species, together with kinetically efficient reduction of oxidized NOx species by TEMPO and other organic nitroxyls. PMID:27162977

  20. 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…

  1. 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…

  2. 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.

  3. NOx CONTROL OPTIONS AND INTEGRATION FOR US COAL FIRED BOILERS

    SciTech Connect

    Mike Bockelie; Marc Cremer; Kevin Davis; Connie Senior; Bob Hurt; Eric Eddings; Larry Baxter

    2002-07-28

    This is the eighth 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 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. CFD modeling studies of RRI in a full scale utility boiler have been performed that provide further insight into the NOx reduction process that occurs if the furnace is not adequately staged. In situ reactivity data indicate thus far that titania sulfates under SCR conditions but there is no indication of vanadia sulfation in agreement with some, but not most literature results. Additional analysis and advanced diagnostics are under way to confirm this result and determine its accuracy. Construction of a catalyst characterization reactor system is nearly complete, with a few remaining details discussed in this report. Shakedown testing of the SCR field reactor was completed at the University of Utah pilot-scale coal furnace. The CEM system has been ordered. Talks continued with American Electric Power about hosting a demonstration at their Rockport plant.

  4. Catalytic hydrolysis of urea with fly ash for generation of ammonia in a batch reactor for flue gas conditioning and NOx reduction

    SciTech Connect

    Sahu, J.N.; Gangadharan, P.; Patwardhan, A.V.; Meikap, B.C.

    2009-01-15

    Ammonia is a highly volatile noxious material with adverse physiological effects, which become intolerable even at very low concentrations and present substantial environmental and operating hazards and risk. Yet ammonia has long been known to be used for feedstock of flue gas conditioning and NOx reduction. Urea as the source of ammonia for the production of ammonia has the obvious advantages that no ammonia shipping, handling, and storage is required. The process of this invention minimizes the risks and hazards associated with the transport, storage, and use of anhydrous and aqueous ammonia. Yet no such rapid urea conversion process is available as per requirement of high conversion in shorter time, so here we study the catalytic hydrolysis of urea for fast conversion in a batch reactor. The catalyst used in this study is fly ash, a waste material originating in great amounts in combustion processes. A number of experiments were carried out in a batch reactor at different catalytic doses, temperatures, times, and at a constant concentration of urea solution 10% by weight, and equilibrium and kinetic studies have been made.

  5. NOx CONTROL OPTIONS AND INTEGRATION FOR US COAL FIRED BOILERS

    SciTech Connect

    Mike Bockelie; Marc Cremer; Kevin Davis; Connie Senior; Bob Hurt; Eric Suuberg; Eric Eddings; Larry Baxter

    2002-01-31

    This is the sixth 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 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. Preliminary results from laboratory and field tests of a corrosion probe to predict waterwall wastage indicate good agreement between the electrochemical noise corrosion rates predicted by the probe and corrosion rates measured by a surface profilometer. Four commercial manufacturers agreed to provide catalyst samples to the program. BYU has prepared two V/Ti oxide catalysts (custom, powder form) containing commercially relevant concentrations of V oxide and one containing a W oxide promoter. Two pieces of experimental apparatus being built at BYU to carry out laboratory-scale investigations of SCR catalyst deactivation are nearly completed. A decision was made to carry out the testing at full-scale power plants using a slipstream of gas instead of at the University of Utah pilot-scale coal combustor as originally planned. Design of the multi-catalyst slipstream reactor was completed during this quarter. One utility has expressed interest in hosting a long-term test at one of their plants that co-fire wood with coal. Tests to study ammonia adsorption onto fly ash have clearly established that the only routes that can play a role in binding significant amounts of ammonia to the ash surface, under practical ammonia slip conditions, are those that must involve co-adsorbates.

  6. NOx CONTROL OPTIONS AND INTEGRATION FOR US COAL FIRED BOILERS

    SciTech Connect

    Mike Bockelie; Marc Cremer; Kevin Davis; Connie Senior; Bob Hurt; Eric Eddings; Larry Baxter

    2002-10-24

    This is the ninth 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 firing US coals. The Electric Power Research Institute (EPRI) is providing cofunding for this program. This program contains multiple tasks and good progress is being made on all fronts. Various subsystems of BYU's Catalyst Characterization System (CCS) were upgraded this quarter. Work on the CCS hardware and software will continue in the coming quarter. A preliminary test matrix of poisoning experiments in the CCS has been drafted that will explore the effects of at least three poisons: sodium, potassium and calcium. During this quarter, we attempted to resolve discrepancies in previous in situ measurements of catalyst sulfation. Modifications were made to the XPS analysis procedure that allowed analyses of uncrushed samples. Although the XPS and FTIR results are now more consistent in that both indicate that the surface is sulfating (unlike the results reported last quarter), they disagree with respect to which species sulfates. The CEM system for the multi-catalyst slipstream reactor arrived this quarter. Minor modifications to the reactor and control system were completed. The reactor will be shipped to AEP Rockport plant next quarter for shakedown and installation. In a parallel effort, we have proposed to make mercury oxidation measurements across the catalysts at the start of the field test. Pending approval from DOE, we will begin the mercury measurements next quarter.

  7. 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.

  8. Modelling NOx emissions of single droplet combustion

    NASA Astrophysics Data System (ADS)

    Moesl, Klaus G.; Schwing, Joachim E.; Sattelmayer, Thomas

    2012-02-01

    An approach for modelling and simulation of the generation of nitrogen oxide (NOx) in the gas phase surrounding single burning droplets is presented. Assuming spherical symmetry (no gravity, no forced convection), the governing equations are derived first. Then simplifications are introduced and it is proven that they are appropriate. The influences of the initial droplet diameter, the ambient conditions, and the droplet pre-vapourisation on NOx are investigated. The fuel of choice is n-decane (C10H22) as it resembles kerosene and diesel fuel best, and the complexity of the reaction mechanism is manageable. Combinations of C10H22 mechanisms and well-established NOx kinetics are evaluated in detail and validated for their applicability in the context of this work. The conducted simulations of droplet combustion in an atmosphere of hot exhaust gas show that NOx formation (by mass of fuel) increases linearly with the droplet diameter. There is a trade-off between available oxygen and ambient temperature. Increasing the equivalence ratio of the exhaust gas leads to higher NOx emissions in the very lean regime, but to lower emissions if the equivalence ratio exceeds 0.85. Pre-vapourisation of fuel at ambient conditions becomes beneficial with respect to NOx emissions only if the degree of vapourisation is above a minimum limit. If less fuel is vapourised before ignition, the NOx emissions remain almost unaffected.

  9. Effect of Ti or Sn doping on the catalytic performance of MnOx/CeO2 catalyst for low temperature selective catalytic reduction of NO with NH3

    NASA Astrophysics Data System (ADS)

    Xiong, Yan; Tang, Changjin; Dong, Lin

    2015-04-01

    The abatement of nitrogen oxides (NOx) emission from exhaust gases of diesel and stationary sources is a significant challenge for economic and social development. Ceria-based solid solutions were synthesized and used as supports to prepare MnOx/Ce0.8Ti0.2O2 and MnOx/Ce0.8Sn0.2O2 catalysts (Mn/CeTi and Mn/CeSn) for low temperature selective catalytic reduction of NO by NH3 (NH3-SCR). The effects of Ti or Sn doping on the catalytic performance of MnOx/CeO2 catalyst were investigated. Experimental results show that doping of Ti or Sn increases the NO removal efficiency of MnOx/CeO2. The NO conversion of Mn/CeTi catalyst is more than 90 % at temperature window of 175 ~ 300 °C under a gas hour space velocity of 60,000 mL•g-1•h-1. Modified catalysts are also found to exhibit greatly improved resistance to sulfur-poisoning. NH3-TPD results suggest that NH3 desorption on the catalysts is observed over a wide temperature range, due to the variability of adsorbed NH3 species with different thermal stabilities. Doping of Ti and Sn into Mn/CeO2 greatly increased the NH3 adsorption ability of the composites which could promote the SCR reaction. Characterization results also indicate that doping of Ti or Sn brings about catalysts with higher BET surface area, enhanced oxygen storage capacity and increased surface acidity. X-ray photoelectron spectroscopy (XPS) analysis of spent catalysts following SCR reaction in the presence of SO2 verify that the loss of surface Mn species was inhibited by doping of Ti, which contributes to extend the catalyst durability.

  10. Design and testing of an independently controlled urea SCR retrofit system for the reduction of NOx emissions from marine diesels.

    PubMed

    Johnson, Derek R; Bedick, Clinton R; Clark, Nigel N; McKain, David L

    2009-05-15

    research with control optimization, urea distribution and possible use of oxidation catalysts is recommended to improve the NOx reduction capabilities while minimizing ammonia slip.

  11. CRISPR/Cas9-mediated knockout of p22phox leads to loss of Nox1 and Nox4, but not Nox5 activity.

    PubMed

    Prior, Kim-Kristin; Leisegang, Matthias S; Josipovic, Ivana; Löwe, Oliver; Shah, Ajay M; Weissmann, Norbert; Schröder, Katrin; Brandes, Ralf P

    2016-10-01

    The NADPH oxidases are important transmembrane proteins producing reactive oxygen species (ROS). Within the Nox family, different modes of activation can be discriminated. Nox1-3 are dependent on different cytosolic subunits, Nox4 seems to be constitutively active and Nox5 is directly activated by calcium. With the exception of Nox5, all Nox family members are thought to depend on the small transmembrane protein p22phox. With the discovery of the CRISPR/Cas9-system, a tool to alter genomic DNA sequences has become available. So far, this method has not been widely used in the redox community. On such basis, we decided to study the requirement of p22phox in the Nox complex using CRISPR/Cas9-mediated knockout. Knockout of the gene of p22phox, CYBA, led to an ablation of activity of Nox4 and Nox1 but not of Nox5. Production of hydrogen peroxide or superoxide after knockout could be rescued with either human or rat p22phox, but not with the DUOX-maturation factors DUOXA1/A2. Furthermore, different mutations of p22phox were studied regarding the influence on Nox4-dependent H2O2 production. P22phox Q130* and Y121H affected maturation and activity of Nox4. Hence, Nox5-dependent O2(•-) production is independent of p22phox, but native p22phox is needed for maturation of Nox4 and production of H2O2.

  12. Composite TiO2/clays materials for photocatalytic NOx oxidation

    NASA Astrophysics Data System (ADS)

    Todorova, N.; Giannakopoulou, T.; Karapati, S.; Petridis, D.; Vaimakis, T.; Trapalis, C.

    2014-11-01

    TiO2 photocatalyst received much attention for air purification applications especially for removal of air pollutants like NOx, VOCs etc. It has been established that the activity of the photocatalyst can be significantly enhanced by its immobilization onto suitable substrates like inorganic minerals, porous silica, hydroxyapatite, adsorbent materials like activated carbon, various co-catalysts such as semiconductors, graphene, reduced graphite oxide, etc. In the present work, photocatalytic composite materials consisted of mineral substrate and TiO2 in weight ratio 1:1 were manufactured and examined for oxidation and removal of nitric oxides NOx (NO and NO2). Commercial titania P25 (Evonik-Degussa) and urea-modified P25 were used as photocatalytically active components. Inorganic minerals, namely kunipia, talk and hydrotalcite were selected as supporting materials due to their layered structure and expected high NOx adsorption capability. Al3+ and Ca2+ intercalation was applied in order to improve the dispersion of TiO2 and its loading into the supporting matrix. The X-ray diffraction analysis and Scanning Electron Microscopy revealed the binary structure of the composites and homogeneous dispersion of the photocatalyst into the substrates. The photocatalytic behavior of the materials in NOx oxidation and removal was investigated under UV and visible light irradiation. The composite materials exhibited superior photocatalytic activity than the bare titania under both types of irradiation. Significant visible light activity was recorded for the composites containing urea-modified titania that was accredited to the N-doping of the semiconductor. Among the different substrates, the hydrotalcite caused highest increase in the NOx removal, while among the intercalation ions the Ca2+ was more efficient. The results were related to the improved dispersion of the TiO2 and the synergetic activity of the substrates as NOx adsorbers.

  13. 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 Section 96.23 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents. (a)...

  14. 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 Section 96.23 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.23 NOX Budget permit contents....

  15. Activity and hydrothermal stability of CeO₂-ZrO₂-WO₃ for the selective catalytic reduction of NOx with NH₃.

    PubMed

    Song, Zhongxian; Ning, Ping; Zhang, Qiulin; Li, Hao; Zhang, Jinhui; Wang, Yancai; Liu, Xin; Huang, Zhenzhen

    2016-04-01

    A series of CeO2-ZrO2-WO3 (CZW) catalysts prepared by a hydrothermal synthesis method showed excellent catalytic activity for selective catalytic reduction (SCR) of NO with NH3 over a wide temperature of 150-550°C. The effect of hydrothermal treatment of CZW catalysts on SCR activity was investigated in the presence of 10% H2O. The fresh catalyst showed above 90% NOx conversion at 201-459°C, which is applicable to diesel exhaust NOx purification (200-440°C). The SCR activity results indicated that hydrothermal aging decreased the SCR activity of CZW at low temperatures (below 300°C), while the activity was notably enhanced at high temperature (above 450°C). The aged CZW catalyst (hydrothermal aging at 700°C for 8 hr) showed almost 80% NOx conversion at 229-550°C, while the V2O5-WO3/TiO2 catalyst presented above 80% NOx conversion at 308-370°C. The effect of structural changes, acidity, and redox properties of CZW on the SCR activity was investigated. The results indicated that the excellent hydrothermal stability of CZW was mainly due to the CeO2-ZrO2 solid solution, amorphous WO3 phase and optimal acidity. In addition, the formation of WO3 clusters increased in size as the hydrothermal aging temperature increased, resulting in the collapse of structure, which could further affect the acidity and redox properties. Copyright © 2015. Published by Elsevier B.V.

  16. Catalyst mixtures

    DOEpatents

    Masel, Richard I.; Rosen, Brian A.

    2017-02-14

    Catalysts that include at least one catalytically active element and one helper catalyst can be used to increase the rate or lower the overpotential of chemical reactions. The helper catalyst can simultaneously act as a director molecule, suppressing undesired reactions and thus increasing selectivity toward the desired reaction. These catalysts can be useful for a variety of chemical reactions including, in particular, the electrochemical conversion of CO.sub.2 or formic acid. The catalysts can also suppress H.sub.2 evolution, permitting electrochemical cell operation at potentials below RHE. Chemical processes and devices using the catalysts are also disclosed, including processes to produce CO, OH.sup.-, HCO.sup.-, H.sub.2CO, (HCO.sub.2).sup.-, H.sub.2CO.sub.2, CH.sub.3OH, CH.sub.4, C.sub.2H.sub.4, CH.sub.3CH.sub.2OH, CH.sub.3COO.sup.-, CH.sub.3COOH, C.sub.2H.sub.6, O.sub.2, H.sub.2, (COOH).sub.2, or (COO.sup.-).sub.2, and a specific device, namely, a CO.sub.2 sensor.

  17. Ammonia-Free NOx Control System

    SciTech Connect

    S. Wu; Z. Fan; R. Herman

    2004-03-31

    Research is being conducted under United States Department of Energy (DOE) Contract DEFC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia. This report describes the work performed during the January 1 to March 31, 2004 time period.

  18. Ammonia-Free NOx Control System

    SciTech Connect

    S. Wu

    2003-12-31

    Research is being conducted under United States Department of Energy (DOE) Contract DEFC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia. This report describes the work performed during the October 1 to December 31, 2003 time period.

  19. Ammonia-Free NOx Control System

    SciTech Connect

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

    2004-09-30

    Research is being conducted under United States Department of Energy (DOE) Contract DEFC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia. This report describes the work performed during the July 1 to September 30, 2004 time period.

  20. Ammonia-Free NOx Control System

    SciTech Connect

    Song Wu; Zhen Fan; Richard G. Herman

    2004-12-31

    Research is being conducted under United States Department of Energy (DOE) Contract DEFC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia. This report describes the work performed during the October 1 to December 30, 2004 time period.

  1. Ammonia-Free NOx Control System

    SciTech Connect

    Zhen Fan; Song Wu; Richard G. Herman

    2004-06-30

    Research is being conducted under United States Department of Energy (DOE) Contract DEFC26-03NT41865 to develop a new technology to achieve very low levels of NOx emissions from pulverized coal fired boiler systems by employing a novel system level integration between the PC combustion process and the catalytic NOx reduction with CO present in the combustion flue gas. The combustor design and operating conditions will be optimized to achieve atypical flue gas conditions. This approach will not only suppress NOx generation during combustion but also further reduce NOx over a downstream catalytic reactor that does not require addition of an external reductant, such as ammonia. This report describes the work performed during the April 1 to June 30, 2004 time period.

  2. 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.

  3. 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

    2004-03-31

    This is the fifteenth 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. At AEP's Gavin Plant, data from the corrosion probes showed that corrosion rate increased as boiler load was increased. During an outage at the plant, the drop in boiler load, sensor temperature and corrosion rate could all be seen clearly. Restarting the boiler saw a resumption of corrosion activity. This behavior is consistent with previous observations made at a 600MWe utility boiler. More data are currently being examined for magnitudes of corrosion rates and changes in boiler operating conditions. Considerable progress was made this quarter in BYU's laboratory study of catalyst deactivation. Surface sulfation appears to partially suppress NO adsorption when the catalyst is not exposed to NH3; NH3 displaces surface-adsorbed NO on SCR catalysts and surface sulfation increases the amount of adsorbed NH3, as confirmed by both spectroscopy and TPD experiments. However, there is no indication of changes in catalyst activity despite changes in the amount of adsorbed NH3. A monolith test reactor (MTR), completed this quarter, provided the first comparative data for one of the fresh and field-exposed monolith SCR catalysts yet developed in this project. Measurements of activity on one of the field-exposed commercial monolith catalysts do not show significant changes in catalyst activity (within experimental error) as compared to the fresh catalyst. The exposed surface of the sample contains large amounts of Ca and Na, neither of which is present in the fresh sample, even after removal of visibly obvious fouling deposits. However, these fouling compounds do not

  4. Selective catalytic reduction operation with heavy fuel oil: NOx, NH3, and particle emissions.

    PubMed

    Lehtoranta, Kati; Vesala, Hannu; Koponen, Päivi; Korhonen, Satu

    2015-04-07

    To meet stringent NOx emission limits, selective catalytic reduction (SCR) is increasingly utilized in ships, likely also in combination with low-priced higher sulfur level fuels. In this study, the performance of SCR was studied by utilizing NOx, NH3, and particle measurements. Urea decomposition was studied with ammonia and isocyanic acid measurements and was found to be more effective with heavy fuel oil (HFO) than with light fuel oil. This is suggested to be explained by the metals found in HFO contributing to metal oxide particles catalyzing the hydrolysis reaction prior to SCR. At the exhaust temperature of 340 °C NOx reduction was 85-90%, while at lower temperatures the efficiency decreased. By increasing the catalyst loading, the low temperature behavior of the SCR was enhanced. The drawback of this, however, was the tendency of particle emissions (sulfate) to increase at higher temperatures with higher loaded catalysts. The particle size distribution results showed high amounts of nanoparticles (in 25-30 nm size), the formation of which SCR either increased or decreased. The findings of this work provide a better understanding of the usage of SCR in combination with a higher sulfur level fuel and also of ship particle emissions, which are a growing concern.

  5. NOx Direct Decomposition: Potentially Enhanced Thermodynamics and Kinetics on Chemically Modified Ferroelectric Surfaces

    NASA Astrophysics Data System (ADS)

    Kakekhani, Arvin; Ismail-Beigi, Sohrab

    2014-03-01

    NOx are regulated pollutants produced during automotive combustion. As part of an effort to design catalysts for NOx decomposition that operate in oxygen rich environment and permit greater fuel efficiency, we study chemistry of NOx on (001) ferroelectric surfaces. Changing the polarization at such surfaces modifies electronic properties and leads to switchable surface chemistry. Using first principles theory, our previous work has shown that addition of catalytic RuO2 monolayer on ferroelectric PbTiO3 surface makes direct decomposition of NO thermodynamically favorable for one polarization. Furthermore, the usual problem of blockage of catalytic sites by strong oxygen binding is overcome by flipping polarization that helps desorb the oxygen. We describe a thermodynamic cycle for direct NO decomposition followed by desorption of N2 and O2. We provide energy barriers and transition states for key steps of the cycle as well as describing their dependence on polarization direction. We end by pointing out how a switchable order parameter of substrate,in this case ferroelectric polarization, allows us to break away from some standard compromises for catalyst design(e.g. the Sabatier principle). This enlarges the set of potentially catalytic metals. Primary support from Toyota Motor Engineering and Manufacturing, North America, Inc.

  6. 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.

  7. Ultrathin 1T-phase MoS2 nanosheets decorated hollow carbon microspheres as highly efficient catalysts for solar energy harvesting and storage

    NASA Astrophysics Data System (ADS)

    Hsiao, Min-Chien; Chang, Chin-Yu; Niu, Li-Juan; Bai, Feng; Li, Lain-Jong; Shen, Hsin-Hui; Lin, Jeng-Yu; Lin, Tsung-Wu

    2017-03-01

    The composite of MoS2 and hollow carbon sphere (MoS2@HCS) is prepared via a glucose-assisted one pot synthesis. The composite consists of hierarchical spheres with a diameter of 0.5-4 μm and these hollow spheres are decorated with a number of curled and interlaced MoS2 nanosheets. After the composite is subject to the lithium intercalation, the MoS2 is converted from 2H to 1T phase. In this current work, the activities of 1T-MoS2@HCS toward photocatalytic hydrogen evolution and the reduction of I3- in dye-sensitized solar cells (DSCs) are systemically investigated. When evaluated as the photocatalyst for hydrogen evolution, the amount of evolved hydrogen over 1T-MoS2@HCS can reach 143 μmol in 2 h, being 3.6 times higher than as-synthesized 2H-MoS2@HCS. Additionally, the 1T-MoS2@HCS can be employed as the counter electrode (CE) material in DSCs. The DSCs based on 1T-MoS2@HCS CE possesses the power conversion efficiency of 8.94%, being higher than that with 2H-MoS2@HCS CE (8.16%) and comparable to that with Pt CE (8.87%). Our study demonstrates that 1T-MoS2@HCS has a great potential as an inexpensive alternative to Pt catalysts.

  8. 40 CFR 96.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 96.388 Section 96.388 Protection of Environment... 2009 through 2014 for which the CAIR NOX Ozone Season opt-in unit is to be allocated CAIR NOX Ozone...

  9. 40 CFR 75.71 - Specific provisions for monitoring NOX and heat input for the purpose of calculating NOX mass...

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... MONITORING NOX Mass Emissions Provisions § 75.71 Specific provisions for monitoring NOX and heat input for... 40 Protection of Environment 17 2014-07-01 2014-07-01 false Specific provisions for monitoring NOX and heat input for the purpose of calculating NOX mass emissions. 75.71 Section 75.71 Protection of...

  10. 40 CFR 75.71 - Specific provisions for monitoring NOX and heat input for the purpose of calculating NOX mass...

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... MONITORING NOX Mass Emissions Provisions § 75.71 Specific provisions for monitoring NOX and heat input for... 40 Protection of Environment 17 2013-07-01 2013-07-01 false Specific provisions for monitoring NOX and heat input for the purpose of calculating NOX mass emissions. 75.71 Section 75.71 Protection of...

  11. 40 CFR 75.71 - Specific provisions for monitoring NOX and heat input for the purpose of calculating NOX mass...

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... MONITORING NOX Mass Emissions Provisions § 75.71 Specific provisions for monitoring NOX and heat input for... 40 Protection of Environment 17 2012-07-01 2012-07-01 false Specific provisions for monitoring NOX and heat input for the purpose of calculating NOX mass emissions. 75.71 Section 75.71 Protection of...

  12. Correlating Engine NOx Emission with Biodiesel Composition

    NASA Astrophysics Data System (ADS)

    Jeyaseelan, Thangaraja; Mehta, Pramod Shankar

    2016-06-01

    Biodiesel composition comprising of saturated and unsaturated fatty acid methyl esters has a significant influence on its properties and hence the engine performance and emission characteristics. This paper proposes a comprehensive approach for composition-property-NOx emission analysis for biodiesel fuels and highlights the pathways responsible for such a relationship. Finally, a procedure and a predictor equation are developed for the assessment of biodiesel NOx emission from its composition details.

  13. Correlating Engine NOx Emission with Biodiesel Composition

    NASA Astrophysics Data System (ADS)

    Jeyaseelan, Thangaraja; Mehta, Pramod Shankar

    2017-06-01

    Biodiesel composition comprising of saturated and unsaturated fatty acid methyl esters has a significant influence on its properties and hence the engine performance and emission characteristics. This paper proposes a comprehensive approach for composition-property-NOx emission analysis for biodiesel fuels and highlights the pathways responsible for such a relationship. Finally, a procedure and a predictor equation are developed for the assessment of biodiesel NOx emission from its composition details.

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

    SciTech Connect

    Mike Bockelie; Kevin Davis; Connie Senior; Darren Shino; Dave Swenson; Larry Baxter; Calvin Bartholomew; William Hecker; Stan Harding

    2004-12-31

    This is the eighteenth 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. Safety equipment for ammonia for the SCR slipstream reactor at Plant Gadsden was installed. The slipstream reactor was started and operated for about 1400 hours during the last performance period. Laboratory analysis of exposed catalyst and investigations of the sulfation of fresh catalyst continued at BYU. Thicker end-caps for the ECN probes were designed and fabricated to prevent the warpage and failure that occurred at Gavin with the previous design. A refurbished ECN probe was successfully tested at the University of Utah combustion laboratory. Improvements were implemented to the software that controls the flow of cooling air to the ECN probes.

  15. Electrochemical NOx Sensor for Monitoring Diesel Emissions

    SciTech Connect

    Woo, L Y; Glass, R S

    2008-11-14

    % NO, balance NO{sub 2}. Since automotive exhaust sensors will probably be required to operate at temperatures > 600 C, NO is the dominant component in thermodynamic equilibrium and the target NOx species. Also, the use of upstream catalysts could further promote the conversion of NO{sub x} species to NO. Therefore, the focus of current work is to investigate the response to NO. Nevertheless, minimizing the sensitivity to a variety of competing species is important in order to obtain the accuracy necessary for achieving the emission limits. Mitigating the effect of interfering gases (e.g., O{sub 2}, water vapor, HCs, etc.) is an area of current study. For impedance metric NO{sub x} sensors, our previous work has demonstrated that the cross-sensitivity to O{sub 2} may be accounted for by comparing measurements at multiple frequencies. Other strategies for compensation are also being explored, including calibration using data from existing sensors located nearby. Our current work has made significant advances in terms of developing prototype sensors more suitable for commercialization. Also, dynamometer testing has provided real-world sensor performance data that will be useful in approaching potential suppliers to whom we can transfer the technology for commercialization. The advances are a direct result of understanding the sensing mechanisms responsible for impedance-based NO{sub x} sensing and the effect of materials choice and sensor design/geometry.

  16. Advancements in low NOx tangential firing systems

    SciTech Connect

    Hein, R. von; Maney, C.; Borio, R.

    1996-12-31

    The most cost effective method of reducing nitrogen oxide emissions when burning fossil fuels, such as coal, is through in-furnace NOx reduction processes. ABB Combustion Engineering, Inc. (ABB CE), through its ABB Power Plant Laboratories has been involved in the development of such low NOx pulverized coal firing systems for many years. This development effort is most recently demonstrated through ABB CE`s involvement with the U.S. Department of Energy`s (DOE) {open_quotes}Engineering Development of Advanced Coal Fired Low-Emission Boiler Systems{close_quotes} (LEBS) project. The goal of the DOE LEBS project is to use {open_quotes}near term{close_quotes} technologies to produce a commercially viable, low emissions boiler. This paper addresses one of the key technologies within this project, the NOx control subsystem. The foundation for the work undertaken at ABB CE is the TFS 2000{trademark} firing system, which is currently offered on a commercial basis. This system encompasses sub-stoichiometric combustion in the main firing zone for reduced NOx formation. Potential enhancements to this firing system focus on optimizing the introduction of the air and fuel within the primary windbox to provide additional horizontal and vertical staging. As is the case with all in-furnace NOx control processes, it is necessary to operate the system in a manner which does not decrease NOx at the expense of reduced combustion efficiency.

  17. OXYGEN ENHANCED COMBUSTION FOR NOx CONTROL

    SciTech Connect

    David R. Thompson; Lawrence E. Bool; Jack C. Chen

    2004-04-01

    Conventional wisdom says adding oxygen to a combustion system enhances product throughput, system efficiency, and, unless special care is taken, increases NOx emissions. This increase in NOx emissions is typically due to elevated flame temperatures associated with oxygen use leading to added thermal NOx formation. Innovative low flame temperature oxy-fuel burner designs have been developed and commercialized to minimize both thermal and fuel NOx formation for gas and oil fired industrial furnaces. To be effective these systems require close to 100% oxy-fuel combustion and the cost of oxygen is paid for by fuel savings and other benefits. For applications to coal-fired utility boilers at the current cost of oxygen, however, it is not economically feasible to use 100% oxygen for NOx control. In spite of this conventional wisdom, Praxair and its team members, in partnership with the US Department of Energy National Energy Technology Laboratory, have developed a novel way to use oxygen to reduce NOx emissions without resorting to complete oxy-fuel conversion. In this concept oxygen is added to the combustion process to enhance operation of a low NOx combustion system. Only a small fraction of combustion air is replaced with oxygen in the process. By selectively adding oxygen to a low NOx combustion system it is possible to reduce NOx emissions from nitrogen-containing fuels, including pulverized coal, while improving combustion characteristics such as unburned carbon. A combination of experimental work and modeling was used to define how well oxygen enhanced combustion could reduce NOx emissions. The results of this work suggest that small amounts of oxygen replacement can reduce the NOx emissions as compared to the air-alone system. NOx emissions significantly below 0.15 lbs/MMBtu were measured. Oxygen addition was also shown to reduce carbon in ash. Comparison of the costs of using oxygen for NOx control against competing technologies, such as SCR, show that this

  18. Combination of biodiesel-ethanol-diesel fuel blend and SCR catalyst assembly to reduce emissions from a heavy-duty diesel engine.

    PubMed

    Shi, Xiaoyan; Yu, Yunbo; He, Hong; Shuai, Shijin; Dong, Hongyi; Li, Rulong

    2008-01-01

    In this study, the efforts to reduce NOx and particulate matter (PM) emissions from a diesel engine using both ethanol-selective catalytic reduction (SCR) of NOx over an Ag/Al2O3 catalyst and a biodiesel-ethanol-diesel fuel blend (BE-diesel) on an engine bench test are discussed. Compared with diesel fuel, use of BE-diesel increased PM emissions by 14% due to the increase in the soluble organic fraction (SOF) of PM, but it greatly reduced the Bosch smoke number by 60%-80% according to the results from 13-mode test of European Stationary Cycle (ESC) test. The SCR catalyst was effective in NOx reduction by ethanol, and the NOx conversion was approximately 73%. Total hydrocarbons (THC) and CO emissions increased significantly during the SCR of NOx process. Two diesel oxidation catalyst (DOC) assemblies were used after Ag/Al2O3 converter to remove CO and HC. Different oxidation catalyst showed opposite effect on PM emission. The PM composition analysis revealed that the net effect of oxidation catalyst on total PM was an integrative effect on SOF reduction and sulfate formation of PM. The engine bench test results indicated that the combination of BE-diesel and a SCR catalyst assembly could provide benefits for NOx and PM emissions control even without using diesel particle filters (DPFs).

  19. DIESEL REFORMERS FOR LEAN NOX TRAP REGENERATION AND OTHER ON-BOARD HYDROGEN APPLICATIONS

    SciTech Connect

    Mauss, M; Wnuck, W

    2003-08-24

    Many solutions to meeting the 2007 and 2010 diesel emissions requirements have been suggested. On board production of hydrogen for in-cylinder combustion and exhaust after-treatment provide promising opportunities for meeting those requirements. Other benefits may include using syngas to rapidly heat up exhaust after-treatment catalysts during engine startup. HydrogenSource's development of a catalytic partial oxidation reformer for generating hydrogen from ultra-low sulfur diesel fuel is presented. The system can operate on engine exhaust and diesel fuel with no water tank. Test data for hydrogen regeneration of a lean NOx trap is presented showing 90% NOx conversion at temperatures as low as 150 degrees C and 99% conversion at 300 degrees C. Finally, additional efforts required to fully understand the benefits and commercial challenges of this technology are discussed.

  20. Simulation of catalytic oxidation and selective catalytic NOx reduction in lean-exhaust hybrid vehicles

    SciTech Connect

    Gao, Zhiming; Daw, C Stuart; Chakravarthy, Veerathu K

    2012-01-01

    We utilize physically-based models for diesel exhaust catalytic oxidation and urea-based selective catalytic NOx reduction to study their impact on drive cycle performance of hypothetical light-duty diesel powered hybrid vehicles. The models have been implemented as highly flexible SIMULINK block modules that can be used to study multiple engine-aftertreatment system configurations. The parameters of the NOx reduction model have been adjusted to reflect the characteristics of Cu-zeolite catalysts, which are of widespread current interest. We demonstrate application of these models using the Powertrain System Analysis Toolkit (PSAT) software for vehicle simulations, along with a previously published methodology that accounts for emissions and temperature transients in the engine exhaust. Our results illustrate the potential impact of DOC and SCR interactions for lean hybrid electric and plug-in hybrid electric vehicles.

  1. Highly dispersed metal catalyst

    DOEpatents

    Xiao, Xin; West, William L.; Rhodes, William D.

    2016-11-08

    A supported catalyst having an atomic level single atom structure is provided such that substantially all the catalyst is available for catalytic function. A process of forming a single atom catalyst unto a porous catalyst support is also provided.

  2. Reforming catalyst

    SciTech Connect

    Baird, W.C. Jr.; Swan, G.A.

    1991-11-19

    This patent describes a catalyst useful for reforming a naphtha feed at high severity reforming conditions. It comprises the metals, platinum, rhenium and iridium on a refractory porous inorganic oxide support, the support consisting essentially of alumina, wherein the concentration by weight of each of the metals platinum and rhenium is at least 0.1 percent and iridium at least 0.15 percent and at least one of the metals is present in a concentration of at least 0.3 percent, and the sum-total; concentration of the metals is greater than 0.9 percent, and wherein each catalyst particle contains all three of the metals platinum, rhenium and iridium. This patent also describes this composition wherein the catalyst contains from about 0.1 percent to about 3 percent of a halogen and from about 0.05 percent to about 0.02 percent sulfur.

  3. Determination of intermediates and mechanism for soot combustion with NOx/O₂ on potassium-supported Mg-Al hydrotalcite mixed oxides by in situ FTIR.

    PubMed

    Zhang, Zhaoliang; Zhang, Yexin; Su, Qingyun; Wang, Zhongpeng; Li, Qian; Gao, Xiyan

    2010-11-01

    The soot combustion with NO(x) and/or O(2) on potassium-supported Mg-Al hydrotalcite mixed oxides under tight contact condition was studied using temperature-programmed oxidation (TPO), isothermal reaction and in situ FTIR techniques. The presence of NO(x) in O(2) favors the soot combustion at lower temperatures (<300 °C). However, a little suppression was observed at higher temperatures (>300 °C), which was accompanied by a substantial NO(x) reduction. The ketene (C═C═O) and isocyanate (NCO(-)) species were determined as the reaction intermediates. In NO(x) + O(2), NO(2) directly interacts with the free carbon sites (C═C*) through two parallel reactions: (1) NO(2) + C═C* → C═C═O + NO; (2) NO(2) + C═C* → NCO(-) + CO(2). The two reactions can proceed easily, which accounts for the promotion effect of NO(x) on soot combustion at lower temperatures. The further oxidation of NCO(-) by NO(2) or O(2) is responsible for the simultaneous reduction of NO(x). However, the reactions between NO(2) and C═C* are limited by the amount of free carbon sites, which can be provided by the oxidation of soot by O(2) at higher temperatures. The interaction of NO(x) and catalyst results in the formation of nitrates and nitrites, which poisoned the active K sites.

  4. Effect of B20 and Low Aromatic Diesel on Transit Bus NOx Emissions Over Driving Cycles with a Range of Kinetic Intensity

    SciTech Connect

    Lammert, M. P.; McCormick, R. L.; Sindler, P.; Williams, A.

    2012-10-01

    Oxides of nitrogen (NOx) emissions for transit buses for up to five different fuels and three standard transit duty cycles were compared to establish whether there is a real-world biodiesel NOx increase for transit bus duty cycles and engine calibrations. Six buses representing the majority of the current national transit fleet and including hybrid and selective catalyst reduction systems were tested on a heavy-duty chassis dynamometer with certification diesel, certification B20 blend, low aromatic (California Air Resources Board) diesel, low aromatic B20 blend, and B100 fuels over the Manhattan, Orange County and UDDS test cycles. Engine emissions certification level had the dominant effect on NOx; kinetic intensity was the secondary driving factor. The biodiesel effect on NOx emissions was not statistically significant for most buses and duty cycles for blends with certification diesel, except for a 2008 model year bus. CARB fuel had many more instances of a statistically significant effect of reducing NOx. SCR systems proved effective at reducing NOx to near the detection limit on all duty cycles and fuels, including B100. While offering a fuel economy benefit, a hybrid system significantly increased NOx emissions over a same year bus with a conventional drivetrain and the same engine.

  5. Reactive Oxygen Species Derived from NOX3 and NOX5 Drive Differentiation of Human Oligodendrocytes

    PubMed Central

    Accetta, Roberta; Damiano, Simona; Morano, Annalisa; Mondola, Paolo; Paternò, Roberto; Avvedimento, Enrico V.; Santillo, Mariarosaria

    2016-01-01

    Reactive oxygen species (ROS) are signaling molecules that mediate stress response, apoptosis, DNA damage, gene expression and differentiation. We report here that differentiation of oligodendrocytes (OLs), the myelin forming cells in the CNS, is driven by ROS. To dissect the OL differentiation pathway, we used the cell line MO3-13, which display the molecular and cellular features of OL precursors. These cells exposed 1–4 days to low levels of H2O2 or to the protein kinase C (PKC) activator, phorbol-12-Myristate-13-Acetate (PMA) increased the expression of specific OL differentiation markers: the specific nuclear factor Olig-2, and Myelin Basic Protein (MBP), which was processed and accumulated selectively in membranes. The induction of differentiation genes was associated with the activation of ERK1-2 and phosphorylation of the nuclear cAMP responsive element binding protein 1 (CREB). PKC mediates ROS-induced differentiation because PKC depletion or bis-indolyl-maleimide (BIM), a PKC inhibitor, reversed the induction of differentiation markers by H2O2. H2O2 and PMA increased the expression of membrane-bound NADPH oxidases, NOX3 and NOX5. Selective depletion of these proteins inhibited differentiation induced by PMA. Furthermore, NOX5 silencing down regulated NOX3 mRNA levels, suggesting that ROS produced by NOX5 up-regulate NOX3 expression. These data unravel an elaborate network of ROS-generating enzymes (NOX5 to NOX3) activated by PKC and necessary for differentiation of OLs. Furthermore, NOX3 and NOX5, as inducers of OL differentiation, represent novel targets for therapies of demyelinating diseases, including multiple sclerosis, associated with impairment of OL differentiation. PMID:27313511

  6. HYDROGEN GENERATION FROM PLASMATRON REFORMERS: A PROMISING TECHNOLOGY FOR NOX ADSORBER REGENERATION AND OTHER AUTOMOTIVE APPLICATIONS

    SciTech Connect

    Bromberg, L.; Crane, S; Rabinovich, A.; Kong, Y; Cohn, D; Heywood, J; Alexeev, N.; Samokhin, A.

    2003-08-24

    Plasmatron reformers are being developed at MIT and ArvinMeritor [1]. In these reformers a special low power electrical discharge is used to promote partial oxidation conversion of hydrocarbon fuels into hydrogen and CO. The partial oxidation reaction of this very fuel rich mixture is difficult to initiate. The plasmatron provides continuous enhanced volume initiation. To minimize electrode erosion and electrical power requirements, a low current, high voltage discharge with wide area electrodes is used. The reformers operate at or slightly above atmospheric pressure. Plasmatron reformers provide the advantages of rapid startup and transient response; efficient conversion of the fuel to hydrogen rich gas; compact size; relaxation or elimination of reformer catalyst requirements; and capability to process difficult to reform fuels, such as diesel and bio-oils. These advantages facilitate use of onboard hydrogen-generation technology for diesel exhaust after-treatment. Plasma-enhanced reformer technology can provide substantial conversion even without the use of a catalyst. Recent progress includes a substantial decrease in electrical power consumption (to about 200 W), increased flow rate (above 1 g/s of diesel fuel corresponding to approximately 40 kW of chemical energy), soot suppression and improvements in other operational features.. Plasmatron reformer technology has been evaluated for regeneration of NOx adsorber after-treatment systems. At ArvinMeritor tests were performed on a dual-leg NOx adsorber system using a Cummins 8.3L diesel engine both in a test cell and on a vehicle. A NOx adsorber system was tested using the plasmatron reformer as a regenerator and without the reformer i.e., with straight diesel fuel based regeneration as the baseline case. The plasmatron reformer was shown to improve NOx regeneration significantly compared to the baseline diesel case. The net result of these initial tests was a significant decrease in fuel penalty, roughly 50% at

  7. Closeout final report on a demonstration test and evaluation of the Cannon Low-NOx Digester System

    SciTech Connect

    1995-04-01

    Cannon Boiler Works Inc. has been investigating a system for removing NOx from the exhaust gases of furnaces, gas turbines, chemical reactors, incinerators, and boilers. Computer simulations, bench-scale and pilot plant tests have proved that the system is capable of removing substantially all of the NOx from natural gas fired equipment exhaust streams. Originally designated as the Cannon NOx Digester, it has recently been renamed the Low Temperature Oxidation (LTO) System for NOx and SOx Reduction. The principal elements in the system are a fan, heat exchanger, oxidation chamber, spray chamber acting as a gas/liquid absorber, demister, an ozone generator, liquid oxygen storage or dry air supply system for the ozonator, chemical storage and metering system for the caustic neutralizer, and a data acquisition and control system. Most of the ozone is consumed in converting NOx to N{sub 2}O{sub 5} which hydrates to nitric acid which is then scrubbed out of the gas as it passes through the absorber. CO also reacts with ozone to form CO{sub 2} which is subsequently scrubbed out with NaOH. A demonstration, planned for the Alta Dena Dairy located near Los Angeles and in violation of California`s air quality regulations for natural gas fired boilers, was started, delayed due to boiler modifications, and will be continued shortly with new funding. This paper describes the LTO process and presents results from the initial demonstration.

  8. High-Potential Electrocatalytic O2 Reduction with Nitroxyl / NOx Mediators: Implications for Fuel Cells and Aerobic Oxidation Catalysis

    SciTech Connect

    Gerken, James B.; Stahl, Shannon S.

    2015-07-15

    Efficient reduction of O2 to water is a central challenge in energy conversion and aerobic oxidation catalysis. In the present study, we investigate the electrochemical reduction of O2 with soluble organic nitroxyl and nitrogen oxide (NOx) mediators. When used alone, neither organic nitroxyls, such as TEMPO (2,2,6,6-tetramethyl-1-piperidinyl-N-oxyl), nor NOx species, such as sodium nitrite, are effective mediators of electrochemical O2 reduction. The combination of nitroxyl/NOx species, however, mediates sustained O2 reduction at electrochemical potentials of 0.19–0.33 V (vs. Fc/Fc+) in acetonitrile containing trifluoroacetic acid. Mechanistic analysis of the coupled redox reactions supports a process in which the nitrogen oxide catalyst drives aerobic oxidation of a nitroxyl mediator to an oxoammonium species, which then is reduced back to the nitroxyl at the cathode. The electrolysis potential is dictated by the oxoammonium/nitroxyl reduction potential. The high potentials observed with this ORR system benefit from the mechanism-based specificity for four-electron reduction of oxygen to water mediated by NOx species, together with kinetically efficient reduction of oxidized NOx species by TEMPO and other organic nitroxyls. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center, funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.

  9. Characteristics of NOx removal combining dielectric barrier discharge plasma with selective catalytic reduction by C2H5OH

    NASA Astrophysics Data System (ADS)

    Wang, Xing-Quan; Chen, Wei; Guo, Qi-Pei; Li, Yi; Lv, Guo-Hua; Sun, Xiu-Ping; Zhang, Xian-Hui; Feng, Ke-Cheng; Yang, Si-Ze

    2009-07-01

    With the assistance of dielectric barrier discharge (DBD) plasma, selective catalytic reduction of NOx by ethanol over Ag/Al2O3 catalysts was studied. Experimental results show that NOx conversion was greatly enhanced due to the presence of DBD plasma at lower temperature. By varying the DBD voltages or power in 13 kHz frequency at different temperatures, NOx conversion was increased to 40.7% from 6.4% at 176 °C, even to 66.8% from 17.3% at 200 °C. NOx conversion could even be improved to 90% at temperature above 255 °C. It was proposed that nonthermal plasma generated by dielectric barrier discharge reactor was very effective for oxidizing NO to NO2 under excess O2 conditions, which possesses high reactivity with C2H5OH to yield CxHyNzO compound. By reacting with CxHyNzO compound and oxygen, NOx is converted to N2 at low temperatures.

  10. Catalyst activator

    DOEpatents

    McAdon, Mark H.; Nickias, Peter N.; Marks, Tobin J.; Schwartz, David J.

    2001-01-01

    A catalyst activator particularly adapted for use in the activation of metal complexes of metals of Group 3-10 for polymerization of ethylenically unsaturated polymerizable monomers, especially olefins, comprising two Group 13 metal or metalloid atoms and a ligand structure including at least one bridging group connecting ligands on the two Group 13 metal or metalloid atoms.

  11. SOx-NOx-Rox Box{trademark} flue gas clean-up demonstration. Final report

    SciTech Connect

    1995-09-01

    Babcock and Wilcox`s (B and W) SOx-NOx-Rox Box{trademark} process effectively removes SOx, NOx and particulate (Rox) from flue gas generated from coal-fired boilers in a single unit operation, a high temperature baghouse. The SNRB technology utilizes dry sorbent injection upstream of the baghouse for removal of SOx and ammonia injection upstream of a zeolitic selective catalytic reduction (SCR) catalyst incorporated in the baghouse to reduce NOx emissions. Because the SOx and NOx removal processes require operation at elevated gas temperatures (800--900 F) for high removal efficiency, high-temperature fabric filter bags are used in the baghouse. The SNRB technology evolved from the bench and laboratory pilot scale to be successfully demonstrated at the 5-MWe field scale. This report represents the completion of Milestone M14 as specified in the Work Plan. B and W tested the SNRB pollution control system at a 5-MWe demonstration facility at Ohio Edison`s R.E. Burger Plant located near Shadyside, Ohio. The design and operation were influenced by the results from laboratory pilot testing at B and W`s Alliance Research Center. The intent was to demonstrate the commercial feasibility of the SNRB process. The SNRB facility treated a 30,000 ACFM flue gas slipstream from Boiler No. 8. Operation of the facility began in May 1992 and was completed in May 1993. About 2,300 hours of high-temperature operation were achieved. The main emissions control performance goals of: greater than 70% SO{sub 2} removal using a calcium-based sorbent; greater than 90% NOx removal with minimal ammonia slip; and particulate emissions in compliance with the New Source Performance Standards (NSPS) of 0.03 lb/million Btu were exceeded simultaneously in the demonstration program when the facility was operated at optimal conditions. Testing also showed significant reductions in emissions of some hazardous air pollutants.

  12. Preparation of highly active manganese oxides supported on functionalized MWNTs for low temperature NOx reduction with NH3

    NASA Astrophysics Data System (ADS)

    Pourkhalil, Mahnaz; Moghaddam, Abdolsamad Zarringhalam; Rashidi, Alimorad; Towfighi, Jafar; Mortazavi, Yadollah

    2013-08-01

    Manganese oxide catalysts (MnOx) supported on functionalized multi-walled carbon nanotubes (FMWNTs) for low temperature selective catalytic reduction (LTSCR) of nitrogen oxides (NOx) with NH3 in the presence of excess O2 were prepared by the incipient wetness impregnation method. These catalysts were characterized by N2 adsorption, Fourier transform infrared spectroscopy (FTIR), transmission electron microscope (TEM), X-ray diffraction (XRD), thermal gravimetric analysis (TGA) and H2-temperature programmed reduction (H2-TPR) methods. The effects of reaction temperature, MnOx loading, calcination temperature and calcination time were investigated. The presence of surface nitrate species under moderate calcination conditions may play a favorable role in the LTSCR of NOx with NH3. Under the reaction conditions of 200 °C, 1 bar, NO = NH3 = 900 ppm, O2 = 5 vol%, GHSV = 30,000 h-1 and 12 wt% MnOx, NOx conversion and N2 selectivity were 97% and 99.5%, respectively. The SCR activity was reduced in the presence of 100 ppm SO2 and 2.5 vol% H2O from 97% to 92% within 6 h at 200 °C, however such an effect was shown to be reversible by exposing the catalyst to a helium flow for 2 h at 350 °C due to thermal decomposition of ammonium sulphate salts.

  13. Enhanced Combustion Low NOx Pulverized Coal Burner

    SciTech Connect

    David Towle; Richard Donais; Todd Hellewell; Robert Lewis; Robert Schrecengost

    2007-06-30

    For more than two decades, Alstom Power Inc. (Alstom) has developed a range of low cost, infurnace technologies for NOx emissions control for the domestic U.S. pulverized coal fired boiler market. This includes Alstom's internally developed TFS 2000{trademark} firing system, and various enhancements to it developed in concert with the U.S. Department of Energy. As of the date of this report, more than 270 units representing approximately 80,000 MWe of domestic coal fired capacity have been retrofit with Alstom low NOx technology. Best of class emissions range from 0.18 lb/MMBtu for bituminous coal to 0.10 lb/MMBtu for subbituminous coal, with typical levels at 0.24 lb/MMBtu and 0.13 lb/MMBtu, respectively. Despite these gains, NOx emissions limits in the U.S. continue to ratchet down for new and existing boiler equipment. On March 10, 2005, the Environmental Protection Agency (EPA) announced the Clean Air Interstate Rule (CAIR). CAIR requires 25 Eastern states to reduce NOx emissions from the power generation sector by 1.7 million tons in 2009 and 2.0 million tons by 2015. Low cost solutions to meet such regulations, and in particular those that can avoid the need for a costly selective catalytic reduction system (SCR), provide a strong incentive to continue to improve low NOx firing system technology to meet current and anticipated NOx control regulations. The overall objective of the work is to develop an enhanced combustion, low NOx pulverized coal burner, which, when integrated with Alstom's state-of-the-art, globally air staged low NOx firing systems will provide a means to achieve: Less than 0.15 lb/MMBtu NOx emissions when firing a high volatile Eastern or Western bituminous coal, Less than 0.10 lb/MMBtu NOx emissions when firing a subbituminous coal, NOx reduction costs at least 25% lower than the costs of an SCR, Validation of the NOx control technology developed through large (15 MWt) pilot scale demonstration, and Documentation required for economic

  14. High temperature durable catalyst development

    NASA Technical Reports Server (NTRS)

    Snow, G. C.; Tong, H.

    1981-01-01

    A program has been carried out to develop a catalytic reactor capable of operation in environments representative of those anticipated for advanced automotive gas turbine engines. A reactor consisting of a graded cell honeycomb support with a combination of noble metal and metal oxide catalyst coatings was built and successfully operated for 1000 hr. At an air preheat temperature of 740 K and a propane/air ratio of 0.028 by mass, the adiabatic flame temperature was held at about 1700 K. The graded cell monolithic reaction measured 5 cm in diameter by 10.2 cm in length and was operated at a reference velocity of 14.0 m/s at 1 atm. Measured NOx levels remained below 5 ppm, while unburned hydrocarbon concentrations registered near zero and carbon monoxide levels were nominally below 20 ppm.

  15. Low NOx heavy fuel combustor concept program

    NASA Technical Reports Server (NTRS)

    White, D. J.; Kubasco, A. J.

    1982-01-01

    Three simulated coal gas fuels based on hydrogen and carbon monoxide were tested during an experimental evaluation with a rich lean can combustor: these were a simulated Winkler gas, Lurgi gas and Blue Water gas. All three were simulated by mixing together the necessary pure component species, to levels typical of fuel gases produced from coal. The Lurgi gas was also evaluated with ammonia addition. Fuel burning in a rich lean mode was emphasized. Only the Blue Water gas, however, could be operated in such fashion. This showed that the expected NOx signature form could be obtained, although the absolute values of NOx were above the 75 ppm goals for most operating conditions. Lean combustion produced very low NOx well below 75 ppm with the Winkler and Lurgi gases. In addition, these low levels were not significantly impacted by changes in operating conditions.

  16. System and method for diagnosing EGR performance using NOx sensor

    DOEpatents

    Mazur, Christopher John

    2003-12-23

    A method and system for diagnosing a condition of an EGR valve used in an engine system. The EGR valve controls the portion exhaust gases produced by such engine system and fed back to an intake of such engine system. The engine system includes a NOx sensor for measuring NOx in such exhaust. The method includes: determining a time rate of change in NOx measured by the NOx sensor; comparing the determined time rate of change in the measured NOx with a predetermined expected time rate of change in measured NOx; and determining the condition of the EGR valve as a function of such comparison. The method also includes: determining from NOx measured by the NOx sensor and engine operating conditions indications of instances when samples of such measured NOx are greater than an expected maximum NOx level for such engine condition and less than an expected minimum NOx level for such engine condition; and determining the condition of the EGR valve as a function of a statistical analysis of such indications. The method includes determining whether the NOx sensor is faulty and wherein the EGR condition determining includes determining whether the NOx sensor is faulty.

  17. Enhancement of NOx and hydrocarbon conversion in plasma-activated catalysis

    NASA Astrophysics Data System (ADS)

    Graham, Bill; Adress, Wahmeed; Goguet, Alexandre; Yang, Hui; De Rosa, Fabio; Hardacre, Christopher; Stere, Cristina

    2016-09-01

    Atmospheric pressure, non-thermal plasma-activated-catalysis is showing real promise in a number of applications. Here we report on how electrical, visible and FTIR spectroscopy and mass spectroscopy measurements in a kHz atmospheric pressure He plasma jet coupled with a Ag/Al2O3 catalyst allowed us produce and confirm a strong enhancement of both NOx and hydrocarbon conversion at a measured gas temperature of <= 250° C. How these and other measurements have provided an insight into the fundamental physical and chemical processes in the plasma environment that have helped us move to a more efficient system and other processes will be discussed.

  18. NOx reduction methods and apparatuses

    DOEpatents

    Tonkyn, Russell G.; Barlow, Stephan E.; Balmer, M. Lou; Maupin, Gary D.

    2004-10-26

    A NO.sub.x reduction method includes treating a first gas containing NO.sub.x, producing a second gas containing NO.sub.2, reducing a portion of the NO.sub.2 in the second gas to N.sub.2, and producing a third gas containing less NO.sub.x than the first gas, substantially all of the third gas NO.sub.x being NO. The method also includes treating the third gas, producing a fourth gas containing NO.sub.2, reducing a portion of the NO.sub.2 in the fourth gas to N.sub.2, and producing a fifth gas containing less NO.sub.x than the third gas, substantially all of the fifth gas NO.sub.x being NO. Treating the first and/or third gas can include treatment with a plasma. Reducing a portion of the NO.sub.2 in the second and/or fourth gas can include reducing with a catalyst. The method can further include controlling energy consumption of the plasmas independent of each other.

  19. 40 CFR 96.160 - Submission of CAIR NOX allowance transfers.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Transfers § 96.160 Submission of CAIR NOX allowance transfers. A...

  20. 40 CFR 96.160 - Submission of CAIR NOX allowance transfers.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Transfers § 96.160 Submission of CAIR NOX allowance transfers. A...

  1. 40 CFR 96.41 - Timing requirements for NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Allocations § 96.41 Timing requirements for NOX allowance allocations. (a)...

  2. 40 CFR 96.41 - Timing requirements for NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Allowance Allocations § 96.41 Timing requirements for NOX allowance allocations. (a)...

  3. 40 CFR 96.153 - Recordation of CAIR NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Tracking System § 96.153 Recordation of CAIR NOX allowance...

  4. 40 CFR 96.153 - Recordation of CAIR NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Tracking System § 96.153 Recordation of CAIR NOX allowance...

  5. 40 CFR 96.154 - Compliance with CAIR NOX emissions limitation.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Tracking System § 96.154 Compliance with CAIR NOX emissions...

  6. 40 CFR 96.186 - Withdrawal from CAIR NOX Annual Trading Program.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Opt-in Units § 96.186 Withdrawal from CAIR NOX Annual...

  7. 40 CFR 96.154 - Compliance with CAIR NOX emissions limitation.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Tracking System § 96.154 Compliance with CAIR NOX emissions...

  8. Control of NOx Emissions from Stationary Combustion Sources

    EPA Science Inventory

    In general, NOx control technologies are categorized as being either primary control technologies or secondary control technologies. Primary control technologies reduce the formation of NOx in the primary combustion zone. In contrast, secondary control technologies destroy the NO...

  9. Improved low NOx firing systems for pulverized coal combustion

    SciTech Connect

    McCarthy, K.; Laux, S.; Grusha, J.; Rosin, T.; Hausman, G.L.

    1999-07-01

    More stringent emission limits or the addition of post combustion NOx control create the need for improvements of NOx emissions from pulverized coal boilers. Many boilers retrofitted with Low NOx technology during Phase 1 and Phase 2 of the CAAA fail or marginally meet their requirements. Technical solutions range from addition of overfire air and state-of-the-art low NOx burners to low cost additions of combustion enhancements. Regardless of the combustion NOx control method used, stoichiometries local to the burners must be maintained at the designed values at all times to provide high NOx performance at low efficiency loss due to unburned fuel. This paper describes Foster Wheeler's approach to NOx emission improvements for existing low NOx firing systems. The technology to measure air and coal flow individually for each burner and to control the parameters for optimum combustion are presented and discussed. Field experience shows the installation and advantages of the technology.

  10. Control of NOx Emissions from Stationary Combustion Sources

    EPA Science Inventory

    In general, NOx control technologies are categorized as being either primary control technologies or secondary control technologies. Primary control technologies reduce the formation of NOx in the primary combustion zone. In contrast, secondary control technologies destroy the NO...

  11. Dithiothreitol activity by particulate oxidizers of SOA produced from photooxidation of hydrocarbons under varied NOx levels

    NASA Astrophysics Data System (ADS)

    Jiang, Huanhuan; Jang, Myoseon; Yu, Zechen

    2017-08-01

    When hydrocarbons (HCs) are atmospherically oxidized, they form particulate oxidizers, including quinones, organic hydroperoxides, and peroxyacyl nitrates (PANs). These particulate oxidizers can modify cellular materials (e.g., proteins and enzymes) and adversely modulate cell functions. In this study, the contribution of particulate oxidizers in secondary organic aerosols (SOAs) to the oxidative potential was investigated. SOAs were generated from the photooxidation of toluene, 1,3,5-trimethylbenzene, isoprene, and α-pinene under varied NOx levels. Oxidative potential was determined from the typical mass-normalized consumption rate (reaction time t = 30 min) of dithiothreitol (DTTt), a surrogate for biological reducing agents. Under high-NOx conditions, the DTTt of toluene SOA was 2-5 times higher than that of the other types of SOA. Isoprene DTTt significantly decreased with increasing NOx (up to 69 % reduction by changing the HC / NOx ratio from 30 to 5). The DTTt of 1,3,5-trimethylbenzene and α-pinene SOA was insensitive to NOx under the experimental conditions of this study. The significance of quinones to the oxidative potential of SOA was tested through the enhancement of DTT consumption in the presence of 2,4-dimethylimidazole, a co-catalyst for the redox cycling of quinones; however, no significant effect of 2,4-dimethylimidazole on modulation of DTT consumption was observed for all SOA, suggesting that a negligible amount of quinones was present in the SOA of this study. For toluene and isoprene, mass-normalized DTT consumption (DTTm) was determined over an extended period of reaction time (t = 2 h) to quantify their maximum capacity to consume DTT. The total quantities of PANs and organic hydroperoxides in toluene SOA and isoprene SOA were also measured using the Griess assay and the 4-nitrophenylboronic acid assay, respectively. Under the NOx conditions (HC / NOx ratio: 5-36 ppbC ppb-1) applied in this study, the amount of organic hydroperoxides was

  12. Direct Measurements of NOx Produced by Lightning

    NASA Astrophysics Data System (ADS)

    Rahman, M.; Cooray, V.; Rakov, V. A.; Uman, M. A.; Liyanage, P.; Decarlo, B. A.; Jerauld, J.; Olsen, R. C.

    2006-12-01

    We present the first direct measurements of NOx generated by lightning. In July 2005, three negative lightning flashes were triggered using the rocket-and-wire technique at the International Center for Lightning Research and Testing (ICLRT) at Camp Blanding, Florida. The NOx produced by these three rocket- triggered flashes was measured, using the chemiluminescence method, by isolating a 3-cm long section of the lightning channel within a discharge chamber whose volume was 0.77 m3. We measured NOx individually for the first flash, which was triggered on July 15, and cumulatively for the other two flashes, which were triggered within about eleven minutes of each other on July 31. The July 15 flash contained only an initial- stage current and no return strokes. Each of the July 31 flashes contained an initial-stage current and either one or two return strokes. The initial-stage current in each case had a duration in the range from 260 to 360 ms, and one return stroke in each July 31 flash was followed by a continuing current whose duration was greater than 40 ms. The NOx production by the July 15 flash without return strokes (total charge transfer of 77 C) was 2.0×10^{22} molecules per meter of lightning channel, and that by the two July 31 flashes with return strokes (total charge transfer of 108 C) was 2.4×10^{22} molecules per meter. The NOx production per unit charge for these two measurements was similar: 2.6×1020 and 2.2×1020 molecules per meter per coulomb. It appears that the NOx production is primarily from long-duration, steady currents, as opposed to microsecond-scale impulsive return stroke currents. This observation implies that cloud discharges, which transfer, on average, larger charges than ground discharges, but do not contain return strokes (although they do contain typically shorter and presumably smaller amplitude microsecond-scale pulses) may be as effective as (or more effective than) cloud-to-ground discharges in producing NOx in the

  13. Design better cerium-based oxidation catalysts

    SciTech Connect

    Trovarelli, A.; Leitenburg, C. de; Dolcetti, G.

    1997-06-01

    Structural and energetic factors play an important role in the development of a new generation of automobile exhaust catalysts containing CeO{sub 2} doped with ZrO{sub 2} and/or other rare earth oxides such as PrO{sub x}, Y{sub 2}O{sub 3}, and La{sub 2}O{sub 3}. These new catalysts possess high oxygen storage capacity, improved thermal stability, and enhanced catalytic properties. These properties are discussed.

  14. Lagrangian Hotspots of In-Use NOX Emissions from Transit Buses.

    PubMed

    Kotz, Andrew J; Kittelson, David B; Northrop, William F

    2016-06-07

    In-use, spatiotemporal NOX emissions were measured from a conventional powertrain transit bus and a series electric hybrid bus over gradients of route kinetic intensity and ambient temperature. This paper introduces a new method for identifying NOX emissions hotspots along a bus route using high fidelity Lagrangian vehicle data to explore spatial interactions that may influence emissions production. Our study shows that the studied transit buses emit higher than regulated emissions because on-route operation does not accurately represent the range of engine operation tested according to regulatory standards. Using the Lagrangian hotspot detection, we demonstrate that NOX hotspots occurred at bus stops, during cold starts, on inclines, and for accelerations. On the selected routes, bus stops resulted in 3.3 times the route averaged emissions factor in grams/km without significant dependence on bus type or climate. The buses also emitted 2.3 times the route averaged NOX emissions factor at the beginning of each route due to cold selective catalytic reduction aftertreatment temperature. The Lagrangian hotspot detection technique demonstrated here could be employed in future connected vehicles empowered by advances in computational power, data storage capability, and improved sensor technology to optimize emissions as a function of spatial location.

  15. Catalyst suppliers consolidate further, offer more catalysts

    SciTech Connect

    Rhodes, A.K.

    1995-10-02

    The list of suppliers of catalysts to the petroleum refining industry has decreased by five since Oil and Gas Journal`s survey of refining catalysts and catalytic additives was last published. Despite the consolidation, the list of catalyst designations has grown to about 950 in this latest survey, compared to 820 listed in 1993. The table divides the catalysts by use and gives data on their primary differentiating characteristics, feedstock, products, form, bulk density,catalyst support, active agents, availability, and manufactures.

  16. CARBON NANOTUBES AND NANO-Ce-Zr OXIDES SUPPORTED H3PW12O40 FOR EFFECTIVE ADSORPTION-DECOMPOSITION OF NOx

    NASA Astrophysics Data System (ADS)

    Cheng, Lin; Wang, Rui

    2012-01-01

    Surface-modified carbon nanotubes (CNTs) and nano-Ce-Zr mixed oxides (CZO) were prepared and employed initially as supports of H3PW12O40 (HPW) for NOx adsorption-decomposition. Both CNTs and nano-CZO are favorable supports for HPW. After loading with HPW, the NOx adsorption efficiency increases, especially for HPW/CZO in which the highest adsorption efficiency can achieve 98% at the HPW loading of 70%, much higher than that of single HPW. NOx adsorption efficiency can be influenced considerably by catalyst preparing conditions, in particularly, ethyl alcohol is superior to water as solvent for HPW loading onto CNTs; the -OH containing CNTs shows better promotion effect on the adsorption of NOx than that containing -COOH when using absolute ethyl alcohol as solvent; mechanical grinding method is superior to incipient impregnation method in loading HPW onto the support of CZO. For both catalysts of HPW/CNTs and HPW/CZO, with the increase of HPW loading, the NOx adsorption efficiency tends to reach a peak value before dropping down. Heated from 150°C to 450°C at a rate of 50°C/min, the adsorbed NO was found to decompose into N2, O2 and N2O, and yields of N2 being 21.8% and 27.3%, respectively for HPW/CNTs and HPW/CZO were obtained.

  17. Hydrocracking catalyst

    SciTech Connect

    Arias, B.; Galiasso, R.; Kum, H.

    1985-02-12

    The invention relates to a particular method for the preparation of a hydrocracking catalyst, using a high iron content bauxite as a basis. This bauxite is ground and screened to a specific size and mixed with three types of additives: a promoter additive of the P, Mo, Co, Ni, W type. A hardener additive of the phosphoric acid type, ammonium phosphate. And a lubricant and pore-generating additive of the polyvinyl alcohol, polyethylene-glycol, starch type. The particularity consists in that the three additives are added simultaneously during the extrusion of the sample. That way, a particular surface composition is obtained which allows for the activity of the catalyst. Extruded products are obtained in sizes of 1/8, 1/16, and 1/32'' and submitted to drying and calcination programs for their activation. The obtained catalyst offers a good mechanical strength, a high content in macropores and a high activity, specifically for the hydrocracking of heavy Venezuelan crudes or residues.

  18. Ammonia and NO/NOx measurement for DE-NOx applications

    SciTech Connect

    Kita, D.

    1996-10-01

    A number of critical environmental goals may be met by controlling nitrogen oxide (NOx) emissions from combustion sources. These goals include responding to 1990 Clean Air Act Amendment requirements, reduction of human exposure to harmful concentrations of nitric oxide (NO) and nitrogen dioxide (NO{sub 2}), acid deposition control, and urban smog abatement. Technologies utilizing either heterogeneous or homogeneous reactions of NOx with ammonia (NH{sub 3}) are considered major control options. Crucial to the use of such technologies is the continuous measurement of NO/NOx and NH{sub 3} in order to access (and control) performance criteria such as NOx conversion efficiency and NH{sub 3} emissions (NH{sub 3} SLIP) .This paper describes a continuous emission sonitoring system for NO, NO{sub 2}, and NH{sub 3} based upon NO chemiluminescence as well as presenting preliminary field data.

  19. Low NOx heavy fuel combustor concept program

    NASA Technical Reports Server (NTRS)

    White, D. J.; Lecren, R. T.; Batakis, A. P.

    1981-01-01

    A total of twelve low NOx combustor configurations, embodying three different combustion concepts, were designed and fabricated as modular units. These configurations were evaluated experimentally for exhaust emission levels and for mechanical integrity. Emissions data were obtained in depth on two of the configurations.

  20. NOx Emission Reduction by Oscillating Combustion

    SciTech Connect

    2005-09-01

    This project focuses on a new technology that reduces NOx emissions while increasing furnace efficiency for both air- and oxygen-fired furnaces. Oscillating combustion is a retrofit technology that involves the forced oscillation of the fuel flow rate to a furnace. These oscillations create successive, fuel-rich and fuel-lean zones within the furnace.

  1. 1989 SYMPOSIUM ON STATIONARY COMBUSTION NOX CONTROL

    EPA Science Inventory

    This paper summarizes information and results presented at the 1989 Symposium on Stationary Combustion NOX Control, held March 6-9, 1989 in San Francisco. Cosponsored by the Electric Power Research Institute (EPRI) and the U.S. Environmental Protection Agency (EPA), the symposiu...

  2. NOX ENZYMES IN ALLERGIC AIRWAY INFLAMMATION

    PubMed Central

    van der Vliet, Albert

    2011-01-01

    Chronic airway diseases such as asthma are linked to oxidative environmental factors and are commonly associated with increased production of reactive oxygen species (ROS). Therefore, it is commonly assumed that oxidative stress is an important contributing factor to asthma disease pathogenesis and that antioxidant strategies may be useful in treatment of asthma. A primary source of ROS production in biological systems is NADPH oxidase (NOX), originally associated primarily with inflammatory cells but currently widely appreciated as an important enzyme system in many cell types, which a wide array of functional properties ranging from antimicrobial host defense to immune regulation and cell proliferation, differentiation and apoptosis. Given the complex nature of asthma disease pathology, with the involvement of many lung cell types that all express NOX homologs, it is not surprising that the contributions of NOX-derived ROS to various aspects of asthma development and progression are highly diverse and multifactorial. It is the purpose of the present review to summarize the current knowledge with respect to the functional aspects of NOX enzymes in various pulmonary cell types, and to discuss their potential importance in asthma pathogenesis. PMID:21397663

  3. Ras and Nox: linked signaling networks?

    PubMed Central

    Wu, Ru Feng; Terada, Lance S.

    2009-01-01

    Both Ras and Nox represent ancient gene families which control a broad range of cellular responses. Both families mediate signals governing motility, differentiation, and proliferation, and both inhabit overlapping subcellular microdomains. Yet little is known of the precise functional relationship between these two ubiquitous families. In this review, we examine the interface where these two large fields meet. PMID:19501154

  4. 40 CFR 96.10 - Authorization and responsibilities of the NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Authorized Account Representative for NOX Budget...) Except as provided under § 96.11, each NOX Budget source, including all NOX Budget units at the...

  5. 40 CFR 96.10 - Authorization and responsibilities of the NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS NOX Authorized Account Representative for NOX Budget...) Except as provided under § 96.11, each NOX Budget source, including all NOX Budget units at the...

  6. Preparation of Mn-Based Selective Catalytic Reduction Catalysts by Three Methods and Optimization of Process Conditions

    PubMed Central

    Xing, Yi; Hong, Chen; Cheng, Bei; Zhang, Kun

    2013-01-01

    Mn-based catalysts enable high NOx conversion in the selective catalytic reduction of NOx with NH3. Three catalyst-production methods, namely, co-precipitation, impregnation, and sol-gel, were used in this study to determine the optimum method and parameters. The maximum catalytic activity was found for the catalyst prepared by sol-gel with a 0.5 Mn/Ti ratio. The denitrification efficiency using this catalyst was >90%, which was higher than those of catalysts prepared by the two other methods. The critical temperature of catalytic activity was 353 K. The optimum manganese acetate concentration and weathering time were 0.10 mol and 24 h, respectively. The gas hourly space velocity and O2 concentration were determined to be 12000 h-1 and 3%, respectively. PMID:24023841

  7. NOx Sensor for Direct Injection Emission Control

    SciTech Connect

    Betteridge, William J

    2006-02-28

    The Electricore/Delphi team continues to leverage the electrochemical planar sensor technology that has produced stoichiometric planar and wide range oxygen sensors as the basis for development of a NOx sensor. Zirconia cell technology with an integrated heater will provide the foundation for the sensor structure. Proven materials and packaging technology will help to ensure a cost-effective approach to the manufacture of this sensor. The electronics technique and interface is considered to be an area where new strategies need to be employed to produce higher S/N ratios of the NOx signal with emphasis on signal stability over time for robustness and durability Both continuous mode and pulse mode control techniques are being evaluated. Packaging the electronics requires careful design and circuit partitioning so that only the necessary signal conditioning electronics are coupled directly in the wiring harness, while the remainder is situated within the ECM for durability and costs reasons. This task continues to be on hold due to the limitation that the definition of the interface electronics was unavailable until very late in the project. The sense element is based on the amperometric method utilizing integrated alumina and zirconia ceramics. Precious metal electrodes are used to form the integrated heater, the cell electrodes and leads. Inside the actual sense cell structure, it is first necessary to separate NOx from the remaining oxygen constituents of the exhaust, without reducing the NOx. Once separated, the NOx will be measured using a measurement cell. Development or test coupons have been used to facilitate material selection and refinement, cell, diffusion barrier, and chamber development. The sense element currently requires elaborate interconnections. To facilitate a robust durable connection, mechanical and metallurgical connections are under investigation. Materials and process refinements continue to play an important role in the development of the

  8. A novel co-precipitation method for preparation of Mn--Ce/TiO2 composites for NOx reduction with NH3 at low temperature.

    PubMed

    Sheng, Zhongyi; Hu, Yufeng; Xue, Jianming; Wang, Xiaoming; Liao, Weiping

    2012-01-01

    Mn--Ce/TiO2 catalyst prepared by a novel co-precipitation method was used in this study for low-temperature selective catalytic reduction (SCR) of NOx with ammonia. The catalyst showed high activity and good SO2 resistance. The NO conversion on the catalyst increased to 100% when 700 ppm of SO2 flowed in, and reached 60.8% in 2.5 h. The characterized results indicated that the catalyst prepared by the new method had good dispersion of the active phase, uniform micro-size particles and large Brunauer-Emmett-Teller surface. The temperature programmed reduction and temperature programmed desorption experiments showed that the improvement in SCR activity on the Mn--Ce/TiO2 catalyst might be due to the increase of active oxygen species and the enhancement of NH3 chemisorption, both of which were conducive to NH3 activation.

  9. 40 CFR 97.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 97.388 Section 97.388 Protection of Environment... approved by the Administrator: (1) For each control period in 2009 through 2014 for which the CAIR NOX...

  10. 40 CFR 96.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season 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 Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 96.388 Section 96.388 Protection of Environment... SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Ozone Season Opt-in Units § 96.388...

  11. 40 CFR 96.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 96.388 Section 96.388 Protection of Environment... SO 2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Ozone Season Opt-in Units § 96.388...

  12. 40 CFR 96.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 96.388 Section 96.388 Protection of Environment... SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Ozone Season Opt-in Units § 96.388...

  13. 40 CFR 96.388 - CAIR NOX Ozone Season allowance allocations to CAIR NOX Ozone Season 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 Ozone Season allowance allocations to CAIR NOX Ozone Season opt-in units. 96.388 Section 96.388 Protection of Environment... SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Ozone Season Opt-in Units § 96.388...

  14. NOX1 and NOX4 are required for the differentiation of mouse F9 cells into extraembryonic endoderm

    PubMed Central

    Spice, Danielle M.

    2017-01-01

    Mouse F9 cells differentiate to primitive endoderm (PrE) when treated with retinoic acid (RA). Differentiation is accompanied by increased reactive oxygen species (ROS) levels, and while treating F9 cells with antioxidants attenuates differentiation, H2O2 treatment alone is sufficient to induce PrE. We identified the NADPH oxidase (NOX) complexes as candidates for the source of this endogenous ROS, and within this gene family, and over the course of differentiation, Nox1 and Nox 4 show the greatest upregulation induced by RA. Gata6, encoding a master regulator of extraembryonic endoderm is also up-regulated by RA and we provide evidence that NOX1 and NOX4 protein levels increase in F9 cells overexpressing Gata6. Pan-NOX and NOX1-specific inhibitors significantly reduced the ability of RA to induce PrE, and this was recapitulated using a genetic approach to knockdown Nox1 and/or Nox4 transcripts. Interestingly, overexpressing either gene in untreated F9 cells did not induce differentiation, even though each elevated ROS levels. Thus, the data suggests that ROS produced during PrE differentiation is dependent in part on increased NOX1 and NOX4 levels, which is under the control of GATA6. Furthermore, these results suggest that the combined activity of multiple NOX proteins is necessary for the differentiation of F9 cells to primitive endoderm. PMID:28152080

  15. Expression of Nox genes in rat organs, mouse oocytes, and sea urchin eggs.

    PubMed

    Maru, Yoshiro; Nishino, Takeshi; Kakinuma, Katsuko

    2005-04-01

    Degenerate primers were designed to isolate new homologs of Nox family genes in rat organs and sea urchin eggs. The primers were capable of amplifying Nox1, Nox2, Nox3, Nox4, Duox1 and Duox2 but not Nox5, and failed to isolate novel homologs in rat. However, a novel homolog (named as Nox-U1) was identified in sea urchin eggs. In the most conserved region (amino acid 336--417 in human Nox2) Nox-U1 has the highest identity with Nox2, which appears to be abundant in mouse oocytes. However, phylogenetic analysis of the entire sequence has revealed that Nox-U1 is closer to Nox4 or Nox5 than Nox2 or Nox3. Histidine residues assumed to be responsible for heme ligation, motifs for FAD- and NADPH-binding, and two asparagine-linked glycosylation sites are conserved.

  16. Effect of metal ions doping (M = Ti4+, Sn4+) on the catalytic performance of MnOx/CeO2 catalyst for low temperature selective catalytic reduction of NO with NH3

    NASA Astrophysics Data System (ADS)

    Xiong, Yan; Tang, Changjin; Dong, Lin

    2015-04-01

    Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, PR China The abatement of nitrogen oxides (NOx) emission from exhaust gases of diesel and stationary sources is a significant challenge for economic and social development. Ceria-based solid solutions were synthesized and used as supports to prepare MnOx/Ce0.8Ti0.2O2 and MnOx/Ce0.8Sn0.2O2 catalysts (Mn/CeTi and Mn/CeSn) for low temperature selective catalytic reduction of NO by NH3 (NH3-SCR). The effects of Ti or Sn doping on the catalytic performance of MnOx/CeO2 catalyst were investigated. Experimental results show that doping of Ti or Sn increases the NO removal efficiency of MnOx/CeO2. The NO conversion of Mn/CeTi catalyst is more than 90 % at temperature window of 175 ~ 300 °C under a gas hour space velocity of 60,000 mL.g-1.h-1. Modified catalysts are also found to exhibit greatly improved resistance to sulfur-poisoning. NH3-TPD results suggest that NH3 desorption on the catalysts is observed over a wide temperature range, due to the variability of adsorbed NH3 species with different thermal stabilities. Doping of Ti and Sn into Mn/CeO2 greatly increased the NH3 adsorption ability of the composites which could promote the SCR reaction. Characterization results also indicate that doping of Ti or Sn brings about catalysts with higher BET surface area, enhanced oxygen storage capacity and increased surface acidity.

  17. Possible Catalytic Effects of Ice Particles on the Production of NOx by Lightning Discharges

    NASA Technical Reports Server (NTRS)

    2010-01-01

    One mechanism by which NO(x) is produced in the atmosphere is heating in lightning discharge channels. Since most viable proposed electrification mechanisms involve ice crystals, it is reasonable to assume that lightning discharge channels frequently pass through fields of ice particles of various kinds. We address the question of whether ice crystals may serve as catalysts for the production of NO(x) by lightning discharges. If so, and if the effect is large, it would need to be taken into account in estimates of global NO(x) production by lightning. In this study, we make a series of plausible assumptions about the temperature and concentration of reactant species in the environment of discharges and we postulate a mechanism by which ice crystals are able to adsorb nitrogen atoms. We then compare production rates between uncatalyzed and catalytic reactions at 2000 K, 3000 K, and 4000 K. Catalyzed NO production rates are greater at 2000 K, whereas uncatalyzed production occurs most rapidly at 4000 K. 2010

  18. BIFUNCTIONAL CATALYSTS FOR THE SELECTIVE CATALYTIC REDUCTION OF NO BY HYDROCARBONS

    SciTech Connect

    Neylon, M; Castagnola, M; Kropf, A.; Marshall, C

    2003-08-24

    Novel bifunctional catalysts combining two active phases, typically Cu-ZSM-5 and a modifier, were prepared and tested for the selective catalytic reduction of nitrogen oxides using propylene in order to overcome the hindering effects of water typically seen for single-phase catalysts such as Cu-ZSM-5. The catalysts were made by typical preparation techniques, but parameters could be varied to influence the catalyst. The physical characterization of the materials showed that the modification phase was added strictly to the external surface of the zeolite without hindering any internal surface area. Chemical characterization by temperature programmed reactions, DRIFTS and x-ray absorption spectroscopy indicated strong interaction between the two phases, primarily producing materials that exhibited lower reduction temperatures. Two improvements in NOx reduction activity (1000 ppm NO, 1000 ppm C3H6, 2% O2, 30,000 hr-1 GHSV) were seen for these catalysts compared with Cu- ZSM-5: a lower temperature of maximum NOx conversion activity (as low at 250 C), and an enhancement of activity when water was present in the system. The use of a second phase provides a way to further tune the properties of the catalyst in order to achieve mechanistic conditions necessary to maximize NOx remediation.

  19. ULTRA LOW NOx INTEGRATED SYSTEM FOR NOx EMISSION CONTROL FROM COAL-FIRED BOILERS

    SciTech Connect

    Galen H. Richards; Charles Q. Maney; Richard W. Borio; Robert D. Lewis

    2002-12-30

    ALSTOM Power Inc.'s Power Plant Laboratories, working in concert with ALSTOM Power's Performance Projects Group, has teamed with the U.S. Department of Energy's National Energy Technology Laboratory (DOE NETL) to conduct a comprehensive study to develop/evaluate low-cost, efficient NOx control technologies for retrofit to pulverized coal fired utility boilers. The objective of this project was to develop retrofit NOx control technology to achieve less than 0.15 lb/MMBtu NOx (for bituminous coals) and 0.10 lb/MMBtu NOx (for subbituminous coals) from existing pulverized coal fired utility boilers at a cost which is at least 25% less than SCR technology. Efficient control of NOx is seen as an important, enabling step in keeping coal as a viable part of the national energy mix in this century, and beyond. Presently 57% of U.S. electrical generation is coal based, and the Energy Information Agency projects that coal will maintain a lead in U.S. power generation over all other fuel sources for decades (EIA 1998 Energy Forecast). Yet, coal-based power is being strongly challenged by society's ever-increasing desire for an improved environment and the resultant improvement in health and safety. The needs of the electric-utility industry are to improve environmental performance, while simultaneously improving overall plant economics. This means that emissions control technology is needed with very low capital and operating costs. This project has responded to the industry's need for low NOx emissions by evaluating ideas that can be adapted to present pulverized coal fired systems, be they conventional or low NOx firing systems. The TFS 2000{trademark} firing system has been the ALSTOM Power Inc. commercial offering producing the lowest NOx emission levels. In this project, the TFS 2000{trademark} firing system served as a basis for comparison to other low NOx systems evaluated and was the foundation upon which refinements were made to further improve NOx emissions and

  20. Gaseous nitrous acid (HONO) and nitrogen oxides (NOx) emission from gasoline and diesel vehicles under real-world driving test cycles.

    PubMed

    Trinh, Ha T; Imanishi, Katsuma; Morikawa, Tazuko; Hagino, Hiroyuki; Takenaka, Norimichi

    2017-04-01

    Reactive nitrogen species emission from the exhausts of gasoline and diesel vehicles, including nitrogen oxides (NOx) and nitrous acid (HONO), contributes as a significant source of photochemical oxidant precursors in the ambient air. Multiple laboratory and on-road exhaust measurements have been performed to estimate the NOx emission factors from various vehicles and their contribution to atmospheric pollution. Meanwhile, HONO emission from vehicle exhaust has been under-measured despite the fact that HONO can contribute up to 60% of the total hydroxyl budget during daytime and its formation pathway is not fully understood. A profound traffic-induced HONO to NOx ratio of 0.8%, established by Kurtenbach et al. since 2001, has been widely applied in various simulation studies and possibly linked to under-estimation of HONO mixing ratios and OH radical budget in the morning. The HONO/NOx ratios from direct traffic emission have become debatable when it lacks measurements for direct HONO emission from vehicles upon the fast-changing emission reduction technology. Several recent studies have reported updated values for this ratio. This study has reported the measurement of HONO and NOx emission as well as the estimation of exhaust-induced HONO/NOx ratios from gasoline and diesel vehicles using different chassis dynamometer tests under various real-world driving cycles. For the tested gasoline vehicle, which was equipped with three-way catalyst after-treatment device, HONO/NOx ratios ranged from 0 to 0.95 % with very low average HONO concentrations. For the tested diesel vehicle equipped with diesel particulate active reduction device, HONO/NOx ratios varied from 0.16 to 1.00 %. The HONO/NOx ratios in diesel exhaust were inversely proportional to the average speeds of the tested vehicles. Photolysis of HONO is a dominant source of morning OH radicals. Conventional traffic-induced HONO/NOx ratio of 0.8% has possibly linked to underestimation of the total HONO budget and

  1. Commercial introduction of the Advanced NOxTECH system

    SciTech Connect

    Sudduth, B.C.

    1997-12-31

    NOxTECH is BACT for diesel electric generators. Emissions of NO{sub x} are reduced 95% or more with substantial concurrent reductions in CO, particulates, and ROG`s. No engine modifications or other exhaust aftertreatments can remove all criteria pollutants as effectively as NOxTECH. The NOxTECH system reliably maintains NH{sub 3} slip below 2 ppm. Unlike other emissions controls, NOxTECH does not generate hazardous by-products. The Advanced NOxTECH system reduces the size, weight, and cost for BACT emissions reductions. Based on the operation of a 150 kW prototype, NOxTECH, Inc. is quoting commercial units for diesel electric generators. Advanced NOxTECH equipment costs about half as much as SCR systems, and NO{sub x} reduction can exceed 95% with guarantees for emissions compliance.

  2. Cracking catalyst

    SciTech Connect

    Otterstedt, J. E. A.; Jaras, S. G.; Pudas, R.; Upson, L. L.

    1985-05-07

    A cracking catalyst having good resistance to metal poisoning has at least two particle fractions of different particle sizes, the cracking catalyzing zeolite material being concentrated to the coarser particle size fractions, and the finer particle size fractions being formed from material having relatively lower or no or insignificant cracking catalyzing activity. The particles of the finer particle size fractions have a matrix of kaolin and amorphous alumina--silica and may contain for example, an SO /SUB x/ eliminating additive such as Al/sub 2/O/sub 3/, CaO and/or MgO. The coarser particle size fractions having cracking catalyzing effect have a mean particle size of from 80 to 125 ..mu..m and the finer particle size fractions a mean particle size of from 30 to 75 ..mu..m. The coarser particle size fractions have a zeolite content of at least 20 weight % and may have a zeolite content of up to 100 weight %, the remainder consisting essentially of material which has relatively lower or no or insignificant cracking-catalyzing activity and which consists of kaolin and amorphous alumina-silica. The catalyst mass as a whole may have a zeolite content of up to 50 weight %.

  3. Energy Storage.

    ERIC Educational Resources Information Center

    Eaton, William W.

    Described are technological considerations affecting storage of energy, particularly electrical energy. The background and present status of energy storage by batteries, water storage, compressed air storage, flywheels, magnetic storage, hydrogen storage, and thermal storage are discussed followed by a review of development trends. Included are…

  4. Energy Storage.

    ERIC Educational Resources Information Center

    Eaton, William W.

    Described are technological considerations affecting storage of energy, particularly electrical energy. The background and present status of energy storage by batteries, water storage, compressed air storage, flywheels, magnetic storage, hydrogen storage, and thermal storage are discussed followed by a review of development trends. Included are…

  5. Reformer assisted lean NO.sub.x catalyst aftertreatment system and method

    DOEpatents

    Kalyanaraman, Mohan [Media, PA; Park, Paul W [Peoria, IL; Ragle, Christie S [Havana, IL

    2010-06-29

    A method and apparatus for catalytically processing a gas stream passing therethrough to reduce the presence of NO.sub.x therein, wherein the apparatus includes a first catalyst composed of a silver-containing alumina that is adapted for catalytically processing the gas stream at a first temperature range, a second catalyst composed of a copper-containing zeolite located downstream from the first catalyst, wherein the second catalyst is adapted for catalytically processing the gas stream at a lower second temperature range relative to the first temperature range, a hydrocarbon compound for injection into the gas stream upstream of the first catalyst to provide a reductant, and a reformer for reforming a portion of the hydrocarbon compound into H.sub.2 and/or oxygenated hydrocarbon for injection into the gas stream upstream of the first catalyst. The second catalyst is adapted to facilitate the reaction of reducing NOx into N.sub.2, whereby the intermediates are produced via the first catalyst reacting with NOx and hydrocarbons.

  6. Pesticides, microglial NOX2, and Parkinson's disease.

    PubMed

    Taetzsch, Thomas; Block, Michelle L

    2013-02-01

    Accumulating evidence indicates that pesticide exposure is associated with an increased risk for developing Parkinson's disease (PD). Several pesticides known to damage dopaminergic (DA) neurons, such as paraquat, rotenone, lindane, and dieldrin also demonstrate the ability to activate microglia, the resident innate immune cell in the brain. While each of these environmental toxicants may impact microglia through unique mechanisms, they all appear to converge on a common final pathway of microglial activation: NADPH oxidase 2 (NOX2) activation. This review will detail the role of microglia in selective DA neurotoxicity, highlight what is currently known about the mechanism of microglial NOX2 activation in these key pesticides, and describe the importance for DA neuron survival and PD etiology.

  7. Pesticides, Microglial NOX2, and Parkinson's disease

    PubMed Central

    Taetzsch, Thomas; Block, Michelle L.

    2013-01-01

    Accumulating evidence indicates that pesticide exposure is associated with an increased risk for developing Parkinson's disease (PD). Several pesticides known to damage dopaminergic (DA) neurons, such as paraquat, rotenone, lindane, and dieldrin also demonstrate the ability to activate microglia, the resident innate immune cell in the brain. While each of these environmental toxicants may impact microglia through unique mechanisms, they all appear to converge on a common final pathway of microglial activation: NADPH oxidase 2 (NOX2) activation. This review will detail the role of microglia in selective DA neurotoxicity, highlight what is currently known about the mechanism of microglial NOX2 activation in these key pesticides, and describe the importance for DA neuron survival and PD etiology. PMID:23349115

  8. Nitrogen Oxides (NOx) Primary NAAQS REVIEW: Integrated ...

    EPA Pesticide Factsheets

    The NOx Integrated Review Plan is the first document generated as part of the National Ambient Air Quality Standards (NAAQS) review process. The Plan presents background information, the schedule for the review, the process to be used in conducting the review, and the key policy-relevant science issues that will guide the review. The integrated review plan also discusses the frameworks for the various assessment documents to be prepared by the EPA as part of the review, including an Integrated Science Assessment (ISA), and as warranted, a Risk/Exposure Assessment (REA), and a Policy Assessment (PA). The primary purpose of the NOx Integrated Review Plan is to highlight the key policy-relevant issues to be considered in the Review of the NO2 primary NAAQS. A draft of the integrated review plan will be the subject of an advisory review with the Clean Air Scientific Advisory Committee (CASAC) and made available to the public for review and comment.

  9. In-use NOx emissions from diesel and liquefied natural gas refuse trucks equipped with SCR and TWC respectively.

    PubMed

    Misra, Chandan; Ruehl, Chris; Collins, John Francis; Chernich, Don; Herner, Jorn

    2017-02-07

    The California Air Resources Board (ARB) and the City of Sacramento undertook this study to characterize the in-use emissions from model year (MY) 2010 or newer diesel, liquefied natural gas (LNG) and hydraulic hybrid diesel engines during real-world refuse truck operation. Emissions from five trucks: two diesels equipped with selective catalytic reduction (SCR), two LNG's equipped with three-way catalyst (TWC) and one hydraulic hybrid diesel equipped with SCR were measured using a portable emissions measurement system (PEMS) in the Sacramento area. Results showed that the brake-specific NOx emissions for the LNG trucks equipped with the TWC catalyst were lowest of all the technologies tested. Results also showed that the brake specific NOx emissions from the conventional diesel engines were significantly higher despite the exhaust temperature being high enough for proper SCR function. Like diesel engines, the brake specific NOx emissions from the hydraulic hybrid diesel also exceeded certification although this can be explained on the basis of the temperature profile. Future studies are warranted to establish whether the below average SCR performance observed in this study is a systemic issue or is it a problem specifically observed during this work.

  10. Promotional mechanism of propane on selective catalytic reduction of NOx by methane over In/H-BEA at low temperature

    NASA Astrophysics Data System (ADS)

    Pan, Hua; Jian, Yanfei; Yu, Yanke; Chen, Ningna; He, Chi; He, Cheng

    2016-12-01

    Effects of propane/methane ratios on NOx reduction by mixtures of methane and propane over In/H-BEA catalyst were investigated at temperatures ranging from 250 to 550 °C. The higher catalytic activity of In/H-BEA was exhibited for CH4-SCR at high temperatures above 450 °C, while the higher NOx conversion was achieved in C3H8-SCR at below 425 °C. A broadened temperature window and enhanced CO2 selectivity were achieved by combining of methane and propane as the co-reductant. The mixtures with propane/methane of 1/2 showed the most superior T50 (325 °C) and T90 (500 °C) temperatures for NOx reduction over In/H-BEA catalyst. For the promotion mechanism of propane on NO reduction by methane at low temperature, the formation of carbonaceous species (e.g. R-COOH) were enhanced by the activation of C3H8 on Brønsted acid sites at low temperature, and further promoted the generation of sbnd NCO species, which was a crucial determining step for NO reduction.

  11. Some theoretical results concerning O3-NOx-VOC chemistry and NOx-VOC indicators

    NASA Astrophysics Data System (ADS)

    Sillman, Sanford; He, Dongyang

    2002-11-01

    A series of model results is shown pertaining to ozone, reactive nitrogen (NOy), and peroxides in polluted regions. The results focus on ratios such as O3/NOy and H2O2/HNO3 that have been proposed as indicators for O3-NOx-VOC sensitivity. These ratios are shown to correlate with predicted NOx-VOC sensitivity for a variety of zero-dimensional (0-D) and 3-D models, but the correlation varies in situations ranging from relatively clean to highly polluted. The previously identified NOx-VOC transition values for indicators appear to be valid for moderately polluted conditions with 80-150 ppb O3. Changes in indicator behavior are linked to odd hydrogen chemistry and in particular to changes in the ratio of O3 to primary radical production. Changes in indicator behavior are also correlated with the values of a test ratio, O3/(2H2O2+NOz) which can be evaluated against measurements. Ratios of the form ΔO3/ΔNOy, representing differences relative to background values, are proposed for analyzing NOx-VOC sensitivity in individual urban plumes. Comparisons are made to extent-of-reaction parameters, which have been proposed for evaluating NOx-VOC sensitivity.

  12. PVN adenovirus-siRNA injections silencing either NOX2 or NOX4 attenuate aldosterone/NaCl-induced hypertension in mice.

    PubMed

    Xue, Baojian; Beltz, Terry G; Johnson, Ralph F; Guo, Fang; Hay, Meredith; Johnson, Alan Kim

    2012-02-01

    Mineralocorticoid excess increases superoxide production by activating NADPH oxidase (NOX), and intracerebroventricular infusions of NADPH oxidase inhibitors attenuate aldosterone (Aldo)/salt-induced hypertension. It has been hypothesized that increased reactive oxygen species (ROS) in the brain may be a key mechanism in the development of hypertension. The present study investigated the brain regional specificity of NADPH oxidase and the role of NOX2 and NOX4 NADPH oxidase subunits in the hypothalamic paraventricular nucleus (PVN) in Aldo/salt-induced hypertension. PVN injections of adenoviral vectors expressing small interfering (si)RNA targeting NOX2 (AdsiRNA-NOX2) or NOX4 (AdsiRNA-NOX4) mRNAs were used to knock down NOX2 and NOX4 proteins. Three days later, delivery of Aldo (0.2 mg·kg(-1)·day(-1) sc) via osmotic pump commenced and 1% NaCl was provided in place of water. PVN injections of either AdsiRNA-NOX2 or AdsiRNA-NOX4 significantly attenuated the development of Aldo/NaCl-induced hypertension. In an additional study, Aldo/salt-induced hypertension was also significantly attenuated in NOX2 (genomic) knockout mice compared with wild-type controls. When animals from both functional studies underwent ganglionic blockade, there was a reduced fall in blood pressure in the NOX2 and NOX4 knockdown/knockout mice. Western blot analyses of the PVN of siRNA-NOX2- or siRNA-NOX4-injected mice confirmed a marked reduction in the expression of NOX2 or NOX4 protein. In cultured PVN neurons, silencing either NOX2 or NOX4 protein production by culturing PVN cells with siRNA-NOX2 or siRNA-NOX4 attenuated Aldo-induced ROS. These data indicate that both NOX2 and NOX4 in the PVN contribute to elevated sympathetic activity and the hypertensivogenic actions induced by mineralocorticoid excess.

  13. Amorphous molybdenum sulfides as hydrogen evolution catalysts.

    PubMed

    Morales-Guio, Carlos G; Hu, Xile

    2014-08-19

    Providing energy for a population projected to reach 9 billion people within the middle of this century is one of the most pressing societal issues. Burning fossil fuels at a rate and scale that satisfy our near-term demand will irreversibly damage the living environment. Among the various sources of alternative and CO2-emission-free energies, the sun is the only source that is capable of providing enough energy for the whole world. Sunlight energy, however, is intermittent and requires an efficient storage mechanism. Sunlight-driven water splitting to make hydrogen is widely considered as one of the most attractive methods for solar energy storage. Water splitting needs a hydrogen evolution catalyst to accelerate the rate of hydrogen production and to lower the energy loss in this process. Precious metals such as Pt are superior catalysts, but they are too expensive and scarce for large-scale applications. In this Account, we summarize our recent research on the preparation, characterization, and application of amorphous molybdenum sulfide catalysts for the hydrogen evolution reaction. The catalysts can be synthesized by electrochemical deposition under ambient conditions from readily available and inexpensive precursors. The catalytic activity is among the highest for nonprecious catalysts. For example, at a loading of 0.2 mg/cm(2), the optimal catalyst delivers a current density of 10 mA/cm(2) at an overpotential of 160 mV. The growth mechanism of the electrochemically deposited film catalysts was revealed by an electrochemical quartz microcrystal balance study. While different electrochemical deposition methods produce films with different initial compositions, the active catalysts are the same and are identified as a "MoS(2+x)" species. The activity of the film catalysts can be further promoted by divalent Fe, Co, and Ni ions, and the origins of the promotional effects have been probed. Highly active amorphous molybdenum sulfide particles can also be prepared

  14. The NADPH oxidase Nox4 has anti-atherosclerotic functions

    PubMed Central

    Schürmann, Christoph; Rezende, Flavia; Kruse, Christoph; Yasar, Yakub; Löwe, Oliver; Fork, Christian; van de Sluis, Bart; Bremer, Rolf; Weissmann, Norbert; Shah, Ajay M.; Jo, Hanjoong; Brandes, Ralf P.; Schröder, Katrin

    2015-01-01

    Aims Oxidative stress is thought to be a risk for cardiovascular disease and NADPH oxidases of the Nox family are important producers of reactive oxygen species. Within the Nox family, the NADPH oxidase Nox4 has a unique position as it is constitutively active and produces H2O2 rather than O2− . Nox4 is therefore incapable of scavenging NO and its low constitutive H2O2 production might even be beneficial. We hypothesized that Nox4 acts as an endogenous anti-atherosclerotic enzyme. Methods and results Tamoxifen-induced Nox4-knockout mice were crossed with ApoE−/− mice and spontaneous atherosclerosis under regular chow as well as accelerated atherosclerosis in response to partial carotid artery ligation under high-fat diet were determined. Deletion of Nox4 resulted in increased atherosclerosis formation in both models. Mechanistically, pro-atherosclerotic and pro-inflammatory changes in gene expression were observed prior to plaque development. Moreover, inhibition of Nox4 or deletion of the enzyme in the endothelium but not in macrophages resulted in increased adhesion of macrophages to the endothelial surface. Conclusions The H2O2-producing NADPH oxidase Nox4 is an endogenous anti-atherosclerotic enzyme. Nox4 inhibitors, currently under clinical evaluation, should be carefully monitored for cardiovascular side-effects. PMID:26385958

  15. Carbon-based metal-free catalysts

    NASA Astrophysics Data System (ADS)

    Liu, Xien; Dai, Liming

    2016-11-01

    Metals and metal oxides are widely used as catalysts for materials production, clean energy generation and storage, and many other important industrial processes. However, metal-based catalysts suffer from high cost, low selectivity, poor durability, susceptibility to gas poisoning and have a detrimental environmental impact. In 2009, a new class of catalyst based on earth-abundant carbon materials was discovered as an efficient, low-cost, metal-free alternative to platinum for oxygen reduction in fuel cells. Since then, tremendous progress has been made, and carbon-based metal-free catalysts have been demonstrated to be effective for an increasing number of catalytic processes. This Review provides a critical overview of this rapidly developing field, including the molecular design of efficient carbon-based metal-free catalysts, with special emphasis on heteroatom-doped carbon nanotubes and graphene. We also discuss recent advances in the development of carbon-based metal-free catalysts for clean energy conversion and storage, environmental protection and important industrial production, and outline the key challenges and future opportunities in this exciting field.

  16. Role of Nox2 in diabetic kidney disease

    PubMed Central

    You, Young-Hyun; Okada, Shinichi; Ly, San; Jandeleit-Dahm, Karin; Barit, David; Namikoshi, Tamehachi

    2013-01-01

    NADPH oxidase (Nox) isoforms have been implicated in contributing to diabetic microvascular complications, but the functional role of individual isoforms in diabetic kidney are unclear. Nox2, in particular, is highly expressed in phagocytes and may play a key inflammatory role in diabetic kidney disease. To determine the role of Nox2, we evaluated kidney function and pathology in wild-type (WT; C57BL/6) and Nox2 knockout (KO) mice with type 1 diabetes. Diabetes was induced in male Nox2 KO and WT mice with a multiple low-dose streptozotocin protocol. Groups were studied for kidney disease after 8 and 20 wk of diabetes. Hyperglycemia and body weights were similar in WT and Nox2 KO diabetic mice. All functional and structural features of early and later stage diabetic kidney disease (albuminuria, mesangial matrix, tubulointerstitial disease, and gene expression of matrix and transforming growth factor-β) were similar in both diabetic groups compared with their respective nondiabetic groups, except for reduction of macrophage infiltration and monocyte chemoattractant protein-1 in the diabetic Nox2 KO mice. Systolic blood pressure by telemetry was surprisingly increased in Nox2 KO mice; however, the systolic blood pressure was reduced in the diabetic WT and Nox2 KO mice by tail-cuff. Interestingly, diabetic Nox2 KO mice had marked upregulation of renal Nox4 at both the glomerular and cortical levels. The present results demonstrate that lack of Nox2 does not protect against diabetic kidney disease in type 1 diabetes, despite a reduction in macrophage infiltration. The lack of renoprotection may be due to upregulation of renal Nox4. PMID:23389458

  17. Integrated diesel engine NOx reduction technology development

    SciTech Connect

    Hoelzer, J.; Zhu, J.; Savonen, C.L.; Kharas, K.C.C.; Bailey, O.H.; Miller, M.; Vuichard, J.

    1997-12-31

    The effectiveness of catalyst performance is a function of the inlet exhaust gas temperature, gas flow rate, concentration of NO{sub x} and oxygen, and reductant quantity and species. Given this interrelationship, it becomes immediately clear that an integrated development approach is necessary. Such an approach is taken in this project. As such, the system development path is directed by an engine-catalyst engineering team. Of the tools at the engine engineer`s disposal the real-time aspects of computer assisted subsystem modeling is valuable. It will continue to be the case as ever more subtle improvements are needed to meet competitive performance, durability, and emission challenges. A review of recent prototype engines has shown that considerable improvements to base diesel engine technology are being made. For example, HSDI NO{sub x} has been reduced by a factor of two within the past ten years. However, additional substantial NO{sub x}/PM reduction is still required for the future. A viable lean NO{sub x} catalyst would be an attractive solution to this end. The results of recent high and low temperature catalyst developments were presented. High temperature base metal catalysts have been formulated to produce very good conversion efficiency and good thermal stability, albeit at temperatures near the upper range of diesel engine operation. Low temperature noble metal catalysts have been developed to provide performance of promising 4-way control but need increased NO{sub x} reduction efficiency.

  18. Application of solid ash based catalysts in heterogeneous catalysis

    SciTech Connect

    Shaobin Wang

    2008-10-01

    Solid wastes, fly ash, and bottom ash are generated from coal and biomass combustion. Fly ash is mainly composed of various metal oxides and possesses higher thermal stability. Utilization of fly ash for other industrial applications provides a cost-effective and environmentally friendly way of recycling this solid waste, significantly reducing its environmental effects. On the one hand, due to the higher stability of its major component, aluminosilicates, fly ash could be employed as catalyst support by impregnation of other active components for various reactions. On the other hand, other chemical compounds in fly ash such as Fe{sub 2}O{sub 3} could also provide an active component making fly ash a catalyst for some reactions. In this paper, physicochemical properties of fly ash and its applications for heterogeneous catalysis as a catalyst support or catalyst in a variety of catalytic reactions were reviewed. Fly-ash-supported catalysts have shown good catalytic activities for H{sub 2} production, deSOx, deNOx, hydrocarbon oxidation, and hydrocracking, which are comparable to commercially used catalysts. As a catalyst itself, fly ash can also be effective for gas-phase oxidation of volatile organic compounds, aqueous-phase oxidation of organics, solid plastic pyrolysis, and solvent-free organic synthesis. 107 refs., 4 figs., 2 tabs.

  19. The role of Nox1 and Nox2 in GPVI-dependent platelet activation and thrombus formation☆

    PubMed Central

    Walsh, T.G.; Berndt, M.C.; Carrim, N.; Cowman, J.; Kenny, D.; Metharom, P.

    2014-01-01

    Background Activation of the platelet-specific collagen receptor, glycoprotein (GP) VI, induces intracellular reactive oxygen species (ROS) production; however the relevance of ROS to GPVI-mediated platelet responses remains unclear. Objective The objective of this study was to explore the role of the ROS-producing NADPH oxidase (Nox)1 and 2 complexes in GPVI-dependent platelet activation and collagen-induced thrombus formation. Methods and results ROS production was measured by quantitating changes in the oxidation-sensitive dye, H2DCF-DA, following platelet activation with the GPVI-specific agonist, collagen related peptide (CRP). Using a pharmacological inhibitor specific for Nox1, 2-acetylphenothiazine (ML171), and Nox2 deficient mice, we show that Nox1 is the key Nox homolog regulating GPVI-dependent ROS production. Nox1, but not Nox2, was essential for CRP-dependent thromboxane (Tx)A2 production, which was mediated in part through p38 MAPK signaling; while neither Nox1 nor Nox2 was significantly involved in regulating CRP-induced platelet aggregation/integrin αIIbβ3 activation, platelet spreading, or dense granule and α-granule release (ATP release and P-selectin surface expression, respectively). Ex-vivo perfusion analysis of mouse whole blood revealed that both Nox1 and Nox2 were involved in collagen-mediated thrombus formation at arterial shear. Conclusion Together these results demonstrate a novel role for Nox1 in regulating GPVI-induced ROS production, which is essential for optimal p38 activation and subsequent TxA2 production, providing an explanation for reduced thrombus formation following Nox1 inhibition. PMID:24494191

  20. Electrochemical catalyst recovery method

    DOEpatents

    Silva, Laura J.; Bray, Lane A.

    1995-01-01

    A method of recovering catalyst material from latent catalyst material solids includes: a) combining latent catalyst material solids with a liquid acid anolyte solution and a redox material which is soluble in the acid anolyte solution to form a mixture; b) electrochemically oxidizing the redox material within the mixture into a dissolved oxidant, the oxidant having a potential for oxidation which is effectively higher than that of the latent catalyst material; c) reacting the oxidant with the latent catalyst material to oxidize the latent catalyst material into at least one oxidized catalyst species which is soluble within the mixture and to reduce the oxidant back into dissolved redox material; and d) recovering catalyst material from the oxidized catalyst species of the mixture. The invention is expected to be particularly useful in recovering spent catalyst material from petroleum hydroprocessing reaction waste products having adhered sulfides, carbon, hydrocarbons, and undesired metals, and as well as in other industrial applications.

  1. Electrochemical catalyst recovery method

    DOEpatents

    Silva, L.J.; Bray, L.A.

    1995-05-30

    A method of recovering catalyst material from latent catalyst material solids includes: (a) combining latent catalyst material solids with a liquid acid anolyte solution and a redox material which is soluble in the acid anolyte solution to form a mixture; (b) electrochemically oxidizing the redox material within the mixture into a dissolved oxidant, the oxidant having a potential for oxidation which is effectively higher than that of the latent catalyst material; (c) reacting the oxidant with the latent catalyst material to oxidize the latent catalyst material into at least one oxidized catalyst species which is soluble within the mixture and to reduce the oxidant back into dissolved redox material; and (d) recovering catalyst material from the oxidized catalyst species of the mixture. The invention is expected to be particularly useful in recovering spent catalyst material from petroleum hydroprocessing reaction waste products having adhered sulfides, carbon, hydrocarbons, and undesired metals, and as well as in other industrial applications. 3 figs.

  2. Nox4 Is Dispensable for Exercise Induced Muscle Fibre Switch

    PubMed Central

    Vogel, Juri; Figueiredo de Rezende, Flávia; Rohrbach, Susanne; Zhang, Min; Schröder, Katrin

    2015-01-01

    Introduction By producing H2O2, the NADPH oxidase Nox4 is involved in differentiation of mesenchymal cells. Exercise alters the composition of slow and fast twitch fibres in skeletal. Here we hypothesized that Nox4 contributes to exercise-induced adaptation such as changes in muscle metabolism or muscle fibre specification and studied this in wildtype and Nox4-/- mice. Results Exercise, as induced by voluntary running in a running wheel or forced running on a treadmill induced a switch from fast twitch to intermediate fibres. However the induced muscle fibre switch was similar between Nox4-/- and wildtype mice. The same held true for exercise-induced expression of PGC1α or AMPK activation. Both are increased in response to exercise, but with no difference was observed between wildtype and Nox4-/- mice. Conclusion Thus, exercise-induced muscle fibre switch is Nox4-independent. PMID:26083642

  3. Long-Life Catalyst

    NASA Technical Reports Server (NTRS)

    1999-01-01

    STC Catalysts, Inc. (SCi) manufactures a noble metal reducible oxide catalyst consisting primarily of platinum and tin dioxide deposited on a ceramic substrate. It is an ambient temperature oxidation catalyst that was developed primarily for Carbon Dioxide Lasers.The catalyst was developed by the NASA Langley Research Center for the Laser Atmospheric Wind Sounder Program (LAWS) which was intended to measure wind velocity on a global basis. There are a number of NASA owned patents covering various aspects of the catalyst.

  4. Investigation into the effects of vermiculite on NOx reduction and additives on sooting and exhaust infrared signature from a gas-turbine combustor. Master's thesis

    SciTech Connect

    Engel, K.R.

    1990-09-01

    An experimental investigation was conducted to determine the feasibility of using catalytic reduction of NOX emissions from a typical jet engine combustor in the test cell environment. A modified T-63 combustor in combination with an instrumented 21 foot augmentation tube containing a vermiculite catalyst was used. Several methods for containing the vermiculite were attempted. Both vermiculite and vermiculite which had been coated with thiourea were used. Up to 19% reduction in NOX concentrations was obtained using the vermiculite coated with thiourea, however the pressure loss across the catalyst bed was measured to be 36 in. H2O. The techniques used proved ineffective and unacceptable for gas turbine engine test cell applications. Tests were conducted using both Wynn's 15/590 and Catane TM (ferrocene) fuel supplements in order to determine their effectiveness for soot reduction and whether or not the exhaust plume could be changed.

  5. 40 CFR 89.317 - NOX converter check.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ...) Turn on the NOX generator O2 (or air) supply and adjust the O2 (or air) flow rate so that the NO... the concentration of NO in this NO+O2 mixture. (h) Switch the NOX generator to the generation mode and... of nitrogen analyzer will indicate the NOX in the NO+O2 mixture. Record this value. (k) Turn off the...

  6. 40 CFR 89.317 - NOX converter check.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ...) Turn on the NOX generator O2 (or air) supply and adjust the O2 (or air) flow rate so that the NO... the concentration of NO in this NO+O2 mixture. (h) Switch the NOX generator to the generation mode and... of nitrogen analyzer will indicate the NOX in the NO+O2 mixture. Record this value. (k) Turn off the...

  7. 40 CFR 89.317 - NOX converter check.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ...) Turn on the NOX generator O2 (or air) supply and adjust the O2 (or air) flow rate so that the NO... the concentration of NO in this NO+O2 mixture. (h) Switch the NOX generator to the generation mode and... of nitrogen analyzer will indicate the NOX in the NO+O2 mixture. Record this value. (k) Turn off the...

  8. Satellite measurements of daily variations in soil NOx emissions

    NASA Astrophysics Data System (ADS)

    Bertram, Timothy H.; Heckel, Andreas; Richter, Andreas; Burrows, John P.; Cohen, Ronald C.

    2005-12-01

    Soil NOx emission from agricultural regions in the western United States has been investigated using satellite observations of NO2 from the SCIAMACHY instrument. We show that the SCIAMACHY observations over a 2 million hectare agricultural region in Montana capture the short intense NOx pulses following fertilizer application and subsequent precipitation and we demonstrate that these variations can be reproduced by tuning the mechanistic parameters in an existing model of soil NOx emissions.

  9. New Insights on NOX Enzymes in the Central Nervous System

    PubMed Central

    Nayernia, Zeynab; Jaquet, Vincent

    2014-01-01

    Abstract Significance: There is increasing evidence that the generation of reactive oxygen species (ROS) in the central nervous system (CNS) involves the NOX family of nicotinamide adenine dinucleotide phosphate oxidases. Controlled ROS generation appears necessary for optimal functioning of the CNS through fine-tuning of redox-sensitive signaling pathways, while overshooting ROS generation will lead to oxidative stress and CNS disease. Recent Advances: NOX enzymes are not only restricted to microglia (i.e. brain phagocytes) but also expressed in neurons, astrocytes, and the neurovascular system. NOX enzymes are involved in CNS development, neural stem cell biology, and the function of mature neurons. While NOX2 appears to be a major source of pathological oxidative stress in the CNS, other NOX isoforms might also be of importance, for example, NOX4 in stroke. Globally speaking, there is now convincing evidence for a role of NOX enzymes in various neurodegenerative diseases, cerebrovascular diseases, and psychosis-related disorders. Critical Issues: The relative importance of specific ROS sources (e.g., NOX enzymes vs. mitochondria; NOX2 vs. NOX4) in different pathological processes needs further investigation. The absence of specific inhibitors limits the possibility to investigate specific therapeutic strategies. The uncritical use of non-specific inhibitors (e.g., apocynin, diphenylene iodonium) and poorly validated antibodies may lead to misleading conclusions. Future Directions: Physiological and pathophysiological studies with cell-type-specific knock-out mice will be necessary to delineate the precise functions of NOX enzymes and their implications in pathomechanisms. The development of CNS-permeant, specific NOX inhibitors will be necessary to advance toward therapeutic applications. Antioxid. Redox Signal. 20: 2815–2837. PMID:24206089

  10. 40 CFR 96.24 - Effective date of initial NOX Budget permit.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Effective date of initial NOX Budget... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.24 Effective date of initial NOX Budget permit. The initial NOX Budget permit...

  11. 40 CFR 97.85 - NOX Budget opt-in 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 opt-in permit contents. 97... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Individual Unit Opt-ins. § 97.85 NOX Budget opt-in permit contents. (a) Each NOX Budget opt-in permit will contain all elements...

  12. 40 CFR 96.21 - Submission of NOX Budget permit applications.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Submission of NOX Budget permit... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.21 Submission of NOX Budget permit applications. (a) Duty to apply. The NOX...

  13. 40 CFR 96.85 - NOX Budget opt-in 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 opt-in permit contents. 96... (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Individual Unit Opt-ins § 96.85 NOX Budget opt-in permit contents. (a) Each NOX Budget opt-in permit...

  14. 40 CFR 97.21 - Submission of NOX Budget permit applications.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false Submission of NOX Budget permit... PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.21 Submission of NOX Budget permit applications. (a) Duty to apply. The NOX authorized account...

  15. 40 CFR 97.186 - Withdrawal from CAIR NOX Annual Trading Program.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false Withdrawal from CAIR NOX Annual... CAIR NOX Opt-In Units § 97.186 Withdrawal from CAIR NOX Annual Trading Program. Except as provided... representative of the CAIR NOX opt-in unit of the acceptance of the withdrawal of the CAIR NOX opt-in unit...

  16. 40 CFR 97.186 - Withdrawal from CAIR NOX Annual Trading Program.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 21 2014-07-01 2014-07-01 false Withdrawal from CAIR NOX Annual... CAIR NOX Opt-In Units § 97.186 Withdrawal from CAIR NOX Annual Trading Program. Except as provided... representative of the CAIR NOX opt-in unit of the acceptance of the withdrawal of the CAIR NOX opt-in unit...

  17. 40 CFR 97.186 - Withdrawal from CAIR NOX Annual Trading Program.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 22 2013-07-01 2013-07-01 false Withdrawal from CAIR NOX Annual... CAIR NOX Opt-In Units § 97.186 Withdrawal from CAIR NOX Annual Trading Program. Except as provided... representative of the CAIR NOX opt-in unit of the acceptance of the withdrawal of the CAIR NOX opt-in unit...

  18. 40 CFR 97.186 - Withdrawal from CAIR NOX Annual Trading Program.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Withdrawal from CAIR NOX Annual... CAIR NOX Opt-In Units § 97.186 Withdrawal from CAIR NOX Annual Trading Program. Except as provided... representative of the CAIR NOX opt-in unit of the acceptance of the withdrawal of the CAIR NOX opt-in unit...

  19. 40 CFR 97.20 - General NOX Budget Trading Program permit requirements.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 20 2010-07-01 2010-07-01 false General NOX Budget Trading Program... (CONTINUED) AIR PROGRAMS (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Permits § 97.20 General NOX Budget Trading Program permit requirements. (a) For each NOX Budget...

  20. 40 CFR 97.85 - NOX Budget opt-in 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 opt-in permit contents. 97... (CONTINUED) FEDERAL NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS Individual Unit Opt-ins. § 97.85 NOX Budget opt-in permit contents. (a) Each NOX Budget opt-in permit will contain all elements...

  1. 40 CFR 96.14 - Objections concerning the NOX authorized account representative.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... AGENCY (CONTINUED) AIR 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... permitting authority or the Administrator under the NOX Budget Trading Program. (c) Neither the...

  2. 40 CFR 96.21 - Submission of NOX Budget permit applications.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.21 Submission of NOX Budget permit applications. (a) Duty to apply. The NOX... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Submission of NOX Budget...

  3. 40 CFR 96.24 - Effective date of initial NOX Budget permit.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.24 Effective date of initial NOX Budget permit. The initial NOX Budget permit... 40 Protection of Environment 21 2011-07-01 2011-07-01 false Effective date of initial NOX...

  4. 40 CFR 96.14 - Objections concerning the NOX authorized account representative.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... AGENCY (CONTINUED) AIR 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... permitting authority or the Administrator under the NOX Budget Trading Program. (c) Neither the...

  5. DeNOx characteristics using two staged radical injection techniques

    SciTech Connect

    Kambara, S.; Kumano, Y.; Yukimura, K.

    2009-06-15

    Ammonia radical injection using pulsed dielectric barrier discharge (DBD) plasma has been investigated as a means to control NOx emissions from combustors. When DBD plasma-generated radicals (NH{sub 2}, NH, N, and H) are injected into a flue gas containing nitrogen oxide (NOx), NOx is removed efficiently by chain reactions in the gas phase. However, because the percentage of NOx removal gradually decreases with increasing oxygen concentrations beyond 1% O{sub 2}, improvement of the DeNOx (removal of nitrogen oxide) characteristics at high O{sub 2} concentrations was necessary for commercial combustors. A two-staged injection of the DeNOx agent was developed based on the detailed mechanisms of electron impact reactions and gas phase reactions. A concentration of H radical was observed to play an important role in NOx formation and removal. The effects of applied voltages, oxygen concentrations, and reaction temperatures on NOx removal were investigated under normal and staged injection. NOx removal was improved by approximately 20% using staged injection at O{sub 2} concentrations of 1 to 4%.

  6. Low NO(x) potential of gas turbine engines

    NASA Technical Reports Server (NTRS)

    Tacina, Robert R.

    1990-01-01

    The purpose is to correlate emission levels of gas turbine engines. The predictions of NO(x) emissions are based on a review of the literature of previous low NO(x) combustor programs and analytical chemical kinetic calculations. Concepts included in the literature review consisted of lean-premixed-prevaporized (LPP), rich burn/quick quench/lean burn (RQL), and direct injection. The NO(x) emissions were found to be an exponential function of adiabatic combustion temperature over a wide range of inlet temperatures, pressures and (lean) fuel-air ratios. A simple correlation of NO(x) formation with time was not found. The LPP and direct injection (using gaseous fuels) concepts have the lowest NO(x) emissions of the three concepts. The RQL data has higher values of NO(x) than the LPP concept, probably due to the stoichiometric temperatures and NO(x) production that occur during the quench step. Improvements in the quick quench step could reduce the NO(x) emissions to the LPP levels. The low NO(x) potential of LPP is offset by the operational disadvantages of its narrow stability limits and its susceptibility to autoignition/flashback. The Rich-Burn/Quick-Quench/Lean-Burn (RQL) and the direct injection concepts have the advantage of wider stability limits comparable to conventional combustors.

  7. System and method for determining an ammonia generation rate in a three-way catalyst

    DOEpatents

    Sun, Min; Perry, Kevin L; Kim, Chang H

    2014-12-30

    A system according to the principles of the present disclosure includes a rate determination module, a storage level determination module, and an air/fuel ratio control module. The rate determination module determines an ammonia generation rate in a three-way catalyst based on a reaction efficiency and a reactant level. The storage level determination module determines an ammonia storage level in a selective catalytic reduction (SCR) catalyst positioned downstream from the three-way catalyst based on the ammonia generation rate. The air/fuel ratio control module controls an air/fuel ratio of an engine based on the ammonia storage level.

  8. Correlation between Cu ion migration behaviour and deNOx activity in Cu-SSZ-13 for the standard NH3-SCR reaction.

    PubMed

    Beale, A M; Lezcano-Gonzalez, I; Slawinksi, W A; Wragg, D S

    2016-05-04

    Here we present the results of a synchrotron-based in situ, time-resolved PXRD study during activation of two Cu-SSZ-13 catalysts under O2/He and one during standard NH3-SCR reaction conditions to obtain insight into the behaviour of Cu ions. The results obtained indicate that deNOx activity is inexorably linked with occupancy of the zeolite 6r.

  9. Analysis of NOx Budget Trading Program Units Brought into the CAIR NOx Ozone Season Trading Program

    EPA Pesticide Factsheets

    EPA analyzed the effect of having the large non-EGU units in the NBP and the CAIR NOX ozone season trading program and evaluated whether or not emissions from this group of units were reduced as a result of their inclusion in those trading programs.

  10. 40 CFR 52.2237 - NOX RACT and NOX conformity exemption.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... PROGRAMS (CONTINUED) APPROVAL AND PROMULGATION OF IMPLEMENTATION PLANS (CONTINUED) Tennessee § 52.2237 NOX... the Tennessee Department of Environment and Conservation on March 21, 1995, for the five county middle Tennessee (Nashville) ozone moderate nonattainment area. This approval exempts the area from implementing...

  11. The selective catalytic reduction of NOx over Ag/Al2O3 with isobutanol as the reductant

    DOE PAGES

    Brookshear, Daniel William; Pihl, Josh A.; Toops, Todd J.; ...

    2016-02-13

    Here, this study investigates the potential of isobutanol (iBuOH) as a reductant for the selective catalytic reduction (SCR) of NOx over 2 wt% Ag/Al2O3 between 150 and 550 °C and gas hourly space velocities (GHSV) between 10,000 and 35,000 h-1. The feed gas consists of 500 ppm NO, 5% H2O, 10% O2, and 375-1500 ppm iBuOH (C1:N ratios of 3-12); additionally, blends of 24 and 48% iBuOH in gasoline are evaluated. Over 90% NOx conversion is achieved between 300 and 400 C using pure iBuOH, including a 40% peak selectivity towards NH3 that could be utilized in a dual HC/NH3more » SCR configuration. The iBuOH/gasoline blends are only able to achieve greater than 90% NOx conversion when operated at a GHSV of 10,000 h-1 and employing a C1:N ratio of 12. Iso-butyraldehyde and NO2 appear to function as intermediates in the iBuOH-SCR mechanism, which mirrors the mechanism observed for EtOH-SCR. In general, the performance of iBuOH in the SCR of NOx over a Ag/Al2O3 catalyst is comparable with that of EtOH, although EtOH/gasoline blends display higher NOx reduction than iBuOH/gasoline blends. The key parameter in employing alcohols in SCR appears to be the C-OH:N ratio rather than the C1:N ratio.« less

  12. REDUCTION OF NOx VIA COAL COMBUSTION CATALYSIS

    SciTech Connect

    George Ford; Stan Harding; Jeff Hare

    2003-04-28

    The primary objective of this investigation is to determine the effect of different iron catalysts on the production of NO{sub x} during fuel-rich and fuel-lean combustion of coal. Iron in various forms and quantities will be introduced with the pulverized coal and tested in a laboratory-scale combustion furnace. The testing protocol is based on simulation of the near burner region in a full-scale boiler. This semi-annual report describes the selection of the iron catalysts used in the program as well as catalyst preparation. A detailed description of the combustion reactor and ancillary equipment is provided combined with a discussion of the test procedures. The first preliminary data have been collected and are presented followed by the plans to complete the project over the next six months.

  13. Deficiency of NOX1 or NOX4 Prevents Liver Inflammation and Fibrosis in Mice through Inhibition of Hepatic Stellate Cell Activation

    PubMed Central

    Lan, Tian; Kisseleva, Tatiana; Brenner, David A.

    2015-01-01

    Reactive oxygen species (ROS) produced by nicotinamide adenine dinucleotide phosphate oxidase (NOX) play a key role in liver injury and fibrosis. Previous studies demonstrated that GKT137831, a dual NOX1/4 inhibitor, attenuated liver fibrosis in mice as well as pro-fibrotic genes in hepatic stellate cells (HSCs) as well as hepatocyte apoptosis. The effect of NOX1 and NOX4 deficiency in liver fibrosis is unclear, and has never been directly compared. HSCs are the primary myofibroblasts in the pathogenesis of liver fibrosis. Therefore, we aimed to determine the role of NOX1 and NOX4 in liver fibrosis, and investigated whether NOX1 and NOX4 signaling mediates liver fibrosis by regulating HSC activation. Mice were treated with carbon tetrachloride (CCl4) to induce liver fibrosis. Deficiency of either NOX1 or NOX4 attenuates liver injury, inflammation, and fibrosis after CCl4 compared to wild-type mice. NOX1 or NOX4 deficiency reduced lipid peroxidation and ROS production in mice with liver fibrosis. NOX1 and NOX4 deficiency are approximately equally effective in preventing liver injury in the mice. The NOX1/4 dual inhibitor GKT137831 suppressed ROS production as well as inflammatory and proliferative genes induced by lipopolysaccharide (LPS), platelet-derived growth factor (PDGF), or sonic hedgehog (Shh) in primary mouse HSCs. Furthermore, the mRNAs of proliferative and pro-fibrotic genes were downregulated in NOX1 and NOX4 knock-out activated HSCs (cultured on plastic for 5 days). Finally, NOX1 and NOX4 protein levels were increased in human livers with cirrhosis compared with normal controls. Thus, NOX1 and NOX4 signaling mediates the pathogenesis of liver fibrosis, including the direct activation of HSC. PMID:26222337

  14. Nox4: A Hydrogen Peroxide-Generating Oxygen Sensor

    PubMed Central

    2015-01-01

    Nox4 is an oddity among members of the Nox family of NADPH oxidases [seven isoenzymes that generate reactive oxygen species (ROS) from molecular oxygen] in that it is constitutively active. All other Nox enzymes except for Nox4 require upstream activators, either calcium or organizer/activator subunits (p47phox, NOXO1/p67phox, and NOXA1). Nox4 may also be unusual as it reportedly releases hydrogen peroxide (H2O2) in contrast to Nox1–Nox3 and Nox5, which release superoxide, although this result is controversial in part because of possible membrane compartmentalization of superoxide, which may prevent detection. Our studies were undertaken (1) to identify the Nox4 ROS product using a membrane-free, partially purified preparation of Nox4 and (2) to test the hypothesis that Nox4 activity is acutely regulated not by activator proteins or calcium, but by cellular pO2, allowing it to function as an O2 sensor, the output of which is signaling H2O2. We find that approximately 90% of the electron flux through isolated Nox4 produces H2O2 and 10% forms superoxide. The kinetic mechanism of H2O2 formation is consistent with a mechanism involving binding of one oxygen molecule, which is then sequentially reduced by the heme in two one-electron reduction steps first to form a bound superoxide intermediate and then H2O2; kinetics are not consistent with a previously proposed internal superoxide dismutation mechanism involving two oxygen binding/reduction steps for each H2O2 formed. Critically, Nox4 has an unusually high Km for oxygen (∼18%), similar to the values of known oxygen-sensing enzymes, compared with a Km of 2–3% for Nox2, the phagocyte NADPH oxidase. This allows Nox4 to generate H2O2 as a function of oxygen concentration throughout a physiological range of pO2 values and to respond rapidly to changes in pO2. PMID:25062272

  15. NOX Activation by Subunit Interaction and Underlying Mechanisms in Disease

    PubMed Central

    Rastogi, Radhika; Geng, Xiaokun; Li, Fengwu; Ding, Yuchuan

    2017-01-01

    Nicotinamide adenine dinucleotide phosphate (NAPDH) oxidase (NOX) is an enzyme complex with the sole function of producing superoxide anion and reactive oxygen species (ROS) at the expense of NADPH. Vital to the immune system as well as cellular signaling, NOX is also involved in the pathologies of a wide variety of disease states. Particularly, it is an integral player in many neurological diseases, including stroke, TBI, and neurodegenerative diseases. Pathologically, NOX produces an excessive amount of ROS that exceed the body’s antioxidant ability to neutralize them, leading to oxidative stress and aberrant signaling. This prevalence makes it an attractive therapeutic target and as such, NOX inhibitors have been studied and developed to counter NOX’s deleterious effects. However, recent studies of NOX have created a better understanding of the NOX complex. Comprised of independent cytosolic subunits, p47-phox, p67-phox, p40-phox and Rac, and membrane subunits, gp91-phox and p22-phox, the NOX complex requires a unique activation process through subunit interaction. Of these subunits, p47-phox plays the most important role in activation, binding and translocating the cytosolic subunits to the membrane and anchoring to p22-phox to organize the complex for NOX activation and function. Moreover, these interactions, particularly that between p47-phox and p22-phox, are dependent on phosphorylation initiated by upstream processes involving protein kinase C (PKC). This review will look at these interactions between subunits and with PKC. It will focus on the interaction involving p47-phox with p22-phox, key in bringing the cytosolic subunits to the membrane. Furthermore, the implication of these interactions as a target for NOX inhibitors such as apocynin will be discussed as a potential avenue for further investigation, in order to develop more specific NOX inhibitors based on the inhibition of NOX assembly and activation. PMID:28119569

  16. NOx emissions in China: historical trends and future perspectives

    NASA Astrophysics Data System (ADS)

    Zhao, B.; Wang, S. X.; Xu, J. Y.; Fu, K.; Klimont, Z.; Hao, J. M.; He, K. B.; Cofala, J.; Amann, M.

    2013-06-01

    Nitrogen oxides (NOx) are key pollutants for the improvement of ambient air quality. Within this study we estimated the historical NOx emissions in China for the period 1995-2010, and calculated future NOx emissions every five years until 2030 under six emission scenarios. Driven by the fast growth of energy consumption, we estimate the NOx emissions in China increased rapidly from 11.0 Mt in 1995 to 26.1 Mt in 2010. Power plants, industry and transportation were major sources of NOx emissions, accounting for 28.4, 34.0, and 25.4% of the total NOx emissions in 2010, respectively. Two energy scenarios, a business as usual scenario (BAU) and an alternative policy scenario (PC), were developed to project future energy consumption. In 2030, total energy consumption is projected to increase by 64 and 27% from 2010 level respectively. Three sets of end-of-pipe pollution control measures, including baseline, progressive, and stringent control case, were developed for each energy scenario, thereby constituting six emission scenarios. By 2030, the total NOx emissions are projected to increase (compared to 2010) by 36% in the baseline while policy cases result in reduction up to 61% in the most ambitious case with stringent control measures. More than a third of the reduction achieved by 2030 between least and most ambitious scenario comes from power sector and more than half is distributed equally between industry and transportation sectors. Selective Catalytic Reduction dominates the NOx emission reductions in power plants, while life style changes, control measures for industrial boilers and cement production are major contributors to reductions in industry. Timely enforcement of legislation on heavy duty vehicles would contribute significantly to NOx emission reductions. About 30% of the NOx emission reduction in 2020, and 40% of the NOx emission reduction in 2030 could be treated as the ancillary benefit of energy conservation. Sensitivity analysis was conducted to

  17. NOx emissions in China: historical trends and future perspectives

    NASA Astrophysics Data System (ADS)

    Zhao, B.; Wang, S. X.; Liu, H.; Xu, J. Y.; Fu, K.; Klimont, Z.; Hao, J. M.; He, K. B.; Cofala, J.; Amann, M.

    2013-10-01

    Nitrogen oxides (NOx) are key pollutants for the improvement of ambient air quality. Within this study we estimated the historical NOx emissions in China for the period 1995-2010, and calculated future NOx emissions every five years until 2030 under six emission scenarios. Driven by the fast growth of energy consumption, we estimate the NOx emissions in China increased rapidly from 11.0 Mt in 1995 to 26.1 Mt in 2010. Power plants, industry and transportation were major sources of NOx emissions, accounting for 28.4%, 34.0%, and 25.4% of the total NOx emissions in 2010, respectively. Two energy scenarios, a business as usual scenario (BAU) and an alternative policy scenario (PC), were developed to project future energy consumption. In 2030, total energy consumption is projected to increase by 64% and 27% from 2010 level respectively. Three sets of end-of-pipe pollution control measures, including baseline, progressive, and stringent control case, were developed for each energy scenario, thereby constituting six emission scenarios. By 2030, the total NOx emissions are projected to increase (compared to 2010) by 36% in the baseline while policy cases result in reduction up to 61% in the most ambitious case with stringent control measures. More than a third of the reduction achieved by 2030 between least and most ambitious scenario comes from power sector, and more than half is distributed equally between industry and transportation sectors. Selective catalytic reduction dominates the NOx emission reductions in power plants, while life style changes, control measures for industrial boilers and cement production are major contributors to reductions in industry. Timely enforcement of legislation on heavy-duty vehicles would contribute significantly to NOx emission reductions. About 30% of the NOx emission reduction in 2020 and 40% of the NOx emission reduction in 2030 could be treated as the ancillary benefit of energy conservation. Sensitivity analysis was conducted to

  18. 40 CFR 96.120 - General CAIR NOX Annual Trading Program permit requirements.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS Permits § 96.120 General CAIR NOX Annual Trading Program...

  19. 40 CFR 96.141 - Timing requirements for CAIR NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Allocations § 96.141 Timing requirements for CAIR...

  20. 40 CFR 96.141 - Timing requirements for CAIR NOX allowance allocations.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... (CONTINUED) AIR PROGRAMS (CONTINUED) NOX BUDGET TRADING PROGRAM AND CAIR NOX AND SO2 TRADING PROGRAMS FOR STATE IMPLEMENTATION PLANS CAIR NOX Allowance Allocations § 96.141 Timing requirements for CAIR...

  1. Tropospheric sources of NOx: lightning and biology

    NASA Technical Reports Server (NTRS)

    Levine, J. S.; Augustsson, T. R.; Anderson, I. C.; Hoell, J. M. Jr

    1984-01-01

    Laboratory experiments to quantify the global production of NOx (NO + NO2) in the troposphere due to atmospheric lightning and biogenic activity in soil are presented. These laboratory experiments, as well as other studies, suggest that the global production of NOx by lightning probably ranges between 2 and 20 MT(N)y-1 of NO and is strongly dependent on the total energy deposited by lightning, a quantity not well-known. In our laboratory experiments, nitrifying micro-organisms is soil were found to be a significant source of both NO and nitrous oxide (N2O). The measured production ratio of NO to N2O averaged 2-3 for oxygen partial pressures of 0.5-10%. Extrapolating these laboratory measurements to the global scale, which is somewhat risky, suggests that nitrifying micro-organisms in soil may account for as much as 10 MT(N) y-1 of NO. Additional experiments with denitrifying micro-organisms gave an NO to N2O production ratio ranging from 2 to 4 for an oxygen partial pressure of 0.5% and a ratio of less than unity for oxygen partial pressures ranging from 1 to 20%. The production of NO and N2O, normalized with respect to micro-organism number indicates that the production of both NO and N2O by denitrifying micro-organisms is at least an order of magnitude less than production by nitrifying micro-organisms for the micro-organisms studied.

  2. ULTRA-LOW NOX ADVANCED VORTEX COMBUSTOR

    SciTech Connect

    Ryan G. Edmonds; Robert C. Steele; Joseph T. Williams; Douglas L. Straub; Kent H. Casleton; Avtar Bining

    2006-05-01

    An ultra lean-premixed Advanced Vortex Combustor (AVC) has been developed and tested. The natural gas fueled AVC was tested at the U.S. Department of Energy’s National Energy Technology Laboratory (USDOE NETL) test facility in Morgantown (WV). All testing was performed at elevated pressures and inlet temperatures and at lean fuel-air ratios representative of industrial gas turbines. The improved AVC design exhibited simultaneous NOx/CO/UHC emissions of 4/4/0 ppmv (all emissions are at 15% O2 dry). The design also achieved less than 3 ppmv NOx with combustion efficiencies in excess of 99.5%. The design demonstrated tremendous acoustic dynamic stability over a wide range of operating conditions which potentially makes this approach significantly more attractive than other lean premixed combustion approaches. In addition, a pressure drop of 1.75% was measured which is significantly lower than conventional gas turbine combustors. Potentially, this lower pressure drop characteristic of the AVC concept translates into overall gas turbine cycle efficiency improvements of up to one full percentage point. The relatively high velocities and low pressure drops achievable with this technology make the AVC approach an attractive alternative for syngas fuel applications.

  3. Ultra-Low NOx Advanced Vortex Combustor

    SciTech Connect

    Edmonds, R.G.; Steele, R.C.; Williams, J.T.; Straub, D.L.; Casleton, K.H.; Bining, Avtar

    2006-05-01

    An ultra lean-premixed Advanced Vortex Combustor (AVC) has been developed and tested. The natural gas fueled AVC was tested at the U.S. Department of Energy’s National Energy Technology Laboratory (USDOE NETL) test facility in Morgantown (WV). All testing was performed at elevated pressures and inlet temperatures and at lean fuel-air ratios representative of industrial gas turbines. The improved AVC design exhibited simultaneous NOx/CO/UHC emissions of 4/4/0 ppmv (all emissions are at 15% O2 dry). The design also achieved less than 3 ppmv NOx with combustion efficiencies in excess of 99.5%. The design demonstrated tremendous acoustic dynamic stability over a wide range of operating conditions which potentially makes this approach significantly more attractive than other lean premixed combustion approaches. In addition, a pressure drop of 1.75% was measured which is significantly lower than conventional gas turbine combustors. Potentially, this lower pressure drop characteristic of the AVC concept translates into overall gas turbine cycle efficiency improvements of up to one full percentage point. The relatively high velocities and low pressure drops achievable with this technology make the AVC approach an attractive alternative for syngas fuel applications.

  4. Tropospheric sources of NOx: lightning and biology

    NASA Technical Reports Server (NTRS)

    Levine, J. S.; Augustsson, T. R.; Anderson, I. C.; Hoell, J. M. Jr

    1984-01-01

    Laboratory experiments to quantify the global production of NOx (NO + NO2) in the troposphere due to atmospheric lightning and biogenic activity in soil are presented. These laboratory experiments, as well as other studies, suggest that the global production of NOx by lightning probably ranges between 2 and 20 MT(N)y-1 of NO and is strongly dependent on the total energy deposited by lightning, a quantity not well-known. In our laboratory experiments, nitrifying micro-organisms is soil were found to be a significant source of both NO and nitrous oxide (N2O). The measured production ratio of NO to N2O averaged 2-3 for oxygen partial pressures of 0.5-10%. Extrapolating these laboratory measurements to the global scale, which is somewhat risky, suggests that nitrifying micro-organisms in soil may account for as much as 10 MT(N) y-1 of NO. Additional experiments with denitrifying micro-organisms gave an NO to N2O production ratio ranging from 2 to 4 for an oxygen partial pressure of 0.5% and a ratio of less than unity for oxygen partial pressures ranging from 1 to 20%. The production of NO and N2O, normalized with respect to micro-organism number indicates that the production of both NO and N2O by denitrifying micro-organisms is at least an order of magnitude less than production by nitrifying micro-organisms for the micro-organisms studied.

  5. NOx SOx Secondary NAAQS: Integrated Review Plan ...

    EPA Pesticide Factsheets

    The NOx SOx Secondary NAAQS Integrated Review Plan is the first document generated as part of the National Ambient Air Quality Standards (NAAQS) review process. The Plan presents background information, the schedule for the review, the process to be used in conducting the review, and the key policy-relevant science issues that will guide the review. The integrated review plan also discusses the frameworks for the various assessment documents to be prepared by the EPA as part of the review, including an Integrated Science Assessment (ISA), and as warranted, a Risk/Exposure Assessment (REA), and a Policy Assessment (PA). The primary purpose of the NOx SOx Secondary NAAQS Integrated Review Plan is to highlight the key policy-relevant issues to be considered in the Review of the Oxides of Nitrogen and Oxides of Sulfur Secondary NAAQS. A draft of the integrated review plan will be the subject of an advisory review with the Clean Air Scientific Advisory Committee (CASAC) and made available to the public for review and comment.

  6. Flashback Arrestor for LPP, Low NOx Combustors

    NASA Technical Reports Server (NTRS)

    Kraemer, Gil; Lee, Chi-Ming

    1998-01-01

    Lean premixed, prevaporized (LPP) high temperature combustor designs as explored for the Advanced Subsonic Transport (AST) and High Speed Civil Transport (HSCT) combustors can achieve low NO(x), emission levels. An enabling device is needed to arrest flashback and inhibit preignition at high power conditions and during transients (surge and rapid spool down). A novel flashback arrestor design has demonstrated the ability to arrest flashback and inhibit preignition in a 4.6 cm diameter tubular reactor at full power inlet temperatures (725 C) using Jet-A fuel at 0.4 less than or equal To phi less than or equal to 3.5. Several low pressure loss (0.2 to 0.4% at 30 m/s) flashback arrestor designs were developed which arrested flashback at all of the test conditions. Flame holding was also inhibited off the flash arrestor face or within the downstream tube even velocities (less than or equal to 3 to 6 m/s), thus protecting the flashback arrestor and combustor components. Upstream flow conditions influence the specific configuration based on using either a 45% or 76% upstream geometric blockage. Stationary, lean premixed dry low NO(x) gas turbine combustors would also benefit from this low pressure drop flashback arrestor design which can be easily integrated into new and existing designs.

  7. NOx SOx Secondary NAAQS: Integrated Review Plan ...

    EPA Pesticide Factsheets

    The NOx SOx Secondary NAAQS Integrated Review Plan is the first document generated as part of the National Ambient Air Quality Standards (NAAQS) review process. The Plan presents background information, the schedule for the review, the process to be used in conducting the review, and the key policy-relevant science issues that will guide the review. The integrated review plan also discusses the frameworks for the various assessment documents to be prepared by the EPA as part of the review, including an Integrated Science Assessment (ISA), and as warranted, a Risk/Exposure Assessment (REA), and a Policy Assessment (PA). The primary purpose of the NOx SOx Secondary NAAQS Integrated Review Plan is to highlight the key policy-relevant issues to be considered in the Review of the Oxides of Nitrogen and Oxides of Sulfur Secondary NAAQS. A draft of the integrated review plan will be the subject of an advisory review with the Clean Air Scientific Advisory Committee (CASAC) and made available to the public for review and comment.

  8. ROS-induced ROS release orchestrated by Nox4, Nox2, and mitochondria in VEGF signaling and angiogenesis.

    PubMed

    Kim, Young-Mee; Kim, Seok-Jo; Tatsunami, Ryosuke; Yamamura, Hisao; Fukai, Tohru; Ushio-Fukai, Masuko

    2017-06-01

    Reactive oxygen species (ROS) derived from NADPH oxidase (NOX) and mitochondria play a critical role in growth factor-induced switch from a quiescent to an angiogenic phenotype in endothelial cells (ECs). However, how highly diffusible ROS produced from different sources can coordinate to stimulate VEGF signaling and drive the angiogenic process remains unknown. Using the cytosol- and mitochondria-targeted redox-sensitive RoGFP biosensors with real-time imaging, here we show that VEGF stimulation in human ECs rapidly increases cytosolic RoGFP oxidation within 1 min, followed by mitochondrial RoGFP oxidation within 5 min, which continues at least for 60 min. Silencing of Nox4 or Nox2 or overexpression of mitochondria-targeted catalase significantly inhibits VEGF-induced tyrosine phosphorylation of VEGF receptor type 2 (VEGFR2-pY), EC migration and proliferation at the similar extent. Exogenous hydrogen peroxide (H2O2) or overexpression of Nox4, which produces H2O2, increases mitochondrial ROS (mtROS), which is prevented by Nox2 siRNA, suggesting that Nox2 senses Nox4-derived H2O2 to promote mtROS production. Mechanistically, H2O2 increases S36 phosphorylation of p66Shc, a key mtROS regulator, which is inhibited by siNox2, but not by siNox4. Moreover, Nox2 or Nox4 knockdown or overexpression of S36 phosphorylation-defective mutant p66Shc(S36A) inhibits VEGF-induced mtROS, VEGFR2-pY, EC migration, and proliferation. In summary, Nox4-derived H2O2 in part activates Nox2 to increase mtROS via pSer36-p66Shc, thereby enhancing VEGFR2 signaling and angiogenesis in ECs. This may represent a novel feed-forward mechanism of ROS-induced ROS release orchestrated by the Nox4/Nox2/pSer36-p66Shc/mtROS axis, which drives sustained activation of angiogenesis signaling program. Copyright © 2017 the American Physiological Society.

  9. Homocysteine-induced apoptosis in endothelial cells coincides with nuclear NOX2 and peri-nuclear NOX4 activity.

    PubMed

    Sipkens, Jessica A; Hahn, Nynke; van den Brand, Carlien S; Meischl, Christof; Cillessen, Saskia A G M; Smith, Desirée E C; Juffermans, Lynda J M; Musters, René J P; Roos, Dirk; Jakobs, Cornelis; Blom, Henk J; Smulders, Yvo M; Krijnen, Paul A J; Stehouwer, Coen D A; Rauwerda, Jan A; van Hinsbergh, Victor W M; Niessen, Hans W M

    2013-11-01

    Apoptosis of endothelial cells related to homocysteine (Hcy) has been reported in several studies. In this study, we evaluated whether reactive oxygen species (ROS)-producing signaling pathways contribute to Hcy-induced apoptosis induction, with specific emphasis on NADPH oxidases. Human umbilical vein endothelial cells were incubated with 0.01-2.5 mM Hcy. We determined the effect of Hcy on caspase-3 activity, annexin V positivity, intracellular NOX1, NOX2, NOX4, and p47(phox) expression and localization, nuclear nitrotyrosine accumulation, and mitochondrial membrane potential (ΔΨ m). Hcy induced caspase-3 activity and apoptosis; this effect was concentration dependent and maximal after 6-h exposure to 2.5 mM Hcy. It was accompanied by a significant increase in ΔΨ m. Cysteine was inactive on these parameters excluding a reactive thiol group effect. Hcy induced an increase in cellular NOX2, p47(phox), and NOX4, but not that of NOX1. 3D digital imaging microscopy followed by image deconvolution analysis showed nuclear accumulation of NOX2 and p47(phox) in endothelial cells exposed to Hcy, but not in control cells, which coincided with accumulation of nuclear nitrotyrosine residues. Furthermore, Hcy enhanced peri-nuclear localization of NOX4 coinciding with accumulation of peri-nuclear nitrotyrosine residues, a reflection of local ROS production. p47(phox) was also increased in the peri-nuclear region. The Hcy-induced increase in caspase-3 activity was prevented by DPI and apocynin, suggesting involvement of NOX activity. The data presented in this article reveal accumulation of nuclear NOX2 and peri-nuclear NOX4 accumulation as potential source of ROS production in Hcy-induced apoptosis in endothelial cells.

  10. DESIGN REPORT: LOW-NOX BURNERS FOR PACKAGE BOILERS

    EPA Science Inventory

    The report describes a low-NOx burner design, presented for residual-oil-fired industrial boilers and boilers cofiring conventional fuels and nitrated hazardous wastes. The burner offers lower NOx emission levels for these applications than conventional commercial burners. The bu...

  11. 40 CFR 96.142 - CAIR NOX allowance allocations.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 22 2012-07-01 2012-07-01 false CAIR NOX allowance allocations. 96.142... 2009 through 2014, and 97 percent for a control period during 2015 and thereafter, of the tons of NOX... allowances equal to 5 percent for a control period in 2009 through 2014, and 3 percent for a control period...

  12. 40 CFR 96.142 - CAIR NOX allowance allocations.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... CAIR NOX Allowance Allocations § 96.142 CAIR NOX allowance allocations. (a)(1) The baseline heat input... the 3 highest amounts of the unit's adjusted control period heat input for 2000 through 2004, with the adjusted control period heat input for each year calculated as follows: (A) If the unit is coal-fired...

  13. Tyrosine kinase FYN negatively regulates NOX4 in cardiac remodeling

    PubMed Central

    Matsushima, Shouji; Kuroda, Junya; Zhai, Peiyong; Liu, Tong; Ikeda, Shohei; Nagarajan, Narayani; Yokota, Takashi; Kinugawa, Shintaro; Hsu, Chiao-Po; Li, Hong; Tsutsui, Hiroyuki

    2016-01-01

    NADPH oxidases (Noxes) produce ROS that regulate cell growth and death. NOX4 expression in cardiomyocytes (CMs) plays an important role in cardiac remodeling and injury, but the posttranslational mechanisms that modulate this enzyme are poorly understood. Here, we determined that FYN, a Src family tyrosine kinase, interacts with the C-terminal domain of NOX4. FYN and NOX4 colocalized in perinuclear mitochondria, ER, and nuclear fractions in CMs, and FYN expression negatively regulated NOX4-induced O2– production and apoptosis in CMs. Mechanistically, we found that direct phosphorylation of tyrosine 566 on NOX4 was critical for this FYN-mediated negative regulation. Transverse aortic constriction activated FYN in the left ventricle (LV), and FYN-deficient mice displayed exacerbated cardiac hypertrophy and dysfunction and increased ROS production and apoptosis. Deletion of Nox4 rescued the exaggerated LV remodeling in FYN-deficient mice. Furthermore, FYN expression was markedly decreased in failing human hearts, corroborating its role as a regulator of cardiac cell death and ROS production. In conclusion, FYN is activated by oxidative stress and serves as a negative feedback regulator of NOX4 in CMs during cardiac remodeling. PMID:27525436

  14. NOX Activity Is Increased in Mild Cognitive Impairment

    PubMed Central

    Gupta, Sunita; Parrino, Taryn E.; Knight, Alecia G.; Ebenezer, Philip J.; Weidner, Adam M.; LeVine, Harry; Keller, Jeffrey N.; Markesbery, William R.

    2010-01-01

    Abstract This study was undertaken to investigate the profile of NADPH oxidase (NOX) in the clinical progression of Alzheimer's disease (AD). Specifically, NOX activity and expression of the regulatory subunit p47phox and the catalytic subunit gp91phox was evaluated in affected (superior and middle temporal gyri) and unaffected (cerebellum) brain regions from a longitudinally followed group of patients. This group included both control and late-stage AD subjects, and also subjects with preclinical AD and with amnestic mild cognitive impairment (MCI) to evaluate the profile of NOX in the earliest stages of dementia. Data show significant elevations in NOX activity and expression in the temporal gyri of MCI patients as compared with controls, but not in preclinical or late-stage AD samples, and not in the cerebellum. Immunohistochemical evaluations of NOX expression indicate that whereas microglia express high levels of gp91phox, moderate levels of gp91phox also are expressed in neurons. Finally, in vitro experiments showed that NOX inhibition blunted the ability of oligomeric amyloid beta peptides to injure cultured neurons. Collectively, these data show that NOX expression and activity are upregulated specifically in a vulnerable brain region of MCI patients, and suggest that increases in NOX-associated redox pathways in neurons might participate in the early pathogenesis of AD. Antioxid. Redox Signal. 12, 1371–1382. PMID:19929442

  15. DESIGN REPORT: LOW-NOX BURNERS FOR PACKAGE BOILERS

    EPA Science Inventory

    The report describes a low-NOx burner design, presented for residual-oil-fired industrial boilers and boilers cofiring conventional fuels and nitrated hazardous wastes. The burner offers lower NOx emission levels for these applications than conventional commercial burners. The bu...

  16. Plume Evolution and NOx Lifetime in the Denver Metropolitan Area

    NASA Astrophysics Data System (ADS)

    Ebben, C. J.; Sparks, T.; Wooldridge, P. J.; Cohen, R. C.

    2016-12-01

    NOx (NOx≡NO+NO2) is abundant in urban areas due to its emission via combustion processes. As NOx is transported away from cities, it undergoes photochemical oxidation to produce a variety of nitrogen oxide products, including peroxynitrates (PNs), alkyl nitrates (ANs), and nitric acid (HNO3). These species have different loss mechanisms and lifetimes, meaning that ongoing nitrogen oxide chemistry may differ greatly in the near- and far-field of cities. Understanding the evolution of NOx and NOy (NOy≡NOx+PNs+ANs+HNO3+…) - including the relative balance between NOx oxidation products and their overall concentrations - as air masses are transported away from cities is imperative to constraining the lifetime of NOx and understanding how air quality regulations aimed at lowering NOx emissions might impact air quality in the near- and far-field of urban areas. We have used observations from the Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ) to investigate the evolution of NOx in air masses originating from the Denver urban area, and our results are contrasted with examples from other cities.

  17. Nitrogen oxides/sulfur oxides (NOx/SOx) Secondary NAAQS ...

    EPA Pesticide Factsheets

    This document assesses the policy basis for setting the secondary NOx/SOx NAAQS. To provide the policy assessment information for the Administrator to make a more informed decision about the basis for retaining or revising the secondary NOx/SOx NAAQS.

  18. Low Temperature Catalyst for NH3 Removal

    NASA Technical Reports Server (NTRS)

    Monje, Oscar; Melendez, Orlando

    2013-01-01

    Air revitalization technologies maintain a safe atmosphere inside spacecraft by the removal of C02, ammonia (NH3), and trace contaminants. NH3 onboard the International Space Station (ISS) is produced by crew metabolism, payloads, or during an accidental release of thermal control refrigerant. Currently, the ISS relies on removing NH3 via humidity condensate and the crew wears hooded respirators during emergencies. A different approach to cabin NH3 removal is to use selective catalytic oxidation (SCO), which builds on thermal catalytic oxidation concepts that could be incorporated into the existing TCCS process equipment architecture on ISS. A low temperature platinum-based catalyst (LTP-Catalyst) developed at KSC was used for converting NH3 to H20 and N2 gas by SCO. The challenge of implementing SCO is to reduce formation of undesirable byproducts like NOx (N20 and NO). Gas mixture analysis was conducted using FTIR spectrometry in the Regenerable VOC Control System (RVCS) Testbed. The RVCS was modified by adding a 66 L semi-sealed chamber, and a custom NH3 generator. The effect of temperature on NH3 removal using the LTP-Catalyst was examined. A suitable temperature was found where NH3 removal did not produce toxic NO, (NO, N02) and N20 formation was reduced.

  19. Ammonia and the NOx budget of the troposphere

    NASA Technical Reports Server (NTRS)

    Levine, J. S.; Augustsson, T. R.; Hoell, J. M.

    1982-01-01

    Liu et al. (1980) suggested that NOx transported from the stratosphere, as opposed to the anthropogenic source of NOx, may be the dominant source that controls the distribution of NOx in the global troposphere. These ideas require a reinvestigation, and, in particular, an assessment of the role of the oxidation of ammonia as a source of NOx. Attention is given to the results of an ammonia measurement program, in which the vertical distribution of ammonia in the troposphere and lower stratosphere could be studied with the aid of the Infrared Heterodyne Radiometer (IHR), a solar-viewing remote sensor. A one-dimensional photochemical model of the troposphere reported by Levine et al. (1980) was employed to study the chemical and physical processes that control the loss of ammonia in the troposphere. The results of the considered investigation suggest that the oxidation of ammonia may indeed be a significant source of NOx in the troposphere.

  20. Redox-mediated signal transduction by cardiovascular Nox NADPH oxidases.

    PubMed

    Brandes, Ralf P; Weissmann, Norbert; Schröder, Katrin

    2014-08-01

    The only known function of the Nox family of NADPH oxidases is the production of reactive oxygen species (ROS). Some Nox enzymes show high tissue-specific expression and the ROS locally produced are required for synthesis of hormones or tissue components. In the cardiovascular system, Nox enzymes are low abundant and function as redox-modulators. By reacting with thiols, nitric oxide (NO) or trace metals, Nox-derived ROS elicit a plethora of cellular responses required for physiological growth factor signaling and the induction and adaptation to pathological processes. The interactions of Nox-derived ROS with signaling elements in the cardiovascular system are highly diverse and will be detailed in this article, which is part of a Special Issue entitled "Redox Signalling in the Cardiovascular System".

  1. The NADPH oxidase Nox4 and aging in the heart.

    PubMed

    Ago, Tetsuro; Matsushima, Shouji; Kuroda, Junya; Zablocki, Daniela; Kitazono, Takanari; Sadoshima, Junichi

    2010-12-01

    Oxidative stress in mitochondria is believed to promote aging. Although passive leakage of electron from the mitochondrial electron transport chain has been considered as a major source of oxidative stress in the heart and the cardiomyocytes therein, enzymes actively producing reactive oxygen species may also exist in mitochondria. We have shown recently that Nox4, a member of the NADPH oxidase family, is localized on intracellular membranes, primarily at mitochondria, in cardiomyocytes. Mitochondrial expression of Nox4 is upregulated by cardiac stress and aging in the heart, where Nox4 could become a major source of oxidative stress. This raises an intriguing possibility that Nox4 may play an important role in mediating aging of the heart. Here we discuss the potential involvement of Nox4 in mitochondrial oxidative stress and aging in the heart.

  2. Verification of NOx emission inventories over North Korea.

    PubMed

    Kim, Na Kyung; Kim, Yong Pyo; Morino, Yu; Kurokawa, Jun-ichi; Ohara, Toshimasa

    2014-12-01

    In this study, the top-down NOx emissions estimated from satellite observations of NO2 vertical column densities over North Korea from 1996 to 2009 were analyzed. Also, a bottom-up NOx emission inventory from REAS 1.1 from 1980 to 2005 was analyzed with several statistics. REAS 1.1 was in good agreement with the top-down approach for both trend and amount. The characteristics of NOx emissions in North Korea were quite different from other developed countries including South Korea. In North Korea, emissions from industry sector was the highest followed by transportation sector in the 1980s. However, after 1990, the NOx emissions from other sector, mainly agriculture, became the 2nd highest. Also, no emission centers such as urban areas or industrial areas were distinctively observed. Finally, the monthly NOx emissions were high during the warm season. Copyright © 2014 Elsevier Ltd. All rights reserved.

  3. Lewis Base Catalysts 6: Carbene Catalysts

    PubMed Central

    Moore, Jennifer L.

    2013-01-01

    The use of N-heterocyclic carbenes as catalysts for organic transformations has received increased attention in the past 10 years. A discussion of catalyst development and nucleophilic characteristics precedes a description of recent advancements and new reactions using N-heterocyclic carbenes in catalysis. PMID:21494949

  4. Deactivation of Oxidation Catalysts

    DTIC Science & Technology

    1991-05-01

    the fresh catalyst . The loss in chromium may be related to the formation of volatile chromium oxychlorde which vaporizes from the catalyst . It is...CeO2 only marginally improved the thtrmal stability. The addition of 2% water vapor inhibited the oxidation of ethanol for all three copper catalysts ...original activity. Field tests of a copper chromite catalyst on process gas containing H2S, methyl mercaptan, n-aldehydes, and furfural showed

  5. NOx Control for Utility Boiler OTR Compliance

    SciTech Connect

    Hamid Farzan

    2003-12-31

    Under sponsorship of the Department of Energy's National Energy Technology Laboratory (NETL), the Babcock and Wilcox Company (B and W), and Fuel Tech teamed together to investigate an integrated solution for NO{sub x} control. The system is comprised of B and W's DRB-4Z{trademark} ultra low-NO{sub x} pulverized coal (PC) burner technology and Fuel Tech's NOxOUT{reg_sign}, a urea-based selective non-catalytic reduction (SNCR) technology. Development of the low-NO{sub x} burner technology has been a focus in B and W's combustion program. The DRB-4Z{trademark} burner is B and W's newest low-NO{sub x} burner capable of achieving very low NO{sub x}. The burner is designed to reduce NO{sub x} by controlled mixing of the fuel and air. Based on data from several 500 to 600 MWe boilers firing PRB coal, NOx emissions levels of 0.15 to 0.20 lb/ 106 Btu have been achieved from the DRB-4Z{trademark} burners in combination with overfire air ports. Although NOx emissions from the DRB-4Z{trademark} burner are nearing the Ozone Transport Rule (OTR) level of 0.15 lb NO{sub x}/106 Btu, the utility boiler owners can still benefit from the addition of an SNCR and/or SCR system in order to comply with the stringent NO{sub x} emission levels facing them. Large-scale testing is planned in B and W's 100-million Btu/hr Clean Environment Development Facility (CEDF) that simulates the conditions of large coal-fired utility boilers. The objective of the project is to achieve a NO{sub x} level below 0.15 lb/106 Btu (with ammonia slip of less than 5 ppm) in the CEDF using PRB coal and B and W's DRB-4Z{trademark} low-NO{sub x} pulverized coal (PC) burner in combination with dual zone overfire air ports and Fuel Tech's NO{sub x}OUT{reg_sign}. During this period B and W prepared and submitted the project management plan and hazardous substance plan to DOE. The negotiation of a subcontract for Fuel Tech has been started.

  6. Oxidation catalysts comprising metal exchanged hexaaluminate wherein the metal is Sr, Pd, La, and/or Mn

    DOEpatents

    Wickham, David; Cook, Ronald

    2008-10-28

    The present invention provides metal-exchanged hexaaluminate catalysts that exhibit good catalytic activity and/or stability at high temperatures for extended periods with retention of activity as combustion catalysts, and more generally as oxidation catalysts, that make them eminently suitable for use in methane combustion, particularly for use in natural gas fired gas turbines. The hexaaluminate catalysts of this invention are of particular interest for methane combustion processes for minimization of the generation of undesired levels (less than about 10 ppm) of NOx species. Metal exchanged hexaaluminate oxidation catalysts are also useful for oxidation of volatile organic compounds (VOC), particularly hydrocarbons. Metal exchanged hexaaluminate oxidation catalysts are further useful for partial oxidation, particularly at high temperatures, of reduced species, particularly hydrocarbons (alkanes and alkenes).

  7. APBF-DEC NOx Adsorber/DPF Project: Light-Duty Passenger Car Platform

    SciTech Connect

    Tomazic, D; Tatur, M; Thornton, M

    2003-08-24

    A 1.9L turbo direct injection (TDI) diesel engine was modified to achieve the upcoming Tier 2 Bin 5 emission standard in combination with a NOx adsorber catalyst (NAC) and a diesel particulate filter (DPF). The primary objective for developing this test bed is to investigating the effects of different fuel sulfur contents on the performance of an advanced emission control system (ECS) in a light-duty application. During the development process, the engine-out emissions were minimized by applying a state-of-the-art combustion system in combination with cooled exhaust gas recirculation (EGR). The subsequent calibration effort resulted in emission levels requiring 80-90 percent nitrogen-oxide (NOx) and particulate matter (PM) conversion rates by the corresponding ECS. The strategy development included ean/rich modulation for NAC regeneration, as well as, the desulfurization of the NAC and the regeneration of the DPF. Two slightly different ECS were investigated and calibrated. The initial vehicle results in an Audi A4 station wagon over the federal test procedure (FTP), US 06, and the highway fuel economy test (HFET) cycle indicate the potential of these configuration to meet the future Tier 2 emission standard.

  8. The poisoning effect of potassium ions doped on MnOx/TiO2 catalysts for low-temperature selective catalytic reduction

    NASA Astrophysics Data System (ADS)

    Zhang, Liangjing; Cui, Suping; Guo, Hongxia; Ma, Xiaoyu; Luo, Xiaogen

    2015-11-01

    The poisoning of alkali metal on MnOx/TiO2 catalysts used for selective catalytic reduction (SCR) of NOx by NH3 was investigated. KNO3, KCl and K2SO4 were doped on MnOx/TiO2 catalysts by sol-gel method, respectively. The SCR activity of each catalyst was measured for the removal of NOx with NH3 in the temperature range 90-330 °C. The experimental results showed that catalyst with KNO3 have a stronger deactivation effect than other catalysts. The properties of the catalysts were characterized by XRD, BET, SEM, XPS, H2-TPR, NH3-TPD and in situ DRIFTS analyses. The characterized results indicated that KNO3, KCl and K2SO4 caused the similar decrease of specific surface area and pore volume, but the quantity of acid sites for KNO3-MnOx/TiO2 catalyst reduced sharply. The main reason for catalyst deactivation is attributed to two aspects: one was physical influences for the decrease of surface area and pore volume, another was chemical influences that the K+ ions decomposed by KNO3 neutralized Brønsted acid sites of catalyst and reduced their reducibility. The chemical influence played a leading role on the deactivation of catalysts.

  9. Reversible hydrogen storage materials

    DOEpatents

    Ritter, James A [Lexington, SC; Wang, Tao [Columbia, SC; Ebner, Armin D [Lexington, SC; Holland, Charles E [Cayce, SC

    2012-04-10

    In accordance with the present disclosure, a process for synthesis of a complex hydride material for hydrogen storage is provided. The process includes mixing a borohydride with at least one additive agent and at least one catalyst and heating the mixture at a temperature of less than about 600.degree. C. and a pressure of H.sub.2 gas to form a complex hydride material. The complex hydride material comprises MAl.sub.xB.sub.yH.sub.z, wherein M is an alkali metal or group IIA metal, Al is the element aluminum, x is any number from 0 to 1, B is the element boron, y is a number from 0 to 13, and z is a number from 4 to 57 with the additive agent and catalyst still being present. The complex hydride material is capable of cyclic dehydrogenation and rehydrogenation and has a hydrogen capacity of at least about 4 weight percent.

  10. NOX isoforms in the development of abdominal aortic aneurysm.

    PubMed

    Siu, Kin Lung; Li, Qiang; Zhang, Yixuan; Guo, Jun; Youn, Ji Youn; Du, Jie; Cai, Hua

    2017-04-01

    Oxidative stress plays an important role in the formation of abdominal aortic aneurysm (AAA), and we have recently established a causal role of uncoupled eNOS in this severe human disease. We have also shown that activation of NADPH oxidase (NOX) lies upstream of uncoupled eNOS. Therefore, identification of the specific NOX isoforms that are required for eNOS uncoupling and AAA formation would ultimately lead to novel therapies for AAA. In the present study, we used the Ang II infused hph-1 mice to examine the roles of NOX isoforms in the development of AAA. We generated double mutants of hph-1-NOX1, hph-1-NOX2, hph-1-p47phox, and hph-1-NOX4. After two weeks of Ang II infusion, the incidence rate of AAA substantially dropped from 76.5% in Ang II infused hph-1 mice (n=34) to 11.1%, 15.0%, 9.5% and 0% in hph-1-NOX1 (n=27), hph-1-NOX2 (n=40), hph-1-p47phox (n=21), and hph-1-NOX4 (n=33) double mutant mice, respectively. The size of abdominal aortas of the four double mutant mice, determined by ultrasound analyses, was significantly smaller than the hph-1 mice. Aortic nitric oxide and H4B bioavailabilities were markedly improved in the double mutants, while superoxide production and eNOS uncoupling activity were substantially diminished. These effects seemed attributed to an endothelial specific restoration of dihydrofolate reductase expression and activity, deficiency of which has been shown to induce eNOS uncoupling and AAA formation in both Ang II-infused hph-1 and apoE null animals. In addition, over-expression of human NOX4 N129S or T555S mutant newly identified in aneurysm patients increased hydrogen peroxide production, further implicating a relationship between NOX and human aneurysm. Taken together, these data indicate that NOX isoforms 1, 2 or 4 lies upstream of dihydrofolate reductase deficiency and eNOS uncoupling to induce AAA formation. These findings may promote development of novel therapeutics for the treatment of the disease by inhibiting NOX signaling.

  11. Diurnal cycles of NOx over the United States: Comprehensive evaluations and implications for NOx emissions

    NASA Astrophysics Data System (ADS)

    Li, J.; Wang, Y.; Smeltzer, C. D.; Zhang, Y.; Zhang, R.; Weinheimer, A. J.; Celarier, E. A.; Herman, J. R.

    2016-12-01

    Reactive nitrogen (NOx=NO+NO2) plays a crucial role in the formation of ozone and has significant impacts on the production of secondary organic and inorganic aerosols, thus affecting global radiation budget and climate. The diurnal cycle of NOx is a function of emissions and photochemistry. Its observations therefore provide useful constraints in our understanding of these factors. We employ a regional chemical transport model (REAM) to simulate the observed diurnal cycles of NO2 concentrations over the United States. The simulated diurnal cycles are evaluated by using the 2011 DISCOVER-AQ campaign (Maryland) measurements, EPA Air Quality System (AQS) observations, and OMI and GOME-2 column measurements. The model simulations are in reasonably good agreement with the observations except that PANDORA measured column NO2 showed much less variation in early morning and late afternoon than simulated in the model. High resolution (4 km in the horizontal) model simulations are also performed to examine the effects of emission distribution. By analyzing model simulations with the observations, we show that the diurnal emission profiles of NOx is different over the weekend from the weekdays and that weekend emissions are about 1/3 lower than weekdays.

  12. Catalyst by Design

    SciTech Connect

    Narula, Chaitanya Kumar; DeBusk, Melanie Moses

    2014-01-01

    The development of new catalytic materials is still dominated by trial and error methods. Although it has been successful, the empirical development of catalytic materials is time consuming and expensive with no guarantee of success. In our laboratories, we are developing a comprehensive catalysts by design that involves state-of-the-art first principle density functional theory calculations, experimental design of catalyst sites, and sub- ngstr m resolution imaging with an aberration-corrected electron microscope to characterize the microstructure. In this chapter, we focus on supported platinum cluster catalyst systems which are one of the most important industrial catalysts and attempt to demonstrate the feasibility of the catalyst by design concept.

  13. Variation of a Lightning NOx Indicator for National Climate Assessment

    NASA Technical Reports Server (NTRS)

    Koshak, William J.; McCaul, Eugene W., Jr.; Peterson, Harold S.; Vant-Hull, Brian

    2014-01-01

    During the past couple of years, an analysis tool was developed by the NASA Marshall Space Flight Center (MSFC) for the National Climate Assessment (NCA) program. The tool monitors and examines changes in lightning characteristics over the conterminous US (CONUS) on a continual basis. In this study, we have expanded the capability of the tool so that it can compute a new climate assessment variable that is called the Lightning NOx Indicator (LNI). Nitrogen oxides (NOx = NO + NO2) are known to indirectly influence our climate, and lightning NOx is the most important source of NOx in the upper troposphere (particularly in the tropics). The LNI is derived using Lightning Imaging Sensor (LIS) data and is computed by summing up the product of flash area x flash brightness over all flashes that occur in a particular region and period. Therefore, it is suggested that the LNI is a proxy to lightning NOx production. Specifically, larger flash areas are consistent with longer channel length and/or more energetic channels, and hence more NOx production. Brighter flashes are consistent with more energetic channels, and hence more NOx production. The location of the flash within the thundercloud and the optical scattering characteristics of the thundercloud are of course complicating factors. We analyze LIS data for the years 2003-2013 and provide geographical plots of the time-evolution of the LNI in order to determine if there are any significant changes or trends between like seasons, or from year to year.

  14. Air spark-like plasma source for antimicrobial NOx generation

    NASA Astrophysics Data System (ADS)

    Pavlovich, M. J.; Ono, T.; Galleher, C.; Curtis, B.; Clark, D. S.; Machala, Z.; Graves, D. B.

    2014-12-01

    We demonstrate and analyse the generation of nitrogen oxides and their antimicrobial efficacy using atmospheric air spark-like plasmas. Spark-like discharges in air in a 1 L confined volume are shown to generate NOx at an initial rate of about 1.5  ×  1016 NOx molecules/J dissipated in the plasma. Such a discharge operating in this confined volume generates on the order of 6000 ppm NOx in 10 min. Around 90% of the NOx is in the form of NO2 after several minutes of operation in the confined volume, suggesting that NO2 is the dominant antimicrobial component. The strong antimicrobial action of the NOx mixture after several minutes of plasma operation is demonstrated by measuring rates of E. coli disinfection on surfaces and in water exposed to the NOx mixture. Some possible applications of plasma generation of NOx (perhaps followed by dissolution in water) include disinfection of surfaces, skin or wound antisepsis, and sterilization of medical instruments at or near room temperature.

  15. A practical procedure for achieving a steady state of NOx concentration in plasma: with special reference to the NOx content of Japanese daily food.

    PubMed

    Himeno, Mariko; Ishibashi, Takaharu; Nakano, Shigeru; Furuya, Keisuke; Kigoshi, Toshikazu; Uchida, Kenzo; Nishio, Matomo

    2003-02-01

    To establish a concrete procedure to achieve a steady state plasma NOx concentration with Japanese daily food, NOx contents of about 200 types of food and beverages consumed daily were measured and NOx concentration in plasma was monitored till steady state after various degree of intake of NOx restricted food. The NOx content was found to be high in dark green leaved vegetables and low in grains, processed food, fresh and processed seafood. Tap water and mineral water were found to contain various amounts of NOx that were drastically reduced by treatment with a reverse osmosis column and remained in trace amounts after ion exchange column treatment. NOx content was low in drinks such as cola, but was extremely high in vegetable juice containing dark green leaved vegetables. The intake of high NOx drinks resulted in elevated plasma NOx concentration, but intake of low NOx drinks did not change the plasma NOx concentration. Based on these findings, a steady state could be achieved by 18 hours fasting after the intake of a moderately NOx-restricted diet (about 370, micromoles/day) and by 13 hours fasting after the intake of an extremely NOx-restricted diet (< 100 micromoles/day). NOx concentrations in randomly collected blood samples without these conditions were sometimes ten times higher than that at steady state. This procedure can be undertaken under normal Japanese daily life and is expected to be applicable even to outpatients.

  16. System for reactivating catalysts

    SciTech Connect

    Ginosar, Daniel M.; Thompson, David N.; Anderson, Raymond P.

    2010-03-02

    A method of reactivating a catalyst, such as a solid catalyst or a liquid catalyst is provided. The method comprises providing a catalyst that is at least partially deactivated by fouling agents. The catalyst is contacted with a fluid reactivating agent that is at or above a critical point of the fluid reactivating agent and is of sufficient density to dissolve impurities. The fluid reactivating agent reacts with at least one fouling agent, releasing the at least one fouling agent from the catalyst. The at least one fouling agent becomes dissolved in the fluid reactivating agent and is subsequently separated or removed from the fluid reactivating agent so that the fluid reactivating agent may be reused. A system for reactivating a catalyst is also disclosed.

  17. NOX4 is an early initiator of neuropathic pain.

    PubMed

    Geis, Christian; Geuss, Eva; Sommer, Claudia; Schmidt, Harald H H W; Kleinschnitz, Christoph

    2017-02-01

    Treatment of neuropathic pain remains challenging as the etiology is heterogeneous and pathomechanisms are incompletely understood. One possible mechanism is oxidative stress due to unphysiological reactive oxygen species (ROS) formation. The only know dedicated enzymatic source of ROS are NADPH oxidases of which the type 4 isoform (NOX4) has been suggested to be involved in the subacute and chronic phase of neuropathic pain. Here, we aim to translate this finding into a treatment strategy by examining the efficacy of the NOX1/4-specific inhibitor GKT136901 using the chronic constriction injury (CCI) mouse model of neuropathic pain. Unexpectedly, post-nerve lesion treatment using GKT136901 was ineffective to reduce pain-related behavior after CCI. We therefore re-investigated the role of NOX4 using an independent KO mouse model. Early after CCI we found an increase in pro-inflammatory cytokines, ROS formation and the oxidative stress marker nitrotyrosine in the lesioned nerve together with an upregulated Nox4 gene expression. In NOX4 KO mice, mechanical allodynia was markedly reduced from day 4 after nerve injury as were all ROS related and acute biomarkers. In addition, we observed a reduction in the CCI-induced upregulation of pro-inflammatory cytokines in the sciatic nerve and dorsal root ganglia along with NOX4-deficiency. Thus, we conclude that NOX4 is involved in the development of neuropathic pain states by producing oxidative stress and subsequent cytokine dysregulation at the lesion site. This appears at very early stages immediately after nerve injury explaining ineffectiveness of post-acute pharmacological NOX inhibition. We suggest that future target validation of NOX4 should now focus on defining the possible therapeutic window in human neuropathic pain. Copyright © 2016 Elsevier Inc. All rights reserved.

  18. Protein Scaffolding for Small Molecule Catalysts

    SciTech Connect

    Baker, David

    2014-09-14

    We aim to design hybrid catalysts for energy production and storage that combine the high specificity, affinity, and tunability of proteins with the potent chemical reactivities of small organometallic molecules. The widely used Rosetta and RosettaDesign methodologies will be extended to model novel protein / small molecule catalysts in which one or many small molecule active centers are supported and coordinated by protein scaffolding. The promise of such hybrid molecular systems will be demonstrated with the nickel-phosphine hydrogenase of DuBois et. al.We will enhance the hydrogenase activity of the catalyst by designing protein scaffolds that incorporate proton relays and systematically modulate the local environment of the catalyticcenter. In collaboration with DuBois and Shaw, the designs will be experimentally synthesized and characterized.

  19. NOx formation in combustion of gaseous fuel in ejection burner

    NASA Astrophysics Data System (ADS)

    Rimár, Miroslav; Kulikov, Andrii

    2016-06-01

    The aim of this work is to prepare model for researching of the formation in combustion of gaseous fuels. NOx formation is one of the main ecological problems nowadays as nitrogen oxides is one of main reasons of acid rains. The ANSYS model was designed according to the calculation to provide full combustion and good mixing of the fuel and air. The current model is appropriate to research NOx formation and the influence of the different principles of NOx reduction method. Applying of designed model should spare both time of calculations and research and also money as you do not need to measure the burner characteristics.

  20. Recent spectroscopic measurements of NOx in the lower stratosphere

    SciTech Connect

    Goldman, A.; Murcray, D.G.

    1982-01-01

    High resolution (0.02 and 0.06 per cm) Fourier transform airborne systems were used for measurements of long path atmospheric absorption spectra, covering many of the NOx infrared bands. Atmospheric emission measurements with liquid helium cooled grating spectrometer systems at 0.5 per cm resolution were also carried out from different altitudes in the NOx bands region. Analysis of the absorption and emission spectra provides quantification of NOx in the lower stratosphere at different latitudes and seasons, as well as diurnal variability.