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Sample records for nox reduction catalysts

  1. Deactivation-resistant catalyst for selective catalyst reduction of NOx

    DEFF Research Database (Denmark)

    2011-01-01

    The present invention relates to a catalyst for selective catalytic reduction of NOx in alkali metal containing flue gas using ammonia as reductant, the catalyst comprising a surface with catalytically active sites, wherein the surface is at least partly coated with a coating comprising at least...... one metal oxide. In another aspect the present invention relates to the use of said catalyst and to a method of producing said catalyst. In addition, the present invention relates to a method of treating an catalyst for conferring thereon an improved resistance to alkali poisoning....

  2. Multiphase catalysts for selective reduction of NOx with hydrocarbons

    International Nuclear Information System (INIS)

    Maisuls, S.E.

    2000-01-01

    Among the existing proposed solutions to reduce emission of NOx there is a promising alternative, the so-called (HC-SCR) selective catalytic reduction of NOx using hydrocarbons as reductant. This thesis is part of a worldwide effort devoted to gain knowledge on the selective catalytic reduction of NOx with hydrocarbons with the final goal to contribute to the development of suitable catalysts for the above mentioned process. Chapter 2 describes the details of the experimental set-up and of the analytical methods employed. Among the catalyst for HC-SCR, Co-based catalyst are known to be active and selective, thus, a study on a series of Co-based catalysts, supported on zeolites, was undertaken and the results are presented in Chapter 3. Correlation between catalytic characteristics and kinetic results are employed to understand the working catalyst and this is used as a basis for catalyst optimization. With the intention to prepare a multi-functional catalyst that will preserve the desired characteristics of the individual components, minimizing their negative aspects, catalysts based on Co-Pt, supported on ZSM-5, were investigated. In Chapter 4 the results of this study are discussed. A bimetallic Co-Pt/ZSM-5 catalysts with low Pt contents (0.1 wt %) showed a synergistic effect by combining high stability and activity of Pt catalysts with the high N2 selectivity of Co catalysts. Furthermore, it was found to be sulfur- and water-tolerant. Its positive qualities brought us to study the mechanism that takes place over this catalyst during HC-SCR. The results of an in-situ i.r mechanistic study over this catalyst is reported in Chapter 5. From the results presented in Chapter 5 a mechanism operating over the Co-Pt/ZSM-5 catalyst is proposed. The modification of Co catalyst with Pt improved the catalysts. However, further improvement was found to be hindered by high selectivity to N2O. Since Rh catalysts are generally less selective to N2O, the modification of Co

  3. Mechanistic Investigation of the Reduction of NOx over Pt- and Rh-Based LNT Catalysts

    Directory of Open Access Journals (Sweden)

    Lukasz Kubiak

    2016-03-01

    Full Text Available The influence of the noble metals (Pt vs. Rh on the NOx storage reduction performances of lean NOx trap catalysts is here investigated by transient micro-reactor flow experiments. The study indicates a different behavior during the storage in that the Rh-based catalyst showed higher storage capacity at high temperature as compared to the Pt-containing sample, while the opposite is seen at low temperatures. It is suggested that the higher storage capacity of the Rh-containing sample at high temperature is related to the higher dispersion of Rh as compared to Pt, while the lower storage capacity of Rh-Ba/Al2O3 at low temperature is related to its poor oxidizing properties. The noble metals also affect the catalyst behavior upon reduction of the stored NOx, by decreasing the threshold temperature for the reduction of the stored NOx. The Pt-based catalyst promotes the reduction of the adsorbed NOx at lower temperatures if compared to the Rh-containing sample, due to its superior reducibility. However, Rh-based material shows higher reactivity in the NH3 decomposition significantly enhancing N2 selectivity. Moreover, formation of small amounts of N2O is observed on both Pt- and Rh-based catalyst samples only during the reduction of highly reactive NOx stored at 150 °C, where NOx is likely in the form of nitrites.

  4. Urea thermolysis and NOx reduction with and without SCR catalysts

    International Nuclear Information System (INIS)

    Fang, Howard L.; DaCosta, Herbert F.M.

    2003-01-01

    Urea-selective catalytic reduction (SCR) has been a leading contender for removal of nitrogen oxides (deNO x ) from diesel engine emissions. Despite its advantages, the SCR technology faces some critical detriments to its catalytic performance such as catalyst surface passivation (caused by deposit formation) and consequent stoichiometric imbalance of the urea consumption. Deposit formation deactivates catalytic performance by not only consuming part of the ammonia produced during urea decomposition but also degrading the structural and thermal properties of the catalyst surface. We have characterized the urea thermolysis with and without the urea-SCR catalyst using both spectroscopic (DRIFTS and Raman) and thermal techniques (thermal gravimetric analysis (TGA) and differential scanning calorimetry (DSC)) to identify the deposit components and their corresponding thermal properties. Urea thermolysis exhibits two decomposition stages, involving ammonia generation and consumption, respectively. The decomposition after the second stage leads to the product of melamine complexes, (HNC=NH) x (HNCO) y , that hinder catalytic performance. The presence of catalyst accompanied with a good spray of the urea solution helps to eliminate the second stage. In this work, kinetics of the direct reduction of NO x by urea is determined and the possibility of using additives to the urea solution in order to rejuvenate the catalyst surface and improve its performance will be discussed

  5. Reduce NOx Emissions by Adsorber-Reduction Catalyst on Lean Burn Gasoline Engine

    Directory of Open Access Journals (Sweden)

    Dongpeng Yue

    2013-09-01

    Full Text Available The effect of a new catalyst system composed of traditional three way catalyst converter and adsorber-reduction catalysis converter on the emission characteristics and BSFC (Breake Specific Fuel Consumption- BSFCof a lean burn gasoline engine operated were investigated in this paper under different schemes of catalyst converter arrangement and different speeds and loads. The results show that the position of Three Way Catalyst is before the NOx adsorber Catalyst was the best scheme of catalyst converter arrangement. Which has the highest converter efficiency of reduction NOx emission in lean burn gasoline engine. The effects of speed on the exhaust emission and BSFC were also related to the ratio of lean burn time to rich burn time and the absolute value of both time of the adsorber-reduction catalyst converter. The load of the engine was the main influential factor to the exhaust emission characteristics and BSFC of lean burn gasoline engine, and the more load of the engine was, the more NOx emission , the less NOx conversion rate (CNOx and the better BSFC were.

  6. Effects space velocity and gas velocity on DeNOx catalyst with HC reductant; HC tenka NOx kangen shokubai no kukan sokudo oyobi gas ryusoku no eikyo

    Energy Technology Data Exchange (ETDEWEB)

    Niimura, K.; Tsujimura, K.

    1995-04-20

    Discussions were given on the hydrocarbon added reduction catalyst method to reduce NOx in diesel engine exhaust gas. An experiment was carried out with actual exhaust gas from a diesel engine by using a copper ion exchanged zeolite catalyst that has been coated on a honeycomb type substrate, and using propylene as a reductant. When the catalyst volume was changed with the exhaust gas space velocity kept constant, the NOx conversion ratio decreased as the catalyst length is decreased, and the activity shifted to the lower temperature side. The NOx reduction efficiency increased if the faster the gas flow velocity. On the other hand, if the gas flow velocity is slow, the NOx reduction can be carried out with relatively small amount of the reductant. When the catalyst volume was changed with the passing gas amount kept constant, the NOx conversion ratio decreased largely if the catalyst length is decreased. Further, the NOx reduction characteristics shift to the higher temperature side. In the catalyst length direction, the NOx reduction activity shows a relatively uniform action. However, a detailed observation reveals that the reaction heat in the catalyst is transmitted to the wake improving the activity, hence the further down the flow, the NOx conversion ratio gets higher in efficiency. 5 refs., 5 figs., 3 tabs.

  7. Numerical simulation of flow in De-NOx catalyst honeycomb with NOx reduction reaction

    Energy Technology Data Exchange (ETDEWEB)

    Tanno, K.; Makino, H. [Electric Power Industry, Kanagawa (Japan). Energy Engineering Research Lab.; Kurose, R.; Komori, S. [Kyoto Univ. (Japan). Dept. of Mechanical Engineering and Science

    2013-07-01

    The effect of flow behavior in a De-NOx honeycomb with NOx reduction reaction is investigated by direct numerical simulation (DNS). As the inlet flow, fully developed turbulent or laminar flow is given. The results show that the surface reaction is strongly affected by inner flow behavior. The surface reaction rate for the turbulent flow is higher than that for the laminar flow. This is due to the difference of inner flow behavior that the diffusion of NOx in the vicinity of the wall is dominated only by molecular diffusion for the laminar flow, whereas it is enhanced by turbulent motions for the turbulent flow. Moreover, surface reaction is suppressed towards downstream even though inlet flow is turbulent. This is due to the flow transition from turbulent to laminar.

  8. Multiphase catalysts for selective reduction of NOx with hydrocarbons

    NARCIS (Netherlands)

    Maisuls, S.E.

    2000-01-01

    The combustion of fuels, to meet the society demands for energy, result in the emissi of large quantities of nitrogen oxides (NOx) to the environment. These pollutants cause severe environmental problems and present a serious hazard to the health. Nowadays, two methods for the control of NOx

  9. Supported Metal Zeolites as Environmental Catalysts for Reduction of NOx Molecules

    International Nuclear Information System (INIS)

    May Nwe Win; Tin Tin Aye; Kyaw Myo Naing; Nyunt Wynn; Maung Maung Htay

    2005-09-01

    The NOx contamination of air is a major pollutant due to its reaction with the volatile organic compounds, which give rise to ground level (tropospheric) ozone. It is a conventional fact that NOx are one of the major components of car exhaust. In view of that fact, to sustain the tropospheric ozone is to reduce the amount of NOx in the air. Therefore, this paper is concerned with the catalytic activity of Fe-loaded zeolite and Cu-loaded zeolite used to decompose NIOx by SCR (selective catalytic reduction) reaction with very high activity have been studied. Their preparations, characterization by XRD, FT-IR and SEM were also studied. Fe and Cu containig were prepared by soild state ion-exchange method under ambient presure and at the temperature of 600C for 4 hours. From this study, selective catalytic reduction rection was observed, showing about 87% conversion of the NOx molecule with the corresponding optimum amount of catalyst (1.0+-0.5)g working under the reactor space volume of 30cm3 at ambient temperature (30-32)C

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

    Science.gov (United States)

    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.

  11. The effects of regeneration conditions on NOx and NH3 release from NOx storage/reduction catalysts

    International Nuclear Information System (INIS)

    Epling, William S.; Yezerets, Aleksey; Currier, Neal W.

    2007-01-01

    A standard protocol developed by the Cross-Cut Lean Exhaust Emissions Reduction Simulations (CLEERS) group was used to investigate the evolution of N-byproduct species and the release of unreduced NO x from a commercial NO x storage/reduction (NSR) catalyst. NH 3 was readily formed at temperatures below 375 C, and the onset of its formation was typically observed coincident with reductant breakthrough. N 2 O was also observed at these lower test temperatures. The rate of NO x release, as both NO and NO 2 , increased with increasing temperature due to decreasing nitrate stability. Reduction of NO x necessarily involved the presence of reductant, which was also used to titrate oxygen species from oxygen-storage components such as ceria. Changes in the release of unreduced NO x from the catalyst as a function of temperature were directly attributable to the temperature dependencies of nitrate stability and decomposition, NO x diffusion to the precious metal sites, the rate of the NO x reduction reaction and the rate of reduction of these oxygen-storage components. Furthermore, by accounting for the amount of reductant needed for titration of the oxygen-storage components and the amount of NO x trapped, mass balance calculations were performed and used to estimate the amounts of residual nitrates on the catalyst surface after regeneration. These calculations indicate that only at the lower temperatures were the regenerations not effective enough to remove all the trapped NO x . (author)

  12. NO_x reduction and N_2O emissions in a diesel engine exhaust using Fe-zeolite and vanadium based SCR catalysts

    International Nuclear Information System (INIS)

    Cho, Chong Pyo; Pyo, Young Dug; Jang, Jin Young; Kim, Gang Chul; Shin, Young Jin

    2017-01-01

    Highlights: • NO_x reduction and N_2O emission of urea-SCR catalysts with the oxidation precatalysts were investigated. • Fe-zeolite and V-based catalysts were noticeably affected by the NO_2/NOx ratio. • Remarkable N_2O formation was observed only for the Fe-zeolite catalyst. - Abstract: Among various approaches used to comply with strict diesel engine exhaust regulations, there is increasing interest in urea based selective catalytic reduction (SCR) as a NO_x reduction technology, due to its high reduction and excellent fuel efficiencies. NO_x reduction by SCR catalysts is affected by variations in the NO_2/NO_x ratio, caused by oxidation catalysts such as the diesel oxidation catalyst (DOC) and diesel particulate filter (DPF) installed in diesel engines. Recently, it has been reported that the greenhouse gas (GHG) variant N_2O, which is a by-product of the NO_x conversion process in the after-treatment system, will be subject to regulation. Using a real diesel engine installed with DOC and DPF, the NO_x reduction and N_2O emission performances of commonly used Fe-zeolite and V_2O_5-WO_3/TiO_2 catalysts were investigated under various operating conditions. The exhaust of the diesel engine used in this study had a NO_2/NO_x ratio of over 50% for temperatures below 400 °C due to the oxidation catalysts, while the NO_2/NO_x ratio was significantly lower for temperatures above 400 °C. Under such conditions, it was found that the Fe-zeolite and V_2O_5-WO_3/TiO_2 catalysts were noticeably affected by the NO_2/NOx ratio and exhaust temperature. Although both catalysts showed satisfactory NO conversions, the V_2O_5-WO_3/TiO_2 catalyst showed decreasing NO_2 conversion rates between 250 °C and 320 °C. The V_2O_5-WO_3/TiO_2 catalyst exhibited NH_3 slip relatively frequently because of its low NH_3 storage capacity. For the Fe-zeolite catalyst, a significant increase in the amount of generated N_2O was observed for high NO_x conversion conditions due to side

  13. Alternative deNOx catalysts and technologies

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes

    The present thesis entitled Alternative deNOx Catalysts and technologies revolves around the topic of removal of nitrogen oxides. Nitrogen oxides, NOx, are unwanted byproducts formed during combustion (e.g. in engines or power plants). If emitted to the atmosphere, they are involved...... in the formation of acid rain and photochemical smog. Some basic concepts and reactions regarding the formation and removal of NOx are presented in chapter 1 and 2. Two approaches are undertaken in the present work to reduce the emission of NOx: by means of catalytic removal, and by NO absorption in ionic liquids....... The commercial catalyst used for the selective catalytic reduction (SCR) of nitrogen oxides exhibits high activity and selectivity towards N2. However, the vanadia-titania-based catalyst used is very sensitive to deactivation by alkali-species (primarily potassium), which are typically present in high amounts...

  14. The selective reduction of NO@#x@# with NH@#3@# over zirconia-supported vanadia catalysts

    NARCIS (Netherlands)

    Szakacs, S.; Altena, G.J.; Altena, G.J.; Fransen, T.; van Ommen, J.G.; Ross, J.R.H.; Ross, J.R.H.

    1993-01-01

    A series of sub-monolayer vanadia-on-zirconia catalysts have been prepared and the activities of these have been measured for the selective reduction of NO with NH3. It has been found that the activity per vanadium surface species depends on the square of the vanadium surface coverage. We therefore

  15. Preparation Effects on the Performance of Silica-Doped Hydrous Titanium Oxide (HTO:Si)-Supported Pt Catalysts for Lean-Burn NOx Reduction by Hydrocarbons; TOPICAL

    International Nuclear Information System (INIS)

    GARDNER, TIMOTHY J.; MCLAUGHLIN, LINDA I.; MOWERY, DEBORAH L.; SANDOVAL, RONALD S.

    2002-01-01

    This report describes the development of bulk hydrous titanium oxide (HTO)- and silica-doped hydrous titanium oxide (HTO:Si)-supported Pt catalysts for lean-burn NOx catalyst applications. The effects of various preparation methods, including both anion and cation exchange, and specifically the effect of Na content on the performance of Pt/HTO:Si catalysts, were evaluated. Pt/HTO:Si catalysts with low Na content ( and lt; 0.5 wt.%) were found to be very active for NOx reduction in simulated lean-burn exhaust environments utilizing propylene as the major reductant species. The activity and performance of these low Na Pt/HTO:Si catalysts were comparable to supported Pt catalysts prepared using conventional oxide or zeolite supports. In ramp down temperature profile test conditions, Pt/HTO:Si catalysts with Na contents in the range of 3-5 wt.% showed a wide temperature window of appreciable NOx conversion relative to low Na Pt/HTO:Si catalysts. Full reactant species analysis using both ramp up and isothermal test conditions with the high Na Pt/HTO:Si catalysts, as well as diffuse reflectance FTIR studies, showed that this phenomenon was related to transient NOx storage effects associated with NaNO(sub 2)/NaNO(sub 3) formation. These nitrite/nitrate species were found to decompose and release NOx at temperatures above 300 C in the reaction environment (ramp up profile). A separate NOx uptake experiment at 275 C in NO/N(sub 2)/O(sub 2) showed that the Na phase was inefficiently utilized for NOx storage. Steady state tests showed that the effect of increased Na content was to delay NOx light-off and to decrease the maximum NOx conversion. Similar results were observed for high K Pt/HTO:Si catalysts, and the effects of high alkali content were found to be independent of the sample preparation technique. Catalyst characterization (BET surface area, H(sub 2) chemisorption, and transmission electron microscopy) was performed to elucidate differences between the HTO- and HTO

  16. Catalytic reduction of NOx with H2/CO/CH4 over PdMOR catalysts

    International Nuclear Information System (INIS)

    Pieterse, Johannis A.Z.; Booneveld, Saskia

    2007-01-01

    Conversion of NO x with reducing agents H 2 , CO and CH 4 , with and without O 2 , H 2 O, and CO 2 were studied with catalysts based on MOR zeolite loaded with palladium and cerium. The catalysts reached high NO x to N 2 conversion with H 2 and CO (>90% conversion and N 2 selectivity) range under lean conditions. The formation of N 2 O is absent in the presence of both H 2 and CO together with oxygen in the feed, which will be the case in lean engine exhaust. PdMOR shows synergic co-operation between H 2 and CO at 450-500 K. The positive effect of cerium is significant in the case of H 2 and CH 4 reducing agent but is less obvious with H 2 /CO mixture and under lean conditions. Cerium lowers the reducibility of Pd species in the zeolite micropores. The catalysts showed excellent stability at temperatures up to 673 K in a feed with 2500 ppm CH 4 , 500 ppm NO, 5% O 2 , 10% H 2 O (0-1% H 2 ), N 2 balance but deactivation is noticed at higher temperatures. Combining results of the present study with those of previous studies it shows that the PdMOR-based catalysts are good catalysts for NO x reduction with H 2 , CO, hydrocarbons, alcohols and aldehydes under lean conditions at temperatures up to 673 K. (author)

  17. deNOx catalysts for biomass combustion

    DEFF Research Database (Denmark)

    Kristensen, Steffen Buus

    The present thesis revolves around the challenges involved in removal of nitrogen oxides in biomass fired power plants. Nitrogen oxides are unwanted byproducts formed to some extent during almost any combustion. In coal fired plants these byproducts are removed by selective catalytic reduction......, however the alkali in biomass complicate matters. Alkali in biomass severely deactivates the catalyst used for the selective catalytic reduction in matter of weeks, hence a more alkali resistant catalyst is needed. In the thesis a solution to the problem is presented, the nano particle deNOx catalyst...

  18. Local Environment and Nature of Cu Active Sites in Zeolite-Based Catalysts for the Selective Catalytic Reduction of NOx

    NARCIS (Netherlands)

    Deka, U.|info:eu-repo/dai/nl/325811202; Lezcano-Gonzalez, I.; Weckhuysen, B.M.|info:eu-repo/dai/nl/285484397; Beale, A.M.|info:eu-repo/dai/nl/325802068

    2013-01-01

    Cu-exchanged zeolites have demonstrated widespread use as catalyst materials in the abatement of NOx, especially from mobile sources. Recent studies focusing on Cu-exchanged zeolites with the CHA structure have demonstrated them to be excellent catalysts in the ammonia-assisted selective catalytic

  19. Electrochemical reduction of NOx

    DEFF Research Database (Denmark)

    Traulsen, Marie Lund

    NO and NO2 (collectively referred to as NOx) are air pollutants, and the largest single contributor to NOx pollution is automotive exhaust. This study investigates electrochemical deNOx, a technology which aims to remove NOx from automotive diesel exhaust by electrochemical reduction of NOx to N2...... and O2. The focus in this study is on improving the activity and selectivity of solid oxide electrodes for electrochemical deNOx by addition of NOx storage compounds to the electrodes. Two different composite electrodes, La0.85Sr0.15MnO3-δ-Ce0.9Gd0.1O1.95 (LSM15-CGO10) and La0.85Sr0.15FeO3-δ-Ce0.9Gd0.1O......1.95 (LSF15-CGO10), have been investigated in combination with three different NOx storage compounds: BaO, K2O and MnOx. The main focus in the investigation has been on conversion measurements and electrochemical characterization, the latter by means of electrochemical impedance spectroscopy...

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

    Energy Technology Data Exchange (ETDEWEB)

    Harold, Michael [Univ. of Houston, TX (United States); Crocker, Mark [Univ. of Kentucky, Lexington, KY (United States); Balakotaiah, Vemuri [Univ. of Houston, TX (United States); Luss, Dan [Univ. of Houston, TX (United States); Choi, Jae-Soon [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Dearth, Mark [Ford Motor Company, Dearborn, MI (United States); McCabe, Bob [Ford Motor Company, Dearborn, MI (United States); Theis, Joe [Ford Motor Company, Dearborn, MI (United States)

    2013-09-30

    Oxides of nitrogen in the form of nitric oxide (NO) and nitrogen dioxide (NO2) commonly referred to as NOx, is one of the two chemical precursors that lead to ground-level ozone, a ubiquitous air pollutant in urban areas. A major source of NOx} is generated by equipment and vehicles powered by diesel engines, which have a combustion exhaust that contains NOx in the presence of excess O2. 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 NOx. Two catalytic technologies that have emerged as effective for NOx abatement are NOx 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 NOx. 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

  1. Selective Catalytic Reduction of NOx over Copper-based Microporous Catalysts

    NARCIS (Netherlands)

    Deka, U.

    2013-01-01

    Increasing concerns in our society regarding the release of harmful gasses into the atmosphere have led to the development and implementation of various technologies that curb the amount of pollutants released from various sources. Heterogeneous catalysts have made a major contribution in the

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

    Science.gov (United States)

    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

  3. Catalytic reduction of NOx in gasoline engine exhaust over copper- and nickel-exchanged X-zeolite catalysts

    International Nuclear Information System (INIS)

    Bhattacharyya, S.; Das, R.K.

    2001-01-01

    Catalytic removal of NO x in engine exhaust gases can be accomplished by non-selective reduction, selective reduction and decomposition. Noble metals are extensively used for non-selective reduction of NO x and up to 90% of engine NO x emissions can be reduced in a stoichiometric exhaust. This requirement of having the stoichiometric fuel-air ratio acts against efficiency improvement of engines. Selective NO x reduction in the presence of different reductants such as, NH 3 , urea or hydrocarbons, requires close control of the amount of reductant being injected which otherwise may be emitted as a pollutant. Catalytic decomposition is the best option for NO x removal. Nevertheless, catalysts which are durable, economic and active for NO x reduction at normal engine exhaust temperature ranges are still being investigated. Three catalysts based on X-zeolite have been developed by exchanging the Na+ ion with copper, nickel and copper-nickel metal ions and applied to the exhaust of a stationary gasoline engine to explore their potential for catalytic reduction of NO x under a wide range of engine and exhaust conditions. Some encouraging results have been obtained. The catalyst Cu-X exhibits much better NO x reduction performance at any temperature in comparison to Cu-Ni-X and Ni-X; while Cu-Ni-X catalyst exhibits slightly better performance than Ni-X catalyst. Maximum NO x efficiency achieved with Cu-X catalyst is 59.2% at a space velocity (sv) of 31 000 h -1 ; while for Cu-Ni-X and Ni-X catalysts the equivalent numbers are 60.4% and 56% respectively at a sv of 22 000 h -1 . Unlike noble metals, the doped X-zeolite catalysts exhibit significant NO x reduction capability for a wide range of air/fuel ratio and with a slower rate of decline as well with increase in air/fuel ratio. (author)

  4. Heteropoly acid promoted catalyst for SCR of NOx with ammonia

    DEFF Research Database (Denmark)

    2012-01-01

    The present invention concerns the selective removal of nitrogen oxides (NOx) from gases. In particular, the invention concerns a process, a highly alkali metal resistant heteropoly acid promoted catalyst and the use of said catalyst for removal of NOx from exhaust or flue gases, said gases...... comprising alkali or earth alkali metals. Such gases comprise for example flue gases arising from the burning of biomass, combined biomass and fossil fuel, and from waste incineration units. The process comprises the selective catalytic reduction (SCR) of NOx, such as nitrogen dioxide (NO2) and nitrogen...

  5. Preparation and Performance of Modified Red Mud-Based Catalysts for Selective Catalytic Reduction of NOx with NH3

    Directory of Open Access Journals (Sweden)

    Jingkun Wu

    2018-01-01

    Full Text Available Bayer red mud was selected, and the NH3-SCR activity was tested in a fixed bed in which the typical flue gas atmosphere was simulated. Combined with XRF, XRD, BET, SEM, TG and NH3-Temperature Programmed Desorption (TPD characterization, the denitration characteristics of Ce-doped red mud catalysts were studied on the basis of alkali-removed red mud. The results showed that typical red mud was a feasible material for denitration catalyst. Acid washing and calcining comprised the best treatment process for raw red mud, which reduced the content of alkaline substances, cleared the catalyst pore and optimized the particle morphology with dispersion. In the temperature range of 300–400 °C, the denitrification efficiency of calcined acid washing of red mud catalyst (ARM was more than 70%. The doping of Ce significantly enhanced NH3 adsorption from weak, medium and strong acid sites, reduced the crystallinity of α-Fe2O3 in ARM, optimized the specific surface area and broadened the active temperature window, which increased the NOx conversion rate by an average of nearly 20% points from 250–350 °C. The denitration efficiency of Ce0.3/ARM at 300 °C was as high as 88%. The optimum conditions for the denitration reaction of the Ce0.3/ARM catalyst were controlled as follows: Gas Hourly Space Velocity (GHSV of 30,000 h−1, O2 volume fraction of 3.5–4% and the NH3/NO molar ratio ([NH3/NO] of 1.0. The presence of SO2 in the feed had an irreversible negative effect on the activity of the Ce0.3/ARM catalyst.

  6. Novel low temperature NOx storage-reduction catalysts for diesel light-duty engine emissions based on hydrotalcite compounds

    International Nuclear Information System (INIS)

    Fornasari, G.; Trifiro, F.; Vaccari, A.; Prinetto, F.; Ghiotti, G.; Centi, G.

    2002-01-01

    A series of Pt and Pt,Cu supported catalysts were prepared by wet impregnation of Mg-Al supports obtained from hydrotalcite-type (HT) precursor compounds. These novel NO x storage-reduction (NO x SR) catalysts show improved performances in NO x storage than Pt,Ba/alumina NO x SR catalysts at reaction temperatures lower than 200C. These catalysts show also improved resistance to deactivation by SO 2 . The effect is attributed to the formation of well dispersed Mg(Al)O particles which show good NO x storage properties. The promoted low temperature activity is explained by the lower basicity of the Mg(Al)O mixed oxide in comparison to BaO, which induces on one hand a lower inhibition on Pt activity (NO to NO 2 oxidation and/or hydrocarbon oxidation) due to electronic effect, and on the other hand a lower thermal stability of the stored NO x . The presence of Cu slightly inhibits activity at low temperature, although improves activity and resistance to deactivation at 300C. On these catalysts FT-IR characterization evidences the formation of a Pt-Cu alloy after reduction

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

    Science.gov (United States)

    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. Copyright © 2015 Elsevier B.V. All rights reserved.

  8. Modeling the selective catalytic reduction of NOx by ammonia over a Vanadia-based catalyst from heavy duty diesel exhaust gases

    International Nuclear Information System (INIS)

    Yun, Byoung Kyu; Kim, Man Young

    2013-01-01

    A numerical simulation for prediction of NO X conversion over a commercial V 2 O 5 catalyst with NH 3 as a reductant was performed for a heavy duty diesel engine applications. The chemical behaviors of the SCR reactor are described by using the global NO X kinetics including standard, fast, and NH 3 oxidation reactions with the Langmuir–Hinshelwood (LH) mechanism incorporated into the commercial Boost code. After introducing mathematical models for the SCR reaction with specific reaction parameters, the effects of various parameters such as space velocities, the O 2 , H 2 O, NO 2 , and NH 3 concentrations on the NOx conversion are thoroughly studied and validated by comparing with the experimental data available in the literature. It is found that NO X conversion increases with decreasing space velocity, H 2 O concentration, and NH 3 /NO X ratio, and increasing O 2 concentration and NO 2 /NO X ratio. The study shows that not only is the present approach adopted is flexible in treating performance of the commercial V 2 O 5 based SCR catalyst, it is also accurate and efficient for the prediction of NO X conversion in diesel exhaust environments. - Highlights: ► To find the reaction parameters for LH mechanism over a commercial V2O5 catalyst. ► To investigate the effects of various parameters on the SCR NO X conversion. ► To present benchmark solutions on SCR behavior with diesel exhaust environments.

  9. Selective catalytic reduction of NOx in lean-burn engine exhaust over a Pt/V/MCM-41 catalyst

    International Nuclear Information System (INIS)

    Jeon, Jong Yeol; Kim, Hee Young; Woo, Seong Ihl

    2003-01-01

    The activities of Pt supported on various metal-substituted MCM-41 (V-, Ti-, Fe-, Al-, Ga-, La-, Co-, Mo-, Ce-, and Zr-MCM-41) and V-impregnated MCM-41 were investigated for the reduction of NO by C 3 H 6 . Among these catalysts, Pt supported on V-impregnated MCM-41 showed the best activity. The maximum conversion of NO into N 2 +N 2 O over this Pt/V/MCM-41 catalyst (Pt=1wt.%, V=3.8wt.%) was 73%, and this maximum conversion was sustained over a temperature range of 70C from 270 to 340C. The high activity of Pt/V/MCM-41 over a broad temperature range resulted from two additional reactions besides the reaction occurring on usual supported Pt, the reaction of NO with surface carbonaceous materials, and the reaction of NO occurring on support V-impregnated MCM-41. The former additional reaction showed an oscillation characteristic, a phenomenon in which the concentrations of parts of reactant and product gases oscillate continuously. At low temperature, some water vapor injected into the reactant gas mixture promoted the reaction occurring on usual supported Pt, whereas at high temperature, it suppressed the additional reaction related to carbonaceous materials. Five-hundred parts per million of SO 2 added to the reactant gas mixture only slightly decreased the NO conversion of Pt/V/MCM-41

  10. Alternative alkali resistant deNOx catalysts

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Kristensen, Steffen Buus; Due-Hansen, Johannes

    2012-01-01

    by onepot sol–gel method. All catalysts were characterized by BET, XRPD and NH3-TPD. Initial SCR activities of 8 out of 9 catalysts showed higher NO conversion at least at one temperature in the temperature range 300–500 ◦C compared to the conventional V2O5-WO3/TiO2 catalyst. After potassium poisoning (100......Alternative alkali resistant deNOx catalysts were prepared using three different supports ZrO2, TiO2 and Mordenite zeolite. The majority of the catalysts were prepared by incipient wetness impregnation of a commercial support, with vanadium, copper or iron precursor, one catalyst was prepared......–130 µmol of K/g of catalyst) the relative drop in SCR activity and acidity was lower for all the alternative catalysts compared to the industrial V2O5-WO3/TiO2 catalyst. Furthermore, Cu/MOR and Nano-V2O5/Sul-TiO2 catalysts showed 8–16 times higher SCR activities than the conventional even after high...

  11. NOx reduction using biomass as reburning fuel

    Energy Technology Data Exchange (ETDEWEB)

    Niu Sheng-li; Lu Chun-mei; Gao Pan; Han Kui-hua; Geng Ping; Cheng Zhong-jie [Shandong University, Jinan (China). School of Energy and Power Engineering

    2008-10-15

    A series of experiments were conducted in a multiple-functional combustion test bed with several kinds of biomass as reburning fuel to reduce NOx. The character and experimental parameters are, emphasized to examine the influences on NOx reduction. The results show that biomass could get about 55% to 70% NOx reduction. Within a certain range of the parameters tested, NOx reduction increases with the increasing temperature of reburning zone and initial concentration of NOx and with decreasing excess air ratio and diameter of fuel particle. Under the same test conditions, cornstalk gets the highest NOx reduction and wheat straw, peanut shell, wood chip follow in turn. 14 refs., 7 figs., 1 tab.

  12. Congressionally Directed Project for Passive NOx Removal Catalysts Research

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, William [Univ. of Notre Dame, IN (United States)

    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.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    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.

  15. Outstanding low temperature HC-SCR of NOx over platinum-group catalysts supported on mesoporous materials expecting diesel-auto emission regulation

    International Nuclear Information System (INIS)

    Komatsu, Tamikuni; Tomokuni, Keizou; Yamada, Issaku

    2006-01-01

    Outstanding low temperature HC-SCR of NOx over platinum-group catalysts supported on mesoporous materials, which does not rely on the conventional NOx-absorption-reduction-catalysts, is presented for the purpose of de-NOx of diesel-auto emissions. The established catalysts basically consist of mesoporous silica or metal-substituted mesoporous silicates for supports and platinum for active species, which is operated under lean- and rich-conditions. The new catalysts are very active at 150-200 o C and free from difficult problems of SOx-deactivation and hydrothermal ageing of the NOx-absorption-reduction catalyst. (author)

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

    Directory of Open Access Journals (Sweden)

    Ralf Moos

    2011-08-01

    Full Text Available 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.

  17. Utilization of Common Automotive Three-Way NOx Reduction Catalyst for Managing Off- Gas from Thermal Treatment of High-Nitrate Waste - 13094

    International Nuclear Information System (INIS)

    Foster, Adam L.; Ki Song, P.E.

    2013-01-01

    Studsvik's Thermal Organic Reduction (THOR) steam reforming process has been tested and proven to effectively treat radioactive and hazardous wastes streams with high nitrate contents to produce dry, stable mineral products, while providing high conversion (>98%) of nitrates and nitrites directly to nitrogen gas. However, increased NO x reduction may be desired for some waste streams under certain regulatory frameworks. In order to enhance the NO x reduction performance of the THOR process, a common Three-Way catalytic NO x reduction unit was installed in the process gas piping of a recently completed Engineering Scale Technology Demonstration (ESTD). The catalytic DeNO x unit was located downstream of the main THOR process vessel, and it was designed to catalyze the reduction of residual NO x to nitrogen gas via the oxidation of the hydrogen, carbon monoxide, and volatile organic compounds that are inherent to the THOR process gas. There was no need for auxiliary injection of a reducing gas, such as ammonia. The unit consisted of four monolith type catalyst sections positioned in series with a gas mixing section located between each catalyst section. The process gas was monitored for NO x concentration upstream and downstream of the catalytic DeNO x unit. Conversion efficiencies ranged from 91% to 97% across the catalytic unit, depending on the composition of the inlet gas. Higher concentrations of hydrogen and carbon monoxide in the THOR process gas increased the NO x reduction capability of the catalytic DeNO x unit. The NO x destruction performance of THOR process in combination with the Three-Way catalytic unit resulted in overall system NO x reduction efficiencies of greater than 99.9% with an average NO x reduction efficiency of 99.94% for the entire demonstration program. This allowed the NO x concentration in the ESTD exhaust gas to be maintained at less than 40 parts per million (ppm), dry basis with an average concentration of approximately 17 ppm, dry

  18. Influence of zeolite structure on the activity and durability of Co-Pd-zeolite catalysts in the reduction of NOx with methane

    International Nuclear Information System (INIS)

    Pieterse, J.A.Z.; Van den Brink, R.W.; Booneveld, S.; De Bruijn, F.A.

    2003-01-01

    Selective catalytic reduction of NO with CH 4 was studied over ZSM-5, MOR, FER and BEA zeolite-based cobalt (Co) and palladium (Pd) catalysts in the presence of oxygen and water. As compared to other catalytic systems reported in literature for CH 4 -SCR in the presence of water, zeolite supported Co-Pd combination catalysts are very active and selective. The most active catalysts, based on MOR and ZSM-5, are characterised by well-dispersed Pd ions in the zeolite that activate methane. Wet ion exchange is a good method to achieve high dispersion of Pd provided that it is carried out in a competitive manner. The presence of cobalt (Co 3 O 4 , Co-oxo ions) boosts SCR activity by oxidising NO to NO 2 . The activity of the zeolite-based Co-Pd combination catalysts decreases with prolonged times on stream. The severity of the deactivation was found to be different for different zeolite topologies. The characterisation and evaluation of freshly calcined catalysts and spent catalysts show two things that occur during reaction: (1) zeolite solvated metal cations disappear in favour of (inactive) metal oxides and presumably larger metal entities, i.e. loss of dispersion; (2) loss of crystallinity affiliated with steam-dealumination and the concomitant formation of extra-framework aluminium (EFAL) in the presence of water. Both phenomena strongly depend on the (reaction) temperature. The deactivation of Co-Pd-zeolite resembles the deactivation of Pd-zeolite. Hence, future research could encompass the stabilisation of Pd (cations) in the zeolite pores by exploring additives other than cobalt. For this, detailed understanding on the siting of Pd in zeolites is important

  19. Plasma and catalyst for the oxidation of NOx

    DEFF Research Database (Denmark)

    Jögi, I.; Erme, K.; Levoll, E.

    2017-01-01

    The removal of NOx from the exhaust gases requires the oxidation of most abundant NO to NO2 or N2O5. The oxidation can be done by non-thermal plasma but the efficiency is limited due to the back-reaction of NO2 to NO by O radicals. Present contribution investigates the role of catalysts in the im......The removal of NOx from the exhaust gases requires the oxidation of most abundant NO to NO2 or N2O5. The oxidation can be done by non-thermal plasma but the efficiency is limited due to the back-reaction of NO2 to NO by O radicals. Present contribution investigates the role of catalysts...... in the improvement of oxidation efficiency based on the stationary and time-dependent studies of the NOx oxidation at different reactor configurations and experimental conditions. The plasma produced active oxygen species (O, O3) were shown to play an important role in the reactions taking place on the catalyst...... surfaces while the exact mechanism and extent of the effect depended on the reactor configuration. The effect of catalyst at different experimental conditions was quantitatively described with the aid of analytical lumped kinetic models derived for the NOx oxidation when the catalyst was directly...

  20. Two-stage Catalytic Reduction of NOx with Hydrocarbons

    Energy Technology Data Exchange (ETDEWEB)

    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. NOx Reduction Technology in Diesel Engine Exhaust by the Plasmatron

    International Nuclear Information System (INIS)

    Joa, Sang Beom

    2008-02-01

    The diesel vehicle is relatively superior to gasoline vehicle on the fuel consumption, durability and combustion efficiency. However, exhaust emissions from diesel vehicles are known to be harmful to human health and environment. An experimental study of the diesel fuel reformation by a plasmatron and diesel engine exhaust cleaning by means of plasma chemical pretreatment of fuel is described. Plasma chemical reformation of fuel was carried by a DC arc plasmatron that was fabricated to increase an ability of the gas activation. Some portion of the fuel was activated in an arc discharge and turned into the hydrogen-rich synthesis gas. The yield of reformation for the diesel fuel showed 80 % ∼ 100 % when the small quantities of fuel (flow rate up to about 6 cc/min) were reformed. The regulation for an emission from the diesel vehicle is getting more stringent, the research in the field of the in-cylinder processing technologies (pretreatment) becomes more important issue as well as the catalyst after-treatment. The used high durability plasmatron has the characteristics of low contamination level, low anode erosion rate, low plasma temperature, and effective activation of the process gas. The developed fuel reformation system with the plasmatron was connected to the air feeding inlet sleeve of the diesel engine Kookje 3T90LT-AC (Korea) in order to study the reduction of NOx content in the engine's emission. Tubular reformation chamber was connected to the engine through the heat exchanger DOVER B10Hx20/1P-SC-S. Its cooling jacket was connected in series with the cooling system of the plasmatron. At the exit of this device gas temperature did not exceed ∼40 .deg. C at plasmatron power up to 1.5 kW which seemed quite acceptable. Gas composition was studied here using RBR-Ecom KD gas analyzer. The design of the DC arc plasmatron applied for the plasma chemical fuel reformation was improved boosting the degree of fuel-air mixture activation that provided the

  2. Microwave catalytic NOx and SO{sub 2} removal using FeCu/zeolite as catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Z.S. Wei; G.H. Zeng; Z.R. Xie; C.Y. Ma; X.H. Liu; J.L. Sun; L.H. Liu [Sun Yat-sen University, Guangzhou (China). School of Environmental Science and Engineering

    2011-04-15

    Non-thermal plasma technology is a promising process for flue gas treatment. Microwave catalytic NOx and SO{sub 2} removal simultaneously has been investigated using FeCu/zeolite as catalyst. The experimental results showed that a microwave reactor with FeCu/zeolite only could be used to microwave catalytic oxidative 91.7% NOx to nitrates and 79.6% SO{sub 2} to sulfate; the reaction efficiencies of microwave catalytic reduction of NOx and SO{sub 2} in a microwave reactor with FeCu/zeolite and ammonium bicarbonate (NH{sub 4}HCO{sub 3}) as a reducing agent could be up to 95.8% and 93.4% respectively. Microwave irradiation accentuates catalytic reduction of SO{sub 2} and NOx treatment, and microwave addition can increases SO{sub 2} removal efficiency from 14.5% to 18.7%, and NOx removal efficiency from 13.4% to 18.7%, separately. FeCu/zeolite catalyst was characterized by X-ray diffraction (XRD), X-ray photoelectron spectrum analysis (XPS), scanning electron microscopy (SEM) and the Brunauer Emmett Teller (BET) method. Microwave catalytic NOx and SO{sub 2} removal follows Langmuir-Hinshelwood (L-H) kinetics. 25 refs., 7 figs., 1 tab.

  3. Integrated diesel engine NOx reduction technology development

    Energy Technology Data Exchange (ETDEWEB)

    Hoelzer, J.; Zhu, J.; Savonen, C.L. [Detroit Diesel Corp., MI (United States); Kharas, K.C.C.; Bailey, O.H.; Miller, M.; Vuichard, J. [Allied Signal Environmental Catalysts, Tulsa, OK (United States)

    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.

  4. Sulfur Deactivation of NOx Storage Catalysts: A Multiscale Modeling Approach

    Directory of Open Access Journals (Sweden)

    Rankovic N.

    2013-09-01

    Full Text Available Lean NOx Trap (LNT catalysts, a promising solution for reducing the noxious nitrogen oxide emissions from the lean burn and Diesel engines, are technologically limited by the presence of sulfur in the exhaust gas stream. Sulfur stemming from both fuels and lubricating oils is oxidized during the combustion event and mainly exists as SOx (SO2 and SO3 in the exhaust. Sulfur oxides interact strongly with the NOx trapping material of a LNT to form thermodynamically favored sulfate species, consequently leading to the blockage of NOx sorption sites and altering the catalyst operation. Molecular and kinetic modeling represent a valuable tool for predicting system behavior and evaluating catalytic performances. The present paper demonstrates how fundamental ab initio calculations can be used as a valuable source for designing kinetic models developed in the IFP Exhaust library, intended for vehicle simulations. The concrete example we chose to illustrate our approach was SO3 adsorption on the model NOx storage material, BaO. SO3 adsorption was described for various sites (terraces, surface steps and kinks and bulk for a closer description of a real storage material. Additional rate and sensitivity analyses provided a deeper understanding of the poisoning phenomena.

  5. NOx Selective Catalytic Reduction (SCR) on Self-Supported V-W-doped TiO2 Nanofibers

    DEFF Research Database (Denmark)

    Marani, Debora; Silva, Rafael Hubert; Dankeaw, Apiwat

    2017-01-01

    Electrospun V–W–TiO2 catalysts, resulting in a solid solution of V and W in the anatase phase, are prepared as nonwoven nanofibers for NOx selective catalytic reduction (SCR). Preliminary catalytic characterization indicates their superior NOx conversion efficiency to the-state-of-the-art materia...

  6. Reduction of Nitrogen Oxides using zeolite catalysts exchanged with cobalt

    International Nuclear Information System (INIS)

    Garcia M, E.A.; Bustamante L, F.; Montes de C, C.

    1999-01-01

    The Selective Catalytic Reduction (SCR) of NOx by methane in excess oxygen was studied over several zeolite catalysts; namely cobalt loaded mordenite, ferrierite, SM-5 and the corresponding acid forms. When NO2 predominated n the NOx mixture the acid forms showed the highest N2 formation rates under dry conditions. Mordenite supported catalysts were the most active ones followed by ferrierite and ZSM-5. The most active Co-Mordenite catalyst was tested using a NOx mixture, containing mostly NO, under dry conditions and in the presence of water and SO2. The addition of 8 % water to the reaction mixture lead to a reversible deactivation, mainly at low temperatures. When the reaction mixture contained 60 ppm SO2, the N2 formation rate decreased about a half likely due to SO2 poisoning

  7. NOx from cement production - reduction by primary measures

    DEFF Research Database (Denmark)

    Jensen, Lars Skaarup

    1999-01-01

    cement production processes cement is typically produced by thermally treating a mixture of limestone and clay minerals in kiln systems consisting of a rotary kiln and a calciner. Clinker burning at a temperature of about 1450 °C takes place in the internally fired rotary kiln and calcination, which...... rotary kilns, while NOx formation from fuel-N and reduction of NOx take place in calciners. NOx formation in the rotary kiln is mainly governed by the necessary clinker burning temperature and is not very amenable to control, while net NOx formation in calciners depends strongly on calciner design......, calciner operation, fuel properties and on the NOx level from the rotary kiln. The low-NOx calciner types presently marketed are based on combinations of reburning, air staging and temperature control and seem equivalent in their ability to restrict NOx formation. If fuels with a significant volatile...

  8. Amorphous saturated Cerium-Tungsten-Titanium oxide nanofibers catalysts for NOx selective catalytic reaction

    DEFF Research Database (Denmark)

    Dankeaw, Apiwat; Gualandris, Fabrizio; Silva, Rafael Hubert

    2018-01-01

    experiments at the best working conditions (dry and in absence of SO2) are performed to characterize the intrinsic catalytic behavior of the new catalysts. At temeprature lower than 300 °C, superior NOx conversion properties of the amorphous TiOx nanofibers over the crystallized TiO2 (anatase) nanofibers......Herein for the first time, Ce0.184W0.07Ti0.748O2-δ nanofibers are prepared by electrospinning to serve as catalyst in the selective catalytic reduction (SCR) process. The addition of cerium is proven to inhibit crystallization of TiO2, yielding an amorphous TiOx-based solid solution stable up...... temperatures (catalysts in a wide range...

  9. Neural networks prove effective at NOx reduction

    Energy Technology Data Exchange (ETDEWEB)

    Radl, B.J. [Pegasus Technologies, Mentor, OH (USA)

    2000-05-01

    The availability of low cost computer hardware and software is opening up possibilities for the use of artificial intelligence concepts, notably neural networks, in power plant control applications, delivering lower costs, greater efficiencies and reduced emissions. One example of a neural network system is the NeuSIGHT combustion optimisation system, developed by Pegasus Technologies, a subsidiary of KFx Inc. It can help reduce NOx emissions, improve heat rate and enable either deferral or elimination of capital expenditures. on other NOx control technologies, such as low NOx burners, SNCR and SCR. This paper illustrates these benefits using three recent case studies. 4 figs.

  10. Sulfur poisoning and regeneration of the Ag/γ-Al2O3 catalyst for H2-assisted SCR of NOx by ammonia

    DEFF Research Database (Denmark)

    Doronkin, Dmitry E.; Khan, Tuhin Suvra; Bligaard, Thomas

    2012-01-01

    Sulfur poisoning and regeneration mechanisms for a 2% Ag/γ-Al2O3 catalyst for the H2-assisted selective catalytic reduction of NOx by NH3 are investigated. The catalyst has medium sulfur tolerance at low temperatures, however a good capability of regeneration at 670°C under lean conditions when H...

  11. Experimental research of technology activating catalysts for SCR DeNOx in boiler

    Science.gov (United States)

    Zeng, Xi; Yang, Zhengde; Li, Yan; Chen, Donglin

    2018-01-01

    In order to improve activity of the catalysts used in SCR DeNOx system of flue gas, a series of catalysts activated by different activating liquids under varied conditions in boiler directly were conducted. Then these catalysts were characterized by SEM, FT-IR and BET technology. And NO conversions of the activated catalysts were studied and compared with that of inactivated catalyst. The above experiment shows that NO conversion of the activated catalyst can be up to 99%, which 30% higher than that of inactivated catalyst, so activity of catalysts were improved greatly. Furthermore, optimal activating liquid labeled L2 and effective technology parameters were gained in the experiment.

  12. Alternative catalysts and technologies for NOx removal from biomass- and wastefired plants

    DEFF Research Database (Denmark)

    Schill, Leonhard

    removed with the selective catalytic reduction (SCR) using a vanadia-tungsta-titania (VWT) catalyst and ammonia (NH3) as reductant. For application in coal- and gas-red power plants this technology is mature. However, when ring biomass the ue gas contains potassium in large amounts which deactivates....... The deNOx activity over Ag/Al2O3 used in ethanol-SCR is practically as much reduced as in the NH3-SCR case over the traditional VWT catalyst. Furthermore, poisoning with potassium leads to unselective oxidation of the hydrocarbons instead of NO reduction and SO2 concentrations as low as 20 ppm can....... At 150 C, in the presence of 10 % H2O, the catalyst under patenting matches the activity of the commercial VWT one at 220 C. However, ue gases at the tail-end position can contain up to 20 % H2O, increasing the temperature of activity parity to 180 C. Furthermore, the catalyst is also sensitive to SO2...

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

    Science.gov (United States)

    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. Copyright © 2014. Published by Elsevier B.V.

  14. NOx Emission Reduction by Oscillating Combustion

    Energy Technology Data Exchange (ETDEWEB)

    None

    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.

  15. Soot oxidation over NOx storage catalysts. Activity and deactivation

    International Nuclear Information System (INIS)

    Krishna, K.; Makkee, M.

    2006-01-01

    Soot oxidation activity and deactivation of NO x storage and reduction (NSR) catalysts containing Pt, K, and Ba supported on Al 2 O 3 , are studied under a variety of reaction conditions. K-containing catalysts decrease soot oxidation temperature with O 2 alone and the presence of Pt further enhance the activity due to synergetic effect. The active species responsible for synergism on Pt/K-Al 2 O 3 are unstable and cannot be regenerated. Soot oxidation temperature decreases by about 150 o C with NO+O 2 exhaust feed gas and under lean conditions NSR system acts as catalysed soot filter (CSF). The reactions that are mainly responsible for decreasing soot oxidation temperature are: (1) soot oxidation with NO 2 followed by NO recycles to NO 2 , and (2) soot oxidation with O 2 assisted by NO 2 . Only a part of the stored NO x that is decomposed at high temperatures under lean conditions is found to be useful for soot oxidation. NO x storage capacity of NSR catalysts decreases upon ageing under soot oxidising conditions. This will lead to a decreased soot oxidation activity on stored nitrate decomposition. Pt/K-Al 2 O 3 catalyst is more active, but least stable compared with Pt/Ba-Al 2 O 3 . (author)

  16. Physico-Chemical and Structural Properties of DeNOx and SO2 Oxidation Catalysts

    DEFF Research Database (Denmark)

    Masters, Stephen Grenville; Oehlers, Cord; Nielsen, Kurt

    1996-01-01

    Commercial catalysts for NOx removal and SO2 oxidation and their model systems have been investigated by spectroscopic, thermal, electrochemical and X-ray methods. Structural information on the vanadium complexes and compounds as well as physico-chemical properties for catalyst model systems have...

  17. COST OF SELECTIVE CATALYTIC REDUCTION (SCR) APPLICATION FOR NOX CONTROL ON COAL-FIRED BOILERS

    Science.gov (United States)

    The report provides a methodology for estimating budgetary costs associated with retrofit applications of selective catalytic reduction (SCR) technology on coal-fired boilers. SCR is a postcombustion nitrogen oxides (NOx) control technology capable of providing NOx reductions >90...

  18. Alkali resistant Cu/zeolite deNOx catalysts for flue gas cleaning in biomass fired applications

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Riisager, Anders; Fehrmann, Rasmus

    2011-01-01

    to investigate the redox and acidic properties of the catalysts. The poisoning resistivity seems to be due to a combination of high surface area and strong acidity of the Cu/zeolite catalysts. The catalysts might be attractive alternatives to conventional catalysts for deNOx of flue gases from biomass fired...... power plants and other stationary industrial installations....

  19. NOx reduction in Opole power plant

    International Nuclear Information System (INIS)

    Higgins, B.; Gong, B.; Pozzobon, E.; Kinal, E.; Pilipionek, J.

    2010-01-01

    In 2008 PGE Elektrownia Opole ordered a 'turn-key' retrofit execution of the combustion system to reduce NO x emission at BP-1150 boiler. The project includes modifications of burners as a first stage, and then ROFA system installation for combustion optimization and primary reduction of NO x , and Rotamix system installation for the further, secondary NO x reduction. The condition to install ROFA and Rotamix systems was keeping the same parameters of the power unit operation, in particular CO emission level, fly ash LOI and bottom ash LOI, ammonia slip, ambient noise, boiler availability and efficiency, material wastage rate, steam flow rate and temperature, as well as consumption of urea, water, electricity and compressed air. The work for this project was performed by a consortium that included Nalco Mobotec, Remak-Rozruch (a Consortium Leader) and SEFAKO

  20. Possibilities for the reduction of NOx emissions

    International Nuclear Information System (INIS)

    Marx, E.

    1993-01-01

    Nitrogen oxides develop mainly in the combustion of fossil fuels based on three mechanisms: process-dependent thermal NO; prompt NO as well as fuel-dependent NO. The reaction either takes places in the area of the root of the flame or with the combustion gases. A main effect on the amount of developing nitrogen oxides have the fuel, the burner design as well as the heat generator. In the last years considerable emission reductions were attained mainly by design changes of the burner, e.g. gas burners with internal circulation, burners with external exhaust gas recirculation, burners with internal recirculation. (BWI) [de

  1. NOx reduction by compact electron beam processing

    International Nuclear Information System (INIS)

    Penetrante, B.M.; Hsiao, M.C.; Merritt, B.T.; Wallman, P.H.; Vogtlin, G.E.

    1995-01-01

    Among the new methods being investigated for the post-combustion removal of nitrogen oxides (NO x ) are based on non-thermal plasmas. These plasmas can be produced by electrical discharge methods or electron beam irradiation. The application of electron beam irradiation for NO x removal in power plant flue gases has been investigated since the early 1970's in both laboratory- and pilot-scale experiments. Electrical discharge methods are relatively new entrants in the field of flue gas cleanup. Pulsed corona and dielectric-barrier discharge techniques are two of the more commonly used electrical discharge methods for producing nonthermal plasmas at atmospheric pressure. There are basically two types of reactions responsible for the depletion of NO by non-thermal plasmas: oxidation and reduction

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

    Science.gov (United States)

    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.

  3. Plasma and catalyst for the oxidation of NOx

    DEFF Research Database (Denmark)

    Jõgi, Indrek; Erme, Kalev; Levoll, Erik

    2018-01-01

    . In the case of indirect oxidation, only ozone could reach the catalyst surface and improve the oxidation of NO2 to N2O5. The effect of catalyst at different experimental conditions was quantitatively described with the aid of simple global chemical kinetic models derived for the NO x oxidation either...... by plasma or ozone. The models allowed to compare the effect of different catalysts and to analyze the limitations for the efficiency improvement by catalyst....... to NO mediated by O radicals in plasma. Indirect NO oxidation by plasma produced ozone allows to circumvent the back-reaction and further oxidize NO2 to N2O5 but the slow reaction rate for the latter process limits the efficiency of this process. Present paper gives an overview of the role of metal...

  4. Plasma and catalyst for the oxidation of NOx

    Science.gov (United States)

    Jõgi, Indrek; Erme, Kalev; Levoll, Erik; Raud, Jüri; Stamate, Eugen

    2018-03-01

    Efficient exhaust gas cleaning from NO x (NO and NO2) by absorption and adsorption based methods requires the oxidation of NO. The application of non-thermal plasma is considered as a promising oxidation method but the oxidation of NO by direct plasma remains limited due to the back-reaction of NO2 to NO mediated by O radicals in plasma. Indirect NO oxidation by plasma produced ozone allows to circumvent the back-reaction and further oxidize NO2 to N2O5 but the slow reaction rate for the latter process limits the efficiency of this process. Present paper gives an overview of the role of metal-oxide catalysts in the improvement of oxidation efficiency for both direct and indirect plasma oxidation of NO x . The plasma produced active oxygen species (O, O3) were shown to play an important role in the reactions taking place on the catalyst surfaces while the exact mechanism and extent of the effect were different for direct and indirect oxidation. In the case of direct plasma oxidation, both short and long lifetime oxygen species could reach the catalyst and participate in the oxidation of NO to NO2. The back-reaction in the plasma phase remained still important factor and limited the effect of catalyst. In the case of indirect oxidation, only ozone could reach the catalyst surface and improve the oxidation of NO2 to N2O5. The effect of catalyst at different experimental conditions was quantitatively described with the aid of simple global chemical kinetic models derived for the NO x oxidation either by plasma or ozone. The models allowed to compare the effect of different catalysts and to analyze the limitations for the efficiency improvement by catalyst.

  5. Generation and Reduction of NOx on Air-Fed Ozonizers

    Science.gov (United States)

    Ehara, Yoshiyasu; Amemiya, Yusuke; Yamamoto, Toshiaki

    A generation and reduction of NOx on air-fed ozonizers using a ferroelectric packed bed reactor have been experimentally investigated. The reactors packed with CaTiO3, SrTiO3 and BaTiO3 pellets are examined for ozone generation. An ac voltage is applied to the reactor to generate partial discharge. Ozone concentration and the different nitrogen oxides at downstream of the packed bed reactor were measured with UV absorption ozone monitor and a Fourier transform infrared spectroscope respectively. The dielectric constant of packed ferroelectric pellets influences the discharge characteristic, ozone and NOx generations are varied by the dielectric constant value. Focusing on a discharge pulse current and maximum discharge magnitude, the ferroelectric packed bed plasma reactors have been evaluated on nitrogen oxide and ozone generated concentrations.

  6. NOx reduction and NO2 emission characteristics in rich-lean combustion of hydrogen

    OpenAIRE

    Shudo, Toshio; Omori, Kento; Hiyama, Osamu

    2008-01-01

    Hydrogen is a clean alternative to conventional hydrocarbon fuels, but it is very important to reduce the nitrogen oxides (NOx) emissions generated by hydrogen combustion. The rich-lean combustion or staged combustion is known to reduce NOx emissions from continuous combustion burners such as gas turbines and boilers, and NOx reduction effects have been demonstrated for hydrocarbon fuels. The authors applied rich-lean combustion to a hydrogen gas turbine and showed its NOx reduction effect in...

  7. INDUSTRIAL BOILER RETROFIT FOR NOX CONTROL: COMBINED SELECTIVE NONCATALYTIC REDUCTION AND SELECTIVE CATALYTIC REDUCTION

    Science.gov (United States)

    The paper describes retrofitting and testing a 590 kW (2 MBtu/hr), oil-fired, three-pass, fire-tube package boiler with a combined selective noncatalytic reduction (SNCR) and selective catalytic reduction (SCR) system. The system demonstrated 85% nitrogen oxides (NOx) reduction w...

  8. NOx and N2O emission control with catalyst's

    International Nuclear Information System (INIS)

    Hiltunen, M.

    1994-01-01

    Due to the increasingly stringent emission regulations, new technologies are needed to be developed for improving emission control in circulating fluidized-bed boilers. The objective of this project is to test the concept of using catalysts for NO x and N 2 O emission control. N 2 O emission is in the range of 30 - 100 ppm from fluidized bed combustors burning coal. Since it is a greenhouse gas an effective means of controlling N 2 O emission is needed

  9. Evaluating the NOx Storage Catalysts (NSC Aging: A Preliminary Analytical Study with Electronic Microscopy

    Directory of Open Access Journals (Sweden)

    Leonarda Bellebuono

    2017-10-01

    Full Text Available This paper describes an expeditious and reliable method for determining the thermal effects in a static condition of commercial NOx storage catalysts (NSCs using scanning electron microscopy with an energy dispersive X-ray analytical system (SEM/EDS. It is worth remarking that possible changes in the morphology and in the elemental composition of the catalyst may be considered as the most important causes of the lower conversion of NOx. The information attained in this work indicates that Pt nanoparticle sintering is strongly increased by the oxygen exposure, and this can be considered a very useful preliminary investigation for the studies already present in the literature on the efficiency of NSCs.

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

    Science.gov (United States)

    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.

  11. Catalytic Reduction of NO and NOx Content in Tobacco Smoke

    Directory of Open Access Journals (Sweden)

    Cvetkovic N

    2014-12-01

    Full Text Available In order to reduce the nitric oxide (NO and nitrogen oxides (NO content in mainstream tobacco smoke, a new class of catalyst based on Cu-ZSM-5 zeolite has been synthesized. The effectiveness of the new catalyst (degree of reduction and specific catalytic ability was tested both by adding Cu-ZSM-5 zeolite directly to the tobacco blend and by addition to the filter. We have determined that adding the catalyst to the tobacco blend does not cause any changes in the physical, chemical or organoleptic properties of the cigarette blend. But, the addition reduces the yield of nitrogen oxides while having no influence on nicotine and “tar” content in the tobacco smoke of the modified blend. The catalyst addition increases the static burning rate (SBR. The changes in the quantity of NO and NOmay be explained by changes in burning conditions due to the increase of Oobtained from catalytic degradation of NO and NO, and adsorptive and diffusive properties of the catalyst. The changes in mainstream smoke analytes are also given on a puff-by-puff basis.

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

    Science.gov (United States)

    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. DeNOx Abatement over Sonically Prepared Iron-Substituted Y, USY and MFI Zeolite Catalysts in Lean Exhaust Gas Conditions

    Science.gov (United States)

    Stachurska, Patrycja; Kuterasiński, Łukasz; Dziedzicka, Anna; Górecka, Sylwia; Chmielarz, Lucjan; Łojewska, Joanna; Sitarz, Maciej

    2018-01-01

    Iron-substituted MFI, Y and USY zeolites prepared by two preparation routes—classical ion exchange and the ultrasound modified ion-exchange method—were characterised by micro-Raman spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), and ultraviolet (UV)/visible diffuse reflectance spectroscopy (UV/Vis DRS). Ultrasound irradiation, a new technique for the preparation of the metal salt suspension before incorporation to the zeolite structure, was employed. An experimental study of selective catalytic reduction (SCR) of NO with NH3 on both iron-substituted reference zeolite catalysts and those prepared through the application of ultrasound conducted during an ion-exchange process is presented. The prepared zeolite catalysts show high activity and selectivity in SCR deNOx abatement. The MFI-based iron catalysts, especially those prepared via the sonochemical method, revealed superior activity in the deNOx process, with almost 100% selectivity towards N2. The hydrothermal stability test confirmed high stability and activity of MFI-based catalysts in water-rich conditions during the deNOx reaction at 450 °C. PMID:29301370

  14. On the Effect of Preparation Methods of PdCe-MOR Catalysts as NOx CH4-SCR System for Natural Gas Vehicles Application

    Directory of Open Access Journals (Sweden)

    Acácio Nobre Mendes

    2015-10-01

    Full Text Available In the present work, the effect of several parameters involved in the preparation of PdCe-HMOR catalysts active for NOx selective catalytic reduction with methane (NOx CH4-SCR was studied. Results show that the catalytic performance of Pd-HMOR is better when palladium is introduced by ion-exchange, namely at room temperature. It was also shown that Pd loading does not influence the formation of cerium species, namely surface Ce4+ (CeO2 species and CeO2 species in interaction with Pd. However, when Ce is introduced before Pd, more surface CeO2 species are stabilized in the support and less CeO2 become in interaction with Pd, which results in a worse NOx CH4-SCR catalytic performance.

  15. Investigation of NOx Reduction by Low Temperature Oxidation Using Ozone Produced by Dielectric Barrier Discharge

    DEFF Research Database (Denmark)

    Stamate, Eugen; Irimiea, Cornelia; Salewski, Mirko

    2013-01-01

    NOx reduction by low temperature oxidation using ozone produced by a dielectric barrier discharge generator is investigated for different process parameters in a 6m long reactor in serpentine arrangement using synthetic dry flue gas with NOx levels below 500 ppm, flows up to 50 slm and temperatures...

  16. Storage of Nitrous Oxide (NOx in Diesel Engine Exhaust Gas using Alumina-Based Catalysts: Preparation, Characterization, and Testing

    Directory of Open Access Journals (Sweden)

    A. Alsobaai

    2017-03-01

    Full Text Available This work investigated the nitrous oxide (NOx storage process using alumina-based catalysts (K2 O/Al2 O3 , CaO/Al2 O3,  and BaO/Al2 O3 . The feed was a synthetic exhaust gas containing 1,000 ppm of nitrogen monoxide (NO, 1,000 ppm i-C4 H10 , and an 8% O2  and N2  balance. The catalyst was carried out at temperatures between 250–450°C and a contact time of 20 minutes. It was found that NOx was effectively adsorbed in the presence of oxygen. The NOx storage capacity of K2 O/Al2 O3 was higher than that of BaO/Al2 O3.  The NOx storage capacity for K2 O/Al2 O3  decreased with increasing temperature and achieved a maximum at 250°C. Potassium loading higher than 15% in the catalyst negatively affected the morphological properties. The combination of Ba and K loading in the catalyst led to an improvement in the catalytic activity compared to its single metal catalysts. As a conclusion, mixed metal oxide was a potential catalyst for de-NOx process in meeting the stringent diesel engine exhaust emissions regulations. The catalysts were characterized by a number of techniques and measurements, such as X-ray diffraction (XRD, electron affinity (EA, a scanning electron microscope (SEM, Brunner-Emmett-Teller (BET to measure surface area, and pore volume and pore size distribution assessments.

  17. Study on the mechanism of a manganese-based catalyst for catalytic NOX flue gas denitration

    Science.gov (United States)

    Zhang, Lei; Wen, Xin; Lei, Zhang; Gao, Long; Sha, Xiangling; Ma, Zhenhua; He, Huibin; Wang, Yusu; Jia, Yang; Li, Yonghui

    2018-04-01

    Manganese-based bimetallic catalysts were prepared with self-made pyrolysis coke as carrier and its denitration performance of low-temperature SCR (selective catalyst reduction) was studied. The effects of different metal species, calcination temperature, calcination time and the metal load quantity on the denitration performance of the catalyst were studied by orthogonal test. The denitration mechanism of the catalyst was analyzed by XRD (X-ray diffraction), SEM (scanning electron microscope), BET test and transient test. The experiments show that: * The denitration efficiency of Mn-based bimetallic catalysts mainly relates to the metal type, the metal load quantity and the catalyst adjuvant type. * The optimal catalyst preparation conditions are as follows: the load quantity of monometallic MnO2 is 10%, calcined at 300°C for 4h, and then loaded with 8% CeO2, calcined at 350°Cfor 3h. * The denitration mechanism of manganese-based bimetallic oxide catalysts is stated as: NH3 is firstly adsorbed by B acid center Mn-OH which nears Mn4+==O to form NH4+, NH4+ was then attacked by the gas phase NO to form N2, H2O and Mn3+-OH. Finally, Mn3+-OH was oxidized by O2 to regenerate Mn4+.

  18. Study on the mechanism of a manganese-based catalyst for catalytic NOX flue gas denitration

    Directory of Open Access Journals (Sweden)

    Lei Zhang

    2018-04-01

    Full Text Available Manganese-based bimetallic catalysts were prepared with self-made pyrolysis coke as carrier and its denitration performance of low-temperature SCR (selective catalyst reduction was studied. The effects of different metal species, calcination temperature, calcination time and the metal load quantity on the denitration performance of the catalyst were studied by orthogonal test. The denitration mechanism of the catalyst was analyzed by XRD (X-ray diffraction, SEM (scanning electron microscope, BET test and transient test. The experiments show that: ① The denitration efficiency of Mn-based bimetallic catalysts mainly relates to the metal type, the metal load quantity and the catalyst adjuvant type. ② The optimal catalyst preparation conditions are as follows: the load quantity of monometallic MnO2 is 10%, calcined at 300°C for 4h, and then loaded with 8% CeO2, calcined at 350°Cfor 3h. ③ The denitration mechanism of manganese-based bimetallic oxide catalysts is stated as: NH3 is firstly adsorbed by B acid center Mn-OH which nears Mn4+==O to form NH4+, NH4+ was then attacked by the gas phase NO to form N2, H2O and Mn3+-OH. Finally, Mn3+-OH was oxidized by O2 to regenerate Mn4+.

  19. Methodology for Analysing the NOx-NH3 Trade-off for the Heavy-duty Automotive SCR Catalyst

    DEFF Research Database (Denmark)

    Åberg, Andreas; Widd, Anders; Abildskov, Jens

    2017-01-01

    This paper presents a methodology where pareto fronts were used to analyse how changes in the control structure for the urea dosing to the automotive SCR catalyst can improve the trade-o_ between NOx slip and NH3 slip. A previously developed simulation model was used to simulate the European...

  20. Fundamental limits on gas-phase chemical reduction of NOx in a plasma

    Energy Technology Data Exchange (ETDEWEB)

    Penetrante, B.M.; Hsiao, M.C.; Merritt, B.T.; Vogtlin, G.E. [Lawrence Livermore National Lab., CA (United States)

    1997-12-31

    In the plasma, the electrons do not react directly with the NOx molecules. The electrons collide mainly with the background gas molecules like N{sub 2}, O{sub 2} and H{sub 2}O. Electron impact on these molecules result partly in dissociation reactions that produce reactive species like N, O and OH. The NOx in the engine exhaust gas initially consist mostly of NO. The ground state nitrogen atom, N, is the only species that could lead to the chemical reduction of NO to N{sub 2}. The O radical oxidizes NO to NO{sub 2} leaving the same amount of NOx. The OH radical converts NO{sub 2} to nitric acid. Acid products in the plasma can easily get adsorbed on surfaces in the plasma reactor and in the pipes. When undetected, the absence of these oxidation products can often be mistaken for chemical reduction of NOx. In this paper the authors will examine the gas-phase chemical reduction of NOx. They will show that under the best conditions, the plasma can chemically reduce 1.6 grams of NOx per brake-horsepower-hour [g(NOx)/bhp-hr] when 5% of the engine output energy is delivered to the plasma.

  1. Tungstated zirconia as promising carrier for DeNOx catalysts with improved resistance towards alkali poisoning

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes; Kustov, Arkadii; Rasmussen, Søren Birk

    2006-01-01

    Use of biomass as an alternative to fossil fuels has achieved increasing interest since it is considered neutral regarding CO2 accumulation in the atmosphere. The by far most energy-efficient use of solid bio-resources in energy production is combustion in combined biomass and coal or oilfired...... of new alternative catalysts that are more resistant towards poisoning with potassium. Vanadia-based catalysts supported on traditional and tungstated zirconia has been prepared and tested in selective catalytic reduction of NO with ammonia. All prepared catalysts were characterized using N2-BET, XRD......, and NH3-TPD methods. The influence of calcination temperature of zirconia modified with tungsten oxide on the textural characteristics, acidity and catalytic performance was studied. The resistance of the catalysts towards model poisoning with potassium was found to depend dramatically...

  2. A Synthetic Pseudo-Rh: NOx Reduction Activity and Electronic Structure of Pd-Ru Solid-solution Alloy Nanoparticles

    Science.gov (United States)

    Sato, Katsutoshi; Tomonaga, Hiroyuki; Yamamoto, Tomokazu; Matsumura, Syo; Zulkifli, Nor Diana Binti; Ishimoto, Takayoshi; Koyama, Michihisa; Kusada, Kohei; Kobayashi, Hirokazu; Kitagawa, Hiroshi; Nagaoka, Katsutoshi

    2016-06-01

    Rh is one of the most important noble metals for industrial applications. A major fraction of Rh is used as a catalyst for emission control in automotive catalytic converters because of its unparalleled activity toward NOx reduction. However, Rh is a rare and extremely expensive element; thus, the development of Rh alternative composed of abundant elements is desirable. Pd and Ru are located at the right and left of Rh in the periodic table, respectively, nevertheless this combination of elements is immiscible in the bulk state. Here, we report a Pd-Ru solid-solution-alloy nanoparticle (PdxRu1-x NP) catalyst exhibiting better NOx reduction activity than Rh. Theoretical calculations show that the electronic structure of Pd0.5Ru0.5 is similar to that of Rh, indicating that Pd0.5Ru0.5 can be regarded as a pseudo-Rh. Pd0.5Ru0.5 exhibits better activity than natural Rh, which implies promising applications not only for exhaust-gas cleaning but also for various chemical reactions.

  3. The Reduction of NOx Using Pulsed Electron Beams

    Science.gov (United States)

    2015-12-30

    instantly with oxygen to form the brown gas NO2. Nitrogen dioxide is toxic . Dinitrogen trioxide (N2O3) exists as a deep blue solid (-21°C), but is... Fluoride Laser System,” Optical Engineering 47, 104202 (2008). [6] M.F. Wolford, M.C. Myers, F. Hegeler, J.D. Sethian, “NOx Removal with Multiple

  4. Model reduction of a lean NOx trap catalyst model

    NARCIS (Netherlands)

    Nauta, K.M.

    2008-01-01

    The desire to increase fuel efficiency and reduce carbon dioxide emissions of vehicles has led to an increased use of vehicles equipped with lean-burn engines, such as diesel and lean-burn gasoline engines. This type of engine uses excess oxygen when compared to the amount required to

  5. Catalyst for reduction of nitrogen oxides

    Science.gov (United States)

    Ott, Kevin C.

    2010-04-06

    A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub.2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub.2O was not detected (detection limit: 0.6 percent N.sub.2O).

  6. Filter bag De-NOx system with powder type catalysts at low temperature

    International Nuclear Information System (INIS)

    Kim, Byung-Hwan; Kim, Jeong-Heon; Kang, Pil-Sun; Yoo, Seung-Kwan; Yoon, Kyoon-Duk

    2010-01-01

    Combustion of carbon source materials (MSW, RDF, sludge, coal etc.) leads to the emission of harmful gaseous pollutants such as SO x , NO x , mercury, particulate matter, and dioxins etc. In particular, the emission of nitrogen oxides (NO x ) from the solid waste incinerator remains a serious air pollution problem. The previous research concerns have focused mainly on NO x reduction of stationary sources at high temperature SCR or SNCR process. Selective catalytic reduction (SCR) with NH 3 is the most widespread system used to control NO x emissions. However, this process suffers from several disadvantages due to the use of thermo fragile honeycomb type module and high temperature (about 300 degree Celsius) operation which consumes additional heating energy. To overcome this hurdle, filter bag De-NO x system with powder type catalysts at low temperature (less than 200 degree Celsius) has been under investigation in recent years and looks interesting because neither additional heat nor honeycomb type modules are required. Filter bag and powder type catalysts are cheap and effective materials to remove NO x at low temperature. In this study, the selective catalytic reduction of NO x was carried out on a filter support reactor with 300 mesh powder type catalysts at low temperature. The experiments were performed by powder type MnO x and V 2 O 5 / TiO 2 catalyst at low temperature ranging between 130 and 250 degree Celsius. Also, the effect of SO 2 and H 2 O on the NO conversion was investigated under our test conditions. The powder type catalysts were characterized by X-ray photoelectron spectrum (XPS) for measuring the state of oxygen on the catalyst surface and X-ray diffraction (XRD). It was observed that NO conversion of the powder type V 2 O 5 / TiO 2 catalyst was 85 % at 200 degree Celsius under presence of oxygen and that of MnO x was 50 % at the same condition. From these results, the powder type V 2 O 5 / TiO 2 catalyst showed an excellent performance on the

  7. Selective catalyst reduction light-off strategy

    Science.gov (United States)

    Gonze, Eugene V [Pinckney, MI

    2011-10-18

    An emissions control system includes a temperature determination module and an emissions control module. The temperature determination module determines a first temperature of a heater element of a diesel particulate filter (DPF) assembly in an exhaust system and determines a second temperature of a catalyst of the DPF assembly. The emissions control module selectively activates the heater element, selectively initiates a predefined combustion process in an engine based upon the first temperature, and selectively starts a reductant injection process based upon the second temperature.

  8. NOx reduction using amine reclaimer wastes (ARW) generated in post combustion CO2 capture

    DEFF Research Database (Denmark)

    Botheju, Deshai; Glarborg, Peter; Tokheim, Lars-Andre

    2012-01-01

    Amine reclaimer wastes (ARW) generated in CO2 capture processes demand suitable disposal means. Such wastes contain remaining amine, NH3 and other degradation compounds. This study investigated the potential of using ARW as a NOx reducing agent, under laboratory conditions in a flow reactor....../NO ratios (waste product, together with its demonstrated NOx reduction capability and its calorific value contribution, makes it attractive as an additive...

  9. Nature of nitrogen specie in coke and their role in NOx formation during FCC catalyst regeneration

    International Nuclear Information System (INIS)

    Babich, I.V.; Seshan, K.; Lefferts, L.

    2005-01-01

    NO x emission during the regeneration of coked fluid catalytic cracking (FCC) catalysts is an environmental problem. In order to follow the route to NO x formation and try to find ways to suppress it, a coked industrial FCC catalyst has been prepared using model N-containing compounds, e.g., pyridine, pyrrole, aniline and hexadecane-pyridine mixture. Nitrogen present in the FCC feed is incorporated as polyaromatic compounds in the coke deposited on the catalyst during cracking. Its functionality has been characterized using XPS. Nitrogen specie of different types, namely, pyridine, pyrrolic or quaternary-nitrogen (Q-N) have been discriminated. Decomposition of the coke during the catalyst regeneration (temperature programmed oxidation (TPO) and isothermal oxidation) has been monitored by GC and MS measurements of the gaseous products formed. The pyrrolic- and pyridinic-type N specie, present more in the outer coke layers, are oxidized under conditions when still large amount of C or CO is available from coke to reduced NO x formed to N 2 . ''Q-N'' type species are present in the inner layer, strongly adsorbed on the acid sites on the catalyst. They are combusted last during regeneration. As most of the coke is already combusted at this point, lack of reductants (C, CO, etc.) results in the presence of NO x in the tail gas

  10. Combustion, performance, and selective catalytic reduction of NOx for a diesel engine operated with combined tri fuel (H_2, CH_4, and conventional diesel)

    International Nuclear Information System (INIS)

    Abu-Jrai, Ahmad M.; Al-Muhtaseb, Ala'a H.; Hasan, Ahmad O.

    2017-01-01

    In this study, the effect of tri fuel (ULSD, H_2, and CH_4) operation under real exhaust gas conditions with different gaseous fuel compositions on the combustion characteristics, engine emissions, and selective catalytic reduction (SCR) after treatment was examined at low, medium, and high engine loads. Pt/Al_2O_3-SCR reactor was used and operated at different exhaust gas temperatures. Results revealed that at low load, the two gaseous fuels (H_2 and CH_4) have the same trend on combustion proccess, where both reduce the in-cylinder pressure and rate of heat release. At the high engine load there was a considerable influence appeared as an increase of the premixed combustion phase and a significant decrease of the total combustion duration. In terms of emissions, it was observed that at high engine load, fuels with high CH_4 content tend to reduce NOx formation, whereas, fuels with high H_2 content tend to reduce PM formation, moreover, combustion of tri fuel with 50:50 fuel mixture resulted in lower BSFC compared to the other ratios and hence, the best engine efficiency. The hydrocarbon-SCR catalyst has shown satisfactory performance in NOx reduction under real diesel exhaust gas in a temperature window of 180–280 °C for all engine loads. - Highlights: • Effect of tri fuel (ULSD, H_2, CH_4) on combustion and engine emissions was examined. • Fuel with high CH_4 content (H50-M50 and H25-M75) tend to reduce NOx formation. • Fuel with high H_2 content (H75-M25 and H50-M50) tend to reduce PM formation. • Increasing the percentage of H_2 in the feed gas improved the NO_x reduction. • The hydrocarbon-SCR catalyst has shown satisfactory performance in NO_x reduction.

  11. Selective catalytic reduction of NOx and N{sub 2}O by NH{sub 3} over Fe-FER; Developpement d'un traitement catalytique combine des NOx et de N{sub 2}O par NH{sub 3} sur Fe-Fer

    Energy Technology Data Exchange (ETDEWEB)

    Kieger, St. [Grande Paroisse, 76 - Grand-Quevilly (France); Navascues, L.; Gry, Ph. [Grande Paroisse, 92 - Paris la Defense (France)

    2001-07-01

    The emission of nitrogen oxides from anthropogenic activities is a major environmental issue. N{sub 2}O is taking part to the global warming and depletion of the stratospheric ozone layer, and NOx to acid rains. At the Kyoto Conference in 1997, the European Union committed itself to reduce by 8% the release of greenhouse gases at the horizon 2010. The selective catalytic reduction (SCR) of NOx by NH{sub 3} is nowadays the main control technology for the emissions from nitric acid plant. Therefore, Grande Paroisse and IRMA have developed a new catalyst (Fe-FER) for the SCR of N{sub 2}O by NH{sub 3}. The catalyst was evaluated in a pilot plant and in the same operating conditions than a DeNOx catalyst. At a space velocity of 9000 to 12000 h{sup -1}, a decomposition of 50% of N{sub 2}O was achieved at 440 deg C. Moreover for the same decomposition level, the temperature could be shifted to 390 deg C by adding ammonia, and the complete reduction of NOx was also observed. This new catalyst is rather bi-functional. Also after months of using, the catalyst did not show major loss of activity nor mechanical strength. (authors)

  12. The Use of Amine Reclaimer Wastes as a NOx Reduction Agent

    DEFF Research Database (Denmark)

    Botheju, Deshai; Glarborg, Peter; Tokheim, Lars-Andre

    2013-01-01

    that of aqueous ammonia, i.e. the most common SNCR chemical reagent used in industry (above 60% NOx reduction efficiency), ARW is nonetheless shown to possess valuable SNCR qualities (at least 20% NOx reduction efficiency) considering its availability as a waste product which has to be safely disposed. A series...... of thermo-gravimetric analyses provided important information on vaporization characteristics of amine reclaimer bottom wastes. The proposed methodology can lead to simultaneous energy and material resource recovery while primarily solving two environmental pollution problems, i.e. toxic ARW wastes...

  13. Effect of Ca-Fe oxides additives on NOx reduction in iron ore sintering

    Institute of Scientific and Technical Information of China (English)

    Zhi-yuan Yu; Xiao-hui Fan; Min Gan; Xu-ling Chen

    2017-01-01

    As the emission control regulations get stricter, the NOx reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain. The NOx emissions from the sintering machine account for 48% of total amount from the iron and steel industry.Thus, it is essential to reduce NOx emissions from the sintering machine, for the achievement of clean production of sinter.Ca-Fe oxides, serving as the main binding phase in the sinter, are therefore used as additives into the sintering mixture to reduce NOx emissions.The results show that the NOx re-duction ratio achieves 27.76% with 8% Ca-Fe oxides additives since the Ca-Fe oxides can advance the ig-nition and inhibit the nitrogen oxidation compared with the conventional condition.Meanwhile, the exist-ence of Ca-Fe oxides was beneficial to the sinter quality since they were typical low melting point com-pounds.The optimal mass fraction of Ca-Fe oxides additives should be less than 8% since the permeability of sintering bed was significantly decreased with a further increase of the Ca-Fe oxides fines, inhibiting the mineralization reaction of sintering mixture.Additionally, the appropriate particle size can be obtained when mixing an equal amount of Ca-Fe oxides additives of -0.5 mm and 0.5-3.0 mm in size.

  14. Influence of Co or Ce addition on the NOx storage and sulfur-resistance performance of the lean-burn NOx trap catalyst Pt/K/TiO{sub 2}-ZrO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Zou Zhiqiang [Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Meng, Ming, E-mail: mengm@tju.edu.cn [Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Tsubaki, Noritatsu [Department of Applied Chemistry, School of Engineering, University of Toyama, Gofuku 3190, Toyama city, Toyama 930 8555 (Japan); He Junjun; Wang Gang; Li Xingang; Zhou Xiaoyan [Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China)

    2009-10-15

    The Pt/K/TiO{sub 2}-ZrO{sub 2} catalysts promoted by Co or Ce were prepared by successive impregnation or mechanically mixing method. The influence of Co or Ce addition on the NOx storage and sulfur-resistance performance of the catalyst was investigated carefully. The techniques of XRD, FT-IR, in-situ DRIFTS, H{sub 2}-TPR and XPS were employed for catalyst characterization. The Co or Ce addition can greatly improve the NOx storage capacity of Pt/K/TiO{sub 2}-ZrO{sub 2} due to the enhanced oxidation ability and the release of more K sites. Ce addition induces higher K/Ti atomic ratio and larger NOx storage capacity as compared with Co addition. After sulfation and regeneration, the promoted catalysts shows more or less decreased NSC than Pt/K/TiO{sub 2}-ZrO{sub 2} due to the formation of more sulfates, especially for the Co-promoted catalysts, which possess better oxidation ability and facilitate the formation of large sulfates. The effect of Ce addition on Pt/K/TiO{sub 2}-ZrO{sub 2} largely depends on the addition mode. The high oxidation ability and the high K/Ti ratio of the mechanically prepared Ce-promoted catalyst make it still possess considerable NOx storage capacity (NSC) of 142 {mu}mol/g after sulfation and regeneration. With the decrease of sulfur content in fuels, the Co- and Ce-promoted catalysts possessing large NOx storage capacity, will be applicable to the purification of lean-burn NOx.

  15. Plasma-assisted heterogeneous catalysis for NOx reduction in lean-burn engine exhaust

    Energy Technology Data Exchange (ETDEWEB)

    Penetrante, B.M.; Hsaio, M.C.; Merritt, B.T.; Vogtlin, G.E. [Lawrence Livermore National Lab., CA (United States); Wan, C.Z.; Rice, G.W.; Voss, K.E. [Engelhard Corp., Iselin, NJ (United States)

    1997-12-31

    This paper discusses the combination of a plasma with a catalyst to improve the reduction of NO{sub x} under lean-burn conditions. The authors have been investigating the effects of a plasma on the NO{sub x} reduction activity and temperature operating window of various catalytic materials. One of the goals is to develop a fundamental understanding of the interaction between the gas-phase plasma chemistry and the heterogeneous chemistry on the catalyst surface. The authors have observed that plasma assisted heterogeneous catalysis can facilitate NO{sub x} reduction under conditions that normally make it difficult for either the plasma or the catalyst to function by itself. By systematically varying the plasma electrode and catalyst configuration, they have been able to elucidate the process by which the plasma chemistry affects the chemical reduction of NO{sub x} on the catalyst surface. They have discovered that the main effect of the plasma is to induce the gas-phase oxidation of NO to NO{sub 21}. The reduction of NO{sub x} to N{sub 2} is then accomplished by heterogeneous reaction of O with activated hydrocarbons on the catalyst surface. The use of a plasma opens the opportunity for a new class of catalysts that are potentially more durable, more active, more selective and more sulfur-tolerant compared to conventional lean-NO{sub x} catalysts.

  16. Multi-Stage Selective Catalytic Reduction of NOx in Lean-Burn Engine Exhaust

    National Research Council Canada - National Science Library

    Penetrante, B

    1997-01-01

    .... A plasma can also be used to oxidize NO to NO2. This paper compares the multi-stage catalytic scheme with the plasma-assisted catalytic scheme for reduction of NOx in lean-burn engine exhausts. The advantages of plasma oxidation over catalytic oxidation are presented.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  18. IR and UV gas absorption measurements during NOx reduction on an industrial natural gas fired power plant

    DEFF Research Database (Denmark)

    Stamate, Eugen; Chen, Weifeng; Jørgensen, L.

    2010-01-01

    NOx reduction of flue gas by plasma-generated ozone was investigated in pilot test experiments on an industrial power plant running on natural gas. Reduction rates higher than 95% have been achieved for a molar ratio O3:NOx slightly below two. Fourier transform infrared and ultraviolet absorption...... spectroscopy were used for spatial measurements of stable molecules and radicals along the reduction reactor. Reactions of O3 injected in the flue gas in the reduction reactor were also modeled. Experiments are in good agreement with numerical simulations. The operation costs for NOx reduction were estimated...

  19. NOx emissions and potential NOx reduction for low volatile Australian coals: End-of-grant report

    International Nuclear Information System (INIS)

    Holcombe, D.; Nelson, P.F.; Kelly, M.D.; Gupta, R.P.; Wall, T.F.

    1994-09-01

    The objective of this project was to improve the understanding of NO x formation from the combustion of low-volatile Australian coals. A secondary objective was to develop NO x reduction techniques which will improve the export market potential of these coals. Low volatile coals frequently have high nitrogen levels. In addition, they differ from high volatile coals in their behaviour in the early part of the combustion process, which largely determines the level of NO x that will be formed. Low volatile coals were examined with respect to the release of nitrogen species during the early stage of PF combustion. These species are precursors to NO x and it is at this stage of combustion that furnace conditions are important in determining whether these species become NO x or are reduced to molecular nitrogen. Pilot scale measurements of NO x concentrations from the combustion of the coals were undertaken under a range of conditions to provide data on the relevance of furnace parameters as well as of coal properties. Finally, mathematical models of coal combustion with NO x formation were developed, to be able to incorporate data on nitrogen species released from coal, and to use this information as well as furnace conditions to predict NO x concentrations. (author). Tabs., figs., refs

  20. Experimental investigation on NOx removal using pulsed dielectric barrier discharges in combination with catalysts

    NARCIS (Netherlands)

    Chirumamilla, V.R.; Hoeben, W.F.L.M.; Beckers, F.J.C.M.; Huiskamp, T.; Pemen, A.J.M.

    2015-01-01

    In this study, an experimental investigation of the removal of NOx has been carried out with a dielectric barrier discharge reactor filled with different catalytic materials. NOx removal efficiency and by-products formation were studied as a function of energy density using plasma catalytic

  1. Reduction of a Ni/Spinel Catalyst for Methane Reforming

    DEFF Research Database (Denmark)

    Kehres, Jan; Andreasen, Jens Wenzel; Fløystad, Jostein Bø

    2015-01-01

    microscopy (HRTEM) was performed on the fresh catalyst sample. The Ni particles in the fresh catalyst sample were observed to exhibit a Ni/NiO core/shell structure. A decrease of the Ni lattice parameter is observed during the reduction in a temperature interval from 413 – 453 K, which can be related...

  2. SSZ-13-supported manganese oxide catalysts for low temperature ...

    Indian Academy of Sciences (India)

    YONGZHOU YE

    Their performances for the selective catalytic reduction (SCR) of NOx with NH3 were evaluated. ... catalysts have received considerable attention.2,3 More- over, catalysts ..... zeolite channels or causing agglomeration on the cat- alyst surface ...

  3. Reduction of NOx emissions when burning low heating value gas

    International Nuclear Information System (INIS)

    Gustafsson, R.; Oskarsson, J.; Waldheim, L.

    1993-09-01

    On the gasification of nitrogen-rich fuel the nitrogen from the fuel goes into the gas phase in the form of ammonia and hydrogen cyanide and also nitrogen containing tars. When the gas is combusted the nitrogen compounds are oxidized to a great extent to NO x and, therefore, high NO x emissions can be found on the combustion of low heating value gas produced from energy forest wood chips as is also the case with direct combustion of nitrogen rich fuels. An experimental study has been carried out where the important parameters for designing a combustion chamber for low heating value gases have been studied in order to obtain maximum reduction of NO x emissions. The effect of tar cracking using dolomite on these emissions and the effect of parameters such as the addition of steam has also been tested. The tests were carried out with energy forest wood chips with 0.3% nitrogen. The gasification was carried out in a pyrolysis reactor, operated to yield a low heating value gas, and which was coupled to a simplified gas turbine combustion chamber at atmospheric pressure. The results show that the main part of the nitrogen in the fuel is found as ammonia in the low heating value gas. With this type of gasification the conversion of fuel nitrogen to ammonia in the gas is equivalent to 500-600 mg/MJ, calculated as NO 2 . Only very low amounts of hydrogen cyanide have been noted and no nitrogen containing tar components have been found. No apparent effect of steam additions has been noted. On the other hand the distribution of air in the combustion chamber and residence time during the under stoichiometric conditions are of great importance for the NO x reduction. Depending on the air distribution the emissions of NO 2 varied between 100 and 250 mg/MJ, calculated as NO 2 . 23 refs, 11 figs, 2 tabs

  4. Reducing NO(x) emissions from a nitric acid plant of domestic petrochemical complex: enhanced conversion in conventional radial-flow reactor of selective catalytic reduction process.

    Science.gov (United States)

    Abbasfard, Hamed; Hashemi, Seyed Hamid; Rahimpour, Mohammad Reza; Jokar, Seyyed Mohammad; Ghader, Sattar

    2013-01-01

    The nitric acid plant of a domestic petrochemical complex is designed to annually produce 56,400 metric tons (based on 100% nitric acid). In the present work, radial-flow spherical bed reactor (RFSBR) for selective catalytic reduction of nitric oxides (NO(x)) from the stack of this plant was modelled and compared with the conventional radial-flow reactor (CRFR). Moreover, the proficiency of a radial-flow (water or nitrogen) membrane reactor was also compared with the CRFR which was found to be inefficient at identical process conditions. In the RFSBR, the space between the two concentric spheres is filled by a catalyst. A mathematical model, including conservation of mass has been developed to investigate the performance of the configurations. The model was checked against the CRFR in a nitric acid plant located at the domestic petrochemical complex. A good agreement was observed between the modelling results and the plant data. The effects of some important parameters such as pressure and temperature on NO(x) conversion were analysed. Results show 14% decrease in NO(x) emission annually in RFSBR compared with the CRFR, which is beneficial for the prevention of NO(x) emission, global warming and acid rain.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. Spent catalyst waste management. A review. Part 1. Developments in hydroprocessing catalyst waste reduction and use

    Energy Technology Data Exchange (ETDEWEB)

    Marafi, M.; Stanislaus, A. [Petroleum Refining Department, Petroleum Research and Studies Center, Kuwait Institute for Scientific Research, P.O. Box 24885, 13109-Safat (Kuwait)

    2008-04-15

    Solid catalysts containing metals, metal oxides or sulfides, which play a key role in the refining of petroleum to clean fuels and many other valuable products, become solid wastes after use. In many refineries, the spent catalysts discarded from hydroprocessing units form a major part of these solid wastes. Disposal of spent hydroprocessing catalysts requires compliance with stringent environmental regulations because of their hazardous nature and toxic chemicals content. Various options such as minimizing spent catalyst waste generation by regeneration and reuse, metals recovery, utilization to produce useful materials and treatment for safe disposal, could be considered to deal with the spent catalyst environmental problem. In this paper, information available in the literature on spent hydroprocessing catalyst waste reduction at source by using improved more active and more stable catalysts, regeneration, rejuvenation and reuse of deactivated catalysts in many cycles, and reusing in other processes are reviewed in detail with focus on recent developments. Available methods for recycling of spent hydroprocessing catalysts by using them as raw materials for the preparation of active new catalysts and many other valuable products are also reviewed. (author)

  7. Alkali resistivity of Cu based selective catalytic reduction catalysts

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Jensen, Anker Degn; Riisager, Anders

    2012-01-01

    The deactivation of V2O5–WO3–TiO2, Cu–HZSM5 and Cu–HMOR plate type monolithic catalysts was investigated when exposed to KCl aerosols in a bench-scale reactor. Fresh and exposed catalysts were characterized by selective catalytic reduction (SCR) activity measurements, scanning electron microscope......–energy dispersive X-ray spectroscopy (SEM–EDX) and NH3-temperature programmed desorption (NH3-TPD). 95% deactivation was observed for the V2O5–WO3–TiO2 catalyst, while the Cu–HZSM5 and Cu–HMOR catalysts deactivated only 58% and 48%, respectively, after 1200 h KCl exposure. SEM analysis of the KCl aerosol exposed...... catalysts revealed that the potassium salt not only deposited on the catalyst surface, but also penetrated into the catalyst wall. Thus, the K/M ratio (M = V or Cu) was high on V2O5–WO3–TiO2 catalyst and comparatively less on Cu–HZSM5 and Cu–HMOR catalysts. NH3-TPD revealed that the KCl exposed Cu–HZSM5...

  8. Kinetic experiments and modeling of NO oxidation and SCR of NOx with decane over Cu- and Fe-MFI catalysts

    Czech Academy of Sciences Publication Activity Database

    Čapek, Libor; Vradman, L.; Sazama, Petr; Herskowitz, M.; Wichterlová, Blanka; Zukerman, R.; Brosius, R.; Martens, J. A.

    2007-01-01

    Roč. 70, 1-4 (2007), s. 53-57 ISSN 0926-3373 Grant - others:European Union(XE) GR5D-CT 2001-00595 Institutional research plan: CEZ:AV0Z40400503 Source of funding: O - operačné programy Keywords : NO oxidation * Nox reduction with hydrocarbons * heterogeneous kinetic s * iron zeolite Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 4.651, year: 2007

  9. Fe-BEA Zeolite Catalysts for NH3-SCR of NOx

    DEFF Research Database (Denmark)

    Frey, Anne Mette; Mert, Selcuk; Due-Hansen, Johannes

    2009-01-01

    Iron-containing zeolites are known to be promising catalysts for the NH3-SCR reaction. Here, we will investigate the catalytic activity of iron-based BEA catalysts, which was found to exhibit improved activities compared to previously described iron-containing zeolite catalysts, such as ZSM-5...... and ZSM-12. Series of Fe-BEA zeolite catalysts were prepared using a range of different preparation methods. Furthermore, we found that an iron concentration around 3 wt% on BEA showed a small optimum in SCR activity compared to the other iron loadings studied....

  10. Catalyst for the reduction of sulfur dioxide to elemental sulfur

    Science.gov (United States)

    Jin, Y.; Yu, Q.; Chang, S.G.

    1996-02-27

    The inventive catalysts allow for the reduction of sulfur dioxide to elemental sulfur in smokestack scrubber environments. The catalysts have a very high sulfur yield of over 90% and space velocity of 10,000 h{sup {minus}1}. They also have the capacity to convert waste gases generated during the initial conversion into elemental sulfur. The catalysts have inexpensive components, and are inexpensive to produce. The net impact of the invention is to make this technology practically available to industrial applications. 21 figs.

  11. Neutron studies of nanostructured CuO-Al2O3 NOx removal catalysts

    International Nuclear Information System (INIS)

    Ozawa, Masakuni; Loong Chun-Keung

    1997-01-01

    Nanostructured powders of automotive catalytic system CuO0Al 2 O 3 , targeted for nitrogen oxides (NOx) removal under lean-burn engine conditions, were investigated using neutron diffraction and small-angle neutron scattering. The crystal phases, structural transformations and microstructure of 10 mol% Cu-Al 2 O 3 powders are characterized according to the heat-treatment conditions. These properties are correlated with the pore structure and NOx removal efficiency determined by nitrogen adsorption isotherm, electron spin resonance, and temperature programmed reaction measurements. The γ-(Cu, Al) 2 O 3 phase and the mass-fractal-like aggregate of particles (size ∼ 26 nm) at annealing temperatures below 900 degrees C were found to be crucial to the high NOx removal performance. The transformation to bulk crystalline phases of α-Al 2 O 3 + CuAl 2 O 4 spinel above ∼1050 degrees C corresponds to a drastic drop of Nox removal efficiency. The usefulness of neutron-scattering techniques as well as their complementarity with other traditional methods of catalytic research are discussed

  12. Multi-stage selective catalytic reduction of NOx in lean burn engine exhaust

    Energy Technology Data Exchange (ETDEWEB)

    Penetrante, B.M.; Hsaio, M.C.; Merritt, B.T.; Vogtlin, G.E. [Lawrence Livermore National Lab., CA (United States)

    1997-12-31

    Many studies suggest that the conversion of NO to NO{sub 2} is an important intermediate step in the selective catalytic reduction (SCR) of NO{sub x} to N{sub 2}. Some effort has been devoted to separating the oxidative and reductive functions of the catalyst in a multi-stage system. This method works fine for systems that require hydrocarbon addition. The hydrocarbon has to be injected between the NO oxidation catalyst and the NO{sub 2} reduction catalyst; otherwise, the first-stage oxidation catalyst will also oxidize the hydrocarbon and decrease its effectiveness as a reductant. The multi-stage catalytic scheme is appropriate for diesel engine exhausts since they contain insufficient hydrocarbons for SCR, and the hydrocarbons can be added at the desired location. For lean-burn gasoline engine exhausts, the hydrocarbons already present in the exhausts will make it necessary to find an oxidation catalyst that can oxidize NO to NO{sub 2} but not oxidize the hydrocarbon. A plasma can also be used to oxidize NO to NO{sub 2}. Plasma oxidation has several advantages over catalytic oxidation. Plasma-assisted catalysis can work well for both diesel engine and lean-burn gasoline engine exhausts. This is because the plasma can oxidize NO in the presence of hydrocarbons without degrading the effectiveness of the hydrocarbon as a reductant for SCR. In the plasma, the hydrocarbon enhances the oxidation of NO, minimizes the electrical energy requirement, and prevents the oxidation of SO{sub 2}. This paper discusses the use of multi-stage systems for selective catalytic reduction of NO{sub x}. The multi-stage catalytic scheme is compared to the plasma-assisted catalytic scheme.

  13. Observations of the temperature dependent response of ozone to NOx reductions in the Sacramento, CA urban plume

    Science.gov (United States)

    Lafranchi, B. W.; Goldstein, A. H.; Cohen, R. C.

    2011-07-01

    Observations of NOx in the Sacramento, CA region show that mixing ratios decreased by 30 % between 2001 and 2008. Here we use an observation-based method to quantify net ozone (O3) production rates in the outflow from the Sacramento metropolitan region and examine the O3 decrease resulting from reductions in NOx emissions. This observational method does not rely on assumptions about detailed chemistry of ozone production, rather it is an independent means to verify and test these assumptions. We use an instantaneous steady-state model as well as a detailed 1-D plume model to aid in interpretation of the ozone production inferred from observations. In agreement with the models, the observations show that early in the plume, the NOx dependence for Ox (Ox = O3 + NO2) production is strongly coupled with temperature, suggesting that temperature-dependent biogenic VOC emissions and other temperature-related effects can drive Ox production between NOx-limited and NOx-suppressed regimes. As a result, NOx reductions were found to be most effective at higher temperatures over the 7 year period. We show that violations of the California 1-h O3 standard (90 ppb) in the region have been decreasing linearly with decreases in NOx (at a given temperature) and predict that reductions of NOx concentrations (and presumably emissions) by an additional 30 % (relative to 2007 levels) will eliminate violations of the state 1 h standard in the region. If current trends continue, a 30 % decrease in NOx is expected by 2012, and an end to violations of the 1 h standard in the Sacramento region appears to be imminent.

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

    Directory of Open Access Journals (Sweden)

    Markus Dietrich

    2017-07-01

    Full Text Available 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.

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

    Science.gov (United States)

    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

  16. Reduction of NOx emission in tangential fired - furnace by changing the, mode of operation

    International Nuclear Information System (INIS)

    Chudnovsky, B.; Talanker, A.; Levin, L.; Kahana, S

    1998-01-01

    The present work analyses tile results of tests on 575 MW units with tangential firing furnace arrangement in sub-stoichiometric combustion. Tangential firing provides good conditions for implementing sub-stoichiometric combustion owing to the delivery scheme of pulverized coal and air. The furnace was tested in several different modes of operation (Over Fire Air, Bunkers Out Of Service, Excess air, Tilt etc.) to achieve low cost NOx reduction. Actual performance data are presented based on experiments made on lEC's boiler in M.D. 'B' power station

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

    Science.gov (United States)

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

    2010-07-20

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

  18. Reduction of NOx in synthetic diesel exhaust via two-step plasma-catalysis treatment

    International Nuclear Information System (INIS)

    Tonkyn, R.G.; Barlow, S.E.; Hoard, John W.

    2003-01-01

    Significant reduction of NO x in synthetic light duty diesel exhaust has been achieved over a broad temperature window by combining atmospheric plasma with appropriate catalysts. The technique relies on the addition of hydrocarbon reductant prior to passing the simulated exhaust through a non-thermal plasma and a catalyst bed. The observed chemistry in the plasma includes conversion of NO to NO 2 as well as the partial oxidation of the hydrocarbon. The overall NO x reduction has a maximum of less than 80%, with this maximum obtained only at high-energy input into the plasma, high concentration of hydrocarbon reductant and low space velocity. We present data in this paper illustrating that a multiple-step treatment strategy, whereby two or more plasma-catalyst reactors are utilized in series, can increase the maximum NO x conversion obtainable. Alternatively, this technique can reduce the energy and/or hydrocarbon requirements for a fixed conversion efficiency. When propene is used as the reductant, the limiting reagent for the overall process is most likely acetaldehyde. The data suggest that acetaldehyde is formed in concert with NO oxidation to NO 2 in the plasma stage. The limited NO x reduction efficiency attained in a single step, even with excess energy, oxygen content and/or hydrocarbon-to-NO x ratio is well explained by this hypothesis, as is the effectiveness of the multiple-step treatment strategy. We present the data here illustrating the advantage of this approach under a wide variety of conditions

  19. New catalyst developed at Argonne National Laboratory could help diesels meet NOx deadlines

    CERN Multimedia

    2003-01-01

    "A new catalyst could help auto makers meet the U.S. Environmental Protection Agency's deadline to eliminate 95 percent of nitrogen-oxide from diesel engine exhausts by 2007, while saving energy" (1 page).

  20. Agricultural Bio-Fueled Generation of Electricity and Development of Durable and Efficent NOx Reduction

    Energy Technology Data Exchange (ETDEWEB)

    Boyd, Rodney

    2007-08-08

    The objective of this project was to define the scope and cost of a technology research and development program that will demonstrate the feasibility of using an off-the-shelf, unmodified, large bore diesel powered generator in a grid-connected application, utilizing various blends of BioDiesel as fuel. Furthermore, the objective of project was to develop an emissions control device that uses a catalytic process and BioDiesel (without the presence of Ammonia or Urea)to reduce NOx and other pollutants present in a reciprocating engine exhaust stream with the goal of redefining the highest emission reduction efficiencies possible for a diesel reciprocating generator. Process: Caterpillar Power Generation adapted an off-the-shelf Diesel Generator to run on BioDiesel and various Petroleum Diesel/BioDiesel blends. EmeraChem developed and installed an exhaust gas cleanup system to reduce NOx, SOx, volatile organics, and particulates. The system design and function was optimized for emissions reduction with results in the 90-95% range;

  1. Combinatorial computational chemistry approach to the design of metal catalysts for deNOx

    International Nuclear Information System (INIS)

    Endou, Akira; Jung, Changho; Kusagaya, Tomonori; Kubo, Momoji; Selvam, Parasuraman; Miyamoto, Akira

    2004-01-01

    Combinatorial chemistry is an efficient technique for the synthesis and screening of a large number of compounds. Recently, we introduced the combinatorial approach to computational chemistry for catalyst design and proposed a new method called ''combinatorial computational chemistry''. In the present study, we have applied this combinatorial computational chemistry approach to the design of precious metal catalysts for deNO x . As the first step of the screening of the metal catalysts, we studied Rh, Pd, Ag, Ir, Pt, and Au clusters regarding the adsorption properties towards NO molecule. It was demonstrated that the energetically most stable adsorption state of NO on Ir model cluster, which was irrespective of both the shape and number of atoms including the model clusters

  2. Heterogeneous photocatalysis on construction materials: effect of catalyst properties on the efficiency for degrading NOx and self cleaning

    Directory of Open Access Journals (Sweden)

    Bengtsson, N.

    2014-05-01

    Full Text Available This paper analyzes the effect of some properties of different catalysts on the photocatalytic activity. The efficiency has been determined for two different processes: NOx abatement and self-cleaning for Rhodamine B and tobacco extract being, the TiO2 based photocatalyst, supported as coatings on white mortar. Eight different catalysts were tested, seven commercial ones and one home-made catalyst with improved visible light absorption properties. Additionally, some of them were submitted to exposition to water and/or calcinations to alter their physical properties. A kinetic approach was used to evaluate the photocatalytic activity, being the first reaction constant (for NO and just empirical constants (for self-cleaning the parameters used for the comparison of the different materials. As a result, the efficiency, even for ranking, is dependent on the type of contaminant used in the experiment. In general, NO oxidation and tobacco followed similar trends while no clear relations were found for Rhodamine B.En este trabajo se analiza el efecto de las propiedades de distintos catalizadores en la actividad fotocatalítica de degradación de NOx y autolimpieza, para Rodamina B y extracto de tabaco. Se han ensayado ocho fotocatalizadores, basados en TiO2 y soportados sobre mortero blanco; siete de ellos comerciales y uno sintetizado en el laboratorio con absorción mejorada en el visible. Adicionalmente, las propiedades físicas de algunos de ellos se alteraron mediante tratamientos con agua y/o por calcinación. La actividad fotocatalítica se ha evaluado mediante aproximación cinética, siendo la constante de reacción de primer orden (para NO y constantes empíricas de ajuste (para autolimpieza los parámetros de comparación entre materiales. Como resultado, la eficiencia depende del contaminante utilizado en el experimento de evaluación. En general, en este estudio, oxidación de NO y de extracto de tabaco presentan tendencias similares

  3. Experimental investigation of N2O formation in selective non-catalytic NOx reduction processes performed in stoker boiler

    Directory of Open Access Journals (Sweden)

    Krawczyk Piotr

    2016-12-01

    Full Text Available Stoker fired boiler plants are common throughout Eastern Europe. Increasingly strict emission standards will require application of secondary NOx abatement systems on such boilers. Yet operation of such systems, in addition to reducing NOx emissions, may also lead to emission of undesirable substances, for example N2O. This paper presents results of experimental tests concerning N2O formation in the selective non-catalytic NOx emission reduction process (SNCR in a stoker boiler (WR 25 type. Obtained results lead to an unambiguous conclusion that there is a dependency between the NOx and N2O concentrations in the exhaust gas when SNCR process is carried out in a coal-fired stoker boiler. Fulfilling new emission standards in the analysed equipment will require 40–50% reduction of NOx concentration. It should be expected that in such a case the N2O emission will be approximately 55–60 mg/m3, with the NOx to N2O conversion factor of about 40%.

  4. Effect of process parameters and injector position on the efficiency of NOx reduction by selective non catalytic reduction technique

    International Nuclear Information System (INIS)

    Hamid, A.; Mehmood, M.A.; Irfan, N.; Javed, M.T.; Waheed, K.

    2009-01-01

    An experimental investigation has been performed to study the effect of atomizer pressure dilution of the reducing reagent and the injector position on the efficiency or the NOx reduction by a selective non-catalytic reduction technique using urea as a reducing agent. Experiments were performed with a flow reactor in which flue gas was generated by the combustion of methane in air at stoichiometric amount of oxygen and the desired levels of initial NOx (400-450 ppm) were achieved by doping the flame with ammonia. The work was directed to investigate the effect of atomizer pressure, dilution of urea reagent and the injector position. The atomizer pressure was varied from 1 to 3bar and 20-25% increase in efficiency was observed by decreasing the pressure. Effect of dilution of urea solution was investigated by varying the strength of the solution from the 8 to 32% and 40-45% increase in the efficiency was observed. Effects of injector position was investigated by injecting the urea solution both in co current and counter current direction of the flue gases and 20-25% increase in the efficiency was observed in counter current direction. (author)

  5. Reduction and reoxidation of cobalt Fischer-Tropsch catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Hilmen, Anne-Mette

    1996-12-31

    The Fischer-Tropsch synthesis involves the hydrogenation of carbon monoxide to produce mainly hydrocarbons, water and carbon dioxide, but also alcohols, aldehydes and acids are formed. The distribution of these products is determined by the choice of catalyst and synthesis conditions. This thesis studies the reduction and reoxidation of 17%Co/Al{sub 2}O{sub 3} and 17%Co-1%Re/Al{sub 2}O{sub 3} by means of several characterization techniques. The effect of small amounts of Re on the reduction properties of Al{sub 2}O{sub 3}-supported Co catalysts has been studied by temperature-programmed reduction (TPR). An intimate mixture of CoAl{sub 2}O{sub 3} and Re/Al{sub 2}O{sub 3} catalysts showed a promoting effect of Re similar to that for co impregnated CoRe/Al{sub 2}O{sub 3}. A loose mixture of Co/Al{sub 2}O{sub 3} + Re/Al{sub 2}O{sub 3} did not show any effect of Re on the reduction of Co. But a promoting effect was observed if the mixture had been pre-treated with Ar saturated with water before the TPR. It is suggested that Re promotes the reduction of Co oxide by hydrogen spillover. It is shown that a high temperature TPK peak at 1200K assigned to Co aluminate is mainly caused by the diffusion of Co ions during the TPR and not during calcination. The Co particle size measured by x-ray diffraction on oxidized catalysts decreased compared to the particle size on the calcined catalysts, while the dispersion measured by volumetric chemisorption decreased somewhat after the oxidation-reduction treatment. The role of water in the deactivation of Co/Al{sub 2}O{sub 3} and CoRe/Al{sub 2}O{sub 3} Fischer-Tropsch catalysts has been extensively studied. There were significant differences in the reducibility of the phases formed for the two catalysts during exposure to H{sub 2}O/He. 113 refs., 76 figs., 18 tabs.

  6. Diesel Emission Control- Sulfur Effects (DECSE) Program- Phase II Summary Report: NOx Adsorber Catalysts; FINAL

    International Nuclear Information System (INIS)

    None

    2000-01-01

    The investigations performed in this project demonstrated the ability to develop a NO(sub x) regeneration strategy including both an improved lean/rich modulation cycle and rich engine calibration, which resulted in a high NO(sub x) conversion efficiency over a range of operating temperatures. A high-temperature cycle was developed to desulfurize the NO(sub x) absorber catalyst. The effectiveness of the desulfurization process was demonstrated on catalysts aged using two different sulfur level fuels. The major findings of this project are as follows: (1) The improved lean/rich engine calibration achieved as a part of this test project resulted in NO(sub x) conversion efficiencies exceeding 90% over a catalyst inlet operating temperature window of 300 C-450 C. This performance level was achieved while staying within the 4% fuel economy penalty target defined for the regeneration calibration. (2) The desulfurization procedure developed showed that six catalysts, which had been exposed to fuel sulfur levels of 3-, 16-, and 30-ppm for as long as 250 hours, could be recovered to greater than 85% NO(sub x) conversion efficiency over a catalyst inlet operating temperature window of 300 C-450 C, after a single desulfurization event. This performance level was achieved while staying within the 4% fuel economy penalty target defined for the regeneration calibration. (3) The desulfurization procedure developed has the potential to meet in-service engine operating conditions and provide acceptable driveability conditions. (4) Although aging with 78-ppm sulfur fuel reduced NO(sub x) conversion efficiency more than aging with 3-ppm sulfur fuel as a result of sulfur contamination, the desulfurization events restored the conversion efficiency to nearly the same level of performance. However, repeatedly exposing the catalyst to the desulfurization procedure developed in this program caused a continued decline in the catalyst's desulfurized performance. Additional work will be

  7. CFD analysis of NOx reduction by domestic natural gas added to coal combustion

    Energy Technology Data Exchange (ETDEWEB)

    Bar-Ziv, E.; Yasur, Y.; Chudnovsky, B. [Ben-Gurion University of the Negev, Beer-Sheva (Israel). Dept. of Mechanical Engineering and Inst. for Applied Research

    2004-07-01

    To date, Israel's electrical energy has been based only on imported fuels. However, with the recently discovered natural gas in the Ashqulon shores, Israel can examine the benefits to its energy resources, environment, and economy of blending its domestic natural gas with imported coal. As for using natural gas, the proposal is to burn it in existing IEC coal-fired boilers in order to significantly reduce NOx emission by reburning. An important aspect is to provide retrofitting in existing IEC boilers by replacing a fraction of the coal by natural gas. This would allow the purchase of coal with a wide range of parameters, which is less expensive. Hence, mixed gas-coal burning would benefit Israel. The authors have made numerical simulations in order to study the optimal conditions of operation and evaluate the economic as well as environmental benefits. Indeed, extensive simulations have shown that there is a significant reduction of NOx emission, as expected, with the addition of relatively small amounts of natural gas. Experiments will now be carried out in a test facility that will provide accurate physicochemical properties of the mixed fuel for more reliable simulations. 19 refs., 6 figs., 1 tab.

  8. Study on the Noise Reduction of Vehicle Exhaust NOX Spectra Based on Adaptive EEMD Algorithm

    Directory of Open Access Journals (Sweden)

    Kai Zhang

    2017-01-01

    Full Text Available It becomes a key technology to measure the concentration of the vehicle exhaust components with the transmission spectra. But in the conventional methods for noise reduction and baseline correction, such as wavelet transform, derivative, interpolation, polynomial fitting, and so forth, the basic functions of these algorithms, the number of decomposition layers, and the way to reconstruct the signal have to be adjusted according to the characteristics of different components in the transmission spectra. The parameter settings of the algorithms above are not transcendental, so with them, it is difficult to achieve the best noise reduction effect for the vehicle exhaust spectra which are sharp and drastic in the waveform. In this paper, an adaptive ensemble empirical mode decomposition (EEMD denoising model based on a special normalized index optimization is proposed and used in the spectral noise reduction of vehicle exhaust NOX. It is shown with the experimental results that the method can effectively improve the accuracy of the spectral noise reduction and simplify the denoising process and its operation difficulty.

  9. NOx reduction over metal-ion exchanged novel zeolite under lean conditions. Activity and hydrothermal stability

    International Nuclear Information System (INIS)

    Subbiah, Ayyappan; Gujar, Amit; Price, Geoffrey L.; Cho, Byong K.; Blint, Richard J.; Yie, Jae E.

    2003-01-01

    Zeolite SUZ-4 was synthesized and tested for its hydrothermal stability using a standard aging procedure coupled with NMR spectroscopy, and was identified as a promising support for lean-NO x catalysts for high temperature applications. Various metals such as Cu, Ag, Fe, Co were ion exchanged onto the SUZ-4 zeolite, and their catalytic activity for NO/NO x conversion was measured in the presence of excess oxygen using ethylene as the reducing agent. Among the metal-ions exchanged, copper proved to be the best metal cation for lean-NO x catalysis with the optimum level of exchange at 29-42%. The optimized, fresh Cu/SUZ-4 catalyst achieved 70-80% of NO/NO x conversion activity over a wide range of temperature from 350 to 600C with the maximum conversion temperature at 450C. The presence of H 2 O and SO 2 reduced the NO/NO x conversion by about 30% of the fresh Cu/SUZ-4 catalyst due possibly to the blocking of active sites for NO/NO x adsorption. Substitution of gasoline vapor for ethylene as the reductant improved the NO x reduction activity of the fresh Cu/SUZ-4 catalyst at high temperatures above 350C. Aging the Cu/SUZ-4 catalyst resulted in a slight shift of activity profile toward higher temperatures, yielding an increase of NO conversion by 16% and a decrease of NO x conversion by 15% at 525C. The effect of H 2 O and SO 2 on the aged catalyst was to reduce the NO activity by 20% and NO x activity by 30% at 500C. The effect of space velocity change was not significant except in the low temperature range where the reaction light-off occurs. Adsorption/desorption measurements indicate that aging Cu/SUZ-4 results in partial migration/agglomeration of Cu particles in the pores thereby reducing the NO/NO x activity. Overall, the NO x conversion efficiency of Cu/SUZ-4, for both fresh and aged, is much better than the benchmark Cu/ZSM-5 in the presence of H 2 O and/or SO 2

  10. Mercury Oxidation over Selective Catalytic Reduction (SCR) Catalysts - Ph.d. thesis Karin Madsen

    DEFF Research Database (Denmark)

    Madsen, Karin

    The vanadium-based SCR catalyst used for NOx-control promotes the oxidation of elemental mercury Hg0 to Hg2+ in flue gases from coal-fired power plants. Hg2+ is water soluble and can effectively be captured in a wet scrubber. This means that the combination of an SCR with a wet FGD can offer an e...

  11. Efficiency Analysis of Technological Methods for Reduction of NOx Emissions while Burning Hydrocarbon Fuels in Heat and Power Plants

    Directory of Open Access Journals (Sweden)

    S. M. Kabishov

    2013-01-01

    Full Text Available The paper contains a comparative efficiency analysis pertaining to application of existing technological methods for suppression of nitric oxide formation in heating boilers of heat generators. A special attention has been given to investigation of NOx  emission reduction while burning hydrocarbon fuel with the help of oxygen-enriched air. The calculations have demonstrated that while enriching oxidizer with the help of oxygen up to 50 % (by volume it is possible to reduce volume of NOx formation (while burning fuel unit by 21 %.

  12. Kinetics of the reduction of uranium oxide catalysts

    International Nuclear Information System (INIS)

    Heynen, H.W.G.; Camp-van Berkel, M.M.; Bann, H.S. van der

    1977-01-01

    The reduction of uranium oxide and uranium oxide on alumina catalysts by ethylbenzene and by hydrogen has been studied in a thermobalance. Ethylbenzene mole fractions between 0.0026 and 0.052 and hydrogen mole fractions between 0.1 and 0.6 were applied at temperatures of 425--530 0 C. During the reduction the uranium oxides are converted into UO 2 . The rate of reduction of pure uranium oxide appears to be constant in the composition region UO/sub 2.6/-UO/sub 2.25/. The extent of this region is independent of the concentration of the reducing agents and of the reaction temperature. The constant rate is explained in terms of a constant oxygen pressure which is in equilibrium with the two solid phases, U 3 O/sub 8-x/ and U 4 O 9 . The reduction rate is first order in hydrogen and zero order in ethylbenzene with activation energies of 120 and 190 kJ mol -1 , respectively. Oxygen diffusion through the lattice is probably not rate limiting. The reduction behavior of uranium oxide on alumina is different from that of pure uranium oxide; the rate of reduction continuously decreases with increasing degree of reduction. An explanation for this behavior has been given by visualizing this catalyst as a set of isolated uranium oxide crystallites with a relative wide variation of diameters, in an alumina matrix. At the beginning of the reduction, carbon dioxide and water are the only reaction products. Thereafter, benzene is found as well and, finally, at U/O ratios below 2.25, styrene also appears in the reactor outlet

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

    Science.gov (United States)

    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.

  14. Catalyst and method for reduction of nitrogen oxides

    Science.gov (United States)

    Ott, Kevin C [Los Alamos, NM

    2008-05-27

    A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub.2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub.2O was not detected (detection limit: 0.6 percent N.sub.2O).

  15. Highly selective NOx reduction for diesel engine exhaust via an electrochemical system

    DEFF Research Database (Denmark)

    Shao, Jing; Tao, Youkun; Kammer Hansen, Kent

    2016-01-01

    It is challenging to reduce the nitrogen oxides (NOx) in diesel engine exhaust due to the inhibiting effect of excess oxygen. In this study, a novel electrochemical deNOx system was developed, which eliminated the need for additional reducing materials or a sophisticated controlling system as used...

  16. Effects of NOX Storage Component on Ammonia Formation in TWC for Passive SCR NOX Control in Lean Gasoline Engines

    Energy Technology Data Exchange (ETDEWEB)

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

    2018-04-01

    A prototype three-way catalyst (TWC) with NOX storage component 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 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. Adding a NOX storage component to a TWC provides two benefits in the context of a passive SCR system: (1) enabling longer lean operation by storing NOX upstream and preserving NH3 inventory on the downstream SCR catalyst; and (2) increasing the quantity and rate of NH3 production during rich operation. Since the fuel penalty associated with passive SCR NOX control depends on the fraction of time that the engine is running rich rather than lean, both benefits (longer lean times and shorter rich times achieved via improved NH3 production) will decrease the passive SCR fuel penalty. However, these benefits are primarily realized at low to moderate temperatures (300-500 °C), where the NOX storage component is able to store NOX, with little to no benefit at higher temperatures (>500 °C), where NOX storage is no longer effective. This study discusses engine parameters and control strategies affecting the NH3 generation over a TWC with NOX storage component.

  17. Catalysts for Environmental Remediation

    DEFF Research Database (Denmark)

    Abrams, B. L.; Vesborg, Peter Christian Kjærgaard

    2013-01-01

    The properties of catalysts used in environmental remediation are described here through specific examples in heterogeneous catalysis and photocatalysis. In the area of heterogeneous catalysis, selective catalytic reduction (SCR) of NOx was used as an example reaction with vanadia and tungsta...

  18. The influence of a silica pillar in lamellar tetratitanate for selective catalytic reduction of NOx using NH3

    International Nuclear Information System (INIS)

    Nogueira da Cunha, Beatriz; Gonçalves, Alécia Maria; Gomes da Silveira, Rafael; Urquieta-González, Ernesto A.; Magalhães Nunes, Liliane

    2015-01-01

    Highlights: • Potassium ions significantly affected the SCR. • The introduction of silica in the catalyst promotes the NH 3 -SCR reaction. • The catalysts activities were not significantly influenced by SO 2 addition. - Abstract: Silica-pillared layered titanate (SiO 2 –Ti 4 O 9 ) was prepared by intercalating organosilanes into the interlayers of a layered K 2 Ti 4 O 9 followed by calcination at 500 °C. The lamellar titanates produced were used as a support to prepare vanadium catalysts (1 and 2 wt%) through wet impregnation for selective catalytic reduction (SCR) of NO. The catalysts were characterized using nitrogen adsorption (BET), X-ray diffraction (XRD), temperature programmed reduction (H 2 -TPR), nuclear magnetic resonance ( 29 Si NMR), and infrared spectroscopy (FT-IR). Reduction of NO by NH 3 was studied in a fixed-bed reactor packed with the catalysts and fed a mixture comprising 1% NH 3 , 1% NO, 10% O 2 , and 34 ppm SO 2 (when used) in helium. The results demonstrate that activity is correlated with the support, i.e., with acidic strength of catalysts. The potassium in the support, K 2 Ti 4 O 9 , significantly affected the reaction and level of vanadium species reduction. The catalyst (1VSiT) with 1 wt% vanadium impregnated on the SiO 2 –Ti 4 O 9 support reduced ∼80% of the NO. Approximately the same conversion rate was generated on the catalyst (2VSiT) with 2 wt% vanadium using the same support. The increased NH 3 adsorption demonstrate that introduction of silica in the catalyst promotes the NH 3 -SCR reaction. More importantly, 2VSiT and 1VSiT were strongly resistant to SO 2 poisoning

  19. Numerical simulation of urea based selective non-catalytic reduction deNOx process for industrial applications

    International Nuclear Information System (INIS)

    Baleta, Jakov; Mikulčić, Hrvoje; Vujanović, Milan; Petranović, Zvonimir; Duić, Neven

    2016-01-01

    Highlights: • SNCR is a simple method for the NOx reduction from large industrial facilities. • Capabilities of the developed mathematical framework for SNCR simulation were shown. • Model was used on the geometry of experimental reactor and municipal incinerator. • Results indicate suitability of the developed model for real industrial cases. - Abstract: Industrial processes emit large amounts of diverse pollutants into the atmosphere, among which NOx takes a significant portion. Selective non-catalytic reduction (SNCR) is a relatively simple method for the NOx reduction in large industrial facilities such as power plants, cement plants and waste incinerator plants. It consists of injecting the urea-water solution in the hot flue gas stream and its reaction with the NOx. During this process flue gas enthalpy is used for the urea-water droplet heating and for the evaporation of water content. After water evaporates, thermolysis of urea occurs, during which ammonia, a known NO_x reductant, and isocyanic acid are generated. In order to cope with the ever stringent environmental norms, equipment manufacturers need to develop energy efficient products that are at the same time benign to environment. This is becoming increasingly complicated and costly, and one way to reduce production costs together with the maintaining the same competitiveness level is to employ computational fluid dynamics (CFD) as a tool, in a process today commonly known under the term “virtual prototyping”. The aim of this paper is to show capabilities of the developed mathematical framework implemented in the commercial CFD code AVL FIRE®, to simulate physical processes of all relevant phenomena occurring during the SNCR process. First, mathematical models for description of SNCR process are presented and afterwards, models are used on the 3D geometry of an industrial reactor and a real industrial case to predict SNCR efficiency, temperature and velocity field. Influence of the main

  20. Enhanced Activity of Nanocrystalline Zeolites for Selective Catalytic Reduction of NOx

    International Nuclear Information System (INIS)

    Sarah C. Larson; Vicki H. Grassian

    2006-01-01

    Nanocrystalline zeolites with discrete crystal sizes of less than 100 nm have different properties relative to zeolites with larger crystal sizes. Nanocrystalline zeolites have improved mass transfer properties and very large internal and external surface areas that can be exploited for many different applications. The additional external surface active sites and the improved mass transfer properties of nanocrystalline zeolites offer significant advantages for selective catalytic reduction (SCR) catalysis with ammonia as a reductant in coal-fired power plants relative to current zeolite based SCR catalysts. Nanocrystalline NaY was synthesized with a crystal size of 15-20 nm and was thoroughly characterized using x-ray diffraction, electron paramagnetic resonance spectroscopy, nitrogen adsorption isotherms and Fourier Transform Infrared (FT-IR) spectroscopy. Copper ions were exchanged into nanocrystalline NaY to increase the catalytic activity. The reactions of nitrogen dioxides (NO x ) and ammonia (NH 3 ) on nanocrystalline NaY and CuY were investigated using FT-IR spectroscopy. Significant conversion of NO 2 was observed at room temperature in the presence of NH 3 as monitored by FT-IR spectroscopy. Copper-exchanged nanocrystalline NaY was more active for NO 2 reduction with NH 3 relative to nanocrystalline NaY

  1. Atmospheric pollution reduction effect and regional predicament: An empirical analysis based on the Chinese provincial NOx emissions.

    Science.gov (United States)

    Ding, Lei; Liu, Chao; Chen, Kunlun; Huang, Yalin; Diao, Beidi

    2017-07-01

    Atmospheric pollution emissions have become a matter of public concern in recent years. However, most of the existing researches on NOx pollution are from the natural science and technology perspective, few studies have been conducted from an economic point, and regional differences have not been given adequate attention. This paper adopts provincial panel data from 2006 to 2013 and the LMDI model to analyze the key driving factors and regional dilemmas of NOx emissions. The results show that significant regional disparities still exit on NO x emissions and its reduction effect 27 provinces didn't accomplish their corresponding reduction targets. Economic development factor is the dominating driving factor of NO x emissions during the study period, while energy efficiency and technology improvement factors offset total NO x emissions in the majority of provinces. In addition, the industrial structure factor plays a more significant role in reducing the NO x emissions after 2011. Therefore, the government should consider all these factors as well as regional heterogeneity in developing appropriate pollution mitigating policies. It's necessary to change NOx emissions control attitude from original key areas control to divided-zone control, not only attaches great importance to the reduction of the original key areas, but also emphasizes the new potential hotspots with high NO x emissions. Copyright © 2017 Elsevier Ltd. All rights reserved.

  2. Hollow Spheres of Iron Carbide Nanoparticles Encased in Graphitic Layers as Oxygen Reduction Catalysts

    DEFF Research Database (Denmark)

    Hu, Yang; Jensen, Jens Oluf; Zhang, Wei

    2014-01-01

    Nonprecious metal catalysts for the oxygen reduction reaction are the ultimate materials and the foremost subject for low‐temperature fuel cells. A novel type of catalysts prepared by high‐pressure pyrolysis is reported. The catalyst is featured by hollow spherical morphologies consisting...

  3. Experimental comparison of biomass chars with other catalysts for tar reduction

    NARCIS (Netherlands)

    Abu El-Rub, Ziad; Bramer, Eduard A.; Brem, Gerrit

    2008-01-01

    In this paper the potential of using biomass char as a catalyst for tar reduction is discussed. Biomass char is compared with other known catalysts used for tar conversion. Model tar compounds, phenol and naphthalene, were used to test char and other catalysts. Tests were carried out in a fixed bed

  4. Final Technical Report on Investigation of Selective Non-Catalytic Processes for In-Situ Reduction of NOx and CO Emissions from Marine Gas Turbines and Diesel Engines

    National Research Council Canada - National Science Library

    Bowman, Craig

    1997-01-01

    .... These observations suggest the possibility of utilizing SNCR for reducing NO(x) emissions from marine gas turbines and Diesel engines by direct injection of a reductant species into the combustion chamber, possibly as a fuel...

  5. Conditions for reduction of ironmolybdenum-tungsten catalyst for ammonia synthesis

    International Nuclear Information System (INIS)

    Simulina, N.A.; Karibdzhanyan, N.A.; Lachinov, S.S.; Anfimov, V.A.; Shumlyakovskij, Ts.I.

    1977-01-01

    The reduction of Fe-Mo-W catalyst MB-5, used for synthesis of ammonia, has been studied in the reactor of extracolumn reduction. The results obtained have been compared with similar results for the catalyst CA-1. It has been shown that reduction of the catalyst MB-5 proceeds more intensive and is completed at lower temperature and for a shorter period of time. The samples of the catalyst MB-5 discharged from different layers in the reactor are more active than CA-1 reduced under identical conditions

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

    International Nuclear Information System (INIS)

    Oh, Kwang Seok; Woo, Seong Ihl

    2011-01-01

    A chemiluminescence-based analyzer of NO x gas species has been applied for high-throughput screening of a library of catalytic materials. The applicability of the commercial NO x 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 Al 2 O 3 substrate was tested for the efficiency of NO x removal using a home-built 64-channel parallel and sequential tubular reactor. The NO x concentrations measured by the NO x analyzer agreed well with the results obtained using micro gas chromatography for a reference catalyst consisting of 1 wt% Pt on γ-Al 2 O 3 . Most alloys showed high efficiency at 275 °C, which is typical of Pt-based catalysts for selective catalytic reduction of NO. The screening with NO x analyzer allowed to select Pt-Ce (X) (X=1–3) and Pt–Fe (2) as the optimal catalysts for NO x removal: 73% NO x 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.

  7. The effect of diluting ruthenium by iron in RuxSey catalyst for oxygen reduction

    International Nuclear Information System (INIS)

    Delacote, Cyril; Lewera, Adam; Pisarek, Marcin; Kulesza, Pawel J.; Zelenay, Piotr; Alonso-Vante, Nicolas

    2010-01-01

    This study has focused on the synthesis of novel oxygen reduction reaction (ORR) chalcogenide catalysts, with Ru partially replaced by Fe in a cluster-type Ru x Se y . The catalysts were obtained by thermal decomposition of Ru 3 (CO) 12 and Fe(CO) 5 in the presence of Se. As indicated by the XPS data, the composition of catalyst nanoparticles depends on the solvent used (either p-xylene or dichlorobenzene). The presence of iron in synthesized catalysts has been confirmed by both EDAX and XPS. Voltammetric activation of the catalysts results in a partial removal of iron and unreacted selenium from the surface. The ORR performance of electrochemically pre-treated catalysts was evaluated using rotating disk and ring-disk electrodes in a sulfuric acid solution. No major change in the ORR mechanism relative to the Se/Ru catalyst has been observed with Fe-containing catalysts.

  8. The activity of supported vanadium oxide catalysts for the selective reduction of NO with ammonia

    NARCIS (Netherlands)

    Bosch, H.; Janssen, Frans J.J.G.; van den Kerkhof, Frans M.G.; Oldenziel, Jaap; van Ommen, J.G.; Ross, Julian R.H.

    1986-01-01

    The activities of monolayer V2O5 catalysts for the selective reduction of NO with NH3 are compared with those of commercial available catalysts containing V and/or W. From steady state and pulse experiments it can be concluded that the reduction of surface sites proceeds either by NH3 + NO or by NH3

  9. Nano-Structured Bio-Inorganic Hybrid Material for High Performing Oxygen Reduction Catalyst.

    Science.gov (United States)

    Jiang, Rongzhong; Tran, Dat T; McClure, Joshua P; Chu, Deryn

    2015-08-26

    In this study, we demonstrate a non-Pt nanostructured bioinorganic hybrid (BIH) catalyst for catalytic oxygen reduction in alkaline media. This catalyst was synthesized through biomaterial hemin, nanostructured Ag-Co alloy, and graphene nano platelets (GNP) by heat-treatment and ultrasonically processing. This hybrid catalyst has the advantages of the combined features of these bio and inorganic materials. A 10-fold improvement in catalytic activity (at 0.8 V vs RHE) is achieved in comparison of pure Ag nanoparticles (20-40 nm). The hybrid catalyst reaches 80% activity (at 0.8 V vs RHE) of the state-of-the-art catalyst (containing 40% Pt and 60% active carbon). Comparable catalytic stability for the hybrid catalyst with the Pt catalyst is observed by chronoamperometric experiment. The hybrid catalyst catalyzes 4-electron oxygen reduction to produce water with fast kinetic rate. The rate constant obtained from the hybrid catalyst (at 0.6 V vs RHE) is 4 times higher than that of pure Ag/GNP catalyst. A catalytic model is proposed to explain the oxygen reduction reaction at the BIH catalyst.

  10. Supported quantum clusters of silver as enhanced catalysts for reduction

    Directory of Open Access Journals (Sweden)

    Leelavathi Annamalai

    2011-01-01

    Full Text Available Abstract Quantum clusters (QCs of silver such as Ag7(H2MSA7, Ag8(H2MSA8 (H2MSA, mercaptosuccinic acid were synthesized by the interfacial etching of Ag nanoparticle precursors and were loaded on metal oxide supports to prepare active catalysts. The supported clusters were characterized using high resolution transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and laser desorption ionization mass spectrometry. We used the conversion of nitro group to amino group as a model reaction to study the catalytic reduction activity of the QCs. Various aromatic nitro compounds, namely, 3-nitrophenol (3-np, 4-nitrophenol (4-np, 3-nitroaniline (3-na, and 4-nitroaniline (4-na were used as substrates. Products were confirmed using UV-visible spectroscopy and electrospray ionization mass spectrometry. The supported QCs remained active and were reused several times after separation. The rate constant suggested that the reaction followed pseudo-first-order kinetics. The turn-over frequency was 1.87 s-1 per cluster for the reduction of 4-np at 35°C. Among the substrates investigated, the kinetics followed the order, SiO2 > TiO2 > Fe2O3 > Al2O3.

  11. Development of a pilot fluidized bed combustion to NOx reduction using natural gas: characterization and dimensioning; Desenvolvimento de um combustor piloto a leito fluidizado para reducao de NOx usando gas natural: caracterizacao e dimensionamento

    Energy Technology Data Exchange (ETDEWEB)

    Santos, Douglas A.; Lucena, Sergio [Universidade Federal de Pernambuco (UFPE), Recife, PE (Brazil)

    2004-07-01

    At the present time, the operation of combustion systems and the design of combustors continue being important problems in the Engineering, and don't involve just the size increase of combustors, but also changes of characteristics in the details of projects. The combustors applications are directly related to the needs, like: material transformation for heating, drying or incineration; and all have the inconvenience of emanating of pollutant gaseous (such like NOx). In combustion systems of gases, NOx is basically created in the reaction between nitrogen and oxygen to high temperatures ({approx} 1200 deg C). Below such conditions, the contribution of thermal NOx is recognisably small. The efficient reduction, safe control and economical elimination of pollutant emissions in the systems of burning are the main focuses of environmental legislation and concern to several industrialized countries, besides Brazil. Furthermore, in appeal at the Environmental Laws and at the rising consumption of combustible gases (Natural Gas), new technologies more attractive and economically viable have been studied, for example the combustion systems in fluidized bed. In this kind of system is possible to obtain high combustion efficiency at low temperatures ({approx} 900 deg C) with NOx reduction. In this work is intended of characterizing and dimensioning an industrial fluidized bed combustor that uses Natural Gas like feedstock in the combustion system, with smaller amounts of emitted NOx. (author)

  12. NO reduction by CO over noble-metal catalysts under cycled feedstreams

    International Nuclear Information System (INIS)

    Muraki, H.; Fujitani, Y.

    1986-01-01

    The reduction of NO with CO was studied over α-Al/sub 2/O/sub 3/-supported Pt, Pd, Rh, Ru, and Ir catalysts. The activities were measured by using cycled feeds and steady noncycled feed. The activity sequence of the catalysts tested was Rh > Ru > Ir > Pd > Pt. The activities of Pt and Pd catalysts were increased under the cycled feed. The periodic operation effect on the Pt catalyst was more predominant than that on the Pd catalyst. The order of periodic operation effect corresponded to the order of their susceptibility to CO self-poisoning

  13. Rutile vanadium antimonates. A new class of catalysts for selective reduction of NO with ammonia

    Energy Technology Data Exchange (ETDEWEB)

    Brazdil, James F.; Ebner, Ann M.; Cavalcanti, Fernando A.P. [BP Chemicals Inc., Cleveland, OH (United States)

    1997-12-31

    This paper describes a new class of vanadium containing oxide catalysts that are active and selective for the selective catalytic reduction of NO with ammonia. Vanadium antimony oxide based catalysts were found to be effective in the conversion of NO with little or no ammonia slippage when tested using gas mixtures containing between 300 and 700ppm NO. X-ray diffraction analyses of the catalysts show that the dominant phase present in the catalyst is vanadium antimonate having a defect rutile crystal structure. The catalysts are active and selective in the ranges of 400-460C and gas hourly space velocities of 3000-8000h{sup -1}

  14. Electrocatalytic Reduction-oxidation of Chlorinated Phenols using a Nanostructured Pd-Fe Modified Graphene Catalyst

    International Nuclear Information System (INIS)

    Shi, Qin; Wang, Hui; Liu, Shaolei; Pang, Lei; Bian, Zhaoyong

    2015-01-01

    A Pd-Fe modified graphene (Pd-Fe/G) catalyst was prepared by the Hummers oxidation method and bimetallic co-deposition method. The catalyst was then characterized by various characterization techniques and its electrochemical property toward the electrocatalytic reduction-oxidation of chlorinated phenols was investigated by using cyclic voltammetry and differential pulse voltammetry. The results of the characterization show that the Pd-Fe/G catalyst in which the weight proportion of Pd and Fe is 1:1 has an optimal surface performance. The diameter of the Pd-Fe particles is approximately 5.2 ± 0.3 nm, with a uniform distribution on the supporting graphene. This is smaller than the Pd particles of a Pd-modified graphene (Pd/G) catalyst. The Pd-Fe/G catalyst shows a higher electrocatalytic activity than the Pd/G catalyst for reductive dechlorination when feeding with hydrogen gas. The reductive peak potentials of −0.188 V, −0.836 V and −0.956 V in the DPV curves are attributed to the dechlorination of ortho-Cl, meta-Cl, and para-Cl in 2-chlorophenol, 3-chlorophenol and 4-chlorophenol, respectively. In accordance with an analysis of the frontier orbital theory, the order of ease of dechlorination with Pd-Fe/G catalyst is 2-chlorophenol > 3-chlorophenol > 4-chlorophenol. The Pd-Fe/G catalyst has a greater activity than the Pd/G catalyst in accelerating the two-electron reduction of O_2 to H_2O_2, which is attributed to the higher current of the reduction peak at approximately −0.40 V when feeding with oxygen gas. Therefore, the Pd-Fe/G catalyst exhibits a higher electrocatalytic activity than the Pd/G catalyst for the reductive dechlorination and acceleration of the two-electron reduction of O_2 to H_2O_2.

  15. Reduction and Analysis of Low Temperature Shift Heterogeneous Catalyst for Water Gas Reaction in Ammonia Production

    Directory of Open Access Journals (Sweden)

    Zečević, N.

    2013-09-01

    Full Text Available In order to obtain additional quantities of hydrogen after the reforming reactions of natural gas and protect the ammonia synthesis catalyst, it is crucial to achieve and maintain maximum possible activity, selectivity and stability of the low temperature shift catalyst for conversion of water gas reaction during its lifetime. Whereas the heterogeneous catalyst comes in oxidized form, it is of the utmost importance to conduct the reduction procedure properly. The proper reduction procedure and continuous analysis of its performance would ensure the required activity, selectivity and stability throughout the catalyst’s service time. For the proper reduction procedure ofthe low temperature shift catalyst, in addition to process equipment, also necessary is a reliable and realistic system for temperature measurements, which will be effective for monitoring the exothermal temperature curves through all catalyst bed layers. For efficiency evaluation of low shift temperature catalyst reduction and its optimization, it is necessary to determine at regular time intervals the temperature approach to equilibrium and temperature profiles of individual layers by means of "S" and "die off" temperature exothermal curves. Based on the obtained data, the optimum inlet temperature could be determined, in order to maximally extend the service life of the heterogeneous catalyst as much as possible, and achieve the optimum equilibrium for conversion of the water gas. This paper presents the methodology for in situ reduction of the low temperature shift heterogeneous catalyst and the developed system for monitoring its individual layers to achieve the minimum possible content of carbon monoxide at the exit of the reactor. The developed system for temperature monitoring through heterogeneous catalyst layers provides the proper procedure for reduction and adjustment of optimum process working conditions for the catalyst by the continuous increase of reactor inlet

  16. Development of supported noble metal catalyst for U(VI) to U(IV) reduction

    International Nuclear Information System (INIS)

    Tyagi, Deepak; Varma, Salil; Bhattacharyya, K.; Tripathi, A.K.; Bharadwaj, S.R.; Jain, V.K.; Sahu, Avinash; Vincent, Tessy; Jagatap, B.N.; Wattal, P.K.

    2015-01-01

    Uranium-plutonium separation is an essential step in the PUREX process employed in spent nuclear fuel reprocessing. This partitioning in the PUREX process is achieved by selective reduction of Pu(IV) to Pu(III) using uranous nitrate as reductant and hydrazine as stabilizer. Currently in our Indian reprocessing plants, the requirement of uranous nitrate is met by electrolytic reduction of uranyl nitrate. This process, however, suffers from a major drawback of incomplete reduction with a maximum conversion of ~ 60%. Catalytic reduction of U(VI) to U(IV) is being considered as one of the promising alternatives to the electro-reduction process due to fast kinetics and near total conversion. Various catalysts involving noble metals like platinum (Adams catalyst, Pt/Al 2 O 3 , Pt/SiO 2 etc.) have been reported for the reduction. Sustained activity and stability of the catalyst under harsh reaction conditions are still the issues that need to be resolved. We present here the results on zirconia supported noble metal catalyst that is developed in BARC for reduction of uranyl nitrate to uranous nitrate. Supported noble metal catalysts with varying metal loadings (0.5 - 2 wt%) were prepared via support precipitation and noble metal impregnation. The green catalysts were reduced either by chemical reduction using hydrazine hydrate or by heating in hydrogen flow or combination of both the steps. These catalysts were characterized by various techniques such as, XRD, SEM, TEM, N 2 adsorption and H 2 chemisorption. Performance of these catalysts was evaluated for U(VI) to U(IV) reduction with uranyl nitrate feed using hydrazine as reductant. The results with the most active catalyst are named as 'BARC-CAT', which was developed in our lab. (author)

  17. NOx storage and reduction over a lean-burn automotive catalyst

    NARCIS (Netherlands)

    Scholz, C.M.L.

    2007-01-01

    Nowadays, there is an increased interest in lean-burn technologies, i.e. diesel and lean-burn gasoline engines, mainly due to their higher fuel efficiency compared to conventional gasoline engines. Lean-burn engines work under excess oxygen and consequently produce oxygen-rich exhaust. This

  18. A new process for NOx reduction in combustion systems for the generation of energy from waste.

    Science.gov (United States)

    Gohlke, Oliver; Weber, Toralf; Seguin, Philippe; Laborel, Yann

    2010-07-01

    In the EU, emissions from energy from waste plants are largely reduced by applying the Waste Incineration Directive with its limit of 200 mg/m3(s) for NO(x) emissions. The need for further improvement is reflected by new German legislation effective as of 27 January 2009, requiring 100 mg/m3(s). Other countries are expected to follow this example due to the national emission ceilings of the Gothenburg protocol and the concluding EU directive 2001/81/EC. On the other hand, an increase in energy efficiency will be encouraged by the EU Waste Framework Directive. This is why there is a need for new technologies that make it possible to reconcile both requirements: reduced emissions and increased energy efficiency. A new process combining the internal recirculation of flue gas with ammonia or urea injection in order to achieve less then 80 mg/m3(s) of NO(x) is described. Important additional features of the process are an R1 efficiency above the required 0.65 of the EU Waste Framework Directive even with standard steam parameters of 40 bar/380 degrees C as well as low ammonia slip in the flue gas at the boiler outlet of below 10 mg/m3(s). Copyright (c) 2010 Elsevier Ltd. All rights reserved.

  19. NOx removal from the flue gas of oil-fired boiler using a multistage plasma-catalyst hybrid system

    International Nuclear Information System (INIS)

    Park, Sung Youl; Deshwal, Bal Raj; Moon, Seung Hyun

    2008-01-01

    The study on removal of NO x from the flue gas of oil-fired boiler has been carried out using non-thermal plasma cum catalyst hybrid reactor at 150 C. Propylene (C 3 H 6 ) was used as a reducing agent. A multistage plasma-catalyst hybrid reactor was newly designed and successfully operated to clean up the flue gas stream having a flow rate of 30 Nm 3 /h. TiO 2 and Pd/ZrO 2 wash-coated on cordierite honeycomb were used as catalysts in the present study. Though the plasma-catalyst hybrid reactor with TiO 2 showed good activity on the removal of NO yet it removed only 50-60% of NO x because a significant portion of NO oxidized to NO 2 . On the contrary, the plasma-catalyst hybrid reactor with Pd/ZrO 2 removed about 50% of inlet NO with a negligible amount of NO oxidation into NO 2 . The plasma/dual-catalysts hybrid system (front two units of plasma-Pd/ZrO 2 + rear two units of plasma/TiO 2 ) proved to be very promising in NO x removal in the presence of C 3 H 6 . DeNO x efficiency of about 74% has been achieved at a space velocity of 3300/h at 150 C. (author)

  20. Soot and NOx simultaneous reduction by use of CO2 mixed fuel; Ekika CO2 yokai nenryo ni yoru diesel kikan no susu, NOx no doji teigen

    Energy Technology Data Exchange (ETDEWEB)

    Senda, J; Yokoyama, T; Ikeda, M; Fujimoto, H [Doshisha University, Kyoto (Japan); Ifuku, Y [Kubota Corp., Osaka (Japan)

    1997-10-01

    We propose the new fuel injection system by use of diesel fuel dissolved with CO2 to reduce both soot and NOx simultaneously. In this paper spray combustion characteristics of CO2 mixed fuel is reported. It is revealed that flame temperature and KL factor at the CO2 mixed fuel combustion are lower than at the only n-tridecane combustion due to separation or partly flashing of CO2component. And the result of exhaust gas measurement shows the capability that CO2 mixed fuel is able to reduce both soot and NOx simultaneously. 12 refs., 7 figs., 1 tab.

  1. Polymer-Supported Raney Nickel Catalysts for Sustainable Reduction Reactions

    Directory of Open Access Journals (Sweden)

    Haibin Jiang

    2016-06-01

    Full Text Available Green is the future of chemistry. Catalysts with high selectivity are the key to green chemistry. Polymer-supported Raney catalysts have been found to have outstanding performance in the clean preparation of some chemicals. For example, a polyamide 6-supported Raney nickel catalyst provided a 100.0% conversion of n-butyraldehyde without producing any detectable n-butyl ether, the main byproduct in industry, and eliminated the two main byproducts (isopropyl ether and methyl-iso-butylcarbinol in the hydrogenation of acetone to isopropanol. Meanwhile, a model for how the polymer support brought about the elimination of byproducts is proposed and confirmed. In this account the preparation and applications of polymer-supported Raney catalysts along with the corresponding models will be reviewed.

  2. Exhaust Recirculation Control for Reduction of NOx from Large Two-Stroke Diesel Engines

    DEFF Research Database (Denmark)

    Nielsen, Kræn Vodder

    Increased awareness of the detrimental effects on climate, ecosystems and human health have led to numerous restrictions of the emissions from internal combustion engines. Recently the International Maritime Organization has introduced the Tier III standard, which includes a significantly stricter...... the automotive industry, but have only recently been introduced commercially to large two-stroke diesel engines. Recirculation of exhaust gas to the cylinders lowers the oxygen availability and increases the heat capacity during combustion, which in turn leads to less formation of NOx. Experience shows...... of the Tier III standard, while still maintaining maneuverability performance without smoke formation. The design methods acknowledge that engine specific parameter tuning is a scarce resource in the industry and controller complexity is kept to a minimum. An existing dynamic model of the engine and EGR...

  3. Analysis and study on the performance variation of SCR DeNOx catalyst of Coal-Fired Boilers

    International Nuclear Information System (INIS)

    Jianxing, Ren; Fangqin, Li; Jiang, Wu; Qingrong, Liu; Yongwen, Yang; Zhongzhu, Qiu

    2010-01-01

    Nitrogen oxides (NO x ) are one kind of harmful substances from the burning process of fossil fuel and air at high temperature. NO x emissions cause serious pollution on atmospheric environment. In this paper, coal-fired utility boilers were chosen as the object, NO x formation mechanism and control were studied, and SCR deNO x technology was used to control NO x emissions from coal-fired boilers. Analyzed the relationship between deNO x efficiency and characteristics of SCR DeNO x catalyst. Through analysis, affecting SCR DeNO x catalyst failure factors, change law of catalytic properties and technical measures to extend the service life of the catalyst were gotten. (author)

  4. Spectroscopic Insights into Copper-Based Microporous Zeolites for NH3-SCR of NOx and Methane-to-Methanol Activation

    OpenAIRE

    Oord, R.

    2017-01-01

    Smog has received a lot of attention and is still a major problem in big cities all over the world. A major contribution to smog are nitrogen oxides (NOx), which are mainly produced by road transport, industrial processes and power plants. A lot of research has been put into the reduction of these pollutants, and heterogeneous catalysts have made a major contribution to this field. Selective catalytic reduction (SCR) is an efficient technology to reduce these NOx, and is already used in diese...

  5. HYBRID SELECTIVE NON-CATALYTIC REDUCTION (SNCR)/SELECTIVE CATALYTIC REDUCTION (SCR) DEMONSTRATION FOR THE REMOVAL OF NOx FROM BOILER FLUE GASES; FINAL

    International Nuclear Information System (INIS)

    Jerry B. Urbas

    1999-01-01

    The U. S. Department of Energy (DOE), Electric Power Research Institute (EPRI), Pennsylvania Electric Energy Research Council, (PEERC), New York State Electric and Gas and GPU Generation, Inc. jointly funded a demonstration to determine the capabilities for Hybrid SNCR/SCR (Selective Non-Catalytic Reduction/Selective Catalytic Reduction) technology. The demonstration site was GPU Generation's Seward Unit No.5 (147MW) located in Seward Pennsylvania. The demonstration began in October of 1997 and ended in December 1998. DOE funding was provided through Grant No. DE-FG22-96PC96256 with T. J. Feeley as the Project Manager. EPRI funding was provided through agreements TC4599-001-26999 and TC4599-002-26999 with E. Hughes as the Project Manager. This project demonstrated the operation of the Hybrid SNCR/SCR NO(sub x) control process on a full-scale coal fired utility boiler. The hybrid technology was expected to provide a cost-effective method of reducing NO(sub x) while balancing capital and operation costs. An existing urea based SNCR system was modified with an expanded-duct catalyst to provide increased NO(sub x) reduction efficiency from the SNCR while producing increased ammonia slip levels to the catalyst. The catalyst was sized to reduce the ammonia slip to the air heaters to less than 2 ppm while providing equivalent NO(sub x) reductions. The project goals were to demonstrate hybrid technology is capable of achieving at least a 55% reduction in NO(sub x) emissions while maintaining less than 2ppm ammonia slip to the air heaters, maintain flyash marketability, verify the cost benefit and applicability of Hybrid post combustion technology, and reduce forced outages due to ammonium bisulfate (ABS) fouling of the air heaters. Early system limitations, due to gas temperature stratification, restricted the Hybrid NO(sub x) reduction capabilities to 48% with an ammonia slip of 6.1 mg/Nm(sup 3) (8 ppm) at the catalyst inlet. After resolving the stratification problem

  6. HYBRID SELECTIVE NON-CATALYTIC REDUCTION (SNCR)/SELECTIVE CATALYTIC REDUCTION (SCR) DEMONSTRATION FOR THE REMOVAL OF NOx FROM BOILER FLUE GASES

    Energy Technology Data Exchange (ETDEWEB)

    Jerry B. Urbas

    1999-05-01

    The U. S. Department of Energy (DOE), Electric Power Research Institute (EPRI), Pennsylvania Electric Energy Research Council, (PEERC), New York State Electric and Gas and GPU Generation, Inc. jointly funded a demonstration to determine the capabilities for Hybrid SNCR/SCR (Selective Non-Catalytic Reduction/Selective Catalytic Reduction) technology. The demonstration site was GPU Generation's Seward Unit No.5 (147MW) located in Seward Pennsylvania. The demonstration began in October of 1997 and ended in December 1998. DOE funding was provided through Grant No. DE-FG22-96PC96256 with T. J. Feeley as the Project Manager. EPRI funding was provided through agreements TC4599-001-26999 and TC4599-002-26999 with E. Hughes as the Project Manager. This project demonstrated the operation of the Hybrid SNCR/SCR NO{sub x} control process on a full-scale coal fired utility boiler. The hybrid technology was expected to provide a cost-effective method of reducing NO{sub x} while balancing capital and operation costs. An existing urea based SNCR system was modified with an expanded-duct catalyst to provide increased NO{sub x} reduction efficiency from the SNCR while producing increased ammonia slip levels to the catalyst. The catalyst was sized to reduce the ammonia slip to the air heaters to less than 2 ppm while providing equivalent NO{sub x} reductions. The project goals were to demonstrate hybrid technology is capable of achieving at least a 55% reduction in NO{sub x} emissions while maintaining less than 2ppm ammonia slip to the air heaters, maintain flyash marketability, verify the cost benefit and applicability of Hybrid post combustion technology, and reduce forced outages due to ammonium bisulfate (ABS) fouling of the air heaters. Early system limitations, due to gas temperature stratification, restricted the Hybrid NO{sub x} reduction capabilities to 48% with an ammonia slip of 6.1 mg/Nm{sup 3} (8 ppm) at the catalyst inlet. After resolving the stratification

  7. Process of activation of a palladium catalyst system

    Science.gov (United States)

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

    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.

  8. Reduction of amine and biological antioxidants on NOx emissions powered by mango seed biodiesel

    Directory of Open Access Journals (Sweden)

    Velmurugan Kolanjiappan

    2017-01-01

    Full Text Available Este estudio analiza la influencia de la amina y algunos antioxidantes biológicos en la reducción de las emisiones de NOx en un motor diesel alimentado con B100 (100% volumen de éster metílico de semillas de mango y B20 (20% en volumen de semillas de mango y 80% en volumen de mezcla de combustible diesel, Se probaron tres antioxidantes de amina, p-fenilendiamina (PPD, etilendiamina (EDA y N, N’-difenil-1,4-fenilendiamina (DPPD y tres antioxidantes biológicos, diclorometano (DCM, acetato de alfa-tocoferol ( α -T y ácido L-ascórbico (L-asc.acid en un motor diesel kirloskar de cuatro tiempos refrigerado por agua, 5,9 KW de potencia. Hay cinco concentraciones usadas en la mezcla antioxidante de mezclas de biodiesel. Es decir, 0,005% -m, 0,010% -m, 0,025% -m, 0,05% -m y 0,1%, valores en los cuales %-m corresponde a la concentración molar empleada en la mezcla antioxidante. Los resultados muestran que la reducción consiguiente de NOx podría ser adquirida por la adhesión de aditivo antioxidante DPPD con la concentración de 0,025% de combustible B20 en un 15,4% y combustible B100 en un 39%. El aditivo DPPD aumentó las emisiones de CO más de 7,42% para el combustible B100 y 6,44% para el combustible B20. El DCM antioxidante biológico exhibe 0,235 g/kWh para combustible B100 y 0,297 g/kWh para combustible B20. Se ha comprobado que la emisión de humo ha aumentado con la adición de antioxidantes. Un ligero incremento en la eficiencia térmica del freno (0,91% se logra con la adición de antioxidantes a plena carga. Los resultados experimentales se comparan con el análisis de varianza y el resultado es simplemente el mismo que el de la experimentación.

  9. Enhanced Activity and Selectivity of Carbon Nanofiber Supported Pd Catalysts for Nitrite Reduction

    KAUST Repository

    Shuai, Danmeng; Choe, Jong Kwon; Shapley, John R.; Werth, Charles J.

    2012-01-01

    Pd-based catalyst treatment represents an emerging technology that shows promise to remove nitrate and nitrite from drinking water. In this work we use vapor-grown carbon nanofiber (CNF) supports in order to explore the effects of Pd nanoparticle size and interior versus exterior loading on nitrite reduction activity and selectivity (i.e., dinitrogen over ammonia production). Results show that nitrite reduction activity increases by 3.1-fold and selectivity decreases by 8.0-fold, with decreasing Pd nanoparticle size from 1.4 to 9.6 nm. Both activity and selectivity are not significantly influenced by Pd interior versus exterior CNF loading. Consequently, turnover frequencies (TOFs) among all CNF catalysts are similar, suggesting nitrite reduction is not sensitive to Pd location on CNFs nor Pd structure. CNF-based catalysts compare favorably to conventional Pd catalysts (i.e., Pd on activated carbon or alumina) with respect to nitrite reduction activity and selectivity, and they maintain activity over multiple reduction cycles. Hence, our results suggest new insights that an optimum Pd nanoparticle size on CNFs balances faster kinetics with lower ammonia production, that catalysts can be tailored at the nanoscale to improve catalytic performance for nitrite, and that CNFs hold promise as highly effective catalyst supports in drinking water treatment. © 2012 American Chemical Society.

  10. Enhanced Activity and Selectivity of Carbon Nanofiber Supported Pd Catalysts for Nitrite Reduction

    KAUST Repository

    Shuai, Danmeng

    2012-03-06

    Pd-based catalyst treatment represents an emerging technology that shows promise to remove nitrate and nitrite from drinking water. In this work we use vapor-grown carbon nanofiber (CNF) supports in order to explore the effects of Pd nanoparticle size and interior versus exterior loading on nitrite reduction activity and selectivity (i.e., dinitrogen over ammonia production). Results show that nitrite reduction activity increases by 3.1-fold and selectivity decreases by 8.0-fold, with decreasing Pd nanoparticle size from 1.4 to 9.6 nm. Both activity and selectivity are not significantly influenced by Pd interior versus exterior CNF loading. Consequently, turnover frequencies (TOFs) among all CNF catalysts are similar, suggesting nitrite reduction is not sensitive to Pd location on CNFs nor Pd structure. CNF-based catalysts compare favorably to conventional Pd catalysts (i.e., Pd on activated carbon or alumina) with respect to nitrite reduction activity and selectivity, and they maintain activity over multiple reduction cycles. Hence, our results suggest new insights that an optimum Pd nanoparticle size on CNFs balances faster kinetics with lower ammonia production, that catalysts can be tailored at the nanoscale to improve catalytic performance for nitrite, and that CNFs hold promise as highly effective catalyst supports in drinking water treatment. © 2012 American Chemical Society.

  11. Ammonia and water sorption properties of the mineral-layered nanomaterials used as the catalysts for NOx removal from exhaust gases

    International Nuclear Information System (INIS)

    Olszewska, D.

    2006-01-01

    The object of the study is the influence of acidity and hydrophilic properties of the surface of catalyst of the selective catalytic reduction (SCR) of nitrogen oxides by NH 3 . A series of catalysts prepared with the ZrO 2 -pillared montmorillonite from Jelsovy Potok have been promoted with manganese oxides. A part of the Na + -montmorillonite form has provisionally been treated with the 20% HCl. The acidity of materials was studied by the ammonia adsorption method at the temperature of 273 and 373K. Acidic properties of catalysts depend on the step of the support preparation-the acidic activation. The activity of the SCR reaction of acid untreated support and the catalyst with MnO x which had few stronger acid centres was lower than the activity of the acid pre-treated catalyst. In this case the support had more strong acid centres. The active material of MnO x increased the NO conversion but not the influence on the amount of ammonia sorption. These centres are probably not acidic centers. The hydrophilic properties were studied by water vapour sorption at the temperature of 298K. All the samples adsorbed the same amount of water, which suggests that the NO conversion does not influence hydrophilic properties. Water molecules were physically sorbed on the surface of materials and they were replaced with NH 3 in the presence of ammonia. (author)

  12. The Poisoning Effect of Na Doping over Mn-Ce/TiO2 Catalyst for Low-Temperature Selective Catalytic Reduction of NO by NH3

    Directory of Open Access Journals (Sweden)

    Liu Yang

    2014-01-01

    Full Text Available Sodium carbonate (Na2CO3, sodium nitrate (NaNO3, and sodium chloride (NaCl were chosen as the precursors to prepare the Na salts deposited Mn-Ce/TiO2 catalysts through an impregnation method. The influence of Na on the performance of the Mn-Ce/TiO2 catalyst for low-temperature selective catalytic reduction of NOx by NH3 was investigated. Experimental results showed that Na salts had negative effects on the activity of Mn-Ce/TiO2 and the precursors of Na salts also affected the catalytic activity. The precursor Na2CO3 had a greater impact on the catalytic activity, while NaNO3 had minimal effect. The characterization results indicated that the significant changes in physical and chemical properties of Mn-Ce/TiO2 were observed after Na was doped on the catalysts. The significant decreases in surface areas and NH3 adsorption amounts were observed after Na was doped on the catalysts, which could be considered as the main reasons for the deactivation of Na deposited Mn-Ce/TiO2.

  13. Polymer supported organic catalysts for O2 reduction in Li-O2 batteries

    International Nuclear Information System (INIS)

    Weng, Wei; Barile, Christopher J.; Du, Peng; Abouimrane, Ali; Assary, Rajeev S.; Gewirth, Andrew A.; Curtiss, Larry A.; Amine, Khalil

    2014-01-01

    Graphical abstract: - Abstract: A novel organic catalyst has been synthesized that contains an anthraquinone moiety supported on a polymer backbone. This oxygen reduction catalyst was successfully incorporated in the cathode of Li-O 2 batteries. The addition of the anthraquinone-based catalyst improved the cycleability of the Li-O 2 battery when cycled in a tetraethylene glycol dimethyl ether electrolyte. Computational studies coupled with a wide range of analytical techniques including differential electrochemical mass spectrometry, cyclic voltammetry, electrochemical impedence spectroscopy, and X-ray diffraction were used to interrogate the Li-O 2 battery with and without the organic catalyst present. This study suggests that organic catalysts may serve as light and inexpensive alternatives to the precious metals frequently used in Li-O 2 batteries

  14. Activity and Stability of Nanoscale Oxygen Reduction Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Shao-Horn, Yang

    2015-07-28

    Design of highly active and stable nanoscale catalysts for electro-oxidation of small organic molecules is of great importance to the development of efficient fuel cells. The amount and instability of Pt-based catalysts in the cathode limits the cost, efficiency and lifetime of proton exchange membrane fuel cells. We developed a microscopic understanding of the factors governing activity and stability in Pt and PtM alloys. Experimental efforts were focused on probing the size and shape dependence of ORR activity of Pt-based nanoparticles supported on carbon nanotubes. A microscopic understanding of the activity was achieved by correlating voltammetry and rotating ring disk electrodes to surface atomic and electronic structures, which were elucidated predominantly by high-resolution transmission electron microscopy (HRTEM), Scanning transmission electron microscopy energy dispersive X-ray Spectroscopy (STEM-EDS) and synchrotron X-ray absorption spectroscopy (XAS).

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

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Jae-Soon [ORNL; Partridge Jr, William P [ORNL; Pihl, Josh A [ORNL; Kim, Miyoung [ORNL; Koci, Petr [Institute of Chemical Technology, Prague, Czech Republic; Daw, C Stuart [ORNL

    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.

  16. Control and reduction of NOx emissions on light hydrocarbons combustion in fluidized bed combustors: a technological prospection surveys; Controle e reducao de emissoes de NOx durante queima de hidrocarbonetos leves em combustores a leito fluidizado: um estudo de prospeccao tecnologica

    Energy Technology Data Exchange (ETDEWEB)

    Santos, Douglas Alves; Winter, Eduardo [Instituto Nacional da Propriedade Industrial (INPI), Rio de Janeiro, RJ (Brazil)

    2008-07-01

    The present paper aims a technological prospecting study of the main technological agents involved in industrial light hydrocarbons combustion process. More specifically, the work approaches technologies applied to nitrogen oxides emissions control and reduction. Nitrogen oxides are typically known as 'NOx' (NO, N{sub 2}O, NO{sub 2}). 'NOx' are byproducts from fuel burning in combustion systems, including also in fluidized bed combustion systems. The technological prospecting study employed 'technology foresight' as tool for evaluating the technological perspectives of the thermal generation, basis on environment protection. Such technological perspectives of the thermal generation were evaluated through invention patent documents. The query methodology for obtaining of patent documents employed a free patent base, known as ESPACENET. Additionally, the documents obtained were evaluated, considering beyond the countries and the publication dates, technological perspectives employed to 'NOx' emissions control and reduction. It is very important to highlight around 70% of the industrial technological information are just found in invention patent documents. (author)

  17. Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol

    DEFF Research Database (Denmark)

    Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank

    2014-01-01

    The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO 2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO...... 2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO 2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni......-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni 5 Ga 3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al 2 O 3 catalysts revealed the same or better methanol synthesis activity, as well as considerably...

  18. Nitrogen-based catalysts for the electrochemical reduction of CO2 to CO.

    Science.gov (United States)

    Tornow, Claire E; Thorson, Michael R; Ma, Sichao; Gewirth, Andrew A; Kenis, Paul J A

    2012-12-05

    The synthesis and application of carbon-supported, nitrogen-based organometallic silver catalysts for the reduction of CO(2) is studied using an electrochemical flow reactor. Their performance toward the selective formation of CO is similar to the performance achieved when using Ag as the catalyst, but comparatively at much lower silver loading. Faradaic efficiencies of the organometallic catalyst are higher than 90%, which are comparable to those of Ag. Furthermore, with the addition of an amine ligand to Ag/C, the partial current density for CO increases significantly, suggesting a possible co-catalyst mechanism. Additional improvements in activity and selectivity may be achieved as greater insight is obtained on the mechanism of CO(2) reduction and on how these complexes assemble on the carbon support.

  19. Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe?N?C Catalysts

    OpenAIRE

    Choi, Chang Hyuck; Choi, Won Seok; Kasian, Olga; Mechler, Anna K.; Sougrati, Moulay Tahar; Br?ller, Sebastian; Strickland, Kara; Jia, Qingying; Mukerjee, Sanjeev; Mayrhofer, Karl J. J.; Jaouen, Fr?d?ric

    2017-01-01

    Abstract Fe?N?C catalysts with high O2 reduction performance are crucial for displacing Pt in low?temperature fuel cells. However, insufficient understanding of which reaction steps are catalyzed by what sites limits their progress. The nature of sites were investigated that are active toward H2O2 reduction, a key intermediate during indirect O2 reduction and a source of deactivation in fuel cells. Catalysts comprising different relative contents of FeN x C y moieties and Fe particles encapsu...

  20. Experiment study on NOx reduction through biomass reburning in an entrained flow reactor

    Energy Technology Data Exchange (ETDEWEB)

    Lu, P.; Wang, Y.; Lu, F.; Liu, Y. [Nanjing Normal Univ. (China). School of Energy and Mechanical Engineering

    2013-07-01

    The reburning experiments with six kinds of biomass (including rice straw, wheat straw, maize stalk, cotton stalk, rice husk and bagasse,) and one biochar (wheat straw char) was carried out in an entrained flow reactor. The effects of biomass type, stoichiometric ratio in the reburning-zone (SR2), reaction temperature in the reburning-zone (t{sub 2}), particle sizes of biomass (d{sub p}), and reburning fuel fraction (R{sub ff}) on NO reduction efficiency analysed. The NO heterogeneous reduction contribute of biochar was also analyzed. The results indicate that NO reduction efficiency behaves a trend of first increase and then decrease with decreasing of SR2 or increasing of R{sub ff}. The higher NO reduction efficiency (more than 50%) can be achieved at the range of SR2 = 0.7-0.8 or R{sub ff} = 20-26% during reburning with six tested biomass. Cotton stalk with higher volatiles and the highest contents of K, Na alkali metals behaves the best performance of NO reduction. In the range of t{sub 2} = 900-1,100 C NO reduction efficiency increases with increasing of reburning-zone reaction temperature at the same SR2. NO reduction efficiency increases insignificantly with decreasing of particle size of biomass while d{sub p} < 425{mu}m. The contribution of NO heterogeneous reduction by wheat straw char to the total NO reduction is in the higher range of 59-68% while R{sub ff} = 10-26%.

  1. Influence of BaO in perovskite electrodes for the electrochemical reduction of NOx

    DEFF Research Database (Denmark)

    Simonsen, Vibe Louise Ernlund; Johnsen, M.M.; Kammer Hansen, Kent

    2007-01-01

    Using the point electrode method, the effect of BaO on electrochemical reduction of NO (x) was investigated using the perovskites La0.85Sr0.15MnO3 (LSM15) and La0.85Sr0.15CoO3 (LSCo15) as electrode materials. The experiments were carried out in the temperature range 400-600 degrees C in 1% NO and...... favored oxygen reduction compared to reduction of nitric oxide. The LSCO15 electrode containing BaO reacted to form a K2NiF4-structure and was not tested further....

  2. Catalysts for the reduction of SO{sub 2} to elemental sulfur

    Energy Technology Data Exchange (ETDEWEB)

    Jin, Y.; Yu, Q.Q.; Chang, S.G. [Lawrence Berkeley Lab., Berkeley, CA (United States)

    1995-11-01

    Catalysts have been prepared for the reduction of SO{sub 2} to elemental sulfur by synthesis gas. A catalyst allows to obtain more than 97% yield of elemental sulfur with a single-stage reactor at 540{degrees}C. A lifetime test has been successfully performed. The mass balance of sulfur and carbon has been checked. The effect of H{sub 2}S, COS, and H{sub 2}O has been studied.

  3. Carbon-supported cubic CoSe2 catalysts for oxygen reduction reaction in alkaline medium

    International Nuclear Information System (INIS)

    Feng Yongjun; Alonso-Vante, Nicolas

    2012-01-01

    Highlights: ► Cubic CoSe 2 a non-precious metal electrocatalyst for oxygen reduction in KOH. ► The catalyst shows four-electron transfer pathway in overall reaction. ► Catalyst has higher methanol tolerance than commercial Pt/C catalyst. - Abstract: A Carbon-supported CoSe 2 nanocatalyst has been developed as an alternative non-precious metal electrocatalyst for oxygen reduction reaction (ORR) in alkaline medium. The catalyst was prepared via a surfactant-free route and its electrocatalytic activity for the ORR has been investigated in detail in 0.1 M KOH electrolyte at 25 °C using rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) techniques. The prepared catalyst showed promising catalytic activity towards ORR in a four-electron transfer pathway and higher tolerance to methanol compared to commercial Pt/C catalyst in 0.1 M KOH. To some extent, the increase of CoSe 2 loading on the electrode favors a faster reduction of H 2 O 2 intermediate to H 2 O.

  4. Modeling analysis of urea direct injection on the NOx emission reduction of biodiesel fueled diesel engines

    International Nuclear Information System (INIS)

    An, H.; Yang, W.M.; Li, J.; Zhou, D.Z.

    2015-01-01

    Highlights: • The effects of urea direct injection on NO x emissions reduction was investigated. • Aqueous urea solution was proposed to be injected after the fuel injection process. • The optimized injection strategy achieved a reduction efficiency of 58%. • There were no severe impacts on the CO emissions and BSFC. - Abstract: In this paper, a numerical simulation study was conducted to explore the possibility of an alternative approach: direct aqueous urea solution injection on the reduction of NO x emissions of a biodiesel fueled diesel engine. Simulation studies were performed using the 3D CFD simulation software KIVA4 coupled with CHEMKIN II code for pure biodiesel combustion under realistic engine operating conditions of 2400 rpm and 100% load. The chemical behaviors of the NO x formation and urea/NO x interaction processes were modeled by a modified extended Zeldovich mechanism and urea/NO interaction sub-mechanism. To ensure an efficient NO x reduction process, various aqueous urea injection strategies in terms of post injection timing, injection angle, and injection rate and urea mass fraction were carefully examined. The simulation results revealed that among all the four post injection timings (10 °ATDC, 15 °ATDC, 20 °ATDC and 25 °ATDC) that were evaluated, 15 °ATDC post injection timing consistently demonstrated a lower NO emission level. The orientation of the aqueous urea injection was also shown to play a critical role in determining the NO x removal efficiency, and 50 degrees injection angle was determined to be the optimal injection orientation which gave the most NO x reduction. In addition, both the urea/water ratio and aqueous urea injection rate demonstrated important roles which affected the thermal decomposition of urea into ammonia and the subsequent NO x removal process, and it was suggested that 50% urea mass fraction and 40% injection rate presented the lowest NO emission levels. At last, with the optimized injection

  5. Reactivity of Aryl Halides for Reductive Dehalogenation in (Seawater Using Polymer-Supported Terpyridine Palladium Catalyst

    Directory of Open Access Journals (Sweden)

    Toshimasa Suzuka

    2015-05-01

    Full Text Available A polymer-supported terpyridine palladium complex was prepared. The complex was found to promote hydrodechlorination of aryl chlorides with potassium formate in seawater. Generally, reductive cleavage of aryl chlorides using transition metal catalysts is more difficult than that of aryl bromides and iodides (reactivity: I > Br > Cl; however, the results obtained did not follow the general trend. Therefore, we investigated the reaction inhibition agents and found a method to remove these inhibitors. The polymeric catalysts showed high catalytic activity and high reusability for transfer reduction in seawater.

  6. Nitrogen-doped carbon-supported cobalt-iron oxygen reduction catalyst

    Science.gov (United States)

    Zelenay, Piotr; Wu, Gang

    2014-04-29

    A Fe--Co hybrid catalyst for oxygen reaction reduction was prepared by a two part process. The first part involves reacting an ethyleneamine with a cobalt-containing precursor to form a cobalt-containing complex, combining the cobalt-containing complex with an electroconductive carbon supporting material, heating the cobalt-containing complex and carbon supporting material under conditions suitable to convert the cobalt-containing complex and carbon supporting material into a cobalt-containing catalyst support. The second part of the process involves polymerizing an aniline in the presence of said cobalt-containing catalyst support and an iron-containing compound under conditions suitable to form a supported, cobalt-containing, iron-bound polyaniline species, and subjecting said supported, cobalt-containing, iron bound polyaniline species to conditions suitable for producing a Fe--Co hybrid catalyst.

  7. Pt Monolayer Shell on Nitrided Alloy Core—A Path to Highly Stable Oxygen Reduction Catalyst

    Directory of Open Access Journals (Sweden)

    Jue Hu

    2015-07-01

    Full Text Available The inadequate activity and stability of Pt as a cathode catalyst under the severe operation conditions are the critical problems facing the application of the proton exchange membrane fuel cell (PEMFC. Here we report on a novel route to synthesize highly active and stable oxygen reduction catalysts by depositing Pt monolayer on a nitrided alloy core. The prepared PtMLPdNiN/C catalyst retains 89% of the initial electrochemical surface area after 50,000 cycles between potentials 0.6 and 1.0 V. By correlating electron energy-loss spectroscopy and X-ray absorption spectroscopy analyses with electrochemical measurements, we found that the significant improvement of stability of the PtMLPdNiN/C catalyst is caused by nitrogen doping while reducing the total precious metal loading.

  8. Nanostructured Mn{sub x}O{sub y} for oxygen reduction reaction (ORR) catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Delmondo, Luisa, E-mail: luisa.delmondo@polito.it [Department of Applied Science and Technology—DISAT, Politecnico di Torino, C.so Duca degli Abruzzi 24, 10129 Torino (Italy); Salvador, Gian Paolo; Muñoz-Tabares, José Alejandro; Sacco, Adriano; Garino, Nadia; Castellino, Micaela [Center for Space Human Robotics @PoliTo, Istituto Italiano di Tecnologia, C.so Trento 21, 10129 Torino (Italy); Gerosa, Matteo; Massaglia, Giulia [Department of Applied Science and Technology—DISAT, Politecnico di Torino, C.so Duca degli Abruzzi 24, 10129 Torino (Italy); Center for Space Human Robotics @PoliTo, Istituto Italiano di Tecnologia, C.so Trento 21, 10129 Torino (Italy); Chiodoni, Angelica; Quaglio, Marzia [Center for Space Human Robotics @PoliTo, Istituto Italiano di Tecnologia, C.so Trento 21, 10129 Torino (Italy)

    2016-12-01

    Highlights: • Good performance catalysts for oxygen reduction reaction. • Nanostructured low-cost catalysts respect to platinum ones. • Synthesis using environmental benign chemical reagents. - Abstract: In the field of fuel cells, oxygen plays a key role as the final electron acceptor. To facilitate its reduction (Oxygen Reduction Reaction—ORR), a proper catalyst is needed and platinum is considered the best one due to its low overpotential for this reaction. By considering the high price of platinum, alternative catalysts are needed and manganese oxides (Mn{sub x}O{sub y}) can be considered promising substitutes. They are inexpensive, environmental friendly and can be obtained into several forms; most of them show significant electro-catalytic performance, even if strategies are needed to increase their efficiency. In particular, by developing light and high-surface area materials and by optimizing the presence of catalytic sites, we can obtain a cathode with improved electro-catalytic performance. In this case, nanofibers and xerogels are two of the most promising nanostructures that can be used in the field of catalysis. In this work, a study of the morphological and catalytic behavior of Mn{sub x}O{sub y} nanofibers and xerogels is proposed. Nanofibers were obtained by electrospinning, while xerogels were prepared by sol-gel and freeze drying techniques. Despite of the different preparation approaches, the obtained nanostructured manganese oxides exhibited similar catalytic performance for the ORR, comparable to those obtained from Pt catalysts.

  9. Coupled Metal/Oxide Catalysts with Tunable Product Selectivity for Electrocatalytic CO2 Reduction.

    Science.gov (United States)

    Huo, Shengjuan; Weng, Zhe; Wu, Zishan; Zhong, Yiren; Wu, Yueshen; Fang, Jianhui; Wang, Hailiang

    2017-08-30

    One major challenge to the electrochemical conversion of CO 2 to useful fuels and chemical products is the lack of efficient catalysts that can selectively direct the reaction to one desirable product and avoid the other possible side products. Making use of strong metal/oxide interactions has recently been demonstrated to be effective in enhancing electrocatalysis in the liquid phase. Here, we report one of the first systematic studies on composition-dependent influences of metal/oxide interactions on electrocatalytic CO 2 reduction, utilizing Cu/SnO x heterostructured nanoparticles supported on carbon nanotubes (CNTs) as a model catalyst system. By adjusting the Cu/Sn ratio in the catalyst material structure, we can tune the products of the CO 2 electrocatalytic reduction reaction from hydrocarbon-favorable to CO-selective to formic acid-dominant. In the Cu-rich regime, SnO x dramatically alters the catalytic behavior of Cu. The Cu/SnO x -CNT catalyst containing 6.2% of SnO x converts CO 2 to CO with a high faradaic efficiency (FE) of 89% and a j CO of 11.3 mA·cm -2 at -0.99 V versus reversible hydrogen electrode, in stark contrast to the Cu-CNT catalyst on which ethylene and methane are the main products for CO 2 reduction. In the Sn-rich regime, Cu modifies the catalytic properties of SnO x . The Cu/SnO x -CNT catalyst containing 30.2% of SnO x reduces CO 2 to formic acid with an FE of 77% and a j HCOOH of 4.0 mA·cm -2 at -0.99 V, outperforming the SnO x -CNT catalyst which only converts CO 2 to formic acid in an FE of 48%.

  10. OPTIMIZED FUEL INJECTOR DESIGN FOR MAXIMUM IN-FURNACE NOx REDUCTION AND MINIMUM UNBURNED CARBON

    Energy Technology Data Exchange (ETDEWEB)

    SAROFIM, A F; LISAUSKAS, R; RILEY, D; EDDINGS, E G; BROUWER, J; KLEWICKI, J P; DAVIS, K A; BOCKELIE, M J; HEAP, M P; PERSHING, D

    1998-01-01

    Reaction Engineering International (REI) has established a project team of experts to develop a technology for combustion systems which will minimize NO x emissions and minimize carbon in the fly ash. This much need technology will allow users to meet environmental compliance and produce a saleable by-product. This study is concerned with the NO x control technology of choice for pulverized coal fired boilers,"in-furnace NOx control," which includes: staged low-NOx burners, reburning, selective non-catalytic reduction (SNCR) and hybrid approaches (e.g., reburning with SNCR). The program has two primary objectives: 1) To improve the performance of "in-furnace" NOx control, processes. 2) To devise new, or improve existing, approaches for maximum "in-furnace" NOx control and minimum unburned carbon. The program involves: 1) fundamental studies at laboratory- and bench-scale to define NO reduction mechanisms in flames and reburning jets; 2) laboratory experiments and computer modeling to improve our two-phase mixing predictive capability; 3) evaluation of commercial low-NOx burner fuel injectors to develop improved designs, and 4) demonstration of coal injectors for reburning and low-NOx burners at commercial scale. The specific objectives of the two-phase program are to: 1 Conduct research to better understand the interaction of heterogeneous chemistry and two phase mixing on NO reduction processes in pulverized coal combustion. 2 Improve our ability to predict combusting coal jets by verifying two phase mixing models under conditions that simulate the near field of low-NOx burners. 3 Determine the limits on NO control by in-furnace NOx control technologies as a function of furnace design and coal type. 5 Develop and demonstrate improved coal injector designs for commercial low-NOx burners and coal reburning systems. 6 Modify the char burnout model in REI's coal

  11. NOx formation and selective non-catalytic reduction (SNCR) in a fluidized bed combustor of biomass

    International Nuclear Information System (INIS)

    Mahmoudi, Shiva; Baeyens, Jan; Seville, Jonathan P.K.

    2010-01-01

    Caledonian Paper (CaPa) is a major paper mill, located in Ayr, Scotland. For its steam supply, it previously relied on the use of a Circulating Fluidized Bed Combustor (CFBC) of 58 MW th , burning coal, wood bark and wastewater treatment sludge. It currently uses a bubbling fluidized bed combustor (BFBC) of 102 MW th to generate steam at 99 bar, superheated to 465 o C. The boiler is followed by steam turbines and a 15 kg/s steam circuit into the mill. Whereas previously coal, wood bark and wastewater treatment sludge were used as fuel, currently only plantation wood (mainly spruce), demolition wood, wood bark and sludge are used. Since these biosolids contain nitrogen, fuel NO x is formed at the combustion temperature of 850-900 o C. NO x emissions (NO + NO 2 ) vary on average between 300 and 600 mg/Nm 3 (dry gas). The current emission standard is 350 mg/Nm 3 but will be reduced in the future to a maximum of 233 mg/Nm 3 for stand-alone biomass combustors of capacity between 50 and 300 MW th according to the EU LCP standards. NO x abatement is therefore necessary. In the present paper we firstly review the NO x formation mechanisms, proving that for applications of fluidized bed combustion, fuel NO x is the main consideration, and the contribution of thermal NO x to the emissions insignificant. We then assess the deNO x techniques presented in the literature, with an updated review and special focus upon the techniques that are applicable at CaPa. From these techniques, Selective Non-catalytic Reduction (SNCR) using ammonia or urea emerges as the most appropriate NO x abatement solution. Although SNCR deNO x is a selective reduction, the reactions of NO x reduction by NH 3 in the presence of oxygen, and the oxidation of NH 3 proceed competitively. Both reactions were therefore studied in a lab-scale reactor and the results were transformed into design equations starting from the respective reaction kinetics. An overall deNO x yield can then be predicted for any

  12. Reactivity of Surface Nitrates in H2-Assisted SCR of NOx Over Ag/Al2O3 Catalyst

    DEFF Research Database (Denmark)

    Sadokhina, N. A.; Doronkin, Dmitry E.; Baeva, G. N.

    2013-01-01

    The role of nitrate ad-species in H2-assisted SCR over Ag/Al2O3 was compared in NH3-SCR and n-C6H14-SCR processes. It was found that nitrates could be reduced by NH3 or n-C6H14 at similar rates with H2 co-feeding which indicates a common rate-limiting step. However, contributions of surface nitrate...... reduction to the overall NH3-SCR or n-C6H14-SCR are different as revealed by comparing the rates of nitrate reduction with the rates of steady-state processes. The rate of the steady-state n-C6H14-SCR is virtually identical to the rate of surface nitrate reduction suggesting a significant contribution...... of the surface nitrates reduction to the overall n-C6H14-SCR process. On the other hand, the steady-state rate of NH3-SCR is by ~15 times higher, which indicates that the reduction of surface nitrates plays a marginal role in the overall NH3-SCR....

  13. Selective catalytic reduction (SCR) NOx control for small natural gas-fired prime movers

    International Nuclear Information System (INIS)

    Shareef, G.S.; Stone, D.K.; Ferry, K.R.; Johnson, K.L.; Locke, K.S.

    1992-01-01

    The application of selective catalytic reduction (SCR) to small natural gas-fired prime movers at cogeneration facilities and compressor stations could possibly increase due to regulatory forces to limit NO x from such sources. The natural gas industry is presently without a current database with which to evaluate the cost and operating characteristics of SCR under the conditions anticipated for small prime movers. This paper presents the results from a two-phase study undertaken to document SCR applications with emphasis on SCR system performance and costs. The database of small natural gas-fired prime mover SCR experience, focusing on prime mover characterization, SCR system performance, and SCR system costs will be described. Result from analysis of performance and cost data will be discussed, including analytical tools developed to project SCR system performance and costs

  14. Evaluation of NOx-reduction with SNCR in a waste-fueled boiler

    International Nuclear Information System (INIS)

    Gromulski, J.; Hinderson, A.; Johansson, A.; Sfiris, G.; Sjoeberg, M.; Westermark, M.

    1994-10-01

    SNCR (Selective Non-Catalytic Reduction) is a method for reducing the level of nitrogen oxides in flue gas that has attracted a lot of attention and has been put to use in several units, both in Sweden and abroad. The chemical basis for this method is the fact that certain nitrogen compounds with a hydrogen content (ammonia, urea, etc) react with nitrogen oxides, forming elementary nitrogen. The maximum NO x removal is obtained when the reducing chemical is injected in the flue gas at a point where the temperature is about 870 - 1010 deg C. The measured removal of NO x using the SNCR system was 30-90%. Most of the observations indicate a NO x removal of 40-60%. The complete picture shows a somewhat improved removal of NO x at lower loads, but also higher emission values for ammonia and nitrous oxide. Within the tested temperature span (870-1020 deg C at high load, and 810-910 deg C at low loads) there is no detectable correlation between temperature and removal of NO x , NH 3 , N 2 O and CO. The dominant factors are stoichiometric ratio and boiler load. The economic evaluation indicates that during 1993, with an average emission reduction of 56%, the NO x emission fee is reduced from 12371 kSEK/yr without flue gas treatment to 5458 kSEK. The total operating costs for the SNCR system (capital cost excluded) being 1248 kSEK/yr, this means a net profit of 5665 kSEK/yr. This means the pay-off time will be about 0.7 year. Note that this figure is computed without regard to capital cost. 74 figs, 9 tabs

  15. Catalytic selective reduction of NO with ethylene over a series of copper catalysts on amorphous silicas

    International Nuclear Information System (INIS)

    Carniti, P.; Gervasini, A.; Modica, V.H.; Ravasio, N.

    2000-01-01

    Catalytic selective reduction of NO to N 2 was studied comparing a series of Cu-based catalysts (ca. 8wt.%) supported over amorphous pure and modified silicas: SiO 2 , SiO 2 -Al 2 O 3 , SiO 2 -TiO 2 , SiO 2 -ZrO 2 . The catalysts were prepared by the chemisorption-hydrolysis method which ensured the formation of a unique copper phase well dispersed over all supports, as confirmed by scanning electron micrographs (SEMs). Temperature-programmed reduction (TPR) analyses confirmed the presence of dispersed copper species which underwent complete reduction at a temperature of about 220C, independently of the support. It was found that the support affects the extent of NO reduction as well as the selectivity to N 2 formation. Maximum N 2 yield was found in the range 275-300C. The catalyst prepared over SiO 2 -Al 2 O 3 was the most active and selective with respect to the other silicas. Competitiveness factors (c.f.'s) as high as 13-20% in the temperature range 200-250C could be calculated. For all catalysts, the temperature of the N 2 peak maximum did not correspond to that of the maximum C 2 H 4 oxidation to CO 2 , suggesting the presence of two different sites for the oxidation and the reduction activity. On the catalyst prepared on SiO 2 -Al 2 O 3 , a kinetic interpretation of catalytic data collected at different contact times and temperatures permitted evaluating the ratio between kinetic coefficients as well as the difference between activation energies of NO reduction by C 2 H 4 and C 2 H 4 oxidation by O 2

  16. Oxygen reduction reaction catalysts of manganese oxide decorated by silver nanoparticles for aluminum-air batteries

    International Nuclear Information System (INIS)

    Sun, Shanshan; Miao, He; Xue, Yejian; Wang, Qin; Li, Shihua; Liu, Zhaoping

    2016-01-01

    In this paper, the hybrid catalysts of manganese oxide decorated by silver nanoparticles (Ag-MnO x ) are fully investigated and show the excellent oxygen reduction reaction (ORR) activity. The Ag-MnO 2 is synthesized by a facile strategy of the electroless plating of silver on the manganese oxide. The catalysts are characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Then, the ORR activities of the catalysts are systematically investigated by the rotating disk electrode (RDE) and aluminum-air battery technologies. The Ag nanoparticles with the diameters at about 10 nm are anchored on the surface of α-MnO 2 and a strong interaction between Ag and MnO 2 components in the hybrid catalyst are confirmed. The electrochemical tests show that the activity and stability of the 50%Ag-MnO 2 composite catalyst (the mass ratio of Ag/MnO 2 is 1:1) toward ORR are greatly enhanced comparing with single Ag or MnO 2 catalyst. Moreover, the peak power density of the aluminum-air battery with 50%Ag-MnO 2 can reach 204 mW cm −2 .

  17. Oxidation of mercury across selective catalytic reduction catalysts in coal-fired power plants

    Energy Technology Data Exchange (ETDEWEB)

    Constance L. Senior [Reaction Engineering International, Salt Lake City, UT (United States)

    2006-01-15

    A kinetic model for predicting the amount of mercury (Hg) oxidation across selective catalytic reduction (SCR) systems in coal-fired power plants was developed and tested. The model incorporated the effects of diffusion within the porous SCR catalyst and the competition between ammonia and Hg for active sites on the catalyst. Laboratory data on Hg oxidation in simulated flue gas and slipstream data on Hg oxidation in flue gas from power plants were modeled. The model provided good fits to the data for eight different catalysts, both plate and monolith, across a temperature range of 280-420{sup o}C, with space velocities varying from 1900 to 5000 hr{sup -1}. Space velocity, temperature, hydrochloric acid content of the flue gas, ratio of ammonia to nitric oxide, and catalyst design all affected Hg oxidation across the SCR catalyst. The model can be used to predict the impact of coal properties, catalyst design, and operating conditions on Hg oxidation across SCRs. 20 refs., 9 figs., 2 tabs.

  18. Evaluation of mechanical properties in metal wire mesh supported selective catalytic reduction (SCR) catalyst structures

    Science.gov (United States)

    Rajath, S.; Siddaraju, C.; Nandakishora, Y.; Roy, Sukumar

    2018-04-01

    The objective of this research is to evaluate certain specific mechanical properties of certain stainless steel wire mesh supported Selective catalytic reduction catalysts structures wherein the physical properties of the metal wire mesh and also its surface treatments played vital role thereby influencing the mechanical properties. As the adhesion between the stainless steel wire mesh and the catalyst material determines the bond strength and the erosion resistance of catalyst structures, surface modifications of the metal- wire mesh structure in order to facilitate the interface bonding is therefore very important to realize enhanced level of mechanical properties. One way to enhance such adhesion properties, the stainless steel wire mesh is treated with the various acids, i.e., chromic acid, phosphoric acid including certain mineral acids and combination of all those in various molar ratios that could generate surface active groups on metal surface that promotes good interface structure between the metal- wire mesh and metal oxide-based catalyst material and then the stainless steel wire mesh is dipped in the glass powder slurry containing some amount of organic binder. As a result of which the said catalyst material adheres to the metal-wire mesh surface more effectively that improves the erosion profile of supported catalysts structure including bond strength.

  19. Efficient oxygen reduction reaction using ruthenium tetrakis(diaquaplatinum)octacarboxyphthalocyanine catalyst supported on MWCNT platform

    CSIR Research Space (South Africa)

    Maxakato, NW

    2011-02-01

    Full Text Available -1 Electroanalysis 2011, 23, No. 2, 325 ? 329 Efficient Oxygen Reduction Reaction Using Ruthenium Tetrakis(diaquaplatinum)Octacarboxyphthalocyanine Catalyst Supported on MWCNT Platform Nobanathi W. Maxakato,a Solomon A. Mamuru,a Kenneth I. Ozoemena*a, b a...

  20. Fuel cell electrocatalsis : oxygen reduction on Pt-based nanoparticle catalysts

    NARCIS (Netherlands)

    Vliet, Dennis Franciscus van der

    2010-01-01

    The thesis contains a discussion on the subject of the Oxygen Reduction Reaction (ORR) on Pt-alloy nanoparticle catalysts in the Rotating Disk Electrode (RDE) method. An insight in some of the difficulties of this method is given with proper solutions and compensations for these problems. Pt3Co,

  1. Comparison of Bimetallic and Trimetallic Catalyst in Reductive Dechlorination; Influence of Copper Addition

    Czech Academy of Sciences Publication Activity Database

    Kaštánek, František; Kaštánek, Petr; Maléterová, Ywetta; Kallistová, A.; Šolcová, Olga

    2015-01-01

    Roč. 2, č. 7 (2015), s. 1954-1958 E-ISSN 3159-0040 R&D Projects: GA TA ČR TA04020700 Institutional support: RVO:67985858 ; RVO:67985831 Keywords : PCB * reductive dechlorination * bimetallic and trimetallic catalysts Subject RIV: CI - Industrial Chemistry, Chemical Engineering http://www.jmest.org/wp-content/uploads/JMESTN42350950.pdf

  2. Oxygen reduction on carbon supported platinum catalysts in high temperature polymer electrolytes

    DEFF Research Database (Denmark)

    Qingfeng, Li; Bergqvist, R. S.; Hjuler, H. A.

    1999-01-01

    Oxygen reduction on carbon supported platinum catalysts has been investigated in H3PO4, H3PO4-doped Nafion and PBI polymer electrolytes in a temperature range from 80 to 190°C. Compared with pure H3PO4, using the H3PO4 doped Nafion and PBI polymer electrolytes can significantly improve the oxygen...

  3. Evaluation of NOx-reduction with SNCR in a waste-fueled boiler

    International Nuclear Information System (INIS)

    Gromulski, J.; Hinderson, A.; Johansson, A.; Sfiris, G.; Sjoeberg, M.; Westermark, M.

    1994-10-01

    SNCR (Selective Non-Catalytic Reduction) is a method for reducing the level of nitrogen oxides in flue gas that has attracted a lot of attention and has been put to use in several units, both in Sweden and abroad. The chemical basis for this method is the fact that certain nitrogen compounds with a hydrogen content (ammonia, urea, etc) react with nitrogen oxides, forming elementary nitrogen. The maximum NO x removal is obtained when the reducing chemical is injected in the flue gas at a point where the temperature is about 870 - 1010 deg C. The measured removal of NO x using the SNCR system was 35-50%. The stoichiometric addition of urea corresponded to 0.55-0.85 moles of urea per mole of NO x in the untreated flue gas. The addition of urea seems to be the main reason for the development of N 2 O gas. Most of the observations (appr 70%) during long-term evaluation indicate a NO x removal of 40-60%. The economic evaluation indicates that during 1993, with an average NO x removal of 46%, the NO x fee was reduced from 5951 kSEK/yr without treatment to 3195 kSEK/yr with treatment. With the total cost of the urea used for the SNCR system being 144 kSEK/yr, the contribution to profit becomes 2612 kSEK/yr, capital, electricity, staff and maintenance costs excluded. Thus, the pay-off time is appr. 1.7 yrs, with an investment of 4500 kSEK. 58 figs, 7 tabs

  4. Assessing the impact of primary measures for NOx reduction on the thermal power plant steam boiler

    International Nuclear Information System (INIS)

    Stupar, Goran; Tucaković, Dragan; Živanović, Titoslav; Belošević, Srdjan

    2015-01-01

    The European normatives prescribe content of 200 mg/Nm 3 NO x for pulverized coal combusting power plants. In order to reduce content of NO x in Serbian thermal power plant (TPP) 'Kostolac B' it's necessary to implement particular measures until 2016. The mathematical model of lignite combustion in the steam boiler furnace is defined and applied to analyze the possibility of implementing certain primary measures for reducing nitrogen oxides and their effects on the steam boiler operation. This model includes processes in the coal-fired furnace and defines radiating reactive two-phase turbulent flow. The model of turbulent flow also contains sub-model of fuel and thermal NO x formation and destruction. This complex mathematical model is related to thermal and aerodynamic calculations of the steam boiler within a unified calculation system in order to analyze the steam boiler overall work. This system provides calculations with a number of influential parameters. The steam boiler calculations for unit 1 (350 MWe) of TPP 'Kostolac B' are implemented for existing and modified combustion system in order to achieve effective, reliable and ecological facility work. The paper presents the influence analysis of large number of parameters on the steam boiler operation with an accepted concept of primary measures. Presented system of calculations is verified against measurements in TPP 'Kostolac B'. - Highlights: • Modern steam boilers need to operate according to ecological standards. • Possibility of applying some of the primary measures of NO x reduction. • Conventional calculations have no possibility to estimate sub-stoichiometric combustion. • Develop a new method of connecting the calculations. • Analysis shows the most favorable operation boiler regime (efficiency and ecology)

  5. Simultaneous reduction of NOx and smoke in a dual fuel DI diesel engine

    International Nuclear Information System (INIS)

    Barik, Debabrata; Murugan, S.

    2014-01-01

    Highlights: • A solution to use the de-oiled cakes disposed from oil industries. • Biogas produced from Karanja de-oiled cakes contains about 73% methane. • Simultaneous reduction of NO and smoke is possible with KME–biogas dual fuel operation. • Up to 30% replacement of KME is possible with induction of biogas at 0.9 kg/h. • Improved part load performance and emission with KME–biogas dual fuel. - Abstract: This paper presents the results of an experimental investigation conducted on a compression ignition (CI) engine, modified to run on dual fuel mode, using biogas as a primary fuel and KME (Karanja methyl ester) as a pilot fuel. The biogas was produced by anaerobic digestion of Pongamia pinnata (Karanja) seed cakes. In dual fuel mode, the biogas was inducted at four different flow rates, viz. 0.3 kg/h, 0.6 kg/h, 0.9 kg/h and 1.2 kg/h through the intake manifold of the engine. The biogas flow rate of 0.9 kg/h gave a better performance and lower emissions, than those of the other flow rates. The NO and smoke emissions were found to be lower by about 34% and 14%, than those of KME operation, at full load. The ignition delay was longer by about 1–2 °CA in the dual fuel operation, than that of KME at full load. The part load performance was found to be better in dual fuel operation, with reduced emissions of NO and smoke, in comparison with KME. The ignition delay at part load in dual fuel operation was also lower than that of KME operation

  6. The effect of diluting ruthenium by iron in Ru{sub x}Se{sub y} catalyst for oxygen reduction

    Energy Technology Data Exchange (ETDEWEB)

    Delacote, Cyril [Laboratory of Electrocatalysis, CNRS, University of Poitiers, F-86022 Poitiers Cedex (France); CEISAM, CNRS, University of Nantes, F-44322 Nantes Cedex 3 (France); Lewera, Adam [University of Warsaw, Department of Chemistry, ul. Pasteura 1, 02-093 Warsaw (Poland); Pisarek, Marcin [Institute of Physical Chemistry, Polish Academy of Sciences, ul. Kasprzaka 44/52, 01-224 Warsaw (Poland); Kulesza, Pawel J. [University of Warsaw, Department of Chemistry, ul. Pasteura 1, 02-093 Warsaw (Poland); Zelenay, Piotr [Materials Physics and Applications, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Alonso-Vante, Nicolas, E-mail: nicolas.alonso.vante@univ-poitiers.f [Laboratory of Electrocatalysis, CNRS, University of Poitiers, F-86022 Poitiers Cedex (France)

    2010-11-01

    This study has focused on the synthesis of novel oxygen reduction reaction (ORR) chalcogenide catalysts, with Ru partially replaced by Fe in a cluster-type Ru{sub x}Se{sub y}. The catalysts were obtained by thermal decomposition of Ru{sub 3}(CO){sub 12} and Fe(CO){sub 5} in the presence of Se. As indicated by the XPS data, the composition of catalyst nanoparticles depends on the solvent used (either p-xylene or dichlorobenzene). The presence of iron in synthesized catalysts has been confirmed by both EDAX and XPS. Voltammetric activation of the catalysts results in a partial removal of iron and unreacted selenium from the surface. The ORR performance of electrochemically pre-treated catalysts was evaluated using rotating disk and ring-disk electrodes in a sulfuric acid solution. No major change in the ORR mechanism relative to the Se/Ru catalyst has been observed with Fe-containing catalysts.

  7. Influence of Reduction Promoters on Stability of Cobalt/g-Alumina Fischer-Tropsch Synthesis Catalysts

    OpenAIRE

    Gary Jacobs; Wenping Ma; Burtron H. Davis

    2014-01-01

    This focused review article underscores how metal reduction promoters can impact deactivation phenomena associated with cobalt Fischer-Tropsch synthesis catalysts. Promoters can exacerbate sintering if the additional cobalt metal clusters, formed as a result of the promoting effect, are in close proximity at the nanoscale to other cobalt particles on the surface. Recent efforts have shown that when promoters are used to facilitate the reduction of small crystallites with the aim of increasing...

  8. Dendrimer encapsulated Silver nanoparticles as novel catalysts for reduction of aromatic nitro compounds

    Science.gov (United States)

    Asharani, I. V.; Thirumalai, D.; Sivakumar, A.

    2017-11-01

    Polyethylene glycol (PEG) core dendrimer encapsulated silver nanoparticles (AgNPs) were synthesized through normal chemical reduction method, where dendrimer acts as reducing and stabilizing agent. The encapsulated AgNPs were well characterized using TEM, DLS and XPS techniques. The synthesized AgNPs showed excellent catalytic activity towards the reduction of aromatic nitro compounds with sodium borohydride as reducing agent and the results substantiate that dendrimer encapsulated AgNPs can be an effective catalyst for the substituted nitro aromatic reduction reactions. Also the kinetics of different nitro compounds reductions was studied and presented.

  9. Highly active Pd–In/mesoporous alumina catalyst for nitrate reduction

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Zhenwei; Zhang, Yonggang; Li, Deyi [State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092 (China); Werth, Charles J. [Civil, Architectural and Environmental Engineering, University of Texas at Austin, 301 East Dean Keeton St., Stop C1786, Austin, TX 78712 (United States); Zhang, Yalei, E-mail: zhangyalei2003@163.com [State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092 (China); Zhou, Xuefei, E-mail: zhouxuefei@tongji.edu.cn [State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092 (China)

    2015-04-09

    Highlights: • Pd–In nanoparticles (6–7 nm) uniformly form in the mesopores of alumina (4 nm). • Pd–In nanoparticles aggregation is prevented during the synthesis process. • The reduction rate of nitrate is efficient by using the obtained catalyst. • The selectivity toward N{sub 2} is ideal by using the obtained catalyst. - Abstract: The catalytic reduction of nitrate is a promising technology for groundwater purification because it transforms nitrate into nitrogen and water. Recent studies have mainly focused on new catalysts with higher activities for the reduction of nitrate. Consequently, metal nanoparticles supported on mesoporous metal oxides have become a major research direction. However, the complex surface chemistry and porous structures of mesoporous metal oxides lead to a non-uniform distribution of metal nanoparticles, thereby resulting in a low catalytic efficiency. In this paper, a method for synthesizing the sustainable nitrate reduction catalyst Pd–In/Al{sub 2}O{sub 3} with a dimensional structure is introduced. The TEM results indicated that Pd and In nanoparticles could efficiently disperse into the mesopores of the alumina. At room temperature in CO{sub 2}-buffered water and under continuous H{sub 2} as the electron donor, the synthesized material (4.9 wt% Pd) was the most active at a Pd–In ratio of 4, with a first-order rate constant (k{sub obs} = 0.241 L min{sup −1} g{sub cata}{sup −1}) that was 1.3× higher than that of conventional Pd–In/Al{sub 2}O{sub 3} (5 wt% Pd; 0.19 L min{sup −1} g{sub cata}{sup −1}). The Pd–In/mesoporous alumina is a promising catalyst for improving the catalytic reduction of nitrate.

  10. Characterization of LSM/CGO Symmetric Cells Modified by NOx Adsorbents for Electrochemical NOx Removal with Impedance Spectroscopy

    DEFF Research Database (Denmark)

    Shao, Jing; Kammer Hansen, Kent

    2013-01-01

    in the resistance of the low-frequency processes, which were ascribed to adsorption, diffusion, and transfer of O2 species and NOx species at or near the triple phase boundary (TPB) region and the formation of the reaction intermediate NO2. The BaO impregnation improved the adsorption of NOx on the LSM....../CGO electrode by selectively trapping NO2 in the form of nitrate over the BaO sites and provided availability for a direct reduction of the stored nitrate. The BaO-Pt-Al2O3 layer enhanced the NOx adsorption and promoted the formation of NO2 due to the NO oxidation ability of the Pt catalyst, but hindered...... the gas diffusion to the reaction sites....

  11. Location of adsorbed species in NO-reduction catalysts by high resolution neutron powder diffraction

    International Nuclear Information System (INIS)

    Fowkes, A.J.; Rosseinsky, M.J.

    1999-01-01

    Complete text of publication follows. Catalysts containing copper ion exchanged into zeolites are attracting considerable attention due to their efficiency for both NO decomposition and the selective catalytic reduction of NO x in so-called lean-burn conditions in automotive exhausts. This presentation will describe the application of in-situ high resolution neutron powder diffraction to study active sites in a Cu-zeolite Y catalyst active for NO decomposition. The study under NO pressure reveals the location of two distinct copper sites for sorption. The influence of copper oxidation state on the structure of both the pristine and NO-loaded zeolites will be discussed. (author)

  12. Controllable synthesis of Co3O4 nanocrystals as efficient catalysts for oxygen reduction reaction

    Science.gov (United States)

    Li, Baoying; Zhang, Yihe; Du, Ruifeng; Liu, Lei; Yu, Xuelian

    2018-03-01

    The electrochemical oxygen reduction reaction (ORR) has received great attention due to its importance in fuel cells and metal-air batteries. Here, we present a simple approach to prepare non-noble metal catalyst-Co3O4 nanocrystals (NCs). The particle size and shape were simply controlled by different types and concentrations of metal precursor. Furthermore, different sizes and shapes of Co3O4 NCs are explored as electrocatalysts for ORR, and it has been observed that particles with a similar shape, and smaller particle size led to greater catalytic current densities because of the greater surface area. For particles with a comparable size, the shape or crystalline structure governed the activity of the electrocatalytic reactions. Most importantly, the 9 nm-Co3O4 were demonstrated to act as low-cost catalysts for the ORR with a similar performance to that of Pt catalysts.

  13. Structure, activity, and stability of platinum alloys as catalysts for the oxygen reduction reaction

    DEFF Research Database (Denmark)

    Vej-Hansen, Ulrik Grønbjerg

    In this thesis I present our work on theoretical modelling of platinum alloys as catalysts for the Oxygen Reduction Reaction (ORR). The losses associated with the kinetics of the ORR is the main bottleneck in low-temperature fuel cells for transport applications, and more active catalysts...... are essential for wide-spread use of this technology. platinum alloys have shown great promise as more active catalysts, which are still stable under reaction conditions. We have investigated these systems on multiple scales, using either Density Functional Theory (DFT) or Effective Medium Theory (EMT......), depending on the length and time scales involved. Using DFT, we show how diffusion barriers in transition metal alloys in the L12 structure depend on the alloying energy, supporting the assumption that an intrinsically more stable alloy is also more stable towards diffusion-related degradation...

  14. A proposed agglomerate model for oxygen reduction in the catalyst layer of proton exchange membrane fuel cells

    International Nuclear Information System (INIS)

    Zhang, Xiaoxian; Gao, Yuan; Ostadi, Hossein; Jiang, Kyle; Chen, Rui

    2014-01-01

    Highlights: • We developed a new agglomerate model to describe oxygen reduction reaction. • We showed how to calculate the model parameters from catalyst layer structure. • We verified the agglomerate model. - Abstract: Oxygen diffusion and reduction in the catalyst layer of PEM fuel cell is an important process in fuel cell modelling, but models able to link the reduction rate to catalyst-layer structure are lack; this paper makes such an effort. We first link the average reduction rate over the agglomerate within a catalyst layer to a probability that an oxygen molecule, which is initially on the agglomerate surface, will enter and remain in the agglomerate at any time in the absence of any electrochemical reaction. We then propose a method to directly calculate distribution function of this probability and apply it to two catalyst layers with contrasting structures. A formula is proposed to describe these calculated distribution functions, from which the agglomerate model is derived. The model has two parameters and both can be independently calculated from catalyst layer structures. We verify the model by first showing that it is an improvement and able to reproduce what the spherical model describes, and then testing it against the average oxygen reductions directly calculated from pore-scale simulations of oxygen diffusion and reaction in the two catalyst layers. The proposed model is simple, but significant as it links the average oxygen reduction to catalyst layer structures, and its two parameters can be directly calculated rather than by calibration

  15. Reduction of NOx and particulate emissions from coal-fired boilers by modification of coal nozzles and combustion tuning

    Energy Technology Data Exchange (ETDEWEB)

    Chudnovsky, B.; Talanker, A.; Mugenstein, A.; Shpon, G.; Vikhansky, A.; Elperin, T.; Bar-Ziv, E.; Bockelie, M.; Eddings, E.; Sarofim, A.F. [Israel Electric Corporation, Haifa (Israel). Engineering Division

    2001-07-01

    In the present paper two issues are discussed: the effect of the burner replacement on boiler performance and NOx emissions and the effect of the burner replacement on performance and efficiency of electrostatic precipitators (ESP). We also have experimented with different coal types and found the coals that together with combustion tuning met commonly accepted emission limits for NOx (less than 600 mg/dNm{sup 3}) and levels of carbon in fly ash (LOI) (approximately 5-6%) for existing boilers without low NOx burners. Our measurements were accompanied by computer simulations of the combustion of the combustion process in the boiler. Special attention was paid to detailed simulation of the flow and ignition in the near-burner zone. 7 refs., 12 figs., 5 tabs.

  16. Temperature-programmed reduction and cyclic voltammetry of Pt/carbon-fibre paper catalysts for methanol electrooxidation

    International Nuclear Information System (INIS)

    Attwood, P.A.; McNicol, B.D.; Short, R.T.

    1981-01-01

    Temperature-programmed reduction (TPR) and cyclic voltammetry (CV) studies of platinum catalysts supported on pyrographite-coated carbon-fibre paper, and prepared by either ion exchange or impregnation, clearly demonstrate the nature of the interactions between the platinum species and the support. After drying the above catalysts at 120 0 C, the ion-exchanged preparation exhibits the stronger interaction with the carbon support, as might be expected since a chemical interaction with carbon surface groups is known to occur in such catalysts. The presence of a fraction of bulk Pt(NH 3 ) 4 (OH) 2 impregnating salt in the impregnated catalyst has been detected using TPR. After air activation at 300 0 C, subambient reduction peaks were observed and the strength of binding of Pt in the ion-exchanged catalyst was reflected by its increased difficulty of reduction in comparison with that of the impregnated catalyst. The stoichiometry of reduction in ion-exchanged catalysts corresponds to Pt 2+ → Pt 0 in both dried and activated catalysts, with a small amount of Pt 4+ present in the latter. Upon activation the impregnated catalyst showed the presence of some Pt metal, which was thought to arise from the decomposition of the fraction of bulk Pt(NH 3 ) 4 (OH) 2 in the dried catalyst. Activation of ion-exchanged catalysts at temperatures higher than 300 0 C led to a progressive weakening of the Pt-support interaction and consequent smaller Pt surface areas. Activation at 500 0 C in air produced Pt metal exclusively and very low Pt surface areas. The strong interaction between Pt and the carbon support upon activation of the ion-exchanged catalyst at 300 0 C is thought to be the origin of the large metal surface area and the high catalytic activity for methanol electrooxidation found upon reduction

  17. Catalyst evaluation for oxygen reduction reaction in concentrated phosphoric acid at elevated temperatures

    Science.gov (United States)

    Hu, Yang; Jiang, Yiliang; Jensen, Jens Oluf; Cleemann, Lars N.; Li, Qingfeng

    2018-01-01

    Phosphoric acid is the common electrolyte for high-temperature polymer electrolyte fuel cells (HT-PEMFCs) that have advantages such as enhanced CO tolerance and simplified heat and water management. The currently used rotating disk electrode technique is limited to tests in dilute solutions at low temperatures and hence is not suitable for catalyst evaluation for HT-PEMFCs. In this study, we have designed and constructed a half-cell setup to measure the intrinsic activities of catalysts towards the oxygen reduction reaction (ORR) in conditions close to HT-PEMFC cathodes. By optimization of the hydrophobic characteristics of electrodes and the catalyst layer thickness, ORR activities of typical Pt/C catalysts are successfully measured in concentrated phosphoric acid at temperatures above 100 °C. In terms of mass-specific activities, the catalyst exhibits about two times higher activity in the half-cell electrode than that observed in fuel cells, indicating the feasibility of the technique as well as the potential for further improvement of fuel cell electrode performance.

  18. Investigation of Au-Pt/C electro-catalysts for oxygen reduction reaction

    International Nuclear Information System (INIS)

    Lin Rui; Zhang Haiyan; Zhao Tiantian; Cao Chunhui; Yang Daijun; Ma Jianxin

    2012-01-01

    Highlights: ► Au-Pt core shell catalyst. ► Seed-mediated growth method. ► Au-Pt (2:4)/C best activity toward ORR. ► Four-electron pathway in acid solution. ► Single cell performance. - Abstract: Carbon-supported Au-Pt core shell nano-structured catalysts were synthesized by the seed-mediated growth method. The nano-structured catalysts were characterized by UV–vis spectroscopy, X-ray photoelectron spectra (XPS) and transmission electron microscopy (TEM) techniques. The oxygen reduction reaction (ORR) activity of the Au-Pt/C was tested by means of linear sweep voltammetry (LSV) by employing rotating disk electrode (RDE). It revealed that Au-Pt (2:4)/C (atomic ratio) catalyst exhibited the best catalytic activity toward ORR. Au-Pt (2:4)/C proceeded by an approximately four-electron pathway in acid solution, through which molecular oxygen was directly reduced to water. The stability of Au-Pt (2:4)/C is tested by cyclic voltammetry for 500 cycles. The performance of the membrane electrode assembly (MEA) prepared by Au-Pt (2:4)/C as the cathode catalyst in a single proton exchange membrane fuel cell (PEMFC) generated a maximum power density of 479 mW cm −2 at 0.431 V using H 2 and O 2 at 80 °C.

  19. Alumina- and titania-based monolithic catalysts for low temperature selective catalytic reduction of nitrogen oxides

    International Nuclear Information System (INIS)

    Blanco, J.; Avila, P.; Suarez, S.; Martin, J.A.; Knapp, C.

    2000-01-01

    The selective catalytic reduction of NO+NO 2 (NO x ) at low temperature (180-230C) with ammonia has been investigated with copper-nickel and vanadium oxides supported on titania and alumina monoliths. The influence of the operating temperature, as well as NH 3 /NO x and NO/NO 2 inlet ratios has been studied. High NO x conversions were obtained at operating conditions similar to those used in industrial scale units with all the catalysts. Reaction temperature, ammonia and nitrogen dioxide inlet concentration increased the N 2 O formation with the copper-nickel catalysts, while no increase was observed with the vanadium catalysts. The vanadium-titania catalyst exhibited the highest DeNO x activity, with no detectable ammonia slip and a low N 2 O formation when NH 3 /NO x inlet ratio was kept below 0.8. TPR results of this catalyst with NO/NH 3 /O 2 , NO 2 /NH 3 /O 2 and NO/NO 2 /NH 3 /O 2 feed mixtures indicated that the presence of NO 2 as the only nitrogen oxide increases the quantity of adsorbed species, which seem to be responsible for N 2 O formation. When NO was also present, N 2 O formation was not observed

  20. Synthesis of 2D Nitrogen-Doped Mesoporous Carbon Catalyst for Oxygen Reduction Reaction

    Directory of Open Access Journals (Sweden)

    Zhipeng Yu

    2017-02-01

    Full Text Available 2D nitrogen-doped mesoporous carbon (NMC is synthesized by using a mesoporous silica film as hard template, which is then investigated as a non-precious metal catalyst for the oxygen reduction reaction (ORR. The effect of the synthesis conditions on the silica template and carbon is extensively investigated. In this work, we employ dual templates—viz. graphene oxide and triblock copolymer F127—to control the textural features of a 2D silica film. The silica is then used as a template to direct the synthesis of a 2D nitrogen-doped mesoporous carbon. The resultant nitrogen-doped mesoporous carbon is characterized by transmission electron microscopy (TEM, nitrogen ad/desorption isotherms, X-ray photoelectron spectroscopy (XPS, cyclic voltammetry (CV, and rotating disk electrode measurements (RDE. The electrochemical test reveals that the obtained 2D-film carbon catalyst yields a highly electrochemically active surface area and superior electrocatalytic activity for the ORR compared to the 3D-particle. The superior activity can be firstly attributed to the difference in the specific surface area of the two catalysts. More importantly, the 2D-film morphology makes more active sites accessible to the reactive species, resulting in a much higher utilization efficiency and consequently better activity. Finally, it is noted that all the carbon catalysts exhibit a higher ORR activity than a commercial Pt catalyst, and are promising for use in fuel cells.

  1. Reductive amination of ethanol to ethylamines over Ni/Al_2O_3 catalysts

    International Nuclear Information System (INIS)

    Park, Jun Hyun; Hong, Eunpyo; An, Sang Hee; Shin, Chae-Ho; Lim, Dong-Hee

    2017-01-01

    Ni(x)/Al_2O_3 (x=wt%) catalysts with Ni loadings of 5-25 wt% were prepared via a wet impregnation method on an γ-Al_2O_3 support and subsequently applied in the reductive amination of ethanol to ethylamines. Among the various catalysts prepared, Ni(10)/Al2O3 exhibited the highest metal dispersion and the smallest Ni particle size, resulting in the highest catalytic performance. To reveal the effects of reaction parameters, a reductive amination process was performed by varying the reaction temperature (T), weight hourly space velocity (WHSV), and NH_3 and H_2 partial pressures in the reactions. In addition, on/off experiments for NH_3 and H_2 were also carried out. In the absence of NH_3 in the reactant stream, the ethanol conversion and selectivities towards the different ethylamine products were significantly reduced, while the selectivity to ethylene was dominant due to the dehydration of ethanol. In contrast, in the absence of H_2, the selectivity to acetonitrile significantly increased due to dehydrogenation of the imine intermediate. Although a small amount of catalyst deactivation was observed in the conversion of ethanol up to 10 h on stream due to the formation of nickel nitride, the Ni(10)/Al_2O_3 catalyst exhibited stable catalytic performance over 90 h under the optimized reaction conditions (i.e., T=190 .deg. C, WHSV=0.9 h"-"1, and EtOH/NH_3/H_2 molar ratio=1/1/6).

  2. Highly active Pd-In/mesoporous alumina catalyst for nitrate reduction.

    Science.gov (United States)

    Gao, Zhenwei; Zhang, Yonggang; Li, Deyi; Werth, Charles J; Zhang, Yalei; Zhou, Xuefei

    2015-04-09

    The catalytic reduction of nitrate is a promising technology for groundwater purification because it transforms nitrate into nitrogen and water. Recent studies have mainly focused on new catalysts with higher activities for the reduction of nitrate. Consequently, metal nanoparticles supported on mesoporous metal oxides have become a major research direction. However, the complex surface chemistry and porous structures of mesoporous metal oxides lead to a non-uniform distribution of metal nanoparticles, thereby resulting in a low catalytic efficiency. In this paper, a method for synthesizing the sustainable nitrate reduction catalyst Pd-In/Al2O3 with a dimensional structure is introduced. The TEM results indicated that Pd and In nanoparticles could efficiently disperse into the mesopores of the alumina. At room temperature in CO2-buffered water and under continuous H2 as the electron donor, the synthesized material (4.9 wt% Pd) was the most active at a Pd-In ratio of 4, with a first-order rate constant (k(obs) = 0.241 L min(-1) g(cata)(-1)) that was 1.3× higher than that of conventional Pd-In/Al2O3 (5 wt% Pd; 0.19 L min(-1) g(cata)(-1)). The Pd-In/mesoporous alumina is a promising catalyst for improving the catalytic reduction of nitrate. Copyright © 2015 Elsevier B.V. All rights reserved.

  3. Optimization of the Pd-Fe-Mo Catalysts for Oxygen Reduction Reaction in Proton-Exchange Membrane Fuel Cells

    International Nuclear Information System (INIS)

    Lee, Yeayeon; Jang, Jeongseok; Lee, Jin Goo; Jeon, Ok Sung; Kim, Hyeong Su; Hwang, Ho Jung; Shul, Yong Gun

    2016-01-01

    Highlights: • Pd-Mo-Fe catalysts show high catalytic activity and stability for oxygen-reduction reactions in acid media. • The optimum compositions were 7.5:1.5:1.0 for Pd-Fe-Mo, and the optimum temperatures were 500 °C. • The Pd-Fe-Mo catalysts were successfully applied to the PEMFC cathode, showing ∼500 mA cm −1 at 0.6 V. • The lattice constant was strongly related to the activity and stability of the catalysts for oxygen-reduction reactions. - Abstract: Highly active and durable non-platinum catalysts for oxygen-reduction reaction (ORR) have been developed for energy conversion devices such as proton-exchange membrane fuel cells (PEMFCs). In this study, Pd-Fe-Mo catalyst is reported as a non-platinum catalyst for ORR. The atomic ratio and annealing temperatures are controlled on the catalysts to understand interplay between their physical and chemical properties and electrochemical activities. The Pd-Fe-Mo catalyst optimized with 7.5:1.5:1.0 of the atomic ratio and 500 °C of the annealing temperature shows 32.18 mA mg −1 PGM (PGM: platinum group metal) of the kinetic current density at 0.9 V for ORR, which is comparable to that of commercial Pt/C catalyst. The current density is degraded to 6.20 mA mg −1 PGM after 3000 cycling of cyclic voltammetry, but it is greatly enhanced value compared to other non-platinum catalysts. In actual application to PEMFCs, the 20% Pd-Fe-Mo catalyst supported on carbons exhibits a high performance of 506 mA cm −2 at 0.6 V. The results suggest that the Pd-Fe-Mo catalyst can be a good candidate for non-platinum ORR catalysts.

  4. Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Hanguang; Hwang, Sooyeon; Wang, Maoyu; Feng, Zhenxing; Karakalos, Stavros; Luo, Langli; Qiao, Zhi; Xie, Xiaohong; Wang, Chongmin; Su, Dong; Shao, Yuyan; Wu, Gang (BNL); (Oregon State U.); (SC); (PNNL); (Buffalo)

    2017-09-26

    It remains a grand challenge to replace platinum group metal (PGM) catalysts with earth-abundant materials for the oxygen reduction reaction (ORR) in acidic media, which is crucial for large-scale deployment of proton exchange membrane fuel cells (PEMFCs). Here, we report a high-performance atomic Fe catalyst derived from chemically Fe-doped zeolitic imidazolate frameworks (ZIFs) by directly bonding Fe ions to imidazolate ligands within 3D frameworks. Although the ZIF was identified as a promising precursor, the new synthetic chemistry enables the creation of well-dispersed atomic Fe sites embedded into porous carbon without the formation of aggregates. The size of catalyst particles is tunable through synthesizing Fe-doped ZIF nanocrystal precursors in a wide range from 20 to 1000 nm followed by one-step thermal activation. Similar to Pt nanoparticles, the unique size control without altering chemical properties afforded by this approach is able to increase the number of PGM-free active sites. The best ORR activity is measured with the catalyst at a size of 50 nm. Further size reduction to 20 nm leads to significant particle agglomeration, thus decreasing the activity. Using the homogeneous atomic Fe model catalysts, we elucidated the active site formation process through correlating measured ORR activity with the change of chemical bonds in precursors during thermal activation up to 1100 °C. The critical temperature to form active sites is 800 °C, which is associated with a new Fe species with a reduced oxidation number (from Fe3+ to Fe2+) likely bonded with pyridinic N (FeN4) embedded into the carbon planes. Further increasing the temperature leads to continuously enhanced activity, linked to the rise of graphitic N and Fe–N species. The new atomic Fe catalyst has achieved respectable ORR activity in challenging acidic media (0.5 M H2SO4), showing a half-wave potential of 0.85 V vs RHE and leaving only a 30 mV gap with Pt/C (60 μgPt/cm2). Enhanced stability

  5. Promotional effect of phosphorus doping on the activity of the Fe-N/C catalyst for the oxygen reduction reaction

    DEFF Research Database (Denmark)

    Hu, Yang; Zhu, Jianbin; Lv, Qing

    2015-01-01

    Cost-effective, active and stable electrocatalysts for the oxygen reduction reaction (ORR) are highly desirable for the wide-spread adoption of technologies such as fuel cells and metal-air batteries. Among the already reported non-precious metal catalysts, carbon-supported transition metal...... to that for the undoped Fe-N/C catalyst. The activity and durability of the catalysts are demonstrated in direct methanol fuel cells....

  6. Pt Catalyst Supported within TiO2 Mesoporous Films for Oxygen Reduction Reaction

    International Nuclear Information System (INIS)

    Huang, Dekang; Zhang, Bingyan; Bai, Jie; Zhang, Yibo; Wittstock, Gunther; Wang, Mingkui; Shen, Yan

    2014-01-01

    In this study, dispersed Pt nanoparticles into mesoporous TiO 2 thin films are fabricated by a facile electrochemical deposition method as electro-catalysts for oxygen reduction reaction. The mesoporous TiO 2 thin films coated on the fluorine-doped tin oxide glass by screen printing allow a facile transport of reactants and products. The structural properties of the resulted Pt/TiO 2 electrode are evaluated by field emission scanning electron microscopy, energy dispersive X-ray spectrometry, X-ray diffraction, and X-ray photoelectron spectroscopy. Cyclic voltammetry measurements are performed to study the electrochemical properties of the Pt/TiO 2 electrode. Further study demonstrates the stability of the Pt catalyst supported within TiO 2 mesoporous films for the oxygen reduction reaction

  7. Oxygen reduction on carbon supported platinum catalysts in high temperature polymer electrolytes

    DEFF Research Database (Denmark)

    Qingfeng, Li; Hjuler, Hans Aage; Bjerrum, Niels

    2000-01-01

    Oxygen reduction on carbon supported platinum catalysts has been investigated in H3PO4, H3PO4-doped Nafion and polybenzimidazole (PBI) polymer electrolytes in a temperature range up to 190 degrees C. Compared with pure H3PO4, the combination of H3PO4 and polymer electrolytes can significantly...... membrane fuel cell based on H3PO4-doped PBI for operation at temperatures between 150 and 200 degrees C. (C) 2000 Elsevier Science Ltd. All rights reserved....

  8. Antioxidant (A-tocopherol acetate) effect on oxidation stability and NOx emission reduction in methyl ester of Annona oil operated diesel engine

    Science.gov (United States)

    Senthil, R.; Silambarasan, R.; Pranesh, G.

    2017-05-01

    There is a major drawback while using biodiesel as a alternate fuel for compression ignition diesel engine due to lower heating value, higher viscosity, higher density and higher oxides of nitrogen emission. To minimize these drawbacks, fuel additives can contribute towards engine performance and exhaust emission reduction either directly or indirectly. In this current work, the test was conducted to investigate the effect of antioxidant additive (A-tocopherol acetate) on oxidation stability and NOx emission in a of Annona methyl ester oil (MEAO) fueled diesel engine. The A-tocopherol acetate is mixed in different concentrations such as 0.01, 0.02, 0.03 and 0.04% with 100% by vol MEAO. It is concluded that the antioxidant additive very effective in increasing the oxidation stability and in controlling the NOx emission. Further, the addition of antioxidant additive is slight increase the HC, CO and smoke emissions. Hence, A-tocopherol acetate is very effective in controlling the NOx emission with MEAO operated diesel engine without any major modification.

  9. Highly Selective TiN-Supported Highly Dispersed Pt Catalyst: Ultra Active toward Hydrogen Oxidation and Inactive toward Oxygen Reduction.

    Science.gov (United States)

    Luo, Junming; Tang, Haibo; Tian, Xinlong; Hou, Sanying; Li, Xiuhua; Du, Li; Liao, Shijun

    2018-01-31

    The severe dissolution of the cathode catalyst, caused by an undesired oxygen reduction reaction at the anode during startup and shutdown, is a fatal challenge to practical applications of polymer electrolyte membrane fuel cells. To address this important issue, according to the distinct structure-sensitivity between the σ-type bond in H 2 and the π-type bond in O 2 , we design a HD-Pt/TiN material by highly dispersing Pt on the TiN surface to inhibit the unwanted oxygen reduction reaction. The highly dispersed Pt/TiN catalyst exhibits excellent selectivity toward hydrogen oxidation and oxygen reduction reactions. With a Pt loading of 0.88 wt %, our catalyst shows excellent hydrogen oxidation reaction activity, close to that of commercial 20 wt % Pt/C catalyst, and much lower oxygen reduction reaction activity than the commercial 20 wt % Pt/C catalyst. The lack of well-ordered Pt facets is responsible for the excellent selectivity of the HD-Pt/TiN materials toward hydrogen oxidation and oxygen reduction reactions. Our work provides a new and cost-effective solution to design selective catalysts toward hydrogen oxidation and oxygen reduction reactions, making the strategy of using oxygen-tolerant anode catalyst to improve the stability of polymer electrolyte membrane fuel cells during startup and shutdown more affordable and practical.

  10. Size and morphology controlled NiSe nanoparticles as efficient catalyst for the reduction reactions

    Energy Technology Data Exchange (ETDEWEB)

    Subbarao, Udumula; Marakatti, Vijaykumar S. [New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India); Amshumali, Mungalimane K. [New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India); Department of Chemistry and Industrial Chemistry, Vijayanagara Sri Krishnadevaraya University, Jnanasagara Campus, Cantonment, Bellary 583105 (India); Loukya, B. [International Center for Materials Science, Jakkur P.O., Bangalore 560064 (India); Singh, Dheeraj Kumar [Chemistry & Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India); Datta, Ranjan [International Center for Materials Science, Jakkur P.O., Bangalore 560064 (India); Peter, Sebastian C., E-mail: sebastiancp@jncasr.ac.in [New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur P.O., Bangalore 560064 (India)

    2016-12-15

    Facile and efficient ball milling and polyol methods were employed for the synthesis of nickel selenide (NiSe) nanoparticle. The particle size of the NiSe nanoparticle has been controlled mechanically by varying the ball size in the milling process. The role of the surfactants in the formation of various morphologies was studied. The compounds were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray energy dispersive spectroscopy (EDS). The efficiency of the NiSe nanoparticle as a catalyst was tested for the reduction of para-nitroaniline (PNA) to para-phenyldiamine (PPD) and para-nitrophenol (PNP) to para-aminophenol (PAP) using NaBH{sub 4} as the reducing agent. Particle size, morphology and the presence of surfactant played a crucial role in the reduction process. - Graphical abstract: NiSe nanoparticles in different size and morphology were synthesized using facile ball milling and polyol methods. Particle size, morphology and the presence of surfactant in these materials played a crucial role in the hydrogenation of PNA and PNP. - Highlights: • NiSe nanoparticles synthesized using ball milling and solution phase methods. • NiSe nanoparticle is an efficient catalyst for the reduction of PNA and PNP. • NiSe is found to be better than the best reported noble metal catalysts.

  11. Size and morphology controlled NiSe nanoparticles as efficient catalyst for the reduction reactions

    International Nuclear Information System (INIS)

    Subbarao, Udumula; Marakatti, Vijaykumar S.; Amshumali, Mungalimane K.; Loukya, B.; Singh, Dheeraj Kumar; Datta, Ranjan; Peter, Sebastian C.

    2016-01-01

    Facile and efficient ball milling and polyol methods were employed for the synthesis of nickel selenide (NiSe) nanoparticle. The particle size of the NiSe nanoparticle has been controlled mechanically by varying the ball size in the milling process. The role of the surfactants in the formation of various morphologies was studied. The compounds were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray energy dispersive spectroscopy (EDS). The efficiency of the NiSe nanoparticle as a catalyst was tested for the reduction of para-nitroaniline (PNA) to para-phenyldiamine (PPD) and para-nitrophenol (PNP) to para-aminophenol (PAP) using NaBH 4 as the reducing agent. Particle size, morphology and the presence of surfactant played a crucial role in the reduction process. - Graphical abstract: NiSe nanoparticles in different size and morphology were synthesized using facile ball milling and polyol methods. Particle size, morphology and the presence of surfactant in these materials played a crucial role in the hydrogenation of PNA and PNP. - Highlights: • NiSe nanoparticles synthesized using ball milling and solution phase methods. • NiSe nanoparticle is an efficient catalyst for the reduction of PNA and PNP. • NiSe is found to be better than the best reported noble metal catalysts.

  12. Mesoporous Fe-containing ZSM-5 zeolite single crystal catalysts for selective catalytic reduction of nitric oxide by ammonia

    DEFF Research Database (Denmark)

    Kustov, Arkadii; Egeblad, Kresten; Kustova, Marina

    2007-01-01

    Mesoporous and conventional Fe-containing ZSM-5 catalysts (0.5–8 wt% Fe) were prepared using a simple impregnationmethod and tested in NO selective catalytic reduction (SCR) with NH3. It was found that mesoporous Fe-ZSM-5 catalysts exhibit higher SCR activities than comparable conventional cataly...

  13. Chemical deactivation of Ag/Al2O3 by sulphur for the selective reduction of NOx using hydrocarbons

    International Nuclear Information System (INIS)

    Houel, Valerie; Millington, Paul; Pollington, Stephen; Poulston, Stephen; Rajaram, Raj R.; Tsolakis, Athanasios

    2006-01-01

    The hydrocarbon-SCR activity of Ag/Al 2 O 3 catalysts is severely deactivated after low temperature (350 o C) sulphur ageing in the form of SO 2 exposure. Catalysts aged with SO 2 , NO and hydrocarbon present accumulate a significantly larger amount of SO 4 2- than those aged in the presence of only O 2 , H 2 O and SO 2 when exposed to an equivalent amount of S. Following sulphation of the catalyst most of the sulphur can be removed by a high temperature (600 o C) treatment in the reaction gas. Regeneration in the absence of hydrocarbon is ineffective. The hydrocarbon-SCR activity of the sulphated catalyst using model hydrocarbons such as n-C 8 H 18 can be restored after a high temperature pre-treatment in the reaction gases. However this desulphation process fails to regenerate the hydrocarbon-SCR activity when diesel fuel is used in the activity test. TPR studies show that a major fraction of the sulphur species present in the catalyst is removed by such pre-treatment, but the slight residual amount of sulphur is sufficient to inhibit the activation of the diesel fuel on the Ag catalyst. The nature of the hydrocarbon species present for the hydrocarbon-SCR reaction and during the regeneration strongly influences the activity. In general aromatics such as C 7 H 8 are less effective for reducing NO x and regenerating the sulphated catalyst. (author)

  14. Enhanced activity and stability of Pt catalysts on functionalized graphene sheets for electrocatalytic oxygen reduction

    Energy Technology Data Exchange (ETDEWEB)

    Kou, Rong; Shao, Yuyan; Wang, Donghai; Engelhard, Mark H.; Kwak, Ja Hun; Wang, Jun; Viswanathan, Vilayanur V.; Wang, Chongmin; Lin, Yuehe; Wang, Yong; Liu, Jun [Pacific Northwest National Laboratory, Richland, WA 99352 (United States); Aksay, Ilhan A. [Department of Chemical Engineering, Princeton University, Princeton, NJ 08544 (United States)

    2009-05-15

    Electrocatalysis of oxygen reduction using Pt nanoparticles supported on functionalized graphene sheets (FGSs) was studied. FGSs were prepared by thermal expansion of graphite oxide. Pt nanoparticles with average diameter of 2 nm were uniformly loaded on FGSs by impregnation methods. Pt-FGS showed a higher electrochemical surface area and oxygen reduction activity with improved stability as compared with the commercial catalyst. Transmission electron microscopy, X-ray photoelectron spectroscopy, and electrochemical characterization suggest that the improved performance of Pt-FGS can be attributed to smaller particle size and less aggregation of Pt nanoparticles on the functionalized graphene sheets. (author)

  15. Metal-phthalocyanine functionalized carbon nanotubes as catalyst for the oxygen reduction reaction: A theoretical study

    Science.gov (United States)

    Orellana, Walter

    2012-07-01

    The covalent functionalization of metallic single-walled carbon nanotubes (CNTs) with transition metal phthalocyanines (MPc, with M = Mn, Fe and Co) are addressed by density functional calculations. The CNT-MPc catalytic activity toward the oxygen reduction reaction (ORR) is investigated through the O2 stretching frequency adsorbed on the phthalocyanine metal center. We find better reduction abilities when the CNT functionalization occurs through sp2-like bonds. Multiple stable-spin states for the M-O2 adduct are also found for M = Mn and Fe, suggesting higher ORR rates. The CNT-MPc complexes show metallic characteristics, suggesting favorable conditions to work as ORR cathode catalysts in fuel cells.

  16. Simultaneous reduction of NOx and smoke using stratified charge compression ignition; Sojo kongoki no asshuku chakka ni yoru NOx smoke no doji teige

    Energy Technology Data Exchange (ETDEWEB)

    Hashizume, T.; Miyamoto, T.; Akagawa, H. [New ACE Institute Co. Ltd., Ibaraki (Japan); Tsujimura, K. [Chiba Institute of Technology, Chiba (Japan)

    2000-12-25

    Simultaneous reduction of NO{sub x} and smoke under high load conditions could be obtained by MULDIC (MULtiple stage DIesel Combustion) where mixture was made stratified before ignition. In this investigation of the basic characteristics of MULDIC, gaseous fuels (DME, Propane) were charged into the intake air which led to the creation of homogeneous lean mixture, and liquid fuel was injected into the cylinder and made rich mixture. The results of the engine test showed that NO{sub x} emissions could be reduced to less than 100 ppm and smoke emissions were also maintained 0 FSN even at higher loads. Moreover, homogeneous rich mixture test results showed that low smoke combustion could be obtained under equivalence ratio of 1.6. In MULDIC, increasing the ignition delay period of injected fuel, soot formation rate was decreased, because over rich region was avoided. (author)

  17. Influence of Reduction Promoters on Stability of Cobalt/g-Alumina Fischer-Tropsch Synthesis Catalysts

    Directory of Open Access Journals (Sweden)

    Gary Jacobs

    2014-03-01

    Full Text Available This focused review article underscores how metal reduction promoters can impact deactivation phenomena associated with cobalt Fischer-Tropsch synthesis catalysts. Promoters can exacerbate sintering if the additional cobalt metal clusters, formed as a result of the promoting effect, are in close proximity at the nanoscale to other cobalt particles on the surface. Recent efforts have shown that when promoters are used to facilitate the reduction of small crystallites with the aim of increasing surface Co0 site densities (e.g., in research catalysts, ultra-small crystallites (e.g., <2–4.4 nm formed are more susceptible to oxidation at high conversion relative to larger ones. The choice of promoter is important, as certain metals (e.g., Au that promote cobalt oxide reduction can separate from cobalt during oxidation-reduction (regeneration cycles. Finally, some elements have been identified to promote reduction but either poison the surface of Co0 (e.g., Cu, or produce excessive light gas selectivity (e.g., Cu and Pd, or Au at high loading. Computational studies indicate that certain promoters may inhibit polymeric C formation by hindering C-C coupling.

  18. Combustion system optimization of a P-62 lignite boiler in ContourGlobal Maritsa East 3 with NOx-reduction and efficiency improvement

    International Nuclear Information System (INIS)

    Petkov, Ch.; Thierbach, Hans-Ulrich; Totev, T.

    2013-01-01

    Steinmueller Engineering GmbH, Gummersbach, Germany, successfully concluded in consortium with Siemens EOOD, Sofia, the combustion system modification of a P62 lignite fired boiler in TPP ContourGlobal Maritsa East 3, which was targeting mainly the reduction of the NOx emissions below 180 mg/Nm 3 at 6 % O 2 . The modification is part of an EPC contract covering the design, fabrication, installation and commissioning works needed to upgrade the boilers at the power station. The Modification concept involves optimization of PF- and Vapor distribution, replacement of the coal burners, installation of new Over-fire air (OFA) system and Side-wall air (SWA) system and minor modification of the existing control system to allow control of the OFAflow. The main results of the modification are: Reduction of the NOx emissions (at ESP exit) from approximately 390 g/Nm³ to below 180 mg/Nm³ at 6% O 2 , Efficiency increase of the furnace by reduction of the excess air ratio from 1.2 to 1.15 (at furnace outlet) and overall increase of the boiler efficiency. (authors)

  19. Palladium nanoparticles as catalysts for reduction of Cr(VI) and Suzuki coupling reaction

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Lilan; Guo, Yali; Iqbal, Anam; Li, Bo; Deng, Min; Gong, Deyan; Liu, Weisheng; Qin, Wenwu, E-mail: qinww@lzu.edu.cn [Lanzhou University, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province and State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering (China)

    2017-04-15

    Herein, six kinds of PdNPs (including icosahedron, sphere, spindle, cube, rod, and wire) were synthesized via simple methods. The catalytic activities were investigated by the reduction reaction of Cr(VI) and Suzuki coupling reaction. Chemically synthesized morphologies of the six catalysis were characterized by transmission electron microscopy, field emission scanning electron microscopy, and X-ray diffraction, etc. Pd icosahedron shows a better catalytic property than other PdNPs with a rate constants 0.42 min{sup −1} for the reduction of Cr(VI). Moreover, the electrocatalyst shows that Pd icosahedron possesses a bigger surface area of 8.56 m{sup 2}/g than other nanoparticles, which is attributed to the better catalyst. The Pd icosahedron possesses a better catalytic property, attributing to the abundant exposed {111} facets with high activity on Pd icosahedron. The catalytic activities are closely related to the surface area with the following order: icosahedrons ≥ sphere > rod > spindle > cube > wire. The Pd icosahedron catalyst represents a strong activity for Suzuki coupling reaction as well, outweighting is 80%. The results reveal that Pd icosahedron acts as an efficient catalyst compared to other PdNPs (wire, rod, sphere, spindle, and cube).

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

    Energy Technology Data Exchange (ETDEWEB)

    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

  1. Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Hanguang [Department; Hwang, Sooyeon [Center; Wang, Maoyu [School; Feng, Zhenxing [School; Karakalos, Stavros [Department; Luo, Langli [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Qiao, Zhi [Department; Xie, Xiaohong [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Wang, Chongmin [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Su, Dong [Center; Shao, Yuyan [Pacific Northwest National Laboratory, Richland, Washington 99352, United States; Wu, Gang [Department

    2017-09-26

    To significantly reduce the cost of proton exchange membrane (PEM) fuel cells, current Pt must be replaced by platinum-metal-group (PGM)-free catalysts for the oxygen reduction reaction (ORR) in acid. We report here a new class of high-performance atomic iron dispersed carbon catalysts through controlled chemical doping of iron ions into zinc-zeolitic imidazolate framework (ZIF), a type of metal-organic framework (MOF). The novel synthetic chemistry enables accurate size control of Fe-doped ZIF catalyst particles with a wide range from 20 to 1000 nm without changing chemical properties, which provides a great opportunity to increase the density of active sites that is determined by the particle size. We elucidated the active site formation mechanism by correlating the chemical and structural changes with thermal activation process for the conversion from Fe-N4 complex containing hydrocarbon networks in ZIF to highly active FeNx sites embedded into carbon. A temperature of 800oC was identified as the critical point to start forming pyridinic nitrogen doping at the edge of the graphitized carbon planes. Further increasing heating temperature to 1100oC leads to increase of graphitic nitrogen, generating possible synergistic effect with FeNx sites to promote ORR activity. The best performing catalyst, which has well-defined particle size around 50 nm and abundance of atomic FeNx sites embedded into carbon structures, achieve a new performance milestone for the ORR in acid including a half-wave potential of 0.85 V vs RHE and only 20 mV loss after 10,000 cycles in O2 saturated H2SO4 electrolyte. The new class PGM-free catalyst with approaching activity to Pt holds great promise for future PEM fuel cells.

  2. Heterogeneous electrochemical CO2 reduction using nonmetallic carbon-based catalysts: current status and future challenges

    Science.gov (United States)

    Ma, Tao; Fan, Qun; Tao, Hengcong; Han, Zishan; Jia, Mingwen; Gao, Yunnan; Ma, Wangjing; Sun, Zhenyu

    2017-11-01

    Electrochemical CO2 reduction (ECR) offers an important pathway for renewable energy storage and fuels production. It still remains a challenge in designing highly selective, energy-efficient, robust, and cost-effective electrocatalysts to facilitate this kinetically slow process. Metal-free carbon-based materials have features of low cost, good electrical conductivity, renewability, diverse structure, and tunability in surface chemistry. In particular, surface functionalization of carbon materials, for example by doping with heteroatoms, enables access to unique active site architectures for CO2 adsorption and activation, leading to interesting catalytic performances in ECR. We aim to provide a comprehensive review of this category of metal-free catalysts for ECR, providing discussions and/or comparisons among different nonmetallic catalysts, and also possible origin of catalytic activity. Fundamentals and some future challenges are also described.

  3. The role of reticular chemistry in the design of CO2 reduction catalysts

    Science.gov (United States)

    Diercks, Christian S.; Liu, Yuzhong; Cordova, Kyle E.; Yaghi, Omar M.

    2018-02-01

    The problem with current state-of-the-art catalysts for CO2 photo- or electroreduction is rooted in the notion that no single system can independently control, and thus optimize, the interplay between activity, selectivity and efficiency. At its core, reticular chemistry is recognized for its ability to control, with atomic precision, the chemical and structural features (activity and selectivity) as well as the output optoelectronic properties (efficiency) of porous, crystalline materials. The molecular building blocks that are in a reticular chemist's toolbox are chosen in such a way that the structures are rationally designed, framework chemistry is performed to integrate catalytically active components, and the manner in which these building blocks are connected endows the material with the desired optoelectronic properties. The fact that these aspects can be fine-tuned independently lends credence to the prospect of reticular chemistry contributing to the design of next-generation CO2 reduction catalysts.

  4. Electro and photo-assisted carbon dioxide reduction on molecular catalysts

    International Nuclear Information System (INIS)

    Stanbury, Matthew

    2016-01-01

    The general context of this thesis is on CO 2 valorisation, and recounts fundamental research aimed at finding new molecular catalysts in order to achieve CO 2 conversion. The results obtained provide additional knowledge in view of developing an efficient and selective catalytic CO 2 reduction process. The first chapter begins with the general picture of CO 2 utilisation and contains a bibliographical overview on the use of molecular catalysts for CO 2 photo- and electroreduction. This short review demonstrates the wide variety of transition metal complexes used as catalysts, in particularly those based on rhenium. An analysis on the current state of CO 2 reduction research using molecular catalyst complexes of the manganese carbonyl type is then reported. In Chapter II, the discussion begins with a brief overview of the research developed during this thesis relating to new complexes of the general formula: [Mn(L)(CO) 3 (X)] (X = Br, n = 0 ou CH 3 CN, n = 1; L = terpyridine derivatives). The interest in these complexes is twofold, as their physico-chemical properties give them potential catalytic CO 2 reduction applications, as well as applications in the field relating to controlled CO release molecules. Developing new complexes based on ligands derived from terpy is one of the main routes that were chosen for catalyst performance optimisation and improvement. In this context, Mn complexes were synthesised, their photo- and electrochemical properties were studied in detail, before testing their activity with respect to catalytic CO 2 reduction. The most remarkable result comes from the unique ability of these species to release one of their carbonyl ligands in a controlled fashion, which led to the discovery of novel Mn dicarbonyl complexes which are selective catalysts for CO 2 reduction, and also to new molecules which are applicable in the release of small quantities of CO for therapeutic purposes. Chapter III covers the study of the complex [Mn

  5. Au/iron oxide catalysts: temperature programmed reduction and X-ray diffraction characterization

    International Nuclear Information System (INIS)

    Neri, G.; Visco, A.M.; Galvagno, S.; Donato, A.; Panzalorto, M.

    1999-01-01

    Gold on iron oxides catalysts have been characterized by temperature programmed reduction (TPR) and X-ray diffraction spectroscopy (XRD). The influence of preparation method, gold loading and pretreatment conditions on the reducibility of iron oxides have been investigated. On the impregnated Au/iron oxide catalysts as well as on the support alone the partial reduction of Fe(III) oxy(hydroxides) to Fe 3 O 4 starts in the 550 and 700 K temperature range. On the coprecipitated samples, the temperature of formation of Fe 3 O 4 is strongly dependent on the presence of gold. The reduction temperature is lowered as the gold loading is increased. The reduction of Fe 3 O 4 to FeO occurs at about 900 K and is not dependent on the presence of gold and the preparation method. It is suggested that the effect of gold on the reducibility of the iron oxides is related to an increase of the structural defects and/or of the surface hydroxyl groups. (Copyright (c) 1999 Elsevier Science B.V., Amsterdam. All rights reserved.)

  6. Metal-polypyridyl catalysts for electro- and photochemical reduction of water to hydrogen.

    Science.gov (United States)

    Zee, David Z; Chantarojsiri, Teera; Long, Jeffrey R; Chang, Christopher J

    2015-07-21

    Climate change, rising global energy demand, and energy security concerns motivate research into alternative, sustainable energy sources. In principle, solar energy can meet the world's energy needs, but the intermittent nature of solar illumination means that it is temporally and spatially separated from its consumption. Developing systems that promote solar-to-fuel conversion, such as via reduction of protons to hydrogen, could bridge this production-consumption gap, but this effort requires invention of catalysts that are cheap, robust, and efficient and that use earth-abundant elements. In this context, catalysts that utilize water as both an earth-abundant, environmentally benign substrate and a solvent for proton reduction are highly desirable. This Account summarizes our studies of molecular metal-polypyridyl catalysts for electrochemical and photochemical reduction of protons to hydrogen. Inspired by concept transfer from biological and materials catalysts, these scaffolds are remarkably resistant to decomposition in water, with fast and selective electrocatalytic and photocatalytic conversions that are sustainable for several days. Their modular nature offers a broad range of opportunities for tuning reactivity by molecular design, including altering ancillary ligand electronics, denticity, and/or incorporating redox-active elements. Our first-generation complex, [(PY4)Co(CH3CN)2](2+), catalyzes the reduction of protons from a strong organic acid to hydrogen in 50% water. Subsequent investigations with the pentapyridyl ligand PY5Me2 furnished molybdenum and cobalt complexes capable of catalyzing the reduction of water in fully aqueous electrolyte with 100% Faradaic efficiency. Of particular note, the complex [(PY5Me2)MoO](2+) possesses extremely high activity and durability in neutral water, with turnover frequencies at least 8500 mol of H2 per mole of catalyst per hour and turnover numbers over 600 000 mol of H2 per mole of catalyst over 3 days at an

  7. Oscillations and patterns in a model of simultaneous CO and C2H2 oxidation and NO(x) reduction in a cross-flow reactor.

    Science.gov (United States)

    Hadač, Otto; Kohout, Martin; Havlica, Jaromír; Schreiber, Igor

    2015-03-07

    A model describing simultaneous catalytic oxidation of CO and C2H2 and reduction of NOx in a cross-flow tubular reactor is explored with the aim of relating spatiotemporal patterns to specific pathways in the mechanism. For that purpose, a detailed mechanism proposed for three-way catalytic converters is split into two subsystems, (i) simultaneous oxidation of CO and C2H2, and (ii) oxidation of CO combined with NOx reduction. The ability of these two subsystems to display mechanism-specific dynamical effects is studied initially by neglecting transport phenomena and applying stoichiometric network and bifurcation analyses. We obtain inlet temperature - inlet oxygen concentration bifurcation diagrams, where each region possessing specific dynamics - oscillatory, bistable and excitable - is associated with a dominant reaction pathway. Next, the spatiotemporal behaviour due to reaction kinetics combined with transport processes is studied. The observed spatiotemporal patterns include phase waves, travelling fronts, pulse waves and spatiotemporal chaos. Although these types of pattern occur generally when the kinetic scheme possesses autocatalysis, we find that some of their properties depend on the underlying dominant reaction pathway. The relation of patterns to specific reaction pathways is discussed.

  8. Impact of catalyst reduction mode on selective hydrogenation of cinnamaldehyde over Ru-Sn sol-gel catalysts

    Czech Academy of Sciences Publication Activity Database

    Hájek, J.; Kumar, N.; Salmi, T.; Murzin, DY.; Karhu, H.; Väyrynen, J.; Červený, L.; Paseka, Ivo

    2003-01-01

    Roč. 42, č. 2 (2003), s. 295-305 ISSN 0888-5885 R&D Projects: GA ČR GA104/00/1009 Institutional research plan: CEZ:AV0Z4032918 Keywords : Supported ruthenium catalysts * Ru-Sn-Al2O3 catalysts * benzene Subject RIV: CA - Inorganic Chemistry Impact factor: 1.317, year: 2003

  9. Characteristics of mordenite-type zeolite catalysts deactivated by SO{sub 2} for the reduction of NO with hydrocarbons

    Energy Technology Data Exchange (ETDEWEB)

    Kim, M.H.; Nam, I.S.; Kim, Y.G. [Pohang Univ. of Science and Technology/Research Inst. of Industrial Science and Technology, Pohang (Korea, Republic of)

    1998-10-25

    The deactivation of mordenite-type zeolite catalysts for the selective reduction of NO by hydrocarbons in the presence of SO{sub 2} was examined in a packed-bed flow reactor system. The physicochemical properties of the deactivated catalysts by SO{sub 2} were extensively characterized by TGA, TPSR, XPS, Raman, XANES, the measurements of surface area and elemental analysis. Not only the surface area and sulfur content of the deactivated catalysts, but their TGA and TPSR patterns strongly suggest the formation of a sulfur species as a deactivating agent on the catalyst surface. It is also observed that the sulfur species exists in the form of sulfate (SO{sub 4}{sup 2{minus}}) by XPS and Raman. It mainly causes the loss of NO removal activity of the catalysts. The sulfate species formed on the deactivated catalysts by SO{sub 2} did not significantly alter the chemical environment of the copper ions contained in the zeolite catalysts such as CuHM and CuNZA. It does not exist in the form of cupric sulfate pentahydrate on the catalyst surface as revealed by Cu K-edge absorption spectra of the catalysts.

  10. Catalytic reduction of NH4NO3 by NO. Effects of solid acids and implications for low temperature DeNOx processes

    International Nuclear Information System (INIS)

    Savara, Aditya; Li, Mei-Jun; Sachtler, Wolfgang M.H.; Weitz, Eric

    2008-01-01

    Ammonium nitrate is thermally stable below 250 C and could potentially deactivate low temperature NO x reduction catalysts by blocking active sites. It is shown that NO reduces neat NH 4 NO 3 above its 170 C melting point, while acidic solids catalyze this reaction even at temperatures below 100 C. NO 2 , a product of the reduction, can dimerize and then dissociate in molten NH 4 NO 3 to NO + + NO 3 - , and may be stabilized within the melt as either an adduct or as HNO 2 formed from the hydrolysis of NO + or N 2 O 4 . The other product of reduction, NH 4 NO 2 , readily decomposes at ≤100 C to N 2 and H 2 O, the desired end products of DeNO x catalysis. A mechanism for the acid catalyzed reduction of NH 4 NO 3 by NO is proposed, with HNO 3 as an intermediate. These findings indicate that the use of acidic catalysts or promoters in DeNO x systems could help mitigate catalyst deactivation at low operating temperatures (<150 C). (author)

  11. Cross-Linked CoMoO4/rGO Nanosheets as Oxygen Reduction Catalyst

    Directory of Open Access Journals (Sweden)

    Jiaqi Fu

    2017-12-01

    Full Text Available Development of inexpensive and robust electrocatalysts towards oxygen reduction reaction (ORR is crucial for the cost-affordable manufacturing of metal-air batteries and fuel cells. Here we show that cross-linked CoMoO4 nanosheets and reduced graphene oxide (CoMoO4/rGO can be integrated in a hybrid material under one-pot hydrothermal conditions, yielding a composite material with promising catalytic activity for oxygen reduction reaction (ORR. Cyclic voltammetry (CV and linear sweep voltammetry (LSV were used to investigate the efficiency of the fabricated CoMoO4/rGO catalyst towards ORR in alkaline conditions. The CoMoO4/rGO composite revealed the main reduction peak and onset potential centered at 0.78 and 0.89 V (vs. RHE, respectively. This study shows that the CoMoO4/rGO composite is a highly promising catalyst for the ORR under alkaline conditions, and potential noble metal replacement cathode in fuel cells and metal-air batteries.

  12. Reduction and Immobilization of Potassium Permanganate on Iron Oxide Catalyst by Fluidized-Bed Crystallization Technology

    Directory of Open Access Journals (Sweden)

    Guang-Xia Li

    2012-03-01

    Full Text Available A manganese immobilization technology in a fluidized-bed reactor (FBR was developed by using a waste iron oxide (i.e., BT-3 as catalyst which is a by-product from the fluidized-bed Fenton reaction (FBR-Fenton. It was found that BT-3 could easily reduce potassium permanganate (KMnO4 to MnO2. Furthermore, MnO2 could accumulate on the surface of BT-3 catalyst to form a new Fe-Mn oxide. Laboratory experiments were carried out to investigate the KMnO4-reduction mechanism, including the effect of KMnO4 concentration, BT-3 dosage, and operational solution pH. The results showed that the pH solution was a significant factor in the reduction of KMnO4. At the optimum level, pHf 6, KMnO4 was virtually reduced in 10 min. A pseudo-first order reaction was employed to describe the reduction rate of KMnO4.

  13. Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction.

    Science.gov (United States)

    Yang, Liu; Cheng, Daojian; Xu, Haoxiang; Zeng, Xiaofei; Wan, Xin; Shui, Jianglan; Xiang, Zhonghua; Cao, Dapeng

    2018-06-26

    It is still a grand challenge to develop a highly efficient nonprecious-metal electrocatalyst to replace the Pt-based catalysts for oxygen reduction reaction (ORR). Here, we propose a surfactant-assisted method to synthesize single-atom iron catalysts (SA-Fe/NG). The half-wave potential of SA-Fe/NG is only 30 mV less than 20% Pt/C in acidic medium, while it is 30 mV superior to 20% Pt/C in alkaline medium. Moreover, SA-Fe/NG shows extremely high stability with only 12 mV and 15 mV negative shifts after 5,000 cycles in acidic and alkaline media, respectively. Impressively, the SA-Fe/NG-based acidic proton exchange membrane fuel cell (PEMFC) exhibits a high power density of 823 mW cm -2 Combining experimental results and density-functional theory (DFT) calculations, we further reveal that the origin of high-ORR activity of SA-Fe/NG is from the Fe-pyrrolic-N species, because such molecular incorporation is the key, leading to the active site increase in an order of magnitude which successfully clarifies the bottleneck puzzle of why a small amount of iron in the SA-Fe catalysts can exhibit extremely superior ORR activity.

  14. Recent developments of nano-structured materials as the catalysts for oxygen reduction reaction

    Science.gov (United States)

    Kang, SungYeon; Kim, HuiJung; Chung, Yong-Ho

    2018-04-01

    Developments of high efficient materials for electrocatalyst are significant topics of numerous researches since a few decades. Recent global interests related with energy conversion and storage lead to the expansion of efforts to find cost-effective catalysts that can substitute conventional catalytic materials. Especially, in the field of fuel cell, novel materials for oxygen reduction reaction (ORR) have been noticed to overcome disadvantages of conventional platinum-based catalysts. Various approaching methods have been attempted to achieve low cost and high electrochemical activity comparable with Pt-based catalysts, including reducing Pt consumption by the formation of hybrid materials, Pt-based alloys, and not-Pt metal or carbon based materials. To enhance catalytic performance and stability, numerous methods such as structural modifications and complex formations with other functional materials are proposed, and they are basically based on well-defined and well-ordered catalytic active sites by exquisite control at nanoscale. In this review, we highlight the development of nano-structured catalytic materials for ORR based on recent findings, and discuss about an outlook for the direction of future researches.

  15. Electrodeposited ultrafine TaOx/CB catalysts for PEFC cathode application: Their oxygen reduction reaction kinetics

    KAUST Repository

    Seo, Jeongsuk

    2014-12-01

    Ultrafine TaOx nanoparticles were electrodeposited on carbon black (CB) powder in a nonaqueous Ta complex solution at room temperature, and the resultant TaOx/CB catalysts were assessed as oxygen reduction reaction (ORR) electrocatalysts for polymer electrolyte fuel cell (PEFC) cathodes. The Ta electrodeposition process was scaled up using a newly designed working electrode containing a CB dense layer, without introducing any binder such as the ionomer Nafion in the electrode for electrodeposition. The electrodeposited TaOx/CB powders were removed from the deposition electrode and subsequent H2 treatment at varying temperatures between 523 and 1073 K was attempted to increase the ORR performance. The TaOx/CB samples were characterized by SEM, STEM, XPS, and EELS measurements. XPS and EELS results indicated the reduced nature of the Ta species caused by the high-temperature treatment in H2, while STEM images clearly revealed that the TaOx particles aggregated as the treatment temperature increased. When the TaOx/CB catalyst, which was treated at 873 K for 2 h, was deposited on a glassy carbon substrate with Nafion ionomer, it resulted in the highest activity among the samples investigated, giving an onset potential of 0.95 VRHE at -2 μA cm-2 in a 0.1 M H2SO4 solution. Moreover, the long-term stability test with 10,000 cycles of the voltammetry only led to a 6% loss in the ORR currents, demonstrating the high stability of the TaOx/CB catalysts. Kinetic analysis by R(R)DE indicated that the four-electron transfer pathway in the ORR process was dominant for this TaOx/CB catalyst, and Tafel plots showed a slope corresponding to a one-electron reaction for the rate-determining step.

  16. Electrodeposited ultrafine TaOx/CB catalysts for PEFC cathode application: Their oxygen reduction reaction kinetics

    KAUST Repository

    Seo, Jeongsuk; Anjum, Dalaver H.; Takanabe, Kazuhiro; Kubota, Jun; Domen, Kazunari

    2014-01-01

    Ultrafine TaOx nanoparticles were electrodeposited on carbon black (CB) powder in a nonaqueous Ta complex solution at room temperature, and the resultant TaOx/CB catalysts were assessed as oxygen reduction reaction (ORR) electrocatalysts for polymer electrolyte fuel cell (PEFC) cathodes. The Ta electrodeposition process was scaled up using a newly designed working electrode containing a CB dense layer, without introducing any binder such as the ionomer Nafion in the electrode for electrodeposition. The electrodeposited TaOx/CB powders were removed from the deposition electrode and subsequent H2 treatment at varying temperatures between 523 and 1073 K was attempted to increase the ORR performance. The TaOx/CB samples were characterized by SEM, STEM, XPS, and EELS measurements. XPS and EELS results indicated the reduced nature of the Ta species caused by the high-temperature treatment in H2, while STEM images clearly revealed that the TaOx particles aggregated as the treatment temperature increased. When the TaOx/CB catalyst, which was treated at 873 K for 2 h, was deposited on a glassy carbon substrate with Nafion ionomer, it resulted in the highest activity among the samples investigated, giving an onset potential of 0.95 VRHE at -2 μA cm-2 in a 0.1 M H2SO4 solution. Moreover, the long-term stability test with 10,000 cycles of the voltammetry only led to a 6% loss in the ORR currents, demonstrating the high stability of the TaOx/CB catalysts. Kinetic analysis by R(R)DE indicated that the four-electron transfer pathway in the ORR process was dominant for this TaOx/CB catalyst, and Tafel plots showed a slope corresponding to a one-electron reaction for the rate-determining step.

  17. Tracking the Structural and Electronic Configurations of a Cobalt Proton Reduction Catalyst in Water

    Energy Technology Data Exchange (ETDEWEB)

    Moonshiram, Dooshaye; Gimbert-Suriñach, Carolina [Institute; Guda, Alexander [International; Picon, Antonio; Lehmann, C. Stefan; Zhang, Xiaoyi; Doumy, Gilles; March, Anne Marie; Benet-Buchholz, Jordi [Institute; Soldatov, Alexander [International; Llobet, Antoni [Institute; Departament; Southworth, Stephen H.

    2016-08-09

    Time resolved X-ray absorption spectroscopy (X-TAS) has been used to study the light induced hydrogen evolution reaction catalyzed by a highly stable cobalt complex, [Ru(bpy)3]2+ photosensitizer and an equimolar mixture of sodium ascorbate/ascorbic acid electron donor in pure water. XANES and EXAFS analysis of a binary mixture of the octahedral Co(III) pre-catalyst and [Ru(bpy)3]2+ after illumination, revealed in-situ formation of a square pyramidal Co(II) intermediate, with electron transfer kinetics of 51 ns. On the other hand, X-TAS experiments of the complete photocatalytic system in the presence of the electron donor showed the formation of a square planar Co(I) intermediate species within a few nanoseconds followed by its decay in the microsecond timescales. The Co(I) structural assignment is supported by calculations based on density functional theory (DFT). At longer reaction times, we observe the formation of the initial Co(III) species concomitant to the decay of Co(I), thus closing the catalytic cycle. The experimental X-ray absorption spectra of the molecular species formed along the catalytic cycle are modeled using a combination of molecular orbital DFT calculations (DFT-MO) and Finite Difference Method (FDM). These findings allowed us to unequivocally assign the full mechanistic pathway followed by the catalyst as well as to determine the rate limiting step of the process, which consists in the protonation of the Co(I). This study provides a complete kinetics scheme for the hydrogen evolution reaction by a cobalt catalyst, revealing unique information for the development of better catalysts for the reductive side of hydrogen fuel cells.

  18. Torrefaction reduction of coke formation on catalysts used in esterification and cracking of biofuels from pyrolysed lignocellulosic feedstocks

    Science.gov (United States)

    Kastner, James R; Mani, Sudhagar; Hilten, Roger; Das, Keshav C

    2015-11-04

    A bio-oil production process involving torrefaction pretreatment, catalytic esterification, pyrolysis, and secondary catalytic processing significantly reduces yields of reactor char, catalyst coke, and catalyst tar relative to the best-case conditions using non-torrefied feedstock. The reduction in coke as a result of torrefaction was 28.5% relative to the respective control for slow pyrolysis bio-oil upgrading. In fast pyrolysis bio-oil processing, the greatest reduction in coke was 34.9%. Torrefaction at 275.degree. C. reduced levels of acid products including acetic acid and formic acid in the bio-oil, which reduced catalyst coking and increased catalyst effectiveness and aromatic hydrocarbon yields in the upgraded oils. The process of bio-oil generation further comprises a catalytic esterification of acids and aldehydes to generate such as ethyl levulinate from lignified biomass feedstock.

  19. In-line localized monitoring of catalyst activity in selective catalytic NO.sub.x reduction systems

    Science.gov (United States)

    Muzio, Lawrence J [Laguna Niguel, CA; Smith, Randall A [Huntington Beach, CA

    2009-12-22

    Localized catalyst activity in an SCR unit for controlling emissions from a boiler, power plant, or any facility that generates NO.sub.x-containing flue gases is monitored by one or more modules that operate on-line without disrupting the normal operation of the facility. Each module is positioned over a designated lateral area of one of the catalyst beds in the SCR unit, and supplies ammonia, urea, or other suitable reductant to the catalyst in the designated area at a rate that produces an excess of the reductant over NO.sub.x on a molar basis through the designated area. Sampling probes upstream and downstream of the designated area draw samples of the gas stream for NO.sub.x analysis, and the catalyst activity is determined from the difference in NO.sub.x levels between the two probes.

  20. Catalysts for cleaner combustion of coal, wood and briquettes sulfur dioxide reduction options for low emission sources

    Energy Technology Data Exchange (ETDEWEB)

    Smith, P.V. [Global Environmental Solutions, Inc., Morton Grove, IL (United States)

    1995-12-31

    Coal fired, low emission sources are a major factor in the air quality problems facing eastern European cities. These sources include: stoker-fired boilers which feed district heating systems and also meet local industrial steam demand, hand-fired boilers which provide heat for one building or a small group of buildings, and masonary tile stoves which heat individual rooms. Global Environmental Systems is marketing through Global Environmental Systems of Polane, Inc. catalysts to improve the combustion of coal, wood or fuel oils in these combustion systems. PCCL-II Combustion Catalysts promotes more complete combustion, reduces or eliminates slag formations, soot, corrosion and some air pollution emissions and is especially effective on high sulfur-high vanadium residual oils. Glo-Klen is a semi-dry powder continuous acting catalyst that is injected directly into the furnace of boilers by operating personnel. It is a multi-purpose catalyst that is a furnace combustion catalyst that saves fuel by increasing combustion efficiency, a cleaner of heat transfer surfaces that saves additional fuel by increasing the absorption of heat, a corrosion-inhibiting catalyst that reduces costly corrosion damage and an air pollution reducing catalyst that reduces air pollution type stack emissions. The reduction of sulfur dioxides from coal or oil-fired boilers of the hand fired stoker design and larger, can be controlled by the induction of the Glo-Klen combustion catalyst and either hydrated lime or pulverized limestone.

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

    Science.gov (United States)

    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.

  2. Enzymatic versus Inorganic Oxygen Reduction Catalysts: Comparison of the Energy Levels in a Free-Energy Scheme

    DEFF Research Database (Denmark)

    Kjærgaard, Christian Hauge; Rossmeisl, Jan; Nørskov, Jens Kehlet

    2010-01-01

    In this paper, we present a method to directly compare the energy levels of intermediates in enzymatic and inorganic oxygen reduction catalysts. We initially describe how the energy levels of a Pt(111) catalyst, operating at pH = 0, are obtained. By a simple procedure, we then convert the energy...... levels of cytochrome c oxidase (CcO) models obtained at physiological pH = 7 to the energy levels at pH = 0, which allows for comparison. Furthermore, we illustrate how different bias voltages will affect the free-energy landscapes of the catalysts. This allows us to determine the so-called theoretical...

  3. Descomposición electrocatalítica del NOx con el catalizador NiO/YSZ= Electrochemical catalytic descomposition of NOx with a NiO/YSZ catalyst

    OpenAIRE

    Alfonso Martínez, María Pilar

    2012-01-01

    Los catalizadores basados en níquel presentan una buena actividad en la descomposición del NOx, pero son fuertemente inhibidos por el oxígeno. En este trabajo se estudió la regeneración de los centros activos del catalizador, obteniéndose una regeneración continua de los mismos cuando se llevaba a cabo una reducción electro-química del catalizador. Se observó un aumento en la selectividad de la celda electroquímica respecto a la reacción de descomposición de los óxidos de nitrógeno con el tie...

  4. Graphene layer encapsulated metal nanoparticles as a new type of non-precious metal catalysts for oxygen reduction

    DEFF Research Database (Denmark)

    Hu, Yang; Zhong, Lijie; Jensen, Jens Oluf

    2016-01-01

    Cheap and efficient non-precious metal catalysts for oxygen reduction have been a focus of research in the field of low-temperature fuel cells. This review is devoted to a brief summary of the recent work on a new type of catalysts, i.e., the graphene layer encapsulated metal nanoparticles....... The discussion is focused on the synthesis, structure, mechanism, performance, and further research....

  5. 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

    Science.gov (United States)

    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.

  6. Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane.

    Science.gov (United States)

    Zhang, Sheng; Kang, Peng; Bakir, Mohammed; Lapides, Alexander M; Dares, Christopher J; Meyer, Thomas J

    2015-12-29

    Developing sustainable energy strategies based on CO2 reduction is an increasingly important issue given the world's continued reliance on hydrocarbon fuels and the rise in CO2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO2 reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd-H sites and Cu-CO sites during electrochemical CO2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO2 resulting in the enhancement of catalytic current densities by threefold. The procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.

  7. Carbon and Mo transformations during the synthesis of mesoporous Mo2C/carbon catalysts by carbothermal hydrogen reduction

    Science.gov (United States)

    Wang, Haiyan; Liu, Shida; Liu, Bing; Montes, Vicente; Hill, Josephine M.; Smith, Kevin J.

    2018-02-01

    The synthesis of mesoporous Mo2C/carbon catalysts by carbothermal hydrogen reduction is reported. Petroleum coke (petcoke) was activated with KOH at 800 °C to obtain high surface area microporous activated petcoke (APC; 2000 m2/g). The APC was wet impregnated with ammonium heptamolybdate (AHM: 10 wt% Mo), dried and reduced in H2 at temperatures from 400 to 800 °C, to yield Mo2C/APC catalysts. Increased reduction temperature increased the Mo2C yield and the mesoporous volume of the Mo2C/APC. At a reduction temperature of 750 °C the mesopore volume of the catalyst doubled compared to the APC support and accounted for 37% of the total pore volume. Maintaining the final CHR temperature for 90 min further increased the Mo2C yield and mesoporosity of the catalyst. The role of Mo2C in the catalytic hydrogenation of the APC and mesopore generation is demonstrated. The activity of the Mo2C/carbon catalysts in the hydrodeoxygenation of 4-methyl phenol increased with increased CHR temperature and catalyst mesoporosity.

  8. Innovative clean coal technology: 500 MW demonstration of advanced wall-fired combustion techniques for the reduction of nitrogen oxide (NOx) emissions from coal-fired boilers. Final report, Phases 1 - 3B

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1998-01-01

    This report presents the results of a U.S. Department of Energy (DOE) Innovative Clean Coal Technology (ICCT) project demonstrating advanced wall-fired combustion techniques for the reduction of nitrogen oxide (NOx) emissions from coal-fired boilers. The project was conducted at Georgia Power Company`s Plant Hammond Unit 4 located near Rome, Georgia. The technologies demonstrated at this site include Foster Wheeler Energy Corporation`s advanced overfire air system and Controlled Flow/Split Flame low NOx burner. The primary objective of the demonstration at Hammond Unit 4 was to determine the long-term effects of commercially available wall-fired low NOx combustion technologies on NOx emissions and boiler performance. Short-term tests of each technology were also performed to provide engineering information about emissions and performance trends. A target of achieving fifty percent NOx reduction using combustion modifications was established for the project. Short-term and long-term baseline testing was conducted in an {open_quotes}as-found{close_quotes} condition from November 1989 through March 1990. Following retrofit of the AOFA system during a four-week outage in spring 1990, the AOFA configuration was tested from August 1990 through March 1991. The FWEC CF/SF low NOx burners were then installed during a seven-week outage starting on March 8, 1991 and continuing to May 5, 1991. Following optimization of the LNBs and ancillary combustion equipment by FWEC personnel, LNB testing commenced during July 1991 and continued until January 1992. Testing in the LNB+AOFA configuration was completed during August 1993. This report provides documentation on the design criteria used in the performance of this project as it pertains to the scope involved with the low NOx burners and advanced overfire systems.

  9. Lanthanides-based graphene catalysts for high performance hydrogen evolution and oxygen reduction

    International Nuclear Information System (INIS)

    Shinde, S.S.; Sami, Abdul; Lee, Jung-Ho

    2016-01-01

    Highlights: • Facile, scalable in-situ synthesis of lanthanide (La, Eu, Yb) doped graphene frameworks. • Efficient electrocatalytic performance towards HER and ORR. • Eu-Gr hybrid shows HER performance; onset & overpotential (81 & 160 mV), & Tafel slope (52 mV dec −1 ). • Eu-Gr exhibits superior activity of ORR; onset potential (0.92 V), electron transfer number (4.03). • Excellent long-term stability in HER and ORR, comparable to those of commercial Pt/C catalysts. - Abstract: The design of efficient electrocatalysts for hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) has received enormous consideration due to their effectiveness in modern renewable energy technologies such as fuel cells, electrolyzers, and metal–air batteries. Herein, we present a facile method to fabricate lanthanides (L = La, Eu, Yb)-doped graphene materials as catalyst for the HER and ORR that show desirable electrocatalytic activities as well as long-term stability. The Eu-graphene hybrid has showed unbeatable HER performance such as small values of onset potential (81 mV), overpotential (160 mV), and Tafel slope (52 mV dec −1 ), along with a high exchange current density (7.55 × 10 −6 A cm −2 ). The L-graphenes also exhibit superior electrocatalytic activity for ORR, including small Tafel slopes (96, 66, and 105 mV dec −1 for La-Gr, Eu-Gr, and Yb-Gr, respectively), positive onset potential (∼0.83–0.92 V), high electron transfer numbers (∼3.84–4.03), and excellent enduring strength, analogous to those of viable Pt/C catalysts. The excellent electrocatalytic performance is attributed to the synergistic effect of abundant edges and doping sites, high electrical conductivity, large active surface areas and fast charge transfer; which renders lanthanide-based graphene hybrids as potentially great candidate for energy conversion systems.

  10. Nanocarbon/oxide composite catalysts for bifunctional oxygen reduction and evolution in reversible alkaline fuel cells: A mini review

    Science.gov (United States)

    Chen, Mengjie; Wang, Lei; Yang, Haipeng; Zhao, Shuai; Xu, Hui; Wu, Gang

    2018-01-01

    A reversible fuel cell (RFC), which integrates a fuel cell with an electrolyzer, is similar to a rechargeable battery. This technology lies on high-performance bifunctional catalysts for the oxygen reduction reaction (ORR) in the fuel cell mode and the oxygen evolution reaction (OER) in the electrolyzer mode. Current catalysts are platinum group metals (PGM) such as Pt and Ir, which are expensive and scarce. Therefore, it is highly desirable to develop PGM-free catalysts for large-scale application of RFCs. In this mini review, we discussed the most promising nanocarbon/oxide composite catalysts for ORR/OER bifunctional catalysis in alkaline media, which is mainly based on our recent progress. Starting with the effectiveness of selected oxides and nanocarbons in terms of their activity and stability, we outlined synthetic methods and the resulting structures and morphologies of catalysts to provide a correlation between synthesis, structure, and property. A special emphasis is put on understanding of the possible synergistic effect between oxide and nanocarbon for enhanced performance. Finally, a few nanocomposite catalysts are discussed as typical examples to elucidate the rules of designing highly active and durable bifunctional catalysts for RFC applications.

  11. Efficient selective catalytic reduction of NO by novel carbon-doped metal catalysts made from electroplating sludge.

    Science.gov (United States)

    Zhang, Jia; Zhang, Jingyi; Xu, Yunfeng; Su, Huimin; Li, Xiaoman; Zhou, Ji Zhi; Qian, Guangren; Li, Li; Xu, Zhi Ping

    2014-10-07

    Electroplating sludges, once regarded as industrial wastes, are precious resources of various transition metals. This research has thus investigated the recycling of an electroplating sludge as a novel carbon-doped metal (Fe, Ni, Mg, Cu, and Zn) catalyst, which was different from a traditional carbon-supported metal catalyst, for effective NO selective catalytic reduction (SCR). This catalyst removed >99.7% NO at a temperature as low as 300 °C. It also removed NO steadily (>99%) with a maximum specific accumulative reduced amount (MSARA) of 3.4 mmol/g. Gas species analyses showed that NO removal was accompanied by evolving N2 and CO2. Moreover, in a wide temperature window, the sludge catalyst showed a higher CO2 selectivity (>99%) than an activated carbon-supported metal catalyst. Structure characterizations revealed that carbon-doped metal was transformed to metal oxide in the sludge catalyst after the catalytic test, with most carbon (2.33 wt %) being consumed. These observations suggest that NO removal over the sludge catalyst is a typical SCR where metals/metal oxides act as the catalytic center and carbon as the reducing reagent. Therefore, our report probably provides an opportunity for high value-added utilizations of heavy-metal wastes in mitigating atmospheric pollutions.

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

    Science.gov (United States)

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

    2017-07-12

    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 NO x 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.

  13. Investigation of a Pt-Fe/C catalyst for oxygen reduction reaction in direct ethanol fuel cells

    International Nuclear Information System (INIS)

    Castro Luna, A. M.; Bonesi, A.; Triaca, W. E.; Blasi, A. Di; Stassi, A.; Baglio, V.; Antonucci, V.; Arico, A. S.

    2010-01-01

    Three cathode catalysts (60% Pt/C, 30% Pt/C and 60% Pt-Fe/C), with a particle size of about 2-3 nm, were prepared to investigate the effect of ethanol cross-over on cathode surfaces. All samples were studied in terms of structure and morphology by using X-ray diffraction (XRD) and transmission electron microscopy (TEM) analyses. Their electrocatalytic behavior in terms of oxygen reduction reaction (ORR) was investigated and compared using a rotating disk electrode (RDE). The tolerance of cathode catalysts in the presence of ethanol was evaluated. The Pt-Fe/C catalyst showed both higher ORR activity and tolerance to ethanol cross-over than Pt/C catalysts. Moreover, the more promising catalysts were tested in 5 cm 2 DEFC single cells at 60 and 80 o C. An improvement in single cell performance was observed in the presence of the Pt-Fe catalyst, due to an enhancement in the oxygen reduction kinetics. The maximum power density was 53 mW cm -2 at 2 bar rel. cathode pressure and 80 o C.

  14. Analysis of proton exchange membrane fuel cell catalyst layers for reduction of platinum loading at Nissan

    International Nuclear Information System (INIS)

    Ohma, Atsushi; Mashio, Tetsuya; Sato, Kazuyuki; Iden, Hiroshi; Ono, Yoshitaka; Sakai, Kei; Akizuki, Ken; Takaichi, Satoshi; Shinohara, Kazuhiko

    2011-01-01

    The biggest issue that must be addressed in promoting widespread use of fuel cell vehicles (FCVs) is to reduce the cost of the fuel cell system. Especially, it is of vital importance to reduce platinum (Pt) loading of catalyst layers (CLs) in the membrane electrode assembly (MEA) of a proton exchange membrane fuel cell (PEMFC). In order to lower the Pt loading of the MEA, mass transport of reactants related to the performance in high current density should be enhanced significantly as well as kinetics of the catalyst, which can result in the better Pt utilization and effectiveness. In this study, we summarized our analytical approach and methods for reduction of Pt loading in CLs. Microstructure, mass transport properties of the reactants, and their relation in CLs were elucidated by applying experimental analyses and computational methods. A simple CL model for I–V performance prediction was then established, where experimentally elucidated parameters of the microstructure and the properties in CLs were taken into account. Finally, we revealed the impact of lowering the Pt loading on the transport properties, polarization, and the I–V performance.

  15. High performance vanadia-anatase nanoparticle catalysts for the selective catalytic reduction of NO by ammonia

    DEFF Research Database (Denmark)

    Kristensen, Steffen Buus; Kunov-Kruse, Andreas Jonas; Riisager, Anders

    2011-01-01

    Highly active nanoparticle SCR deNO(x) catalysts composed of amorphous vanadia on crystalline anatase have been prepared by a sol-gel, co-precipitation method using decomposable crystallization seeds. The catalysts were characterized by means of XRPD, TEM/SEM, FT-IR, nitrogen physisorption and NH(3......) catalysts reported in the literature in the examined temperature range of 200-400 degrees C. The catalysts showed very high resistivity towards potassium poisoning maintaining a 15-30 times higher activity than the equally poisoned industrial reference catalyst, upon impregnation by 280 mu mole potassium....../g of catalyst. (C) 2011 Elsevier Inc. All rights reserved....

  16. Use of Biomass as a Sustainable and Green Fuel with Alkali-Resistant DeNOx Catalysts based on Sulfated or Tungstated Zirconia

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes; Fehrmann, Rasmus; Christensen, Claus H.

    poisons is the use of supports with highly acidic properties, which would interact stronger with potassium than the vanadium species. Among those, sulfated and tungstated zirconica appears very attractive, since their surface acidity can be tuned in a wide range by varying the preparation procedure, WOX......, sulfated, and tungstated zirconia were prepared and tested. The influence of potassium additives on the acidity and activity was studied and the results were compared with traditional V2O5-WO3/TiO2 catalyst. Resistance of the catalysts towards poisoning with potassium was found to depend dramatically...... on the crystallinity and surface acidity of the support used. Better resistance of the samples based on sulfated and tungstated zirconia seems to be connected with the fact that a significant part of the potassium on the surface of the catalyst preferentially interact with strong acid sites of the support thus...

  17. Modelling the aqueous and nonaqueous interfaces for CO2 electro-reduction over Sn catalysts

    Science.gov (United States)

    Sheng, Tian; Sun, Shi-Gang

    2018-01-01

    In CO2 electroreduction, Sn catalysts with a high overpotential for hydrogen evolution reaction and a high selectivity towards formic acid formation are very attractive. Many efforts have been made for improving the catalytic performance and for understanding the mechanisms. In electrochemistry, the role of solvents for surface reactions was deserved to be investigated, in particular for some nonaqueous solvents. Here, we have modeled the aqueous (water) and nonaqueous (acetonitrile and dichloromethane) for investigation of CO2 electroreduction on Sn surface, by constrained ab initio molecular dynamics simulations and thermodynamic integrations, including a number of explicit solvent molecules in computational models. It was found that CO2 reduction is initiated from formate formation and solvents, in particular, water can effectively facilitate the reaction.

  18. Effect of solvent on Se-modified ruthenium/carbon catalyst for oxygen reduction

    Directory of Open Access Journals (Sweden)

    Chuanxiang Zhang

    2014-12-01

    Full Text Available Se-modified ruthenium supporting on carbon (Sex–Ru/C electrocatalyst was prepared by solvothermal one-step synthesis method. The reaction mechanism was revealed after discussing impact of different solvents (i-propanol and EG in solvotermal reaction. The result showed that the grain size of Se-modified ruthenium electrocatalyst was as small as 1 to 3 nm and highly dispersed on carbon surface. X-ray photoelectron spectroscopy (XPS presented that selenium mainly existed in the catalyst in the form of elemental selenium and selenium oxides when the solvent was EG and i-propanol, respectively. The oxygen reduction reaction (ORR performance was improved by appearance of selenium oxides.

  19. Chitosan supported bimetallic Pd/Co nanoparticles as a heterogeneous catalyst for the reduction of nitroaromatics to amines

    Directory of Open Access Journals (Sweden)

    Sajjad Keshipour

    2017-01-01

    Full Text Available A new bimetallic nanocomposite of chitosan was prepared. Pd and Co nanoparticles were deposited on chitosan to produce a new heterogeneous recyclable catalyst for use in the bimetallic catalytic reduction reaction. The catalyst was characterized with common analysis methods for nanocomposites including Energy Dispersive X-Ray Spectroscopy, X-Ray Diffraction pattern, Thermal Gravimetric Analysis, Flame Atomic Absorption Spectroscopy and Scanning Electron Microscopy, and applied in the reduction reaction of nitroaromatics using NaBH4 at room temperature. The bimetallic system gave good results compared to each of the applied metals. Various aromatic amines and diamines were used in the reduction reaction. The aromatic amines were obtained as the sole product of the reduction reaction with 15 mol% Pd and 12 mol% Co during 2h. This reaction had some advantages such as mild reaction conditions, high yield, green solvent, and a recyclable catalyst. Also, the recovered catalyst was applicable in the reduction reaction without a significant decrease in the activity for up to six times.

  20. Uniformity index measurement technology using thermocouples to improve performance in urea-selective catalytic reduction systems

    Science.gov (United States)

    Park, Sangki; Oh, Jungmo

    2018-05-01

    The current commonly used nitrogen oxides (NOx) emission reduction techniques employ hydrocarbons (HCs), urea solutions, and exhaust gas emissions as the reductants. Two of the primary denitrification NOx (DeNOx) catalyst systems are the HC-lean NOx trap (HC-LNT) catalyst and urea-selective catalytic reduction (urea-SCR) catalyst. The secondary injection method depends on the type of injector, injection pressure, atomization, and spraying technique. In addition, the catalyst reaction efficiency is directly affected by the distribution of injectors; hence, the uniformity index (UI) of the reductant is very important and is the basis for system optimization. The UI of the reductant is an indicator of the NOx conversion efficiency (NCE), and good UI values can reduce the need for a catalyst. Therefore, improving the UI can reduce the cost of producing a catalytic converter, which are expensive due to the high prices of the precious metals contained therein. Accordingly, measurement of the UI is an important process in the development of catalytic systems. Two of the commonly used methods for measuring the reductant UI are (i) measuring the exhaust emissions at many points located upstream/downstream of the catalytic converter and (ii) acquisition of a reductant distribution image on a section of the exhaust pipe upstream of the catalytic converter. The purpose of this study is to develop a system and measurement algorithms to measure the exothermic response distribution in the exhaust gas as the reductant passes through the catalytic converter of the SCR catalyst system using a set of thermocouples downstream of the SCR catalyst. The system is used to measure the reductant UI, which is applied in real-time to the actual SCR system, and the results are compared for various types of mixtures for various engine operating conditions and mixer types in terms of NCE.

  1. Selective catalytic reduction of nitric oxide with acetaldehyde over NaY zeolite catalyst in lean exhaust feed

    International Nuclear Information System (INIS)

    Schmieg, Steven J.; Cho, Byong K.; Oh, Se H.

    2004-01-01

    Steady-state selective catalytic reduction (SCR) of nitric oxide (NO) was investigated under simulated lean-burn conditions using acetaldehyde (CH 3 CHO) as the reductant. This work describes the influence of catalyst space velocity and the impact of nitric oxide, acetaldehyde, oxygen, sulfur dioxide, and water on NO x reduction activity over NaY zeolite catalyst. Results indicate that with sufficient catalyst volume 90% NO x conversion can be achieved at temperatures relevant to light-duty diesel exhaust (150-350C). Nitric oxide and acetaldehyde react to form N 2 , HCN, and CO 2 . Oxygen is necessary in the exhaust feed stream to oxidize NO to NO 2 over the catalyst prior to reduction, and water is required to prevent catalyst deactivation. Under conditions of excess acetaldehyde (C 1 :N>6:1) and low temperature ( x conversion is apparently very high; however, the NO x conversion steadily declines with time due to catalytic oxidation of some of the stored (adsorbed) NO to NO 2 , which can have a significant impact on steady-state NO x conversion. With 250ppm NO in the exhaust feed stream, maximum NO x conversion at 200C can be achieved with =400ppm of acetaldehyde, with higher acetaldehyde concentrations resulting in production of acetic acid and breakthrough of NO 2 causing lower NO x conversion levels. Less acetaldehyde is necessary at lower NO concentrations, while more acetaldehyde is required at higher temperatures. Sulfur in the exhaust feed stream as SO 2 can cause slow deactivation of the catalyst by poisoning the adsorption and subsequent reaction of nitric oxide and acetaldehyde, particularly at low temperature

  2. Fe/Ni-N-CNFs electrochemical catalyst for oxygen reduction reaction/oxygen evolution reaction in alkaline media

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhuang [MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001 (China); Li, Mian [Faculty of Chemistry, Northeast Normal University, Changchun 130024 (China); Fan, Liquan; Han, Jianan [MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001 (China); Xiong, Yueping, E-mail: ypxiong@hit.edu.cn [MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001 (China)

    2017-04-15

    Highlights: • Novel Fe/Ni-N-CNFs electrocatalysts are prepared by electrospinning technique. • The Fe1Ni1-N-CNFs catalyst exhibits the excellent ORR and OER catalytic activity. • Synergy of Fe/Ni alloy is responsible for the excellent catalytic performance. - Abstract: The novel of iron, nickel and nitrogen doped carbon nanofibers (Fe/Ni-N-CNFs) as bifunctional electrocatalysts are prepared by electrospinning technique. In alkaline media, the Fe/Ni-N-CNFs catalysts (especially for Fe1Ni1-N-CNFs) exhibit remarkable electrocatalytic performances of oxygen reduction reaction (ORR)/oxygen evolution reaction (OER). For ORR catalytic activity, Fe1Ni1-N-CNFs catalyst offers a higher onset potential of 0.903 V, a similar four-electron reaction pathway, and excellent stability. For OER catalytic activity, Fe1Ni1-N-CNFs catalyst possesses a lower onset potential of 1.528 V and a smaller charge transfer resistance of 48.14 Ω. The unparalleled catalytic activity of ORR and OER for the Fe1Ni1-N-CNFs is attributed to the 3D porous cross-linked microstructures of carbon nanofibers with Fe/Ni alloy, N dopant, and abundant M-N{sub x} and NiOOH as catalytic active sites. Thus, Fe1Ni1-N-CNFs catalyst can be acted as one of the efficient and inexpensive catalysts of metal-air batteries.

  3. Metal-air batteries: from oxygen reduction electrochemistry to cathode catalysts.

    Science.gov (United States)

    Cheng, Fangyi; Chen, Jun

    2012-03-21

    Because of the remarkably high theoretical energy output, metal-air batteries represent one class of promising power sources for applications in next-generation electronics, electrified transportation and energy storage of smart grids. The most prominent feature of a metal-air battery is the combination of a metal anode with high energy density and an air electrode with open structure to draw cathode active materials (i.e., oxygen) from air. In this critical review, we present the fundamentals and recent advances related to the fields of metal-air batteries, with a focus on the electrochemistry and materials chemistry of air electrodes. The battery electrochemistry and catalytic mechanism of oxygen reduction reactions are discussed on the basis of aqueous and organic electrolytes. Four groups of extensively studied catalysts for the cathode oxygen reduction/evolution are selectively surveyed from materials chemistry to electrode properties and battery application: Pt and Pt-based alloys (e.g., PtAu nanoparticles), carbonaceous materials (e.g., graphene nanosheets), transition-metal oxides (e.g., Mn-based spinels and perovskites), and inorganic-organic composites (e.g., metal macrocycle derivatives). The design and optimization of air-electrode structure are also outlined. Furthermore, remarks on the challenges and perspectives of research directions are proposed for further development of metal-air batteries (219 references).

  4. Alternative SILP-SCR Catalysts based on Guanidinium Chromates

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes; Riisager, Anders; Ståhl, Kenny

    There is an increasing global concern about human caused emissions of pollutants like sulfur and nitrogen oxides to the atmosphere leading to, e.g. smog and acid rain damaging to the human health and the environment. Selective catalytic reduction (SCR) of NOx with ammonia as reductant is the most...... duct. There is therefore a demand for alkali-resistant SCR catalysts more flexible regarding temperature of operation and position in the duct. Supported ionic liquid phase (SILP) catalysts with 1,1,3,3-Tetramethylguanidinium (TMGH+) and a chromium oxide anion supported on anatase have exhibited...

  5. Selective hydrogenation of phenol to cyclohexanone over Pd@CN (N-doped porous carbon): Role of catalyst reduction method

    Science.gov (United States)

    Hu, Shuo; Yang, Guangxin; Jiang, Hong; Liu, Yefei; Chen, Rizhi

    2018-03-01

    Selective phenol hydrogenation is a green and sustainable technology to produce cyclohexanone. The work focused on investigating the role of catalyst reduction method in the liquid-phase phenol hydrogenation to cyclohexanone over Pd@CN (N-doped porous carbon). A series of reduction methods including flowing hydrogen reduction, in-situ reaction reduction and liquid-phase reduction were designed and performed. The results highlighted that the reduction method significantly affected the catalytic performance of Pd@CN in the liquid-phase hydrogenation of phenol to cyclohexanone, and the liquid-phase reduction with the addition of appropriate amount of phenol was highly efficient to improve the catalytic activity of Pd@CN. The influence mechanism was explored by a series of characterizations. The results of TEM, XPS and CO chemisorption confirmed that the reduction method mainly affected the size, surface composition and dispersion of Pd in the CN material. The addition of phenol during the liquid-phase reduction could inhibit the aggregation of Pd NPs and promote the reduction of Pd (2+), and then improved the catalytic activity of Pd@CN. The work would aid the development of high-performance Pd@CN catalysts for selective phenol hydrogenation.

  6. Graphene hydrogels with embedded metal nanoparticles as efficient catalysts in 4-nitrophenol reduction and methylene blue decolorization

    Directory of Open Access Journals (Sweden)

    Żelechowska Kamila

    2016-12-01

    Full Text Available Synthesis and characterization of the graphene hydrogels with three different metallic nanoparticles, that is Au, Ag and Cu, respectively is presented. Synthesized in a one-pot approach graphene hydrogels with embedded metallic nanoparticles were tested as heterogeneous catalysts in a model reaction of 4-nitrophenol reduction. The highest activity was obtained for graphene hydrogel with Cu nanoparticles and additional reaction of methylene blued degradation was evaluated using this system. The obtained outstanding catalytic activity arises from the synergistic effect of graphene and metallic nanoparticles. The hydrogel form of the catalyst benefits in the easiness in separation from the reaction mixture (for example using tweezers and reusability.

  7. Heteropoly acid promoted Cu and Fe catalysts for the selective catalytic reduction of NO with ammonia

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Mossin, Susanne L.; Riisager, Anders

    2011-01-01

    Cu/TiO2, Fe/TiO2 and heteropoly acid promoted Cu/TiO2, Fe/TiO2 catalysts were prepared and characterized by N2 physisorption, XRPD, NH3-TPD, H2-TPR and EPR. The catalysts exhibited only crystalline TiO2 phases with the active metals and promoters in highly dispersed state. The acidic properties...... activity and acidity was lower for promoted catalysts than for unpromoted catalysts. In the heteropoly acid promoted catalysts the SCR active Cu and Fe metals were protected from potassium poisons by bonding of the potassium to the Brønsted acid centres. Thus heteropoly acid promoted catalysts might...... be suitable for biomass fired power plant SCR applications....

  8. Program to reduce NOx emissions of HNO{sub 3} plants with selective catalytic reduction; Programme visant a reduire les emissions de NOx d'ateliers d'HNO{sub 3} par reduction catalytique selective

    Energy Technology Data Exchange (ETDEWEB)

    Gry, Ph. [Grande Paroisse SA, Group ATOFINA, 92 - Paris la Defense (France)

    2001-07-01

    Grande Paroisse well known as G.P. has been created in 1919. Nowadays, it is an affiliated company of ATOFINA. The Company is the first French producer of fertilizers and the third West European. In its sites G.P. controls 1.3 millions metric tons per year of nitric acid, on 13 units. Continuous improvement of its technology together with productivity development make G.P. one of the most competitive fertilizer manufacturer. A technical team achieves this objective and maintains a world wide reputable technology. For the past 15 years, industry has tried to reduce NO{sub x} atmospheric pollution. The SCR (Selective Catalytic Reduction) is most used with ammonia for nitric acid units and described here under. (author)

  9. Ti and Si doping as a way to increase low temperature activity of sulfated Ag/Al2O3 in H2-assisted NH3-SCR of NOx

    DEFF Research Database (Denmark)

    Doronkin, Dmitry E.; Fogel, Sebastian; Gabrielsson, Pär

    2013-01-01

    Ag/Al2O3 catalysts modified by Si, Ti, Mg and W were studied to obtain higher NOx SCR activity and potentially also higher SO2 resistance than the pure silver-based catalyst for automotive applications. Addition of Ti or Si to the alumina support leads to a better NOx removal at low temperature i......-TPR) and temperature-programmed desorption of ammonia (NH3-TPD). The obtained results suggest a better silver dispersion and better regeneration capability in the case of Ti- and Si-modified Ag/Al2O3 catalysts........e. reduces the SCR onset temperature by about 10°C under the applied conditions. However, it does not increase the SO2 resistance. The catalysts and the supports have been characterized by BET, conventional and synchrotron XRD, X-ray absorption spectroscopy during temperature-programmed reduction (XAS......Ag/Al2O3 catalysts modified by Si, Ti, Mg and W were studied to obtain higher NOx SCR activity and potentially also higher SO2 resistance than the pure silver-based catalyst for automotive applications. Addition of Ti or Si to the alumina support leads to a better NOx removal at low temperature i...

  10. System and method for controlling ammonia levels in a selective catalytic reduction catalyst using a nitrogen oxide sensor

    Science.gov (United States)

    None

    2017-07-25

    A system according to the principles of the present disclosure includes an air/fuel ratio determination module and an emission level determination module. The air/fuel ratio determination module determines an air/fuel ratio based on input from an air/fuel ratio sensor positioned downstream from a three-way catalyst that is positioned upstream from a selective catalytic reduction (SCR) catalyst. The emission level determination module selects one of a predetermined value and an input based on the air/fuel ratio. The input is received from a nitrogen oxide sensor positioned downstream from the three-way catalyst. The emission level determination module determines an ammonia level based on the one of the predetermined value and the input received from the nitrogen oxide sensor.

  11. Durability Improvement of Pt/RGO Catalysts for PEMFC by Low-Temperature Self-Catalyzed Reduction.

    Science.gov (United States)

    Sun, Kang Gyu; Chung, Jin Suk; Hur, Seung Hyun

    2015-12-01

    Pt/C catalyst used for polymer electrolyte membrane fuel cells (PEMFCs) displays excellent initial performance, but it does not last long because of the lack of durability. In this study, a Pt/reduced graphene oxide (RGO) catalyst was synthesized by the polyol method using ethylene glycol (EG) as the reducing agent, and then low-temperature hydrogen bubbling (LTHB) treatment was introduced to enhance the durability of the Pt/RGO catalyst. The cyclic voltammetry (CV), oxygen reduction reaction (ORR) analysis, and transmittance electron microscopy (TEM) results suggested that the loss of the oxygen functional groups, because of the hydrogen spillover and self-catalyzed dehydration reaction during LTHB, reduced the carbon corrosion and Pt agglomeration and thus enhanced the durability of the electrocatalyst.

  12. Method and apparatus for combination catalyst for reduction of NO.sub.x in combustion products

    Science.gov (United States)

    Socha, Richard F.; Vartuli, James C.; El-Malki, El-Mekki; Kalyanaraman, Mohan; Park, Paul W.

    2010-09-28

    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, and 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.

  13. Influence of hydrogen treatment on SCR catalysts

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes

    stream, i.e. by in situ treatment of the Pt-catalyst by reductive H2-gas. However, the introduction of H2 gas in the gas stream could also affect other units in the tail pipe gas cleaning system. Of special interest in this study is the effect of hydrogen gas on the performance of the selective catalytic...... reduction (SCR) process, i.e. the catalytic removal of NOx from the flue gas. A series of experiments was conducted to reveal the impact on the NO SCR activity of a industrial DeNOX catalyst (3%V2O5-7%WO3/TiO2) by treatment of H2. Standard conditions were treatment of the SCR catalyst for 60 min with three...... different concentrations of H2 (0-2%) in a 8% O2/N2 mixture, where the SCR activity was measured before and after the hydrogen treatment. The results show that the activity of the SCR catalyst is only negligible affected during exposure to the H2/O2 gas and in all cases it returned reversibly to the initial...

  14. A novel method for synthesis of phosphomolybdic acid-modified Pd/C catalysts for oxygen reduction reaction

    Science.gov (United States)

    Zhu, Mingyuan; Gao, Xiaoling; Luo, Guangqin; Dai, Bin

    2013-03-01

    This manuscript reports a convenient method for immobilizing phosphomolybdic acid (HPMo) on polyaniline (PAN-) functionalized carbon supports. The obtained HPMo-PAN-C sample is used as the support to prepare a Pd/HPMo-PAN-C catalyst. The samples are characterized by Fourier transform infrared spectroscopy, transmission electron microscopy and X-ray diffraction analysis. The results suggest that HPMo retains its Keggin structure and that the presence of HPMo reduces the average particle size of the Pd nano-particles in the obtained Pd/HPMo-PAN-C catalyst. Electro-chemical measurements in 0.5 M HClO4 solution reveal that the Pd/HPMo-PAN-C catalyst has higher catalytic activity for oxygen reduction reactions than does a Pd/C catalyst prepared using a similar procedure. The stability of the Pd/HPMo-PAN-C catalyst is evaluated by multiple-cycle voltammetry techniques; the mass catalytic activity decreases by only 10% after 100 scanning cycles.

  15. Quaternized chitosan/rectorite/AgNP nanocomposite catalyst for reduction of 4-nitrophenol

    Energy Technology Data Exchange (ETDEWEB)

    Ling, Yunzhi [State Key Laboratory of Pulp & Paper Engineering, South China University of Technology, Guangzhou 510640 (China); Zeng, Xianjie [School of Business Administration, South China University of Technology, Guangzhou 510640 (China); Tan, Weirui [State Key Laboratory of Pulp & Paper Engineering, South China University of Technology, Guangzhou 510640 (China); Luo, Jiwen, E-mail: holdit@126.com [Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education, School of Chemistry and Environment, South China Normal University, Guangzhou 510006 (China); State Key Laboratory of Pulp & Paper Engineering, South China University of Technology, Guangzhou 510640 (China); Liu, Shijie, E-mail: sjliu@163.com [State Key Laboratory of Pulp & Paper Engineering, South China University of Technology, Guangzhou 510640 (China); China Department of Paper and Bioprocess Engineering, State University of New York, College of Environmental Science and Forestry, 1 Forestry Drive, Syracuse, NY 13210 (United States)

    2015-10-25

    This study investigated a one-step green fabrication of exfoliated quaternized chitosan/rectorite/AgNP nanocomposites under microwave radiation method. The nanocomposites were characterized by FT-IR, XRD, XPS and TEM. The results revealed that quaternized chitosan and rectorite acted as reducing and stabilizing agents, spherical AgNPs were synthesized greenly and rapidly, meanwhile the layers of rectorite were exfoliated, and when the ratio of quaternized chitosan, rectorite and silver nitrate was 100 mg: 10 mg: 2 mmol, the AgNP content reached the maximum of 2.73%. Then, the quaternized chitosan/rectorite/AgNP nanocomposite was fabricated as a film, which was used in the catalytic reduction from 4-nitrophenol to 4-aminophenol by NaBH{sub 4}. The film showed excellent catalytic efficiency with an activation energy of 29.76 kJ mol{sup −1} and outstanding reusable performance even after catalysis for 10 times. - Graphical abstract: Quaternized chitosan/rectorite/AgNP nanocomposite catalyst was prepared greenly in one pot and fabricated as a film, which showed excellent catalytic efficiency and reusable performance. - Highlights: • Quaternized chitosan and rectorite acted as reducing and stabilizing agents. • Spherical Ag NPs were synthesized greenly and rapidly. • AgNP dispersed well on the surface and the interlayer of exfoliated rectorite. • Quaternized chitosan/rectorite/AgNP nanocomposite was prepared as a film. • The film showed excellent catalytic efficiency and reusable performance.

  16. New Homogeneous Chromophore/Catalyst Concepts for the Solar-Driven Reduction of Carbon Dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Hopkins, Michael D. [The University of Chicago, Chicago, IL (United States)

    2015-06-22

    One of the major scientific and technical challenges of this century is to develop chemical means to store solar energy in the form of fuels. This can be accomplished by developing light-absorbing and catalytic compounds that function cooperatively to rearrange the chemical bonds of feedstocks in a way that allows solar energy to be stored and released on demand. The research conducted during this project was directed toward addressing fundamental questions that underlie the conversion of CO2 to a solar fuel using homogeneous molecular systems. The research focused particularly on developing methods for extracting the reducing equivalents for these photochemical conversions from H2, which is a renewable molecule sourced to water. The research followed two main lines. One effort focused on understanding the general principles that govern how light-absorbing molecules interact with independent H2 oxidation and CO2 reduction catalysts to produce a functional cycle for driving the energy-storing reverse water-gas-shift reaction with light. The second effort centered on developing the excited-state properties and H2 activation chemistry of tungsten–alkylidyne complexes. These chromophores were found to be powerful excited-state reducing agents, which could be incorporated into light-light-harvesting assemblies, and to hold the potential to be regenerated using H2.

  17. Design of heterogeneous catalysts

    DEFF Research Database (Denmark)

    Frey, Anne Mette

    was inspired by a computational screening, suggesting that alloys such as Ni-Fe, Co-Ni, and Co-Fe should show superior activity to the industrially used nickel catalyst. Especially the Ni-Fe system was considered to be interesting, since such alloy catalysts should be both more active and cheaper than the Ni...... catalyst. The results from the screening were experimentally verified for CO hydrogenation, CO2 hydrogenation, and simultaneous CO and CO2 hydrogenation by bimetallic Ni-Fe catalysts. These catalysts were found to be highly active and selective. The Co-Ni and Co-Fe systems were investigated for CO...... well, and the best catalyst prepared had a C5+ yield almost a factor of two higher than a standard air calcined Co catalyst. In the NH3-SCR reaction it is desirable to develop an active and stable catalyst for NOx removal in automotive applications, since the traditionally used vanadium-based catalyst...

  18. Supramolecular tetracluster-cobalt porphyrin: a four-electron transfer catalyst for dioxygen reduction

    International Nuclear Information System (INIS)

    Winnischofer, Herbert; Otake, Vesper Yoshiyuki; Dovidauskas, Sergio; Nakamura, Marcelo; Toma, Henrique Eisi; Araki, Koiti

    2004-01-01

    Electrocatalysis by CoTCP {CoTCP meso-tetrakis(4-pyridyl)porphynatocobalt(III)} coordinated to four [Ru 3 (μ 3 -O)(μ 2 -CH 3 CO 2 ) 6 (py) 2 ] + complexes in the four-electron reduction of dioxygen, has been unequivocally demonstrated in this work by using two types of electrostatically assembled films of CoTCP and anionic zinc or free-base meso-tetrakis(4-sulfonatophenyl)porphyrins (ZnTPPS or H 2 TPPS), as well as, by employing different electrode materials. An enhanced electrocatalytic activity has been observed, in spite of the fact that the typical bis-coordination of dioxygen to two cobalt porphyrin sites is precluded in such CoTCP/ZnTPPS or CoTCP/H 2 TPPS bilayered films. In addition, negligible ring currents have been observed in ring-disk voltammetry measurements, yielding straight Levich and Koutecky-Levich plots, whose slopes approached the theoretical 4e - curve in air, or in O 2 saturated solutions (pH 3-5). The use of gold instead of glassy carbon (GC) electrodes has not also significantly perturbed the mechanism. By ruling out any influence from the electrode materials, a well known critical point in the catalysis by cobalt porphyrins, the results have shown that CoTCP is acting as a four-electron transfer catalyst for dioxygen reduction. Also, by excluding the possibility of bis-coordination of dioxygen, it was shown that the electronic and supramolecular effects exerted by the peripheral ruthenium cluster complexes should be triggering the four-electron catalytic activity of the cobalt porphyrin center

  19. Feasibility of plasma aftertreatment for simultaneous control of NOx and particulates

    International Nuclear Information System (INIS)

    Brusasco, R M; Merritt, B T; Penetrante, B; Pitz, W J; Vogtlin, G E

    1999-01-01

    Plasma reactors can be operated as a particulate trap or as a NOx converter. Particulate trapping in a plasma reactor can be accomplished by electrostatic precipitation. The soluble organic fraction of the trapped particulates can be utilized for the hydrocarbon-enhanced oxidation of NO to NO2 . The NO2 can then be used to non-thermally oxidize the carbon fraction of the particulates. The oxidation of the carbon fraction by NO2 can lead to reduction of NOx or backconversion of NO2 to NO. This paper examines the hydrocarbon and electrical energy density requirements in a plasma for maximum NOx conversion in both heavy-duty and light-duty diesel engine exhaust. The energy density required for complete oxidation of hydrocarbons is also examined and shown to be much greater than that required for maximum NOx conversion. The reaction of NO2 with carbon is shown to lead mainly to backconversion of NO2 to NO. These results suggest that the combination of the plasma with a catalyst will be required to reduce the NOx and oxidize the hydrocarbons. The plasma reactor can be operated occasionally in the arc mode to thermally oxidize the carbon fraction of the particulates

  20. Photocatalytic NO_x abatement. Theory, applications, current research, and limitations

    International Nuclear Information System (INIS)

    Bloh, Jonathan Z.

    2017-01-01

    Nitrogen oxides are one of the major air pollutants that threaten our air quality and health. As a consequence, increasingly stricter regulations are in place forcing action to reduce the concentration of these dangerous compounds. Conventional methods of reducing the NO_x pollution level are reducing the emission directly at the source or restrictive measures such as low emission zones. However, there are recent reports questioning the efficacy of the strategy to reduce ambient NO_x levels solely by reducing their emissions and existing threshold values are still frequently exceeded in many European cities. Semiconductor photocatalysis presents an appealing alternative capable of removing NO_x and other air pollutants from the air once they have already been released and dispersed. Recent field tests have shown that a reduction of a few percent in NO_x values is possible with available photocatalysts. Current research focuses on further increasing the catalysts' efficacy as well as their selectivity to suppress the formation of undesired by-products. Especially using these improved materials, photocatalytic NO_x abatement could prove a very valuable contributor to better air quality.

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

    Energy Technology Data Exchange (ETDEWEB)

    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. Regeneration of Pt-catalysts deactivated in municipal waste flue gas with H2/N2 and the effect of regeneration step on the SCR catalyst

    DEFF Research Database (Denmark)

    Due-Hansen, Johannes; Rasmussen, Søren Birk; Kustov, Arkadii

    Municipal waste flue gas was previously found to deactivate the Pt-based CO oxidation catalyst severely. In the specific case studied, siloxanes were found to cause the deactivation. An on-site method for complete regeneration of the catalyst activity was found without shutdown of the flue gas...... stream, i.e. by in situ treatment of the Pt-catalyst by reductive H2-gas. However, introduction of H2 gas in the gas stream could also affect other units in the tail pipe gas cleaning system. Of special interest here, is the effect of hydrogen gas on the performance of the deNOx + SCR catalytic process...

  3. Asymmetric reduction of ketones with catecholborane using 2,6-BODOL complexes of titanium(IV) as catalysts.

    Science.gov (United States)

    Sarvary, I; Almqvist, F; Frejd, T

    2001-05-18

    Reductions performed with Ti(IV) complexes of ligands based on bicyclo[2.2.2]octane diols 5 and 6 are effective catalysts in the reduction of prochiral ketones to optically active alcohols, with catecholborane as the reducing agent. Methyl ketones are favored and enantiomeric excesses (ee) of octanone, which gave 2-octanol in 87% ee. Further details of the method were examined, for example, temperature, solvent composition, amount of molecular sieves (4 A), and catecholborane quality, as well as the sensitivity of the ligands towards acids. NMR spectroscopic methods were used to gain some insight into the complexes formed between the ligands and [Ti(OiPr)4]. A dimeric structure is proposed for the pre-catalyst.

  4. Year-round N2O production by benthic NOx reduction in a monomictic south-alpine lake

    Science.gov (United States)

    Freymond, C. V.; Wenk, C. B.; Frame, C. H.; Lehmann, M. F.

    2013-12-01

    Nitrous oxide (N2O) is a potent greenhouse gas, generated through microbial nitrogen (N) turnover processes, such as nitrification, nitrifier denitrification, and denitrification. Previous studies quantifying natural sources have mainly focused on soils and the ocean, but the potential role of terrestrial water bodies in the global N2O budget has been widely neglected. Furthermore, the biogeochemical controls on the production rates and the microbial pathways that produce benthic N2O in lakes are essentially unknown. In this study, benthic N2O fluxes and the contributions of the microbial pathways that produce N2O were assessed using 15N label flow-through sediment incubations in the eutrophic, monomictic south basin of Lake Lugano in Switzerland. The sediments were a significant source of N2O throughout the year, with production rates ranging between 140 and 2605 nmol N2O h-1 m-2, and the highest observed rates coinciding with periods of water column stratification and stably anoxic conditions in the overlying bottom water. Nitrate (NO3-) reduction via denitrification was found to be the major N2O production pathway in the sediments under both oxygen-depleted and oxygen-replete conditions in the overlying water, while ammonium oxidation did not contribute significantly to the benthic N2O flux. A marked portion (up to 15%) of the total NO3- consumed by denitrification was reduced only to N2O, without complete denitrification to N2. These fluxes were highest when the bottom water had stabilized to a low-oxygen state, in contrast with the notion that stable anoxia is particularly conducive to complete denitrification without accumulation of N2O. This study provides evidence that lake sediments are a significant source of N2O to the overlying water and may produce large N2O fluxes to the atmosphere during seasonal mixing events.

  5. Reduction of nanowire diameter beyond lithography limits by controlled catalyst dewetting

    International Nuclear Information System (INIS)

    Calahorra, Yonatan; Kerlich, Alexander; Gavrilov, Arkady; Cohen, Shimon; Ritter, Dan; Amram, Dor

    2016-01-01

    Catalyst assisted vapour-liquid–solid is the most common method to realize bottom-up nanowire growth; establishing a parallel process for obtaining nanoscale catalysts at pre-defined locations is paramount for further advancement towards commercial nanowire applications. Herein, the effect of a selective area mask on the dewetting of metallic nanowire catalysts, deposited within lithography-defined mask pinholes, is reported. It was found that thin disc-like catalysts, with diameters of 120–450 nm, were transformed through dewetting into hemisphere-like catalysts, having diameters 2–3 fold smaller; the process was optimized to about 95% yield in preventing catalyst splitting, as would otherwise be expected due to their thickness-to-diameter ratio, which was as low as 1/60. The catalysts subsequently facilitated InP and InAs nanowire growth. We suggest that the mask edges prevent surface migration mediated spreading of the dewetted metal, and therefore induce its agglomeration into a single particle. This result presents a general strategy to diminish lithography-set dimensions for NW growth, and may answer a fundamental challenge faced by bottom-up nanowire technology. (paper)

  6. Reduction of nanowire diameter beyond lithography limits by controlled catalyst dewetting

    Science.gov (United States)

    Calahorra, Yonatan; Kerlich, Alexander; Amram, Dor; Gavrilov, Arkady; Cohen, Shimon; Ritter, Dan

    2016-04-01

    Catalyst assisted vapour-liquid-solid is the most common method to realize bottom-up nanowire growth; establishing a parallel process for obtaining nanoscale catalysts at pre-defined locations is paramount for further advancement towards commercial nanowire applications. Herein, the effect of a selective area mask on the dewetting of metallic nanowire catalysts, deposited within lithography-defined mask pinholes, is reported. It was found that thin disc-like catalysts, with diameters of 120-450 nm, were transformed through dewetting into hemisphere-like catalysts, having diameters 2-3 fold smaller; the process was optimized to about 95% yield in preventing catalyst splitting, as would otherwise be expected due to their thickness-to-diameter ratio, which was as low as 1/60. The catalysts subsequently facilitated InP and InAs nanowire growth. We suggest that the mask edges prevent surface migration mediated spreading of the dewetted metal, and therefore induce its agglomeration into a single particle. This result presents a general strategy to diminish lithography-set dimensions for NW growth, and may answer a fundamental challenge faced by bottom-up nanowire technology.

  7. Characterization of Cu/CeO2/Al2O3 catalysts by temperature programmed reduction and activity for CO oxidation

    International Nuclear Information System (INIS)

    Cataluna, Renato; Baibich, Ione M.; Dallago, R.M.; Picinini, C.; Martinez-Arias, A.; Soria, J.

    2001-01-01

    The kinetic parameters for the CO oxidation reaction using copper/alumina-modified ceria as catalysts were determined. The catalysts with different concentrations of the metals were prepared using impregnation methods. In addition, the reduction-oxidation behaviour of the catalysts were investigated by temperature-programmed reduction. The activity results show that the mechanism for CO oxidation is bifunctional: oxygen is activated on the anionic vacancies of ceria surface, while carbon monoxide is adsorbed preferentially on the higher oxidation copper site. Therefore, the reaction occurs on the interfacial active centers. Temperatures-programmed Reduction patterns show a higher dispersion when cerium oxide is present. (author)

  8. The Reduction Reaction of Dissolved Oxygen in Water by Hydrazine over Platinum Catalyst Supported on Activated Carbon Fiber

    Energy Technology Data Exchange (ETDEWEB)

    Park, K.K.; Moon, J.S. [Korea Electric Power Research Institute, Taejon (Korea)

    1999-07-01

    The reduction reaction of dissolved oxygen (DO) by hydrazine was investigated on activated carbon fiber (ACF) and Pt/ACF catalysts using a batch reactor with an external circulating loop. The ACF itself showed catalytic activity and this was further improved by supporting platinum on ACF. The catalytic role platinum is ascribed to its acceleration of hydrazine decomposition, based on electric potential and current measurements as well as the kinetic study. (author). 15 refs., 13 figs.

  9. Metalloporphyrin catalysts for oxygen reduction developed using computer-aided molecular design

    Energy Technology Data Exchange (ETDEWEB)

    Ryba, G.N.; Hobbs, J.D.; Shelnutt, J.A. [and others

    1996-04-01

    The objective of this project is the development of a new class of metalloporphyrin materials used as catalsyts for use in fuel cell applications. The metalloporphyrins are excellent candidates for use as catalysts at both the anode and cathode. The catalysts reduce oxygen in 1 M potassium hydroxide, as well as in 2 M sulfuric acid. Covalent attachment to carbon supports is being investigated. The computer-aided molecular design is an iterative process, in which experimental results feed back into the design of future catalysts.

  10. Iron alloy Fischer-tropsch catalysts--1. Oxidation-reduction studies of the Fe-Ni system

    Energy Technology Data Exchange (ETDEWEB)

    Unmuth, E.E.; Schwartz, L.H.; Butt, J.B.

    1980-01-01

    Catalysts containing 5% iron, nickel, or 4:1 iron-nickel on silica were hydrogen-reduced at 425/sup 0/C for 12 or 24 hr, reoxidized in air for 2 or 4 hr, reduced again in hydrogen for 12 hr, and studied at each treatment step by Moessbauer spectroscopy, X-ray diffraction, and temperature-programed desorption. The nickel was reduced directly to the metal, redispersed during the oxidation, and gave 20% smaller particles in the second reduction than in the first reduction. The ..cap alpha..-Fe/sub 2/O/sub 3/ reduced via an Fe/sub 3/O/sub 4/ intermediate and yielded approx. 70% metallic iron and the second reduction produced about the same particle size as the first reduction. The alloy catalyst reduced into a mixture of two phases, a face-centered cubic phase containing approx. 37.5% Ni, i.e., the bulk equilibrium value, and a body-centered cubic phase, and the particle sizes obtained in the first and second reductions were similar. The activation energies for the reduction were determined.

  11. Porous boron doped diamonds as metal-free catalysts for the oxygen reduction reaction in alkaline solution

    Science.gov (United States)

    Suo, Ni; Huang, Hao; Wu, Aimin; Cao, Guozhong; Hou, Xiaoduo; Zhang, Guifeng

    2018-05-01

    Porous boron doped diamonds (BDDs) were obtained on foam nickel substrates with a porosity of 80%, 85%, 90% and 95% respectively by hot filament chemical vapor deposition (HFCVD) technology. Scanning electron microscopy (SEM) reveals that uniform and compact BDDs with a cauliflower-like morphology have covered the overall frame of the foam nickel substrates. Raman spectroscopy shows that the BDDs have a poor crystallinity due to heavily doping boron. X-ray photoelectron spectroscopy (XPS) analysis effectively demonstrates that boron atoms can be successfully incorporated into the crystal lattice of diamonds. Electrochemical measurements indicate that the oxygen reduction potential is unaffected by the specific surface area (SSA), and both the onset potential and the limiting diffusion current density are enhanced with increasing SSA. It is also found that the durability and methanol tolerance of the boron doped diamond catalysts are attenuated as the increasing of SSA. The SSA of the catalyst is directly proportional to the oxygen reduction activity and inversely to the durability and methanol resistance. These results provide a reference to the application of porous boron doped diamonds as potential cathodic catalysts for the oxygen reduction reaction in alkaline solution by adjusting the SSA.

  12. Brief Communication: CATALYST - a multi-regional stakeholder Think Tank for fostering capacity development in disaster risk reduction and climate change adaptation

    NARCIS (Netherlands)

    Terwisscha van Scheltinga, C.T.H.M.; Hare, M.P.; Bers, van C.; Keur, van der P.

    2014-01-01

    This brief communication presents the work and objectives of the CATALYST project on "Capacity Development for Hazard Risk Reduction and Adaptation" funded by the European Commission (October 2011–September 2013). CATALYST set up a multi-regional think tank covering four regions (Central America and

  13. A Best Practices Notebook for Disaster Risk Reduction and Climate Change Adaptation: Guidance and Insights for Policy and Practice from the CATALYST Project

    NARCIS (Netherlands)

    Hare, M.; Bers, van C.; Mysiak, J.; Calliari, E.; Haque, A.; Warner, K.; Yuzva, K.; Zissener, M.; Jaspers, A.M.J.; Timmerman, J.G.

    2014-01-01

    This publication, A Best Practices Notebook for Disaster Risk Reduction and Climate Change Adaptation: Guidance and Insights for Policy and Practice from the CATALYST Project is one of two main CATALYST knowledge products that focus on the transformative approaches and measures that can support

  14. Catalytic reduction of nitrate and nitrite ions by hydrogen : investigation of the reaction mechanism over Pd and Pd-Cu catalysts

    NARCIS (Netherlands)

    Ilinitch, OM; Nosova, LV; Gorodetskii, VV; Ivanov, VP; Trukhan, SN; Gribov, EN; Bogdanov, SV; Cuperus, FP

    2000-01-01

    The catalytic behavior of mono- and bimetallic catalysts with Pd and/or Cu supported over gamma-Al2O3 in the reduction of aqueous nitrate and nitrite ions by hydrogen was investigated. The composition of the supported metal catalysts was analysed using secondary ion mass spectroscopy (SIMS) and

  15. High Performance Fe- and N- Doped Carbon Catalyst with Graphene Structure for Oxygen Reduction

    Science.gov (United States)

    Peng, Hongliang; Mo, Zaiyong; Liao, Shijun; Liang, Huagen; Yang, Lijun; Luo, Fan; Song, Huiyu; Zhong, Yiliang; Zhang, Bingqing

    2013-05-01

    Proton exchange membrane fuel cells are promising candidates for a clean and efficient energy conversion in the future, the development of carbon based inexpensive non-precious metal ORR catalyst has becoming one of the most attractive topics in fuel cell field. Herein we report a Fe- and N- doped carbon catalyst Fe-PANI/C-Mela with graphene structure and the surface area up to 702 m2 g-1. In 0.1 M HClO4 electrolyte, the ORR onset potential for the catalyst is high up to 0.98 V, and the half-wave potential is only 60 mV less than that of the Pt/C catalyst (Loadings: 51 μg Pt cm-2). The catalyst shows high stability after 10,000 cyclic voltammetry cycles. A membrane electrode assembly made with the catalyst as a cathode is tested in a H2-air single cell, the maximum power density reached ~0.33 W cm2 at 0.47 V.

  16. Integrated Removal of NOx with Carbon Monoxide as Reductant, and Capture of Mercury in a Low Temperature Selective Catalytic and Adsorptive Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Neville Pinto; Panagiotis Smirniotis; Stephen Thiel

    2010-08-31

    Coal will likely continue to be a dominant component of power generation in the foreseeable future. This project addresses the issue of environmental compliance for two important pollutants: NO{sub x} and mercury. Integration of emission control units is in principle possible through a Low Temperature Selective Catalytic and Adsorptive Reactor (LTSCAR) in which NO{sub x} removal is achieved in a traditional SCR mode but at low temperature, and, uniquely, using carbon monoxide as a reductant. The capture of mercury is integrated into the same process unit. Such an arrangement would reduce mercury removal costs significantly, and provide improved control for the ultimate disposal of mercury. The work completed in this project demonstrates that the use of CO as a reductant in LTSCR is technically feasible using supported manganese oxide catalysts, that the simultaneous warm-gas capture of elemental and oxidized mercury is technically feasible using both nanostructured chelating adsorbents and ceria-titania-based materials, and that integrated removal of mercury and NO{sub x} is technically feasible using ceria-titania-based materials.

  17. Manganese catalysts with bulky bipyridine ligands for the electrocatalytic reduction of carbon dioxide: eliminating dimerization and altering catalysis.

    Science.gov (United States)

    Sampson, Matthew D; Nguyen, An D; Grice, Kyle A; Moore, Curtis E; Rheingold, Arnold L; Kubiak, Clifford P

    2014-04-09

    With the goal of improving previously reported Mn bipyridine electrocatalysts in terms of increased activity and reduced overpotential, a bulky bipyridine ligand, 6,6'-dimesityl-2,2'-bipyridine (mesbpy), was utilized to eliminate dimerization in the catalytic cycle. Synthesis, electrocatalytic properties, X-ray diffraction (XRD) studies, and infrared spectroelectrochemistry (IR-SEC) of Mn(mesbpy)(CO)3Br and [Mn(mesbpy)(CO)3(MeCN)](OTf) are reported. Unlike previously reported Mn bipyridine catalysts, these Mn complexes exhibit a single, two-electron reduction wave under nitrogen, with no evidence of dimerization. The anionic complex, [Mn(mesbpy)(CO)3](-), is formed at 300 mV more positive potential than the corresponding state is formed in typical Mn bipyridine catalysts. IR-SEC experiments and chemical reductions with KC8 provide insights into the species leading up to the anionic state, specifically that both the singly reduced and doubly reduced Mn complexes form at the same potential. When formed, the anionic complex binds CO2 with H(+), but catalytic activity does not occur until a ~400 mV more negative potential is present. The Mn complexes show high activity and Faradaic efficiency for CO2 reduction to CO with the addition of weak Brønsted acids. IR-SEC experiments under CO2/H(+) indicate that reduction of a Mn(I)-CO2H catalytic intermediate may be the cause of this unusual "over-reduction" required to initiate catalysis.

  18. Commercial introduction of the Advanced NOxTECH system

    Energy Technology Data Exchange (ETDEWEB)

    Sudduth, B.C. [NOxTECH, Inc., Irvine, CA (United States)

    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.

  19. Selective catalytic reduction of nitric oxide by ethylene over metal-modified ZSM-5- and {gamma}-Al{sub 2}O{sub 3}-catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Eraenen, K; Kumar, N; Lindfors, L E [Aabo Akademi, Turku (Finland). Lab. of Industrial Chemistry

    1997-12-31

    Metal-modified ZSM-5 and {gamma}-Al{sub 2}O{sub 3} catalysts were tested in reduction of nitric oxide by ethylene. Different metals were introduced into the ZSM-5 catalyst by ion-exchange and by introduction of metals during the zeolite synthesis. To prepare bimetallic catalysts a combination of these methods was used. The {gamma}-Al{sub 2}O{sub 3} was impregnated with different metals by the incipient wetness technique and by adsorption. Activity measurements showed that the ZSM-5 based catalysts were more active than the {gamma}-Al{sub 2}O{sub 3} based catalysts. The highest conversion was obtained over a ZSM-5 catalyst prepared by introduction of Pd during synthesis of the zeolite and subsequently ion-exchanged with copper. (author)

  20. Selective catalytic reduction of nitric oxide by ethylene over metal-modified ZSM-5- and {gamma}-Al{sub 2}O{sub 3}-catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Eraenen, K.; Kumar, N.; Lindfors, L.E. [Aabo Akademi, Turku (Finland). Lab. of Industrial Chemistry

    1996-12-31

    Metal-modified ZSM-5 and {gamma}-Al{sub 2}O{sub 3} catalysts were tested in reduction of nitric oxide by ethylene. Different metals were introduced into the ZSM-5 catalyst by ion-exchange and by introduction of metals during the zeolite synthesis. To prepare bimetallic catalysts a combination of these methods was used. The {gamma}-Al{sub 2}O{sub 3} was impregnated with different metals by the incipient wetness technique and by adsorption. Activity measurements showed that the ZSM-5 based catalysts were more active than the {gamma}-Al{sub 2}O{sub 3} based catalysts. The highest conversion was obtained over a ZSM-5 catalyst prepared by introduction of Pd during synthesis of the zeolite and subsequently ion-exchanged with copper. (author)

  1. Improvement of activated carbons as oxygen reduction catalysts in neutral solutions by ammonia gas treatment and their performance in microbial fuel cells

    KAUST Repository

    Watson, Valerie J.; Nieto Delgado, Cesar; Logan, Bruce E.

    2013-01-01

    Commercially available activated carbon (AC) powders from different precursor materials (peat, coconut shell, coal, and hardwood) were treated with ammonia gas at 700 C to improve their performance as oxygen reduction catalysts in neutral p

  2. Poly(neutral red) as a NAD{sup +} reduction catalyst and a NADH oxidation catalyst: Towards the development of a rechargeable biobattery

    Energy Technology Data Exchange (ETDEWEB)

    Arechederra, Marguerite N.; Addo, Paul K. [Department of Chemistry, Saint Louis University, 3501 Laclede Ave., St. Louis, MO 63103 (United States); Minteer, Shelley D., E-mail: minteers@slu.ed [Department of Chemistry, Saint Louis University, 3501 Laclede Ave., St. Louis, MO 63103 (United States)

    2011-01-01

    In this paper, we have established that poly(neutral red), PNR, functions as an electrocatalyst for the reduction and oxidation of NAD{sup +}/NADH in a rechargeable biobattery environment. The reversibility of this catalyst was possible only with the addition of Zn{sup 2+} for complexation to the redox polymer. The zinc ion complexation with the polymer facilitates electron and proton transfer to/from the substrate and the NAD{sup +}/NADH coenzyme without forming covalent bonds between the nicotinamide and the substrate surface. This research presents use of this reversible catalyst in a rechargeable biobattery. The rechargeable battery includes a Prussian blue cathode and a bioanode including NAD{sup +}-dependent alcohol dehydrogenase and zinc complexed PNR. This bioanode was coupled to the cathode with Nafion 212 acting as the ion exchange membrane separator between the two compartments. The biobattery has an open circuit potential of 0.545({+-}0.009) V when first assembled and 0.053({+-}0.005) V when fully discharged. However, when fully charged, the biobattery has an open circuit potential of 1.263({+-}0.051) V, a maximum power density of 16.3({+-}4.03) {mu}W cm{sup -3} and a maximum current density of 221({+-}13.2) {mu}A cm{sup -3}. The efficiency and stability of the biobattery were studied by cycling continuously at a discharging rate of 1 C and the results obtained showed reasonable stability over 50 cycles.

  3. Reductive dechlorination of trichloroacetic acid (TCAA) by electrochemical process over Pd-In/Al_2O_3 catalyst

    International Nuclear Information System (INIS)

    Liu, Yanzhen; Mao, Ran; Tong, Yating; Lan, Huachun; Zhang, Gong; Liu, Huijuan; Qu, Jiuhui

    2017-01-01

    Highlights: • TCAA was efficiently removed by Pd-In/Al_2O_3 based electro-reductive process. • The active species for TCAA electroreduction involved electron (e"−) and atomic H*. • The atomic H* played a major contribution to TCAA removal. - Abstract: Electrochemical reduction treatment was found to be a promising method for dechlorination of Trichloroacetic acid (TCAA), and acceleration of electron transfer or enhancement of the concentration of atomic H* significantly improve the electrochemical dechlorination process. Bimetallic Pd-based catalysts have the unique property of simultaneously catalyzing the production of atomic H* and reducing target pollutants. Herein, a bimetallic Pd–In electrocatalyst with atomic ratio of 1:1 was evenly deposited on an Al_2O_3 substrate, and the bimetallic Pd-In structure was confirmed via X-ray photoelectron spectroscopy (XPS). Electrochemical removal of trichloroacetic acid (TCAA) by the Pd-In/Al_2O_3 catalyst was performed in a three-dimensional reactor. 94% of TCAA with the initial concentration of 500 μg L"−"1 could be degraded within 30 min under a relatively low current density (0.9 mA cm"−"2). In contrast to the presence of refractory intermediates (dichloroacetic acid (DCAA)) found in the Pd/Al_2O_3 system, TCAA could be thoroughly reduced to monochloroacetic acid (MCAA) using Pd-In/Al_2O_3 catalysts. According to scavenger experiments, an electron transfer process and atomic H* formation function both existed in the TCAA reduction process, and the enhanced indirect atomic H* reduction process (confirmed by ESR signals) played a chief role in the TCAA removal. Moreover, the synergistic effects of Pd and In were proven to be able to enhance both direct electron transfer and indirect atomic H* formation, indicating a promising prospect for bimetallic electrochemical reduction treatment.

  4. Reductive dechlorination of tetrachlorobisphenol A by Pd/Fe bimetallic catalysts

    International Nuclear Information System (INIS)

    Huang, Qiang; Liu, Wen; Peng, Ping’an; Huang, Weilin

    2013-01-01

    Highlights: • TCBPA can be rapidly and completely dechlorinated by Pd/Fe bimetallic catalysts. • The observed rate constants are functions of dosages, initial concentration, Pd coverage and solution pH. • Pd dosage is the major factor in the observed rates of the reaction. • This is the first report investigating the dechlorination of TCBPA by Pd/Fe catalysts. -- Abstract: The Pd/Fe bimetallic catalysts of micron sizes were synthesized and the rates of tetrachlorobisphenol A (TCBPA) degradation were measured under various conditions using a batch reactor system. The results showed that TCBPA was rapidly dechlorinated to tri-, di- and mono-chlorobisphenol A and to bisphenol A (BPA). The observed rate constants (k obs ) were found to increase as functions of the Pd coverage on the Fe particles and the dosages of the catalysts within the reactors. The k obs value decreased as the initial TCBPA concentration increased, suggesting that the TCBPA dechlorination may follow a surface-site limiting Langmuir–Hinshelwood rate model. The weakly acidic solution, especially at or near pH 6.0, also favored the dechlorination of TCBPA. At pH 6.0, Pd coverage of 0.044 wt% and catalyst dosage of 5 g L −1 , TCBPA with an initial concentration of 20 μM was completely transformed within 60 min, and BPA was detected as the major product through the reaction time. Meanwhile, the k obs values measured at constant solution pH correlated linearly with the mass of particle-bound Pd introduced to the reactors, regardless of Pd/Fe catalyst dosage or Pd surface coverage. This study suggested that Pd/Fe catalysts could be potentially employed to rapidly degrade TCBPA in the contaminated environment

  5. In Situ UV-Visible Assessment of Iron-Based High-Temperature Water-Gas Shift Catalysts Promoted with Lanthana: An Extent of Reduction Study

    Directory of Open Access Journals (Sweden)

    Basseem B. Hallac

    2018-02-01

    Full Text Available The extent of reduction of unsupported iron-based high-temperature water-gas shift catalysts with small (<5 wt % lanthana contents was studied using UV-visible spectroscopy. Temperature- programmed reduction measurements showed that lanthana content higher than 0.5 wt % increased the extent of reduction to metallic Fe, while 0.5 wt % of lanthana facilitated the reduction to Fe3O4. In situ measurements on the iron oxide catalysts using mass and UV-visible spectroscopies permitted the quantification of the extent of reduction under temperature-programmed reduction and high-temperature water-gas shift conditions. The oxidation states were successfully calibrated against normalized absorbance spectra of visible light using the Kubelka-Munk theory. The normalized absorbance relative to the fully oxidized Fe2O3 increased as the extent of reduction increased. XANES suggested that the average bulk iron oxidation state during the water-gas shift reaction was Fe+2.57 for the catalyst with no lanthana and Fe+2.54 for the catalysts with 1 wt % lanthana. However, the UV-vis spectra suggest that the surface oxidation state of iron would be Fe+2.31 for the catalyst with 1 wt % lanthana if the oxidation state of iron in the catalyst with 0 wt % lanthana were Fe+2.57. The findings of this paper emphasize the importance of surface sensitive UV-visible spectroscopy for determining the extent of catalyst reduction during operation. The paper highlights the potential to use bench-scale UV-visible spectroscopy to study the surface chemistry of catalysts instead of less-available synchrotron X-ray radiation facilities.

  6. Engineering Ru@Pt Core-Shell Catalysts for Enhanced Electrochemical Oxygen Reduction Mass Activity and Stability

    Directory of Open Access Journals (Sweden)

    Ariel Jackson

    2018-01-01

    Full Text Available Improving the performance of oxygen reduction reaction (ORR electrocatalysts is essential for the commercial efficacy of many renewable energy technologies, including low temperature polymer electrolyte fuel cells (PEFCs. Herein, we report highly active and stable carbon-supported Ru@Pt core-shell nanoparticles (Ru@Pt/C prepared by a wet chemical synthesis technique. Through rotating disc electrode testing, the Ru@Pt/C achieves an ORR Pt mass-based activity of 0.50 A mgPt−1 at 0.9 V versus the reversible hydrogen electrode (RHE, which exceeds the activity of the state-of-the-art commercial Pt/C catalyst as well as the Department of Energy 2020 PEFC electrocatalyst activity targets for transportation applications. The impact of various synthetic parameters, including Pt to Ru ratios and catalyst pretreatments (i.e., annealing are thoroughly explored. Pt-based mass activity of all prepared Ru@Pt/C catalysts was found to exceed 0.4 mgPt−1 across the range of compositions investigated, with the maximum activity catalyst having a Ru:Pt ratio of 1:1. This optimized composition of Ru@Pt/C catalyst demonstrated remarkable stability after 30,000 accelerated durability cycles (0.6 to 1.0 V vs. RHE at 125 mV s−1, maintaining 85% of its initial mass activity. Scanning transmission electron microscopy energy dispersive spectroscopy (STEM-EDS analysis at various stages of electrochemical testing demonstrated that the Pt shell can provide sufficient protection against the dissolution of the otherwise unstable Ru core.

  7. Engineering Ru@Pt Core-Shell Catalysts for Enhanced Electrochemical Oxygen Reduction Mass Activity and Stability.

    Science.gov (United States)

    Jackson, Ariel; Strickler, Alaina; Higgins, Drew; Jaramillo, Thomas Francisco

    2018-01-12

    Improving the performance of oxygen reduction reaction (ORR) electrocatalysts is essential for the commercial efficacy of many renewable energy technologies, including low temperature polymer electrolyte fuel cells (PEFCs). Herein, we report highly active and stable carbon-supported Ru@Pt core-shell nanoparticles (Ru@Pt/C) prepared by a wet chemical synthesis technique. Through rotating disc electrode testing, the Ru@Pt/C achieves an ORR Pt mass-based activity of 0.50 A mg Pt -1 at 0.9 V versus the reversible hydrogen electrode (RHE), which exceeds the activity of the state-of-the-art commercial Pt/C catalyst as well as the Department of Energy 2020 PEFC electrocatalyst activity targets for transportation applications. The impact of various synthetic parameters, including Pt to Ru ratios and catalyst pretreatments (i.e., annealing) are thoroughly explored. Pt-based mass activity of all prepared Ru@Pt/C catalysts was found to exceed 0.4 mg Pt -1 across the range of compositions investigated, with the maximum activity catalyst having a Ru:Pt ratio of 1:1. This optimized composition of Ru@Pt/C catalyst demonstrated remarkable stability after 30,000 accelerated durability cycles (0.6 to 1.0 V vs. RHE at 125 mV s -1 ), maintaining 85% of its initial mass activity. Scanning transmission electron microscopy energy dispersive spectroscopy (STEM-EDS) analysis at various stages of electrochemical testing demonstrated that the Pt shell can provide sufficient protection against the dissolution of the otherwise unstable Ru core.

  8. ZIF-67 incorporated with carbon derived from pomelo peels: A highly efficient bifunctional catalyst for oxygen reduction/evolution reactions

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Hao; Yin, Feng-Xiang; Chen, Biao-Hua; He, Xiao-Bo; Lv, Peng-Liang; Ye, Cai-Yun; Liu, Di-Jia

    2017-05-01

    Developing carbon catalyst materials using natural, abundant and renewable resources as precursors plays an increasingly important role in clean energy generation and environmental protection. In this work, N-doped pomelo-peel-derived carbon (NPC) materials were prepared using a widely available food waste-pomelo peels and melamine. The synthetic NPC exhibits well-defined porosities and a highly doped-N content (e.g. 6.38 at% for NPC-2), therefore affords excellent oxygen reduction reaction (ORR) catalytic activities in alkaline electrolytes. NPC was further integrated with ZIF-67 to form ZIF-67@NPC hybrids through solvothermal reactions. The hybrid catalysts show substantially enhanced ORR catalytic activities comparable to that of commercial 20 wa Pt/C. Furthermore, the catalysts also exhibit excellent oxygen evolution reaction (OER) catalytic activities. Among all prepared ZIF-67@NPC hybrids, the optimal composition with ZIF-67 to NPC ratio of 2:1 exhibits the best ORR and OER bifunctional catalytic performance and the smallest Delta E (E-OER@10 mA cm(-2)-E-ORR@-1 mA cm(-2)) value of 0.79 V. The catalyst also demonstrated desirable 4-electron transfer pathways and superior catalytic stabilities. The Co-N-4 in ZIF-67, electrochemical active surface area, and the strong interactions between ZIF-67 and NPC are attributed as the main contributors to the bifunctional catalytic activities. These factors act synergistically, resulting in substantially enhanced bifunctional catalytic activities and stabilities; consequently, this hybrid catalyst is among the best of the reported bifunctional electrocatalysts and is promising for use in metal-air batteries and fuel cells. (C) 2016 Elsevier B.V. All rights reserved.

  9. Reductive amination of ethanol to ethylamines over Ni/Al{sub 2}O{sub 3} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Park, Jun Hyun [Korea Research Institute of Chemical Technology, Daejeon (Korea, Republic of); Hong, Eunpyo; An, Sang Hee; Shin, Chae-Ho; Lim, Dong-Hee [Chungbuk National University, Chungju (Korea, Republic of)

    2017-10-15

    Ni(x)/Al{sub 2}O{sub 3} (x=wt%) catalysts with Ni loadings of 5-25 wt% were prepared via a wet impregnation method on an γ-Al{sub 2}O{sub 3} support and subsequently applied in the reductive amination of ethanol to ethylamines. Among the various catalysts prepared, Ni(10)/Al2O3 exhibited the highest metal dispersion and the smallest Ni particle size, resulting in the highest catalytic performance. To reveal the effects of reaction parameters, a reductive amination process was performed by varying the reaction temperature (T), weight hourly space velocity (WHSV), and NH{sub 3} and H{sub 2} partial pressures in the reactions. In addition, on/off experiments for NH{sub 3} and H{sub 2} were also carried out. In the absence of NH{sub 3} in the reactant stream, the ethanol conversion and selectivities towards the different ethylamine products were significantly reduced, while the selectivity to ethylene was dominant due to the dehydration of ethanol. In contrast, in the absence of H{sub 2}, the selectivity to acetonitrile significantly increased due to dehydrogenation of the imine intermediate. Although a small amount of catalyst deactivation was observed in the conversion of ethanol up to 10 h on stream due to the formation of nickel nitride, the Ni(10)/Al{sub 2}O{sub 3} catalyst exhibited stable catalytic performance over 90 h under the optimized reaction conditions (i.e., T=190 .deg. C, WHSV=0.9 h{sup -1}, and EtOH/NH{sub 3}/H{sub 2} molar ratio=1/1/6).

  10. Combined Particle Filter and Selective Catalytic Reduction Catalyst for Diesel Engines

    DEFF Research Database (Denmark)

    Hvam, Jeanette

    Abstract Silicon carbide has many outstanding properties. It is an extremely hard and tough material with a high thermal and chemical stability, in addition to being an important semiconductor material. Silicon carbide macro-, micro- and nanostructures can be tailored to fit specific needs, making...... and better solutions for exhaust purification systems, and porous silicon carbide has superior characteristics for this purpose. The continuously increasing requirements for low emission levels of both toxic and polluting nitric oxides (NOxes) and health damaging sod particles, requires novel methods...

  11. Turbostratic carbon supported palladium as an efficient catalyst for reductive purification of water from trichloroethylene

    Directory of Open Access Journals (Sweden)

    Emil Kowalewski

    2017-12-01

    Full Text Available This work investigates the catalytic properties of turbostratic carbon supported Pd catalyst in hydrodechlorination of trichloroethylene (TCE HDC in aqueous phase. 1.57 wt% Pd/C was thoroughly characterized by BET, TPHD, CO chemisorption, PXRD, STEM, XPS and used as the catalyst in removal of trichloroethylene from drinking water in batch and continuous-flow reactors. The studies showed that catalytic performance of Pd/C depended on the hydrophobicity and textural properties of carbon support, which influenced noble metal dispersion and increased catalyst tolerance against deactivation by chlorination. Palladium in the form of uniformly dispersed small (~3.5 nm nanoparticles was found to be very active and stable in purification of water from TCE both in batch and continuous-flow operation.

  12. Reversible-Deactivation Radical Polymerization of Methyl Methacrylate Induced by Photochemical Reduction of Various Copper Catalysts

    Directory of Open Access Journals (Sweden)

    Jaroslav Mosnáček

    2014-11-01

    Full Text Available Photochemically mediated reversible-deactivation radical polymerization of methyl methacrylate was successfully performed using 50–400 ppm of various copper compounds such as CuSO4·5H2O, copper acetate, copper triflate and copper acetylacetonate as catalysts. The copper catalysts were reduced in situ by irradiation at wavelengths of 366–546 nm, without using any additional reducing agent. Bromopropionitrile was used as an initiator. The effects of various solvents and the concentration and structure of ligands were investigated. Well-defined polymers were obtained when at least 100 or 200 ppm of any catalyst complexed with excess tris(2-pyridylmethylamine as a ligand was used in dimethyl sulfoxide as a solvent.

  13. Selective catalytic reduction system and process using a pre-sulfated zirconia binder

    Science.gov (United States)

    Sobolevskiy, Anatoly; Rossin, Joseph A.

    2010-06-29

    A selective catalytic reduction (SCR) process with a palladium catalyst for reducing NOx in a gas, using hydrogen as a reducing agent is provided. The process comprises contacting the gas stream with a catalyst system, the catalyst system comprising (ZrO.sub.2)SO.sub.4, palladium, and a pre-sulfated zirconia binder. The inclusion of a pre-sulfated zirconia binder substantially increases the durability of a Pd-based SCR catalyst system. A system for implementing the disclosed process is further provided.

  14. Effect of the sol-gel conditions on the morphology and SCR performance of electrospun V-W-TiO2 catalysts

    DEFF Research Database (Denmark)

    Marani, Debora; Silva, Rafael Hubert; Dankeaw, Apiwat

    2018-01-01

    V-W-TiO2 catalysts are prepared as nanofibers for the removal of the NOx in exhausts via the NH3 Selective Catalytic Reduction (SCR) method. By combining electrospinning and soft chemistry, materials are processed as nanofibers with the catalytic components (e. g. V2O5-WO3) incorporated as dopant...

  15. Remarkably enhanced density and specific activity of active sites in Al-rich Cu-, Fe- and Co-beta zeolites for selective catalytic reduction of NOx

    Czech Academy of Sciences Publication Activity Database

    Sazama, Petr; Pilař, Radim; Mokrzycki, Lukasz; Vondrová, Alena; Kaucký, Dalibor; Plšek, Jan; Sklenák, Štěpán; Šťastný, Petr; Klein, Petr

    2016-01-01

    Roč. 189, JUL 2016 (2016), s. 65-74 ISSN 0926-3373 R&D Projects: GA TA ČR(CZ) TH01021259 Institutional support: RVO:61388955 Keywords : SCR-NOx * Al-rich beta zeolite (*BEA) * Cobalt Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 9.446, year: 2016

  16. High-performance bimetallic alloy catalyst using Ni and N co-doped composite carbon for the oxygen electro-reduction.

    Science.gov (United States)

    Jung, Won Suk

    2018-03-15

    In this study, a novel synthesis method for the bimetallic alloy catalyst is reported, which is subsequently used as an oxygen reduction catalyst in polymer electrolyte membrane fuel cells (PEMFCs). The support prepared from the Ni-chelate complex shows a mesoporous structure with a specific surface area of ca. 400 m 2  g -1 indicating the suitable support for PEMFC applications. Ethylenediamine is converted to the nitrogen and carbon layers to protect the Ni particles which will diffuse into the Pt lattice at 800 °C. The PtNi/NCC catalyst with PtNi cores and Pt-rich shells is successfully formed when acid-treated as evidenced by line scan profiles. The catalyst particles thus synthesized are well-dispersed on the N-doped carbon support, while the average particle size is ca. 3 nm. In the PEMFC test, the maximum power density of the PtNi/NCC catalyst shows approximately 25% higher than that of the commercial Pt/C catalyst. The mass activity of the PtNi/NCC catalyst showed approximately 3-fold higher than that of the commercial Pt/C catalyst. The mass activity strongly depends on the ratio of Pt to Ni since the strain effect can be strong for catalysts due to the mismatch of lattice parameters of the Ni and Pt. Copyright © 2017 Elsevier Inc. All rights reserved.

  17. N, S co-doped carbon spheres with highly dispersed CoO as non-precious metal catalyst for oxygen reduction reaction

    Science.gov (United States)

    Chen, Linlin; Guo, Xingpeng; Zhang, Guoan

    2017-08-01

    It is still a great challenge in preparing non-precious metal catalysts with high activity and long-term stability to substitute for precious metal catalysts for oxygen reduction reaction (ORR) in fuel cells. Herein, we report a novel and facile catalyst-N, S co-doped carbon spheres with highly dispersed CoO (CoO@NS-CSs), where biomass glucose spheres act as carbon precursor and H2S, NH3 derived from the decomposition of thiourea not only provide N, S sources but also can etch carbon spheres to produce nanoporous structure. CoO@NS-CSs catalyst exhibits excellent ORR activity with a high onset potential of 0.946 V vs. RHE (reversible hydrogen electrode) and a half-wave potential of 0.821 V vs. RHE through a four-electron pathway in alkaline solution, which is comparable to commercial Pt/C catalyst (onset potential: 0.926 V vs. RHE, half-wave potential: 0.827 V vs. RHE). Furthermore, both the long-term stability and methanol-tolerance of CoO@NS-CSs catalyst are superior to those of commercial Pt/C catalyst. The excellent ORR performance of CoO@NS-CSs catalyst can be attributed to its micro-mesopore structure, high specific surface area (667 m2 g-1), and highly dispersed CoO. This work manifests that the obtained CoO@NS-CSs catalyst is promising to be applied to fuel cells.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  19. Selective Reduction of CO2 to CH4 by Tandem Hydrosilylation with Mixed Al/B Catalysts

    KAUST Repository

    Chen, Jiawei

    2016-04-04

    This contribution reports the first example of highly selective reduction of CO2 into CH4 via tandem hydrosilylation with mixed main-group organo-Lewis acid (LA) catalysts [Al(C6F5)3 + B(C6F5)3] {[Al] + [B]}. As shown by this comprehensive experimental and computational study, in this unique tandem catalytic process, [Al] effectively mediates the first step of the overall reduction cycle, namely the fixation of CO2 into HCOOSiEt3 (1) via the LA-mediated C=O activation, while [B] is incapable of promoting the same transformation. On the other hand, [B] is shown to be an excellent catalyst for the subsequent reduction steps 2–4, namely the hydrosilylation of the more basic intermediates [1 to H2C(OSiEt3)2 (2) to H3COSiEt3 (3) and finally to CH4] through the frustrated-Lewis-pair (FLP)-type Si–H activation. Hence, with the required combination of [Al] and [B], a highly selective hydrosilylative reduction of CO2 system has been developed, achieving high CH4 production yield up to 94%. The remarkably different catalytic behaviors between [Al] and [B] are attributed to the higher overall Lewis acidity of [Al] derived from two conflicting factors (electronic and steric effects), which renders the higher tendency of [Al] to form stable [Al]–substrate (intermediate) adducts with CO2 as well as subsequent intermediates 1, 2 and 3. Overall, the roles of [Al] and [B] are not only complementary but also synergistic in the total reduction of CO2, which render both [Al]-mediated first reduction step and [B]-mediated subsequent steps catalytic.

  20. Selective Reduction of CO2 to CH4 by Tandem Hydrosilylation with Mixed Al/B Catalysts

    KAUST Repository

    Chen, Jiawei; Falivene, Laura; Caporaso, Lucia; Cavallo, Luigi; Chen, Eugene Y.-X.

    2016-01-01

    This contribution reports the first example of highly selective reduction of CO2 into CH4 via tandem hydrosilylation with mixed main-group organo-Lewis acid (LA) catalysts [Al(C6F5)3 + B(C6F5)3] {[Al] + [B]}. As shown by this comprehensive experimental and computational study, in this unique tandem catalytic process, [Al] effectively mediates the first step of the overall reduction cycle, namely the fixation of CO2 into HCOOSiEt3 (1) via the LA-mediated C=O activation, while [B] is incapable of promoting the same transformation. On the other hand, [B] is shown to be an excellent catalyst for the subsequent reduction steps 2–4, namely the hydrosilylation of the more basic intermediates [1 to H2C(OSiEt3)2 (2) to H3COSiEt3 (3) and finally to CH4] through the frustrated-Lewis-pair (FLP)-type Si–H activation. Hence, with the required combination of [Al] and [B], a highly selective hydrosilylative reduction of CO2 system has been developed, achieving high CH4 production yield up to 94%. The remarkably different catalytic behaviors between [Al] and [B] are attributed to the higher overall Lewis acidity of [Al] derived from two conflicting factors (electronic and steric effects), which renders the higher tendency of [Al] to form stable [Al]–substrate (intermediate) adducts with CO2 as well as subsequent intermediates 1, 2 and 3. Overall, the roles of [Al] and [B] are not only complementary but also synergistic in the total reduction of CO2, which render both [Al]-mediated first reduction step and [B]-mediated subsequent steps catalytic.

  1. Silver/iron oxide/graphitic carbon composites as bacteriostatic catalysts for enhancing oxygen reduction in microbial fuel cells

    Science.gov (United States)

    Ma, Ming; You, Shijie; Gong, Xiaobo; Dai, Ying; Zou, Jinlong; Fu, Honggang

    2015-06-01

    Biofilms from anode heterotrophic bacteria are inevitably formed over cathodic catalytic sites, limiting the performances of single-chamber microbial fuel cells (MFCs). Graphitic carbon (GC) - based nano silver/iron oxide (AgNPs/Fe3O4/GC) composites are prepared from waste pomelo skin and used as antibacterial oxygen reduction catalysts for MFCs. AgNPs and Fe3O4 are introduced in situ into the composites by one-step carbothermal reduction, enhancing their conductivity and catalytic activity. To investigate the effects of Fe species on the antibacterial and catalytic properties, AgNPs/Fe3O4/GC is washed with sulfuric acid (1 mol L-1) for 0.5 h, 1 h, and 5 h and marked as AgNPs/Fe3O4/GC-x (x = 0.5 h, 1 h and 5 h, respectively). A maximum power density of 1712 ± 35 mW m-2 is obtained by AgNPs/Fe3O4/GC-1 h, which declines by 4.12% after 17 cycles. Under catalysis of all AgNP-containing catalysts, oxygen reduction reaction (ORR) proceeds via the 4e- pathway, and no toxic effects to anode microorganisms result from inhibiting the cathodic biofilm overgrowth. With the exception of AgNPs/Fe3O4/GC-5 h, the AgNPs-containing composites exhibit remarkable power output and coulombic efficiency through lowering proton transfer resistance and air-cathode biofouling. This study provides a perspective for the practical application of MFCs using these efficient antibacterial ORR catalysts.

  2. Critical appraisal on the role of catalysts for the oxygen reduction reaction in lithium-oxygen batteries

    International Nuclear Information System (INIS)

    Lodge, Andrew W.; Lacey, Matthew J.; Fitt, Matthew; Garcia-Araez, Nuria; Owen, John R.

    2014-01-01

    This work reports a detailed characterization of the reduction of oxygen in pyrrolidinium-based ionic liquids for application to lithium-oxygen batteries. It is found that, in the absence of Li + , all electron transfer kinetics are fast, and therefore, the reactions are limited by the mass transport rate. Reversible reduction of O 2 to O 2 • − and O 2 • − to O 2 2− take place at E 0 = 2.1 V and 0.8 V vs. Li + /Li, respectively. In the presence of Li + , O 2 is reduced to LiO 2 first and then to Li 2 O 2 . The solubility product constant of Li 2 O 2 is found to be around 10 −51 , corroborating the hypothesis that electrode passivation by Li 2 O 2 deposition is an important issue that limits the capacity delivered by lithium-oxygen batteries. Enhancing the rate of Li 2 O 2 formation by using different electrode materials would probably lead to faster electrode passivation and hence smaller charge due to oxygen reduction (smaller capacity of the battery). On the contrary, soluble redox catalysts can not only increase the reaction rate of Li 2 O 2 formation but also avoid electrode passivation since the fast diffusion of the soluble redox catalyst would displace the formation of Li 2 O 2 at a sufficient distance from the electrode surface

  3. Pt/Cr and Pt/Ni catalysts for oxygen reduction reaction: to alloy or not to alloy?

    Science.gov (United States)

    Escaño, Mary Clare; Gyenge, Elod; Nakanishi, Hiroshi; Kasai, Hideaki

    2011-04-01

    Bimetallic systems such as Pt-based alloys or non-alloys have exhibited interesting catalytic properties but pose a major challenge of not knowing a priori how the electronic and chemical properties will be modified relative to the parent metals. In this work, we present the origin of the changes in the reactivity of Pt/Cr and Pt/Ni catalysts, which have been of wide interest in fuel cell research. Using spin-polarized density functional theory calculations, we have shown that the modification of Pt surface reactivity in Pt/Ni is purely of geometric origin (strain). We have also found that the Pt-Ni bonding is very weak, which explains the observed instability of Pt-Ni catalysts under electrochemical measurements. On the other hand, Pt/Cr systems are governed by strong ligand effect (metal-metal interaction), which explains the experimentally observed reactivity dependence on the relative composition of the alloying components. The general characteristics of the potential energy curves for O2 dissociative adsorption on the bimetallic systems and the pure Pt clarify why the d-band center still works for Pt/Cr despite the strong Pt-Cr bonding and high spin polarization of Pt d-states. On the basis of the above clarifications, viable Pt-Cr and Pt-Ni structures, which involve nano-sized alloys and non-alloy bulk catalyst, which may strike higher than the currently observed oxidation reduction reaction activity are proposed.

  4. One step bioconversion of waste precious metals into Serratia biofilm-immobilized catalyst for Cr(VI) reduction.

    Science.gov (United States)

    Yong, P; Liu, W; Zhang, Z; Beauregard, D; Johns, M L; Macaskie, L E

    2015-11-01

    For reduction of Cr(VI) the Pd-catalyst is excellent but costly. The objectives were to prove the robustness of a Serratia biofilm as a support for biogenic Pd-nanoparticles and to fabricate effective catalyst from precious metal waste. Nanoparticles (NPs) of palladium were immobilized on polyurethane reticulated foam and polypropylene supports via adhesive biofilm of a Serratia sp. The biofilm adhesion and cohesion strength were unaffected by palladization and catalytic biofilm integrity was also shown by magnetic resonance imaging. Biofilm-Pd and mixed precious metals on biofilm (biofilm-PM) reduced 5 mM Cr(VI) to Cr(III) when immobilized in a flow-through column reactor, at respective flow rates of 9 and 6 ml/h. The lower activity of the latter was attributed to fewer, larger, metal deposits on the bacteria. Activity was lost in each case at pH 7 but was restored by washing with 5 mM citrate solution or by exposure of columns to solution at pH 2, suggesting fouling by Cr(III) hydroxide product at neutral pH. A 'one pot' conversion of precious metal waste into new catalyst for waste decontamination was shown in a continuous flow system based on the use of Serratia biofilm to manufacture and support catalytic Pd-nanoparticles.

  5. Photocatalytic carbon dioxide reduction with rhodium-based catalysts in solution and heterogenized within metal-organic frameworks.

    Science.gov (United States)

    Chambers, Matthew B; Wang, Xia; Elgrishi, Noémie; Hendon, Christopher H; Walsh, Aron; Bonnefoy, Jonathan; Canivet, Jérôme; Quadrelli, Elsje Alessandra; Farrusseng, David; Mellot-Draznieks, Caroline; Fontecave, Marc

    2015-02-01

    The first photosensitization of a rhodium-based catalytic system for CO2 reduction is reported, with formate as the sole carbon-containing product. Formate has wide industrial applications and is seen as valuable within fuel cell technologies as well as an interesting H2 -storage compound. Heterogenization of molecular rhodium catalysts is accomplished via the synthesis, post-synthetic linker exchange, and characterization of a new metal-organic framework (MOF) Cp*Rh@UiO-67. While the catalytic activities of the homogeneous and heterogeneous systems are found to be comparable, the MOF-based system is more stable and selective. Furthermore it can be recycled without loss of activity. For formate production, an optimal catalyst loading of ∼10 % molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H2 . There is no precedent for a MOF catalyzing the latter reaction so far. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  6. Macrodynamic study and catalytic reduction of NO by ammonia under mild conditions over Pt-La-Ce-O/Al2O3 catalysts

    International Nuclear Information System (INIS)

    Wang, Yanhui; Zhu, Jingli; Ma, Runyu

    2007-01-01

    Catalytic reduction of NO using ammonia upon series prepared catalysts under 423-573 K in a fixed bed reactor was investigated. Results showed that the performance of supported platinum catalyst could be improved by addition of La and Ce to it. Experimental studies indicated that the suitable molar ratio of Pt:La:Ce would be 1.0:3.78:3.56, Pt-La-Ce (c). Results also found Pt-La-Ce (c) catalyst had good stability and tolerance to certain amounts of sulfur compounds under the used experimental conditions. Characterization for the fresh and used catalysts showed the Pt-La-Ce (c) catalyst had a stable structure. In addition, based on experimental data and using a nonlinear regression algorithm method, an empirical macrodynamic equation was obtained in this study

  7. Spillover effect induced Pt-TiO2/C as ethanol tolerant oxygen reduction reaction catalyst for direct ethanol fuel cells

    International Nuclear Information System (INIS)

    Meenakshi, S.; Nishanth, K.G.; Sridhar, P.; Pitchumani, S.

    2014-01-01

    Hypo-hyper-d-electronic interactive nature is used to develop a new carbon supported HT-Pt-TiO 2 composite catalyst comprising Pt and Ti in varying atomic ratio, namely 1:1, 2:1 and 3:1. The electro-catalysts are characterized by XRD, TEM, SEM-EDAX, Cyclic Voltammetry (CV) and Linear sweep voltammetry (LSV) techniques. HT-Pt-TiO 2 /C catalysts exhibit significant improvement in oxygen reduction reaction (ORR) over Pt/C. The effect of composition towards ORR with and without ethanol has been studied. The direct ethanol fuel cell (DEFC) with HT-Pt-TiO 2 /C cathode catalyst exhibits an enhanced peak power density of 41 mW cm −2 , whereas 21 mW cm −2 is obtained for the DEFCs with carbon-supported Pt catalyst operating under identical conditions

  8. Steam Reforming of Ethylene Glycol over Ni/Al2O3 Catalysts: Effect of the Preparation Method and Reduction Temperature

    International Nuclear Information System (INIS)

    Choi, Dong Hyuck; Park, Jung Eun; Park, Eun Duck

    2015-01-01

    The effect of preparation method on the catalytic activities of the Ni/Al 2 O 3 catalysts on steam reforming of ethylene glycol was investigated. The catalysts were prepared with various preparation methods such as an incipient wetness impregnation, wet impregnation, and coprecipitation method. In the case of coprecipitation method, various precipitants such as KOH, K 2 CO 3 , and NH 4 OH were compared. The prepared catalysts were characterized by using N 2 physisorption, inductively coupled plasma-atomic emission spectroscopy, X-ray diffraction, temperature programmed reduction, pulsed H 2 chemisorption, temperature-programmed oxidation, scanning electron microscopy, and thermogravimetric analysis. Among the catalysts reduced at 773 K, the Ni/Al 2 O 3 catalyst prepared by a coprecipitation with KOH or K 2 CO 3 as precipitants showed the best catalytic performance. The preparation method affected the particle size of Ni, reducibility of nickel oxides, catalytic performance (activity and stability), and types of coke formed during the reaction. The Ni/Al 2 O 3 catalyst prepared by a coprecipitation with KOH showed the increasing catalytic activity with an increase in the reduction temperature from 773 to 1173 K because of an increase in the reduction degree of Ni oxide species even though the particle size of Ni increased with increasing reduction temperature

  9. An Investigation of Palladium Oxygen Reduction Catalysts for the Direct Methanol Fuel Cell

    Directory of Open Access Journals (Sweden)

    G. F. Álvarez

    2011-01-01

    Full Text Available A comparative study of Pd and Pt was carried out in DMFC using different methanol concentrations and under different operating conditions. Cell performance was compared at methanol concentrations of 1, 3, 5, and 7 M and at temperatures of 20, 40, and 60°C. Homemade Pd nanoparticles were prepared on Vulcan XC-72R using ethylene glycol as the reducing agent at pH 11. The resulting catalyst, Pd/C, with metal nanoparticles of approximately 6 nm diameter, was tested as a cathode catalyst in DMFC. At methanol concentrations of 5 M and higher, the Pd cathode-based cell performed better than that with Pt at 60°C with air.

  10. AN EXPERIMENTAL NOX REDUCTION POTENTIAL INVESTIGATION OF THE PARTIAL HCCI APPLICATION, ON A HIGH PRESSURE FUEL INJECTION EQUIPPED DIESEL ENGINE BY IMPLEMENTING FUMIGATION OF GASOLINE PORT INJECTION

    OpenAIRE

    ERGENÇ, Alp Tekin; YÜKSEK, Levent; ÖZENER, Orkun; IŞIN, Övün

    2016-01-01

    This work investigates the effects of partial HCCI (Homogeneous charge compression ignition) application on today's modern diesel engine tail pipe NOx emissions. Gasoline fumigation is supplied via a port fuel injection system located in the intake port of DI(Direct injection) diesel engine to maintain partial HCCI conditions and also diesel fuel injected directly into the combustion chamber before TDC(Top dead center). A single cylinder direct injection diesel research engine equipped w...

  11. Enhanced hydrothermal stability of Cu-ZSM-5 catalyst via surface modification in the selective catalytic reduction of NO with NH_3

    International Nuclear Information System (INIS)

    Zhang, Tao; Shi, Juan; Liu, Jian; Wang, Daxi; Zhao, Zhen; Cheng, Kai; Li, Jianmei

    2016-01-01

    Highlights: • The hydrothermal stability of Cu-ZSM-5 catalyst was enhanced after surface modification. • An inert silica layer was deposited on the surface of Cu-ZSM-5 and formed a protective layer. • The contact between Si and Cu and Al atoms could form Si-O-Al and Si- O−Cu bonds. • The redox and acidity properties of Cu-ZSM-5-CLD-Aged catalyst were largely retained. • The adsorption and activation of NO and NH_3 was almost unchanged over Cu-ZSM-5-CLD catalyst before and after hydrothermal treatment. - Abstract: The surface of Cu-ZSM-5 catalyst was modified by chemical liquid deposition (CLD) of tetraethoxysilane (TEOS) for enhancing its hydrothermal stability in the selective catalytic reduction of NO with NH_3. After hydrothermal aging at 750 °C for 13 h, the catalytic performance of Cu-ZSM-5-Aged catalyst was significantly reduced for NO reduction in the entire temperature range, while that of Cu-ZSM-5-CLD-Aged catalyst was affected very little. The characterization results indicated that an inert silica layer was deposited on the surface of Cu-ZSM-5 and formed a protective layer, which prevents the detachment of Cu"2"+ from ZSM-5 ion-exchange positions and the dealumination of zeolite during the hydrothermal aging process. Based on the data it is hypothesized to be the primary reason for the high hydrothermal stability of Cu-ZSM-5-CLD catalyst.

  12. Nb-doped TiO2 cathode catalysts for oxygen reduction reaction of polymer electrolyte fuel cells

    KAUST Repository

    Arashi, Takuya

    2014-09-01

    Nb-doped TiO2 particles were studied as electrocatalysts for the oxygen reduction reaction (ORR) under acidic conditions. The Nb-doped TiN nanoparticles were first synthesized by meso-porous C3N4 and then fully oxidized to Nb-doped TiO2 by immersing in 0.1 M H 2SO4 at 353 K for 24 h. Although the ORR activity of the as-obtained sample was low, a H2 treatment at relatively high temperature (1173 K) dramatically improved the ORR performance. An onset potential as high as 0.82 VRHE was measured. No degradation of the catalysts was observed during the oxidation-reduction cycles under the ORR condition for over 127 h. H2 treatment at temperatures above 1173 K caused the formation of a Ti4O7 phase, resulting in a decrease in ORR current. Elemental analysis indicated that the Nb-doped TiO 2 contained 25 wt% residual carbon. Calcination in air at 673 or 973 K eliminated the residual carbon in the catalyst, which was accompanied by a dramatic decrease in ORR activity. This post-calcination process may reduce the conductivity of the sample by filling the oxygen vacancies, and the carbon residue in the particle aggregates may enhance the electrocatalytic activity for ORR. The feasibility of using conductive oxide materials as electrocatalysts is discussed. © 2013 Elsevier B.V.

  13. Novel RuCoSe as non-platinum catalysts for oxygen reduction reaction in microbial fuel cells

    Science.gov (United States)

    Rozenfeld, Shmuel; Schechter, Michal; Teller, Hanan; Cahan, Rivka; Schechter, Alex

    2017-09-01

    Microbial electrochemical cells (MECs) are explored for the conversion of acetate directly to electrical energy. This device utilizes a Geobacter sulfurreducens anode and a novel RuCoSe air cathode. RuCoSe synthesized in selected compositions by a borohydride reduction method produces amorphous structures of powdered agglomerates. Oxygen reduction reaction (ORR) was measured in a phosphate buffer solution pH 7 using a rotating disc electrode (RDE), from which the kinetic current (ik) was measured as a function of potential and composition. The results show that ik of RuxCoySe catalysts increases in the range of XRu = 0.25 > x > 0.7 and y < 0.15 for all tested potentials. A poisoning study of RuCoSe and Pt catalysts in a high concentration acetate solution shows improved tolerance of RuCoSe to this fuel at acetate concentration ≥500 mM. MEC discharge plots under physiological conditions show that ∼ RuCo2Se (sample S3) has a peak power density of 750 mW cm-2 which is comparable with Pt 900 mW cm-2.

  14. Nb-doped TiO2 cathode catalysts for oxygen reduction reaction of polymer electrolyte fuel cells

    KAUST Repository

    Arashi, Takuya; Seo, Jeongsuk; Takanabe, Kazuhiro; Kubota, Jun; Domen, Kazunari

    2014-01-01

    Nb-doped TiO2 particles were studied as electrocatalysts for the oxygen reduction reaction (ORR) under acidic conditions. The Nb-doped TiN nanoparticles were first synthesized by meso-porous C3N4 and then fully oxidized to Nb-doped TiO2 by immersing in 0.1 M H 2SO4 at 353 K for 24 h. Although the ORR activity of the as-obtained sample was low, a H2 treatment at relatively high temperature (1173 K) dramatically improved the ORR performance. An onset potential as high as 0.82 VRHE was measured. No degradation of the catalysts was observed during the oxidation-reduction cycles under the ORR condition for over 127 h. H2 treatment at temperatures above 1173 K caused the formation of a Ti4O7 phase, resulting in a decrease in ORR current. Elemental analysis indicated that the Nb-doped TiO 2 contained 25 wt% residual carbon. Calcination in air at 673 or 973 K eliminated the residual carbon in the catalyst, which was accompanied by a dramatic decrease in ORR activity. This post-calcination process may reduce the conductivity of the sample by filling the oxygen vacancies, and the carbon residue in the particle aggregates may enhance the electrocatalytic activity for ORR. The feasibility of using conductive oxide materials as electrocatalysts is discussed. © 2013 Elsevier B.V.

  15. FeRu/TiO2 and Fe/TiO2 catalysts after reduction and Fischer-Tropsch synthesis studied by Moessbauer spectroscopy

    International Nuclear Information System (INIS)

    Kraan, A.M. van der; Nonnekens, R.C.H.; Niemantsverdriet, J.W.

    1986-01-01

    A series of TiO 2 -supported bimetallic FeRu catalysts with different Fe:Ru ratios (infinity; 10:1; 3:1; 1:1; 1:3) has been studied by means of in situ Moessbauer spectroscopy. The influence of reduction and Fischer-Tropsch synthesis on the state of iron in the FeRu/TiO 2 catalysts is derived. (Auth.)

  16. The effect of soot on ammonium nitrate species and NO2 selective catalytic reduction over Cu-zeolite catalyst-coated particulate filter.

    Science.gov (United States)

    Mihai, Oana; Tamm, Stefanie; Stenfeldt, Marie; Olsson, Louise

    2016-02-28

    A selective catalytic reduction (SCR)-coated particulate filter was evaluated by means of dynamic tests performed using NH3, NO2, O2 and H2O. The reactions were examined both prior to and after soot removal in order to study the effect of soot on ammonium nitrate formation and decomposition, ammonia storage and NO2 SCR. A slightly larger ammonia storage capacity was observed when soot was present in the sample, which indicated that small amounts of ammonia can adsorb on the soot. Feeding of NO2 and NH3 in the presence of O2 and H2O at low temperature (150, 175 and 200°C) leads to a large formation of ammonium nitrate species and during the subsequent temperature ramp using H2O and argon, a production of nitrous oxides was observed. The N2O formation is often related to ammonium nitrate decomposition, and our results showed that the N2O formation was clearly decreased by the presence of soot. We therefore propose that in the presence of soot, there are fewer ammonium nitrate species on the surface due to the interactions with the soot. Indeed, we do observe CO2 production during the reaction conditions also at 150°C, which shows that there is a reaction with these species and soot. In addition, the conversion of NOx due to NO2 SCR was significantly enhanced in the presence of soot; we attribute this to the smaller amount of ammonium nitrate species present in the experiments where soot is available since it is well known that ammonium nitrate formation is a major problem at low temperature due to the blocking of the catalytic sites. Further, a scanning electron microscopy analysis of the soot particles shows that they are about 30-40 nm and are therefore too large to enter the pores of the zeolites. There are likely CuxOy or other copper species available on the outside of the zeolite crystallites, which could have been enhanced due to the hydrothermal treatment at 850°C of the SCR-coated filter prior to the soot loading. We therefore propose that soot is

  17. Hydrogen energy share improvement along with NOx (oxides of nitrogen) emission reduction in a hydrogen dual-fuel compression ignition engine using water injection

    International Nuclear Information System (INIS)

    Chintala, V.; Subramanian, K.A.

    2014-01-01

    Highlights: • H 2 energy share increased from 20% without water to 39% with SWC 270 g/kWh. • Specific water consumption (SWC) 200 g/kWh was selected as the optimum quantity. • NO x decreased about 24% with the optimum water quantity at 20% H 2 energy share. • At 20% H 2 share, energy efficiency decreased about 5.5% with the optimum water. • HC, CO and smoke emissions increased 38%, 100% and 69% with optimum water at 20% H 2 share. - Abstract: The study aims at enhancement of Hydrogen (H 2 ) energy share and reduction of Oxides of Nitrogen (NO x ) emission in a 7.4 kW-CI engine at 1500 rpm using water injection. The test engine was modified to run under dual-fuel operation with diesel–biodiesel blend (B20) and H 2 fuels for different Specific Water Consumption (SWC) of 130, 200, and 270 g/kWh. Under conventional H 2 dual-fuel mode, energy efficiency and NO x emission increased significantly while Hydrocarbon (HC), Carbon Monoxide (CO) and smoke emissions decreased. The maximum H 2 energy share increased from 20% without water to 32%, 36%, and 39% with SWC of 130, 200, and 270 g/kWh respectively. However, SWC of 200 g/kWh was selected as an optimum water quantity for knock free operation, better performance and lower emissions. At the optimum SWC with 20% H 2 energy share, the NO x emission and energy efficiency decreased about 24% and 5.7%, while HC and smoke emissions increased about 38% and 69%. At 20% H 2 energy share, the CO emission increased from 0.0 g/kWh without water to 1.2 g/kWh with the optimum SWC. However, reduction of these HC and CO emissions using oxidation catalysts needs to be studied further. A new methodology for determining heat release rate with consideration of crevice gas was proposed in the study

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

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    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.

  19. Selective hydrodechlorination of 1,2-dichloroethane to ethylene over Pd-Ag/Al_2O_3 catalysts prepared by surface reduction

    International Nuclear Information System (INIS)

    Han, Yuxiang; Gu, Guangfeng; Sun, Jingya; Wang, Wenjuan; Wan, Haiqin; Xu, Zhaoyi; Zheng, Shourong

    2015-01-01

    Graphical abstract: - Highlights: • Surface reduction method was used for preparation of Pd-Ag(Cu) bimetallic catalysts. • Hydrodechlorination of 1,2-dichloroethane was investigated for production of ethylene. • Ag(Cu) selectively deposited on Pd surface during surface reduction process. • Ethylene selectivity was enhanced over Pd-Ag(Cu)/Al_2O_3 catalyst prepared by surface reduction. • Isolated Pd site is the key species for ethylene selectivity. - Abstract: Alumina supported Pd-Ag and (Cu) bimetallic catalysts (denoted as sr-Pd-Ag/Al_2O_3 or sr-Pd-Cu/Al_2O_3) with varied Pd/Ag (or Cu) ratios were prepared using the surface reduction method, and the gas-phase catalytic hydrodechlorination of 1,2-dichloroethane over the catalysts were investigated. For comparison, Pd-Ag bimetallic catalysts were prepared by the conventional co-impregnation method (denoted as im-Pd-Ag/Al_2O_3). The catalysts were characterized by N_2 adsorption, X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and CO chemisorption. Characterization results indicated that surface reduction led to selective deposition of metallic Ag on the surface of Pd particles, while Pd and Ag just disorderly mixed in the catalyst prepared by impregnation method. Therefore, sr-Pd-Ag/Al_2O_3 exhibited a higher ethylene selectivity than im-Pd-Ag/Al_2O_3 for hydrodechlorination of 1,2-dichloroethane at a similar Ag loading amount. Moreover, among sr-Pd-Ag/Al_2O_3, sr-Pd-Cu/Al_2O_3 and im-Pd-Ag/Al_2O_3 catalysts, the ethylene selectivity decreased over these catalysts following the order: sr-Pd-Ag/Al_2O_3 > sr-Pd-Cu/Al_2O_3 > im-Pd-Ag/Al_2O_3. The present results indicate that surface reduction can be used as a potential method to synthesize catalyst with enhanced ethylene selectivity in hydrodechlorination of 1,2-dichloroethane.

  20. Graphitic Layer Encapsulated Iron Based Non‐precious Catalysts for the Oxygen Reduction Reaction

    DEFF Research Database (Denmark)

    Zhong, Lijie

    consisting of uniform metallic nanoparticles encapsulated in graphitic layers. The thesis work is conducted aiming at three major objectives: further optimization of the pyrolysis to achieve improved performance of catalysts, investigation of the complex Fe-containing components, and exploration...... of the nitrogen functionalities. Two anions in the electrolyte are used to probe the iron containing active sites towards the ORR, cyanide (CN-) in alkaline and thiocyanate (SCN-) in acidic medium, which seem supporting the above conclusions. These findings provide new insights to the encapsulation structure...

  1. Constitutive NADPH-dependent electron transferase activity of the Nox4 dehydrogenase domain.

    Science.gov (United States)

    Nisimoto, Yukio; Jackson, Heather M; Ogawa, Hisamitsu; Kawahara, Tsukasa; Lambeth, J David

    2010-03-23

    NADPH oxidase 4 (Nox4) is constitutively active, while Nox2 requires the cytosolic regulatory subunits p47(phox) and p67(phox) and activated Rac with activation by phorbol 12-myristate 13-acetate (PMA). This study was undertaken to identify the domain on Nox4 that confers constitutive activity. Lysates from Nox4-expressing cells exhibited constitutive NADPH- but not NADH-dependent hydrogen peroxide production with a K(m) for NADPH of 55 +/- 10 microM. The concentration of Nox4 in cell lysates was estimated using Western blotting and allowed calculation of a turnover of approximately 200 mol of H(2)O(2) min(-1) (mol of Nox4)(-1). A chimeric protein (Nox2/4) consisting of the Nox2 transmembrane (TM) domain and the Nox4 dehydrogenase (DH) domain showed H(2)O(2) production in the absence of cytosolic regulatory subunits. In contrast, chimera Nox4/2, consisting of the Nox4 TM and Nox2 DH domains, exhibited PMA-dependent activation that required coexpression of regulatory subunits. Nox DH domains from several Nox isoforms were purified and evaluated for their electron transferase activities. Nox1 DH, Nox2 DH, and Nox5 DH domains exhibited barely detectable activities toward artificial electron acceptors, while the Nox4 DH domain exhibited significant rates of reduction of cytochrome c (160 min(-1), largely superoxide dismutase-independent), ferricyanide (470 min(-1)), and other electron acceptors (artificial dyes and cytochrome b(5)). Rates were similar to those observed for H(2)O(2) production by the Nox4 holoenzyme in cell lysates. The activity required added FAD and was seen with NADPH but not NADH. These results indicate that the Nox4 DH domain exists in an intrinsically activated state and that electron transfer from NADPH to FAD is likely to be rate-limiting in the NADPH-dependent reduction of oxygen by holo-Nox4.

  2. Catalytic reduction of NO{sub x} in gasoline engine exhaust over copper- and nickel-exchanged X-zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Bhattacharyya, S. [Indian Inst. of Technology, Kharagpur (India). Dept. of Mechanical Engineering; Das, R.K. [Indian School of Mines, Dhanbad (India). Dept. of Engineering and Mining Machinery

    2001-10-11

    Catalytic removal of NO{sub x} in engine exhaust gases can be accomplished by non-selective reduction, selective reduction and decomposition. Noble metals are extensively used for non-selective reduction of NO{sub x} and up to 90% of engine NO{sub x} emissions can be reduced in a stoichiometric exhaust. This requirement of having the stoichiometric fuel-air ratio acts against efficiency improvement of engines. Selective NO{sub x} reduction in the presence of different reductants such as, NH{sub 3}, urea or hydrocarbons, requires close control of the amount of reductant being injected which otherwise may be emitted as a pollutant. Catalytic decomposition is the best option for NO{sub x} removal. Nevertheless, catalysts which are durable, economic and active for NO{sub x} reduction at normal engine exhaust temperature ranges are still being investigated. Three catalysts based on X-zeolite have been developed by exchanging the Na+ ion with copper, nickel and copper-nickel metal ions and applied to the exhaust of a stationary gasoline engine to explore their potential for catalytic reduction of NO{sub x} under a wide range of engine and exhaust conditions. Some encouraging results have been obtained. The catalyst Cu-X exhibits much better NO{sub x} reduction performance at any temperature in comparison to Cu-Ni-X and Ni-X; while Cu-Ni-X catalyst exhibits slightly better performance than Ni-X catalyst. Maximum NO{sub x} efficiency achieved with Cu-X catalyst is 59.2% at a space velocity (sv) of 31 000 h{sup -1}; while for Cu-Ni-X and Ni-X catalysts the equivalent numbers are 60.4% and 56% respectively at a sv of 22 000 h{sup -1}. Unlike noble metals, the doped X-zeolite catalysts exhibit significant NO{sub x} reduction capability for a wide range of air/fuel ratio and with a slower rate of decline as well with increase in air/fuel ratio. (author)

  3. Reduction of Furfural to Furfuryl Alcohol in Liquid Phase over a Biochar-Supported Platinum Catalyst

    Directory of Open Access Journals (Sweden)

    Ariadna Fuente-Hernández

    2017-02-01

    Full Text Available In this work, the liquid phase hydrogenation of furfural has been studied using a biochar-supported platinum catalyst in a batch reactor. Reactions were performed between 170 °C and 320 °C, using 3 wt % and 5 wt % of Pt supported on a maple-based biochar under hydrogen pressure varying from 500 psi to 1500 psi for reaction times between 1 h and 6 h in various solvents. Under all reactive conditions, furfural conversion was significant, whilst under specific conditions furfuryl alcohol (FA was obtained in most cases as the main product showing a selectivity around 80%. Other products as methylfuran (MF, furan, and trace of tetrahydrofuran (THF were detected. Results showed that the most efficient reaction conditions involved a 3% Pt load on biochar and operations for 2 h at 210 °C and 1500 psi using toluene as solvent. When used repetitively, the catalyst showed deactivation although only a slight variation in selectivity toward FA at the optimal experimental conditions was observed.

  4. Selective Catalytic Reduction of NO with NH3 Over V-MCM-41 Catalyst.

    Science.gov (United States)

    Kwon, Woo Hyun; Park, Sung Hoon; Kim, Ji Man; Park, Su Bin; Jung, Sang-Chul; Kim, Sang Chai; Jeon, Jong-Ki; Park, Young-Kwon

    2016-02-01

    V-MCM-41, a mesoporous catalyst doped with V2O5, was applied for the first time to the removal of atmospheric NO. The quantity of V2O5 added was 10 wt% and 30 wt%. The characteristics of the synthesized catalysts were examined using XRD, N2 soprtion, and NH3-TPD. With increasing quantity of V2O5 added, specific surface area decreased and pore size increased. When the quantity of V2O5 was 10 wt%, the MCM-41 structure was retained, whereas considerable collapse of mesoporous structure was observed when 30 wt% V2O5 was added. The examination of acid characteristics using NH3-TPD showed that 30 wt% V-MCM-41 had the higher NH3 adsorption ability, implying that it would exhibit high activity for NH3 SCR reaction. In the NO removal experiments, 30 wt% V-MCM-41 showed much higher NO removal efficiency than 10 wt% V-MCM-41, which was attributed to its high NH3 adsorption ability.

  5. Catalytic activity of dual catalysts system based on nano-manganese oxide and cobalt octacyanophthalocyanine toward four-electron reduction of oxygen in alkaline media

    International Nuclear Information System (INIS)

    Zhang, Dun; Chi, Dahe; Okajima, Takeyoshi; Ohsaka, Takeo

    2007-01-01

    The electrocatalysis of the dual functional catalysts system composed of electrolytic nano-manganese oxide (nano-MnOx) and cobalt octacyanophthalocyanine (CoPcCN) toward 4-electron reduction of oxygen (O 2 ) in alkaline media was studied. Nano-MnOx electrodeposited on the CoPcCN monolayer-modified glassy carbon (GC) electrode was clarified as the nano-rods with ca. 10-20 nm diameter by scanning electron microscopy. The peak current for O 2 reduction at the dual catalysts-modified GC electrode increases largely and the peak potential shifts by ca. 160 mV to the positive direction in cyclic voltammograms compared with those obtained at the bare GC electrode. The Koutecky-Levich plots indicate that the O 2 reduction at the dual catalysts-modified GC electrode is an apparent 4-electron process. Collection efficiencies obtained at the dual catalysts-modified GC electrode are much lower than those at the GC electrode and are almost similar to those at the Pt nano-particles modified GC electrode. The obtained results demonstrate that the dual catalysts system possesses a bifuctional catalytic activity for redox-mediating 2-electron reduction of O 2 to HO 2 - by CoPcCN as well as catalyzing the disproportionation of HO 2 - to OH - and O 2 by nano-MnOx, and enables an apparent 4-electron reduction of O 2 at a relatively low overpotential in alkaline media. In addition, it has been found that the cleaning of the dual catalysts-modified electrode by soaking in 0.1 M sulfuric acid solution enhances its catalytic activity toward the reduction of O 2

  6. Hemoglobin-carbon nanotube derived noble-metal-free Fe5C2-based catalyst for highly efficient oxygen reduction reaction

    Science.gov (United States)

    Vij, Varun; Tiwari, Jitendra N.; Lee, Wang-Geun; Yoon, Taeseung; Kim, Kwang S.

    2016-02-01

    High performance non-precious cathodic catalysts for oxygen reduction reaction (ORR) are vital for the development of energy materials and devices. Here, we report an noble metal free, Fe5C2 nanoparticles-studded sp2 carbon supported mesoporous material (CNTHb-700) as cathodic catalyst for ORR, which was prepared by pyrolizing the hybrid adduct of single walled carbon nanotubes (CNT) and lyophilized hemoglobin (Hb) at 700 °C. The catalyst shows onset potentials of 0.92 V in 0.1 M HClO4 and in 0.1 M KOH which are as good as commercial Pt/C catalyst, giving very high current density of 6.34 and 6.69 mA cm-2 at 0.55 V vs. reversible hydrogen electrode (RHE), respectively. This catalyst has been confirmed to follow 4-electron mechanism for ORR and shows high electrochemical stability in both acidic and basic media. Catalyst CNTHb-700 possesses much higher tolerance towards methanol than the commercial Pt/C catalyst. Highly efficient catalytic properties of CNTHb-700 could lead to fundamental understanding of utilization of biomolecules in ORR and materialization of proton exchange membrane fuel cells for clean energy production.

  7. ALKALI RESISTANT CATALYST

    DEFF Research Database (Denmark)

    2008-01-01

    The present invention concerns the selective removal of nitrogen oxides (NOx) from gasses. In particular, the invention concerns a process, a catalyst and the use of a catalyst for the selective removal of nitrogen oxides in the presence of ammonia from gases containing a significant amount...... of alkali metal and/or alkali-earth compounds which process comprises using a catalyst combined of (i) a formed porous superacidic support, said superacidic support having an Hammett acidity stronger than Ho=-12, and (ii) a metal oxide catalytic component deposited on said superacidic support selected from...

  8. Solid State Electrochemical DeNOx

    DEFF Research Database (Denmark)

    Kammer Hansen, Kent

    2010-01-01

    The literature on direct electrochemical reduction of NOx in a solid state cell has been reviewed. It is shown that that the reduction of nitric oxide either occurs on the electrode or on the electrolyte if F-centers are formed. It is also shown that some oxide based electrodes has a high apparent...

  9. Preparation of a Carbon-Based Solid Acid Catalyst by Sulfonating Activated Carbon in a Chemical Reduction Process

    Directory of Open Access Journals (Sweden)

    Xiao-Yan Liu

    2010-10-01

    Full Text Available Sulfonated (SO3H-bearing activated carbon (AC-SO3H was synthesized by an aryl diazonium salt reduction process. The obtained material had a SO3H density of 0.64 mmol·g-1 and a specific surface area of 602 m2·g-1. The catalytic properties of AC-SO3H were compared with that of two commercial solid acid catalysts, Nafion NR50 and Amberlyst-15. In a 10-h esterification reaction of acetic acid with ethanol, the acid conversion with AC-SO3H (78% was lower than that of Amberlyst-15 (86%, which could be attributed to the fact that the SO3H density of the sulfonated carbon was lower than that of Amberlyst-15 (4.60 mmol·g-1. However, AC-SO3H exhibited comparable and even much higher catalytic activities than the commercial catalysts in the esterification of aliphatic acids with longer carbon chains such as hexanoic acid and decanoic acid, which may be due to the large specific surface area and mesoporous structures of the activated carbon. The disadvantage of AC-SO3H is the leaching of SO3H group during the reactions.

  10. Identifying Different Types of Catalysts for CO2 Reduction by Ethane through Dry Reforming and Oxidative Dehydrogenation.

    Science.gov (United States)

    Porosoff, Marc D; Myint, Myat Noe Zin; Kattel, Shyam; Xie, Zhenhua; Gomez, Elaine; Liu, Ping; Chen, Jingguang G

    2015-12-14

    The recent shale gas boom combined with the requirement to reduce atmospheric CO2 have created an opportunity for using both raw materials (shale gas and CO2 ) in a single process. Shale gas is primarily made up of methane, but ethane comprises about 10 % and reserves are underutilized. Two routes have been investigated by combining ethane decomposition with CO2 reduction to produce products of higher value. The first reaction is ethane dry reforming which produces synthesis gas (CO+H2 ). The second route is oxidative dehydrogenation which produces ethylene using CO2 as a soft oxidant. The results of this study indicate that the Pt/CeO2 catalyst shows promise for the production of synthesis gas, while Mo2 C-based materials preserve the CC bond of ethane to produce ethylene. These findings are supported by density functional theory (DFT) calculations and X-ray absorption near-edge spectroscopy (XANES) characterization of the catalysts under in situ reaction conditions. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. Tailored Combination of Low Dimensional Catalysts for Efficient Oxygen Reduction and Evolution in Li-O2 Batteries.

    Science.gov (United States)

    Yoon, Ki Ro; Kim, Dae Sik; Ryu, Won-Hee; Song, Sung Ho; Youn, Doo-Young; Jung, Ji-Won; Jeon, Seokwoo; Park, Yong Joon; Kim, Il-Doo

    2016-08-23

    The development of efficient bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is a key issue pertaining high performance Li-O2 batteries. Here, we propose a heterogeneous electrocatalyst consisting of LaMnO3 nanofibers (NFs) functionalized with RuO2 nanoparticles (NPs) and non-oxidized graphene nanoflakes (GNFs). The Li-O2 cell employing the tailored catalysts delivers an excellent electrochemical performance, affording significantly reduced discharge/charge voltage gaps (1.0 V at 400 mA g(-1) ), and superior cyclability for over 320 cycles. The outstanding performance arises from (1) the networked LaMnO3 NFs providing ORR/OER sites without severe aggregation, (2) the synergistic coupling of RuO2 NPs for further improving the OER activity and the electrical conductivity on the surface of the LaMnO3 NFs, and (3) the use of GNFs providing a fast electronic pathway as well as improved ORR kinetics. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Reduction of CO2 by nickel (II) macrocycle catalyst at HMDE

    Indian Academy of Sciences (India)

    Unknown

    CO is the major product in the gaseous phase and. HCOOH the sole product formed in the solution phase. Keywords. Nickel (II) azamacrocycle; electrocatalytic reduction of CO2; electrochemical reduction. 1. Introduction. Electrochemical processes for the conversion of carbon dioxide (CO2) to organic substances have ...

  13. Nitrogen Isotope Composition of Thermally Produced NOx from Various Fossil-Fuel Combustion Sources.

    Science.gov (United States)

    Walters, Wendell W; Tharp, Bruce D; Fang, Huan; Kozak, Brian J; Michalski, Greg

    2015-10-06

    The nitrogen stable isotope composition of NOx (δ(15)N-NOx) may be a useful indicator for NOx source partitioning, which would help constrain NOx source contributions in nitrogen deposition studies. However, there is large uncertainty in the δ(15)N-NOx values for anthropogenic sources other than on-road vehicles and coal-fired energy generating units. To this end, this study presents a broad analysis of δ(15)N-NOx from several fossil-fuel combustion sources that includes: airplanes, gasoline-powered vehicles not equipped with a three-way catalytic converter, lawn equipment, utility vehicles, urban buses, semitrucks, residential gas furnaces, and natural-gas-fired power plants. A relatively large range of δ(15)N-NOx values was measured from -28.1‰ to 8.5‰ for individual exhaust/flue samples that generally tended to be negative due to the kinetic isotope effect associated with thermal NOx production. A negative correlation between NOx concentrations and δ(15)N-NOx for fossil-fuel combustion sources equipped with selective catalytic reducers was observed, suggesting that the catalytic reduction of NOx increases δ(15)N-NOx values relative to the NOx produced through fossil-fuel combustion processes. Combining the δ(15)N-NOx measured in this study with previous published values, a δ(15)N-NOx regional and seasonal isoscape was constructed for the contiguous U.S., which demonstrates seasonal and regional importance of various NOx sources.

  14. Temperature dependence of the oxygen reduction kinetics on Ru{sub x}Se{sub y}/C catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Leveratto, D.; Racz, A.; Savinova, E.R.; Stimming, U. [Technische Universitaet Muenchen, Department of Physics E19, James-Franck-Str. 1, D-85748 Garching (Germany)

    2006-07-15

    The temperature dependence of the oxygen reduction kinetics on carbon-supported Ru{sub x}Se{sub y} catalysts is studied using a rotating disc electrode in 0.5 M H{sub 2}SO{sub 4} in the temperature interval from 25 C to 65 C. When the absolute value of the overpotential is below ca. 0.65 V, the reaction is limited by a one-electron charge transfer step, where the transfer coefficient is independent of the temperature and equal to 0.44. The apparent activation enthalpy at zero overpotential is 0.49 eV and the pre-exponential factor is independent of the temperature. (Abstract Copyright [2006], Wiley Periodicals, Inc.)

  15. Catalytic conversion of CO, NO and SO2 on supported sulfide catalysts. Part 2. Catalytic reduction of NO and SO2 by CO

    International Nuclear Information System (INIS)

    Zhuang, S.-X.; Yamazaki, M.; Omata, K.; Takahashi, Y.; Yamada, M.

    2001-01-01

    To investigate the possibility of simultaneous catalytic reduction of NO and SO 2 by CO, reactions of NO, NO-CO, and NO-SO 2 -CO were performed on γ-alumina-supported sulfides of transition metals including Co, Mo, CoMo and FeMo. NO was decomposed into N 2 O and N 2 accompanied with the formation of SO 2 ; this serious oxidation of lattice sulfur resulted in the deactivation of the catalysts. The addition of CO to the NO stream suppressed SO 2 formation and yielded COS instead. A stoichiometric conversion of NO and CO to N 2 and CO 2 was observed above 350C on the CoMo and the FeMo catalysts. Although the CO addition lengthened catalyst life, it was not enough to maintain activity. After the NO-CO reaction, an XPS analysis showed the growth of Mo 6+ and SO 4 2- peaks, especially for the sulfided FeMo/Al 2 O 3 ; the FeMo catalyst underwent strong oxidation in the NO-CO reaction. The NO and the NO-CO reactions proceeded non-catalytically, consuming catalyst lattice sulfur to yield SO 2 or COS. The addition of SO 2 in the NO-CO system enabled in situ regeneration of the catalysts; the catalysts oxidized through abstraction of lattice sulfur experienced anew reduction and sulfurization through the SO 2 -CO reaction at higher temperature. NO and SO 2 were completely and catalytically converted at 400C on the sulfided CoMo/Al 2 O 3 . By contrast, the sulfided FeMo/Al 2 O 3 was easily oxidized by NO and hardly re-sulfided under the test conditions. Oxidation states of the metals before and after the reactions were determined. Silica and titania-supported CoMo catalysts were also evaluated to study support effects

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2004-06-30

    This is the sixteenth 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. During an unplanned outage, damage occurred to the electrochemical noise corrosion probes installed at the AEP Gavin plant; testing is expected to resume in August. The KEMCOP corrosion coupons were not affected by the unplanned outage; the coupons were removed and sent for analysis. BYU conducted a series of tests before the ISSR lab was relocated. Ammonia adsorption experiments provided clear evidence of the types of acidic sites present on catalyst surfaces. Data collected this quarter indicate that surface sulfation decreases Lewis acid site concentrations for all catalysts thus far studied, confirming that catalytic activity under commercial coal-based SCR conditions occurs primarily on Br{o}nsted acid sites and would be susceptible to basic impurities such as alkali and alkaline earth oxides, chlorides, and sulfates. SCR activity tests based on MS analysis showed that increasing sulfation generally increases NO reduction activity for both 0% and 1% vanadia catalysts. During this quarter, the slipstream reactor at Rockport operated for 720 hours on flue gas. Catalyst exposure time reached 4500 hours since installation. The reactor is out of service at the Rockport plant and plans are being made to move it to the Gadsden Plant. At Gadsden, modifications have begun in preparation for installation of the slipstream reactor next quarter.

  17. NOx processing on Solar gas turbines; Turbines, traitement des nox sur les turbines a gaz solar

    Energy Technology Data Exchange (ETDEWEB)

    Chausse, X. [Spie Trindel, 95 - Cergy (France). Service TAG

    1997-12-31

    The Solar Company, in cooperation with Tuma Turbomach, has developed the SoLoNOx combustion system with a dry, lean, premixed compound, allowing for reduced NOx and CO emission levels (respectively 42 ppmv and 50 ppmv at 15 pc O{sub 2}). The combustor size is larger than a conventional combustor in order to maintain combustion efficiency and reduce carbon monoxide levels. Leaner combustion occurs at lower temperatures which produce less nitrogen oxides but require more volume to complete the combustion process. New developments should allow for a further reduction of NOx level at 25 ppmv

  18. Influence of Micropore and Mesoporous in Activated Carbon Air-cathode Catalysts on Oxygen Reduction Reaction in Microbial Fuel Cells

    International Nuclear Information System (INIS)

    Liu, Yi; Li, Kexun; Ge, Baochao; Pu, Liangtao; Liu, Ziqi

    2016-01-01

    In this study, carbon samples with different micropore and mesoporous structures are prepared as air-cathode catalyst layer to explore the role of pore structure on oxygen reduction reaction. The results of linear sweep voltammetry and power density show that the commercially-produced activated carbon (CAC) has the best electrochemical performance, and carbon samples with only micropore or mesoporous show lower performance than CAC. Nitrogen adsorption-desorption isotherms analysis confirm that CAC has highest surface area (1616 m 2 g −1 ) and a certain amount of micropore and mesoporous. According to Tafel plot and rotating disk electrode, CAC behaves the highest kinetic activity and electron transfer number, leading to the improvement of oxygen reduction reaction. The air permeability test proves that mesoporous structure enhance oxygen permeation. Carbon materials are also analyzed by In situ Fourier Transform Infrared Spectroscopy and H 2 temperature programmed reduction, which indicate that micropore provide active sites for catalysis. In a word, micropore and mesoporous together would improve the electrochemical performance of carbon materials.

  19. A New Bioinspired Perchlorate Reduction Catalyst with Significantly Enhanced Stability via Rational Tuning of Rhenium Coordination Chemistry and Heterogeneous Reaction Pathway.

    Science.gov (United States)

    Liu, Jinyong; Han, Mengwei; Wu, Dimao; Chen, Xi; Choe, Jong Kwon; Werth, Charles J; Strathmann, Timothy J

    2016-06-07

    Rapid reduction of aqueous ClO4(-) to Cl(-) by H2 has been realized by a heterogeneous Re(hoz)2-Pd/C catalyst integrating Re(O)(hoz)2Cl complex (hoz = oxazolinyl-phenolato bidentate ligand) and Pd nanoparticles on carbon support, but ClOx(-) intermediates formed during reactions with concentrated ClO4(-) promote irreversible Re complex decomposition and catalyst deactivation. The original catalyst design mimics the microbial ClO4(-) reductase, which integrates Mo(MGD)2 complex (MGD = molybdopterin guanine dinucleotide) for oxygen atom transfer (OAT). Perchlorate-reducing microorganisms employ a separate enzyme, chlorite dismutase, to prevent accumulation of the destructive ClO2(-) intermediate. The structural intricacy of MGD ligand and the two-enzyme mechanism for microbial ClO4(-) reduction inspired us to improve catalyst stability by rationally tuning Re ligand structure and adding a ClOx(-) scavenger. Two new Re complexes, Re(O)(htz)2Cl and Re(O)(hoz)(htz)Cl (htz = thiazolinyl-phenolato bidentate ligand), significantly mitigate Re complex decomposition by slightly lowering the OAT activity when immobilized in Pd/C. Further stability enhancement is then obtained by switching the nanoparticles from Pd to Rh, which exhibits high reactivity with ClOx(-) intermediates and thus prevents their deactivating reaction with the Re complex. Compared to Re(hoz)2-Pd/C, the new Re(hoz)(htz)-Rh/C catalyst exhibits similar ClO4(-) reduction activity but superior stability, evidenced by a decrease of Re leaching from 37% to 0.25% and stability of surface Re speciation following the treatment of a concentrated "challenge" solution containing 1000 ppm of ClO4(-). This work demonstrates the pivotal roles of coordination chemistry control and tuning of individual catalyst components for achieving both high activity and stability in environmental catalyst applications.

  20. Impact of FCC regenerator design in the NOx emissions

    Energy Technology Data Exchange (ETDEWEB)

    Pereira, Hugo Borges; Sandes, Emanuel Freire; Gilbert, William Richard; Roncolatto, Rodolfo Eugenio; Gobbo, Rodrigo; Casavechia, Luiz Carlos; Candido, William Victor Carlos [Petroleo Brasileiro S.A. (PETROBRAS), Rio de Janeiro, RJ (Brazil); Bridi, Patricia Elaine [Possebon Engenharia, Sao Mateus do Sul, PR (Brazil)

    2012-07-01

    Fluid Catalytic Cracking (FCC) is the main point source of NOx in the refinery and it is responsible for at least 20% of the total NOx emissions from the refineries. The thermal NOx formation in the FCC regenerator is negligible. However, half of the feed nitrogen is converted to coke, and is burned in the regenerator. The majority of coke nitrogen is reduced to N2 and less than 10% is converted to NOx. This number may vary significantly with the oxygen excess in the flue gas and other operational conditions. With the purpose of evaluating the impact of different regenerator designs in NOx formation, several tests were carried out in the PETROBRAS FCC prototype unit. The test unit is equipped with adiabatic insulation and a CO boiler, allowing it to reproduce the heat balance of a commercial FCC and to operate either in full combustion or partial combustion. Two different designs of FCC regenerators were evaluated: single stage regenerator (the existing configuration) and two stage regenerator, with the catalyst bed divided into two sections by a structured packing baffle. It was observed in the tests that the combustion regime had a very strong effect on NOx formation. In full combustion, the effect of the FCC operating variables: excess oxygen, combustion promoter content in catalyst and regenerator design could be identified. The two stage configuration was capable of decreasing NOx emissions by 30%. In partial combustion, the effect of the CO-boiler variables on NOx emissions was overwhelming, but the use of the structured packing baffle was able to improve the catalyst regeneration.(author)

  1. Al- or Si-decorated graphene oxide: A favorable metal-free catalyst for the N2O reduction

    International Nuclear Information System (INIS)

    Esrafili, Mehdi D.; Sharifi, Fahimeh; Nematollahi, Parisa

    2016-01-01

    Highlights: • The reduction of N 2 O by CO molecule is investigated over Al- and Si-decorated graphene oxides (Al-/Si-GO). • The N 2 O decomposition process can take place with a negligible activation energy over both surfaces. • Al-GO and Si-GO can be used as an efficient metal-free catalyst for the reduction of N 2 O molecule at ambient conditions. - Abstract: The structural and catalytic properties of Al- or Si-decorated graphene oxide (Al-/Si-GO) are studied by means of density functional theory calculations. The relatively large adsorption energy together with the small Al−O or Si−O binding distances indicate that the epoxy groups over the GO surface can strongly stabilize the single Al or Si atom. Hence, Al-GO and Si-GO are stable enough to be utilized in catalytic reduction of N 2 O by CO molecule. It is found that the adsorption and decomposition of N 2 O molecule over Si-GO is more favorable than over Al-GO, due to its larger adsorption energy (E ads ) and charge transfer (q CT ) values. On the other hand, the CO molecule is physically adsorbed over both surfaces, with relatively small E ads and q CT values. Therefore, at the presence of N 2 O and CO molecules as the reaction gas, the Al or Si atom of the surface should be dominantly covered by N 2 O molecule. Our results indicate that the N 2 O decomposition process can take place with a negligible activation energy over Al-/Si-GO surface, where the N 2 molecule can be easily released from the surface. Then, the activated oxygen atom (O ads ) which remains over the surface reacts with the CO molecule to form the CO 2 molecule via the reaction O ads + CO → CO 2 . Based on the calculated activation energies, it is suggested that both Al-GO and Si-GO can be used as an efficient metal-free catalyst for the reduction of N 2 O molecule at ambient conditions.

  2. Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts.

    Science.gov (United States)

    Yin, Peiqun; Yao, Tao; Wu, Yuen; Zheng, Lirong; Lin, Yue; Liu, Wei; Ju, Huanxin; Zhu, Junfa; Hong, Xun; Deng, Zhaoxiang; Zhou, Gang; Wei, Shiqiang; Li, Yadong

    2016-08-26

    A new strategy for achieving stable Co single atoms (SAs) on nitrogen-doped porous carbon with high metal loading over 4 wt % is reported. The strategy is based on a pyrolysis process of predesigned bimetallic Zn/Co metal-organic frameworks, during which Co can be reduced by carbonization of the organic linker and Zn is selectively evaporated away at high temperatures above 800 °C. The spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements both confirm the atomic dispersion of Co atoms stabilized by as-generated N-doped porous carbon. Surprisingly, the obtained Co-Nx single sites exhibit superior ORR performance with a half-wave potential (0.881 V) that is more positive than commercial Pt/C (0.811 V) and most reported non-precious metal catalysts. Durability tests revealed that the Co single atoms exhibit outstanding chemical stability during electrocatalysis and thermal stability that resists sintering at 900 °C. Our findings open up a new routine for general and practical synthesis of a variety of materials bearing single atoms, which could facilitate new discoveries at the atomic scale in condensed materials. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Dodecahedral W@WC Composite as Efficient Catalyst for Hydrogen Evolution and Nitrobenzene Reduction Reactions.

    Science.gov (United States)

    Chen, Zhao-Yang; Duan, Long-Fa; Sheng, Tian; Lin, Xiao; Chen, Ya-Feng; Chu, You-Qun; Sun, Shi-Gang; Lin, Wen-Feng

    2017-06-21

    Core-shell composites with strong phase-phase contact could provide an incentive for catalytic activity. A simple, yet efficient, H 2 O-mediated method has been developed to synthesize a mesoscopic core-shell W@WC architecture with a dodecahedral microstructure, via a one-pot reaction. The H 2 O plays an important role in the resistance of carbon diffusion, resulting in the formation of the W core and W-terminated WC shell. Density functional theory (DFT) calculations reveal that adding W as core reduced the oxygen adsorption energy and provided the W-terminated WC surface. The W@WC exhibits significant electrocatalytic activities toward hydrogen evolution and nitrobenzene electroreduction reactions, which are comparable to those found for commercial Pt/C, and substantially higher than those found for meso- and nano-WC materials. The experimental results were explained by DFT calculations based on the energy profiles in the hydrogen evolution reactions over WC, W@WC, and Pt model surfaces. The W@WC also shows a high thermal stability and thus may serve as a promising more economical alternative to Pt catalysts in these important energy conversion and environmental protection applications. The current approach can also be extended or adapted to various metals and carbides, allowing for the design and fabrication of a wide range of catalytic and other multifunctional composites.

  4. Heteropoly acid promoted V2O5/TiO2 catalysts for NO abatement with ammonia in alkali containing flue gases

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Jensen, Anker Degn; Riisager, Anders

    2011-01-01

    V2O5/TiO2 and heteropoly acid promoted V2O5/TiO2 catalysts were prepared and characterized by N2 physisorption, XRPD and NH3-TPD. The influence of the calcination temperature from 400 to 700 1C on crystallinity and acidic properties was studied and compared with the activity for the selective...... catalytic reduction (SCR) of NO with ammonia. The SCR activity of heteropoly acid promoted catalysts was found to be much higher than for unpromoted catalysts. The stability of heteropoly acid promoted catalysts is dependent on calcination temperature and there is a gradual decrease in SCR activity...... and acidity with increase in calcination temperatures. Furthermore, the heteropoly acid promoted V2O5/TiO2 catalysts showed excellent alkali deactivation resistance and might therefore be alternative deNOx catalysts in biomass fired power plants....

  5. Promoted V2O5/TiO2 catalysts for selective catalytic reduction of NO with NH3 at low temperatures

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Schill, Leonhard; Godiksen, Anita

    2016-01-01

    characterized by N2 physisorption, XRPD, NH3-TPD, H2-TPR, Raman, FTIR and EPR spectroscopy to investigate the properties of the catalysts. XRPD, Raman and FTIR showed that promotion with 15 wt.% HPA does not cause V2O5 to be present in crystalline form, also at a loading of 5 wt.% V2O5. Hence, use of HPAs does......The influence of varying the V2O5 content (3–6 wt.%) was studied for the selective catalytic reduction (SCR) of nitrogen oxides by ammonia on heteropoly acid (HPA)- and tungsten oxide (WO3)-promoted V2O5/TiO2 catalysts. The SCR activity and alkali deactivation resistance of HPA-promoted V2O5/TiO2...... catalysts was found to be much higher than for WO3-promoted catalysts. By increasing the vanadium content from 3 to 5 wt.% the catalysts displayed a two fold increase in activity at 225 °C and retained their initial activity after alkali doping at a molar K/V ratio of 0.181. Furthermore, the catalysts were...

  6. A facile template approach for the synthesis of mesoporous Fe3C/Fe-N-doped carbon catalysts for efficient and durable oxygen reduction reaction

    Institute of Scientific and Technical Information of China (English)

    Shuai Li; Bo Li; Liang Ma; Jia Yang; Hangxun Xu

    2017-01-01

    Facile synthetic approaches toward the development of efficient and durable nonprecious metal catalysts for the oxygen reduction reaction (ORR) are very important for commercializing advanced electrochemical devices such as fuel cells and metal-air batteries.Here we report a novel template approach to synthesize mesoporous Fe-N-doped carbon catalysts encapsulated with Fe3C nanoparticles.In this approach,the layer-structured FeOCl was first used as a template for the synthesis of a three-dimensional polypyrrole (PPy) structure.During the removal of the FeOCl template,the Fe3+ can be absorbed by PPy and then converted into Fe3C nanoparticles and Fe-N-C sites during the pyrolyzing process.As a result,the as-prepared catalysts could exhibit superior electrocatalytic ORR performance to the commercial Pt/C catalyst in alkaline solutions.Furthermore,the Zn-air battery assembled using the mesoporous carbon catalyst as the air electrode could surpass the commercial Pt/C catalyst in terms of the power density and energy density.

  7. Deactivation of La-Fe-ZSM-5 catalyst for selective catalytic reduction of NO with NH{sup 3}. Field study results

    Energy Technology Data Exchange (ETDEWEB)

    Qi, Gongshin; Yang, Ralph T. [Department of Chemical Engineering, University of Michigan, Ann Arbor, MI 48109 (United States); Chang, Ramsay; Cardoso, Sylvio [Air Pollution Control, Power Generation, Electric Power Research Institute, Palo Alto, CA 94304-1395 (United States); Smith, Randall A. [Fossil Energy Research Corporation, Laguna Hills, CA 92653 (United States)

    2004-11-08

    Results are summarized for a study on the effects of poisons on the La-Fe-ZSM-5 catalyst activity for the selective catalytic reduction of NO by ammonia. The deactivation of La-Fe-ZSM-5 honeycombs was studied in field tests. A honeycomb catalyst containing 25%La-Fe-ZSM-5 had an overall activity similar to that of a commercial vanadia honeycomb catalyst. Long-term activity test results show that the 25%La-Fe-ZSM-5 catalyst activity decreased to 50% after 300h and 25% after 1769h of on-stream flue gas exposure. The deactivation is correlated to the amounts of poisons deposited on the catalyst. Poisons include alkali and alkaline earth metals, As and Hg. Hg was found to be ion-exchanged from HgCl{sup 2} to form Hg-ZSM-5, and Hg was found to be among the strongest poisons. The poisoning effects of these elements appeared to be additive. Thus, from the chemical analysis of the deactivated catalyst, the deactivation of Fe-ZSM-5 can be predicted.

  8. Ethanol-selective catalytic reduction of NO by Ag/Al2O3 catalysts: Activity and deactivation by alkali salts

    DEFF Research Database (Denmark)

    Schill, Leonhard; Putluru, Siva Sankar Reddy; Jacobsen, Casper Funk

    2012-01-01

    Ag/Al2O3 catalysts with and without potassium doping were prepared by incipient wetness impregnation and characterized by N2 physisorption, XRPD, NH3-TPD and SEM. The influence of the Ag content from 1 to 5 wt.% was investigated for the selective catalytic reduction (SCR) of NO with ethanol. The 3...... wt.% Ag/Al2O3 catalyst was found to be the most active and CO2 selective over a wide temperature window (300–500 ◦C). Addition of 500 ppm of H2 has a mild promotional effect on the activity while SO2 has a strong negative influence on the SCR activity. Furthermore, the Ag/Al2O3 ethanol-SCR catalyst......3 ethanol-SCR catalyst compared to the conventional NH3-SCR catalyst. The still low potassium resistance, in combination with the high sensitivity to SO2, seems not to make these catalysts a real option for biomass fired boilers....

  9. Synthesis of self-supported non-precious metal catalysts for oxygen reduction reaction with preserved nanostructures from the polyaniline nanofiber precursor

    DEFF Research Database (Denmark)

    Hu, Yang; Zhao, Xiao; Huang, Yunjie

    2013-01-01

    Non-precious metal catalysts (NPMCs) for the oxygen reduction reaction (ORR) are an active subject of recent research on proton exchange membrane fuel cells. In this study, we report a new approach to preparation of self-supported and nano-structured NPMCs using pre-prepared polyaniline (PANI...

  10. Catalytic Destruction of a Surrogate Organic Hazardous Air Pollutant as a Potential Co-benefit for Coal-fired Selective Catalyst Reduction Systems

    Science.gov (United States)

    Catalytic destruction of benzene (C6H6), a surrogate for organic hazardous air pollutants (HAPs) produced from coal combustion, was investigated using a commercial selective catalytic reduction (SCR) catalyst for evaluating the potential co-benefit of the SCR technology for reduc...

  11. NOx trade. Case studies

    International Nuclear Information System (INIS)

    Jantzen, J.

    2002-01-01

    Some of the questions with respect to the trade of nitrogen oxides that businesses in the Netherlands have to deal with are dealt with: should a business buy or sell rights for NOx emission; which measures must be taken to reduce NOx emission; how much must be invested; and how to deal with uncertainties with regard to prices. Simulations were carried out with the MOSES model to find the answers to those questions. Results of some case studies are presented, focusing on the chemical sector in the Netherlands. Finally, the financial (dis)advantages of NOx trade and the related uncertainties for a single enterprise are discussed [nl

  12. Targeted design of α-MnO2 based catalysts for oxygen reduction

    Czech Academy of Sciences Publication Activity Database

    Lehtimäki, M.; Hoffmannová, Hana; Boytsová, O.; Bastl, Zdeněk; Bush, M.; Halck, N. B.; Rossmeisl, J.; Krtil, Petr

    2016-01-01

    Roč. 191, FEB 2016 (2016), s. 452-461 ISSN 0013-4686 EU Projects: European Commission(XE) 214936 - ELCAT Institutional support: RVO:61388955 Keywords : electrocatalysis * oxygen reduction * MnO2 Subject RIV: CG - Electrochemistry Impact factor: 4.798, year: 2016

  13. Ebselen: A thioredoxin reductase-dependent catalyst for α-tocopherol quinone reduction

    International Nuclear Information System (INIS)

    Fang Jianguo; Zhong Liangwei; Zhao Rong; Holmgren, Arne

    2005-01-01

    The thioredoxin system, composed of thioredoxin (Trx), thioredoxin reductase (TrxR), and NADPH, is a powerful protein disulfide reductase system with a broad substrate specificity. Recently the selenazol drug ebselen was shown to be a substrate for both mammalian TrxR and Trx. We examined if α-tocopherol quinone (TQ), a product of α-tocopherol oxidation, is reduced by ebselen in the presence of TrxR, since TQ was not a substrate for the enzyme itself. Ebselen reduction of TQ in the presence of TrxR was caused by ebselen selenol, generated from fast reduction of ebselen by the enzyme. TQ has no intrinsic antioxidant activity, while the product of reduction of TQ, α-tocopherolhydroquinone (TQH 2 ), is a potent antioxidant. The thioredoxin system dependence of ebselen to catalyze reduction of other oxidized species, such as hydrogen peroxide, dehydroascorbate, and peroxynitrite, is discussed. The ability of ebselen to reduce TQ via the thioredoxin system is a novel mechanism to explain the effects of the drug as an antioxidant in vivo

  14. Lithium-Vanadium bronzes as model catalysts for the selective reduction of nitric oxide

    NARCIS (Netherlands)

    Bosch, H.; Bongers, Annemie; Enoch, Gert; Snel, Ruud; Ross, Julian R.H.

    1989-01-01

    The effect of alkali metals on the selective reduction of nitric oxide with ammonia has been studied on bulk iron oxide and bulk vanadium oxide. The influence of additions of LiOH, NaOH and KOH on the activity was screened by pulse experiments carried out in the absence of gaseous oxygen; FTIR

  15. Targeted design of α-MnO2 based catalysts for oxygen reduction

    DEFF Research Database (Denmark)

    Lehtimaeki, Matti; Hoffmannova, Hana; Boytsova, Olga

    2016-01-01

    The paper focuses on theoretical and experimental aspects of an oxide surface optimization for oxygen reduction reaction (ORR). Various doped α-MnO2 based electrocatalysts were prepared by microwave-assisted hydrothermal synthesis and electrochemically characterized to validate density functional...

  16. Covalent versus Charge Transfer Modification of Graphene/Carbon-Nanotubes with Vitamin B1: Co/N/S-C Catalyst toward Excellent Oxygen Reduction.

    Science.gov (United States)

    Vij, Varun; Tiwari, Jitendra N; Kim, Kwang S

    2016-06-29

    High-performance nonprecious cathodic catalysts for oxygen reduction are highly demanded for low-temperature polymer electrolyte membrane fuel cells (PEMFCs). Here, we report a noble-meta- free, nitrogen and sulfur codoped graphene(G)/carbon-nanotube(CNT) material decorated with Co nanoparticles (NPs), which serve as catalytic sites for excellent oxygen reduction reaction (ORR) in basic and acidic media. Out of the cathodic catalysts synthesized by either covalent (cov) or charge transfer (CT) modification of graphen oxide (GO) with thiamine (Th: Vitamin B1), ThG/CNT/Co-cov shows more promising ORR properties than ThG/CNT/Co-CT. Catalyst ThG/CNT/Co-cov exhibits onset/halfwave potentials of 0.95/0.86 V in 0.1 M KOH and 0.92/0.83 V in 0.1 M HClO4, which are comparable to those of commercial catalyst Pt/C (0.95/0.86 V). As compared to Pt/C, our catalyst shows higher current densities of 6.72 mA cm(-2) in basic medium and 7.08 mA cm(-2) in acidic medium at 0.55 V (vs reversible hydrogen electrode (RHE)). It also exhibits better catalytic stability and methanol tolerance. High catalytic efficiency and stability of ThG/CNT/Co-cov show a promising prospect of materialization of PEMFCs for clean energy production.

  17. Deoxyribonucleic acid directed metallization of platinum nanoparticles on graphite nanofibers as a durable oxygen reduction catalyst for polymer electrolyte fuel cells

    Science.gov (United States)

    Peera, S. Gouse; Sahu, A. K.; Arunchander, A.; Nath, Krishna; Bhat, S. D.

    2015-11-01

    Effective surface functionalization to the hydrophobic graphite nanofibers (GNF) is performed with the biomolecule, namely deoxy-ribo-nucleic-acid (DNA) via π-π interactions. Pt nanoparticles are impregnated on GNF-DNA composite by ethylene glycol reduction method (Pt/GNF-DNA) and its effect on electro catalytic activity for oxygen reduction reaction (ORR) is systemically studied. Excellent dispersion of Pt nanoparticles over GNF-DNA surfaces with no evidence on particle aggregation is a remarkable achievement in this study. This result in higher electro chemical surface area of the catalyst, enhanced ORR behavior with significant enhancement in mass activity. The catalyst is validated in H2-O2 polymer electrolyte fuel cell (PEFC) and a peak power density of 675 mW cm-2 is achieved at a load current density of 1320 mA cm-2 with a minimal catalyst loading of 0.1 mg cm-2 at a cell temperature of 70 °C and 2 bar absolute pressure. Repeated potential cycling up to 10000 cycles in acidic media is also performed for this catalyst and found excellent stability with only 60 mV drop in the ORR half wave potential. The superior behavior of Pt/GNF-DNA catalyst is credited to the robust fibrous structure of GNF and its effective surface functionalization process via π-π interaction.

  18. Enhanced hydrothermal stability of Cu-ZSM-5 catalyst via surface modification in the selective catalytic reduction of NO with NH{sub 3}

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Tao; Shi, Juan; Liu, Jian, E-mail: liujian@cup.edu.cn; Wang, Daxi; Zhao, Zhen, E-mail: zhenzhao@cup.edu.cn; Cheng, Kai; Li, Jianmei

    2016-07-01

    Highlights: • The hydrothermal stability of Cu-ZSM-5 catalyst was enhanced after surface modification. • An inert silica layer was deposited on the surface of Cu-ZSM-5 and formed a protective layer. • The contact between Si and Cu and Al atoms could form Si-O-Al and Si- O−Cu bonds. • The redox and acidity properties of Cu-ZSM-5-CLD-Aged catalyst were largely retained. • The adsorption and activation of NO and NH{sub 3} was almost unchanged over Cu-ZSM-5-CLD catalyst before and after hydrothermal treatment. - Abstract: The surface of Cu-ZSM-5 catalyst was modified by chemical liquid deposition (CLD) of tetraethoxysilane (TEOS) for enhancing its hydrothermal stability in the selective catalytic reduction of NO with NH{sub 3}. After hydrothermal aging at 750 °C for 13 h, the catalytic performance of Cu-ZSM-5-Aged catalyst was significantly reduced for NO reduction in the entire temperature range, while that of Cu-ZSM-5-CLD-Aged catalyst was affected very little. The characterization results indicated that an inert silica layer was deposited on the surface of Cu-ZSM-5 and formed a protective layer, which prevents the detachment of Cu{sup 2+} from ZSM-5 ion-exchange positions and the dealumination of zeolite during the hydrothermal aging process. Based on the data it is hypothesized to be the primary reason for the high hydrothermal stability of Cu-ZSM-5-CLD catalyst.

  19. 40 CFR 76.12 - Phase I NOX compliance extension.

    Science.gov (United States)

    2010-07-01

    ... 40 Protection of Environment 16 2010-07-01 2010-07-01 false Phase I NOX compliance extension. 76.12 Section 76.12 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) ACID RAIN NITROGEN OXIDES EMISSION REDUCTION PROGRAM § 76.12 Phase I NOX compliance extension. (a...

  20. Electrooxidations of ethanol, acetaldehyde and acetic acid using PtRuSn/C catalysts prepared by modified alcohol-reduction process

    Energy Technology Data Exchange (ETDEWEB)

    Wu, Gang [Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208 (United States); Swaidan, Raja [Department of Chemical Engineering, Cooper Union, New York, NY 10003 (United States); Cui, Guofeng [School of Chemistry and Chemical Engineering, Sun-Yat Sen University, Guangzhou 510275 (China)

    2007-10-11

    Well-dispersed ternary PtRuSn catalysts of various atomic ratios (60:30:10, 60:20:20 and 60:10:30) were deposited onto carbon using modified alcohol-reduction process for electrochemical oxidation of ethanol. The alloy phase structure and surface morphology for each variation of the PtRuSn/C catalysts were determined by XRD and HRTEM. In order to evaluate the contributions of Ru and Sn in the different stages of ethanol oxidation, electrochemical oxidations of adsorbed CO, ethanol, acetaldehyde and acetic acid were performed on each PtRuSn/C catalyst. The results indicated that the Ru-rich PtRuSn/C catalyst (60:30:10) exhibited the lowest onset potential for the electrooxidations of adsorbed CO, ethanol and acetaldehyde, revealing that the removal through oxidation of the intermediate C{sub 1} and C{sub 2} species from Pt sites is primarily attributed to the Ru and Pt{sub 3}Sn alloy structures. However, for the overall oxidation of ethanol, the Sn-rich PtRuSn/C catalyst (60:10:30) containing PtSn phase and SnO{sub 2} structure is favorable for the activation of C-C bond breaking, thereby generating higher current density (mass activity) at higher potentials. Moreover, in the electrooxidation of acetic acid, a remarkable improvement for oxidizing acetic acid to C{sub 1} species was observed in the Sn-rich PtRuSn/C catalyst (60:10:30), while the Ru-rich PtRuSn/C catalyst (60:30:10) was almost incapable of breaking the C-C bond to further oxidize acetic acid. The possible reasons for the different reactivities on the studied PtRuSn/C catalysts were discussed based on the removal of intermediates and activation of the C-C bonds on the different surfaces. (author)

  1. Oxygen reduction activities compared in rotating-disk electrode and proton exchange membrane fuel cells for highly active Fe-N-C catalysts

    International Nuclear Information System (INIS)

    Jaouen, F.; Goellner, V.; Lefèvre, M.; Herranz, J.; Proietti, E.; Dodelet, J.P.

    2013-01-01

    In the past three years, two novel synthesis methods for non-precious metal catalysts resulting in a breakthrough of their activity and performance at the cathode of the proton-exchange membrane fuel cell (PEMFC) have been reported by the group of Prof. Dodelet. While the activity of these novel Fe-based catalysts for the oxygen reduction reaction is very high in PEMFC, our preliminary activity measurements with the rotating disk electrode (RDE) technique on one of them showed an activity being a factor 30–100 lower than the one measured in PEMFC at 80 °C. The present work explains to a large extent this huge difference. Two Fe-N-C catalysts synthesized via our novel approaches and one Fe-N-C catalyst synthesized via our classical approach were investigated in RDE and PEMFC. In both systems, the effect of the ink formulation (Nafion-to-catalyst ratio) was investigated. Optimization of the RDE ink formulation explains a factor between 5 and 10 in the two-decade gap mentioned above. Then, the effect of temperature in the RDE system was investigated. An increase from 20 to 80 °C was found to result in a theoretical maximum twofold increase in activity. However, in practice, decreased O 2 solubility with increased temperature cancels this effect. After taking into account these two parameters, a difference in ORR activity between RDE and PEMFC of ca a factor five still remained for one of the two novel Fe-N-C catalysts investigated here. The lower initial activity measured in RDE for this catalyst is shown to be due to the fast adsorption of anions (HSO 4 − ) from the liquid H 2 SO 4 electrolyte on protonated nitrogen atoms (NH + ) found on its surface. The phenomenon of anion adsorption and associated decreased ORR activity also applies to the other novel Fe-N-C catalyst, but is slower and does not immediately occur in RDE.

  2. Improved Oxygen Reduction Activity and Durability of Dealloyed PtCox Catalysts for Proton Exchange Membrane Fuel Cells: Strain, Ligand, and Particle Size Effects

    Science.gov (United States)

    Jia, Qingying; Caldwell, Keegan; Strickland, Kara; Ziegelbauer, Joseph M.; Liu, Zhongyi; Yu, Zhiqiang; Ramaker, David E.; Mukerjee, Sanjeev

    2015-01-01

    The development of active and durable catalysts with reduced platinum content is essential for fuel cell commercialization. Herein we report that the dealloyed PtCo/HSC and PtCo3/HSC nanoparticle (NP) catalysts exhibit the same levels of enhancement in oxygen reduction activity (~4-fold) and durability over pure Pt/C NPs. Surprisingly, ex situ high-angle annular dark field scanning transmission electron microscopy (HAADF STEM) shows that the bulk morphologies of the two catalysts are distinctly different: D-PtCo/HSC catalyst is dominated by NPs with solid Pt shells surrounding a single ordered PtCo core; however, the D-PtCo3/HSC catalyst is dominated by NPs with porous Pt shells surrounding multiple disordered PtCo cores with local concentration of Co. In situ X-ray absorption spectroscopy (XAS) reveals that these two catalysts possess similar Pt–Pt and Pt–Co bond distances and Pt coordination numbers (CNs), despite their dissimilar morphologies. The similar activity of the two catalysts is thus ascribed to their comparable strain, ligand, and particle size effects. Ex situ XAS performed on D-PtCo3/HSC under different voltage cycling stage shows that the continuous dissolution of Co leaves behind the NPs with a Pt-like structure after 30k cycles. The attenuated strain and/or ligand effects caused by Co dissolution are presumably counterbalanced by the particle size effects with particle growth, which likely accounts for the constant specific activity of the catalysts along with voltage cycling. PMID:26413384

  3. The atomistic origin of the extraordinary oxygen reduction activity of Pt3Ni7 fuel cell catalysts.

    Science.gov (United States)

    Fortunelli, Alessandro; Goddard Iii, William A; Sementa, Luca; Barcaro, Giovanni; Negreiros, Fabio R; Jaramillo-Botero, Andrés

    2015-07-01

    Recently Debe et al. reported that Pt 3 Ni 7 leads to extraordinary Oxygen Reduction Reaction (ORR) activity. However, several reports show that hardly any Ni remains in the layers of the catalysts close to the surface ("Pt-skin effect"). This paradox that Ni is essential to the high catalytic activity with the peak ORR activity at Pt 3 Ni 7 while little or no Ni remains close to the surface is explained here using large-scale first-principles-based simulations. We make the radical assumption that processing Pt-Ni catalysts under ORR conditions would leach out all Ni accessible to the solvent. To simulate this process we use the ReaxFF reactive force field, starting with random alloy particles ranging from 50% Ni to 90% Ni and containing up to ∼300 000 atoms, deleting the Ni atoms, and equilibrating the resulting structures. We find that the Pt 3 Ni 7 case and a final particle radius around 7.5 nm lead to internal voids in communication with the exterior, doubling the external surface footprint, in fair agreement with experiment. Then we examine the surface character of these nanoporous systems and find that a prominent feature in the surface of the de-alloyed particles is a rhombic structure involving 4 surface atoms which is crystalline-like but under-coordinated. Using density-functional theory, we calculate the energy barriers of ORR steps on Pt nanoporous catalysts, focusing on the O ad -hydration reaction (O ad + H 2 O ad → OH ad + OH ad ) but including the barriers of O 2 dissociation (O 2ad → O ad + O ad ) and water formation (OH ad + H ad → H 2 O ad ). We find that the reaction barrier for the O ad -hydration rate-determining-step is reduced significantly on the de-alloyed surface sites compared to Pt(111). Moreover we find that these active sites are prevalent on the surface of particles de-alloyed from a Pt-Ni 30 : 70 initial composition. These simulations explain the peak in surface reactivity at Pt 3 Ni 7 , and provide a rational guide to

  4. Nanodiamonds as pH-switchable oxidation and reduction catalysts with enzyme-like activities for immunoassay and antioxidant applications.

    Science.gov (United States)

    Chen, T M; Tian, X M; Huang, L; Xiao, J; Yang, G W

    2017-10-19

    Nanodiamonds (NDs) have recently become a focus of interest from the viewpoints of both science and technology. Their intriguing properties make them suitable as biologically active substrates, in biosensor applications as well as diagnostic and therapeutic biomedical imaging probes. Here, we demonstrate that NDs, as oxidation and reduction catalysts, possess intrinsic enzyme mimetic properties of oxidase, peroxidase and catalase, and these behaviors can be switched by modulating the pH value. NDs not only catalyze the reduction of oxygen (O 2 ) and hydrogen peroxide (H 2 O 2 ) at acidic pH, but also catalyze the dismutation decomposition of H 2 O 2 to produce O 2 at alkaline pH. It was proposed that the molecular mechanism of their peroxidase-like activity is electron-transfer acceleration, the source of which is likely derived from oxygen containing functional groups on their surface. Based on the color reaction, a nanodiamond-based enzyme linked immunosorbent assay (ELISA) was established for the detection of immunoglobulin G (IgG). Surprisingly, NDs display an excellent antioxidant activity due to the protective effect against H 2 O 2 -induced cellular oxidative damage. These findings make NDs a promising enzyme mimetic candidate and expand their applications in biocatalysis, bioassays and nano-biomedicine.

  5. Rhenium Complexes Based on 2-Pyridyl-1,2,3-triazole Ligands: A New Class of CO2 Reduction Catalysts.

    Science.gov (United States)

    Ching, H Y Vincent; Wang, Xia; He, Menglan; Perujo Holland, Noemi; Guillot, Régis; Slim, Cyrine; Griveau, Sophie; Bertrand, Hélène C; Policar, Clotilde; Bedioui, Fethi; Fontecave, Marc

    2017-03-06

    A series of [Re(N^N)(CO) 3 (X)] (N^N = diimine and X = halide) complexes based on 4-(2-pyridyl)-1,2,3-triazole (pyta) and 1-(2-pyridyl)-1,2,3-triazole (tapy) diimine ligands have been prepared and electrochemically characterized. The first ligand-based reduction process is shown to be highly sensitive to the nature of the isomer as well as to the substituents on the pyridyl ring, with the peak potential changing by up to 700 mV. The abilities of this class of complexes to catalyze the electroreduction and photoreduction of CO 2 were assessed for the first time. It is found that only Re pyta complexes that have a first reduction wave with a peak potential at ca. -1.7 V vs SCE are active, producing CO as the major product, together with small amounts of H 2 and formic acid. The catalytic wave that is observed in the CVs is enhanced by the addition of water or trifluoroethanol as a proton source. Long-term controlled potential electrolysis experiments gave total Faradaic yield close to 100%. In particular, functionalization of the triazolyl ring with a 2,4,6-tri-tert-butylphenyl group provided the catalyst with a remarkable stability.

  6. Cu-ZSM-5 zeolite highly active in reduction of NO with decane - Effect of zeolite structural parameters on the catalyst performance

    Czech Academy of Sciences Publication Activity Database

    Čapek, Libor; Dědeček, Jiří; Wichterlová, Blanka; Cider, L.; Jobson, E.; Tokarová, V.

    2005-01-01

    Roč. 60, 3-4 (2005), s. 147-153 ISSN 0926-3373 R&D Projects: GA ČR GD203/03/H140; GA AV ČR 1ET400400413 Grant - others:European Union(XE) GR5D-CT2001-00595 Institutional research plan: CEZ:AV0Z40400503 Keywords : Cu-ZSM-5 * NO reduction * SCR-NOx * lean burn conditions * decane Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.809, year: 2005

  7. The Doha Round Declaration on Cotton: A Catalyst for Poverty Reduction in Africa?

    OpenAIRE

    Blasco, Lorea Barron; Devadoss, Stephen; Stodick, Leroy

    2006-01-01

    Cotton plays a strategic role in the development policies and poverty reduction programs of a number of African countries. Several African countries have introduced reforms in the cotton sector to improve its quality and competitiveness. The impact of these reforms has to date been virtually nullified by the fact that certain WTO Members continue to apply support measures and subsidies that distort global market prices. These are the arguments behind the Cotton Initiative raised in 2003 in th...

  8. Electrochemical promotion of NO reduction by hydrogen on a platinum/polybenzimidazole catalyst

    DEFF Research Database (Denmark)

    Petrushina, Irina; Bandur, Viktor; Cappeln, Frederik Vilhelm

    2003-01-01

    The electrochemical promotion of catalytic NO reduction by hydrogen was studied using a (NO, H-2, Ar), Pt polybenzimidazole (PBI)-H3PO4\\Pt, (H-2, Ar) fuel cell at 135degreesC. A mixture of NO/H-2/Ar was used as the working mixture at one electrode and a mixture of H-2/Ar was used as reference and...... at the negative polarization can be attributed to the electrochemical production of the promoters. At low gas flow rates, a charge-induced change of the strength of chemisorptive bonds can take place.......The electrochemical promotion of catalytic NO reduction by hydrogen was studied using a (NO, H-2, Ar), Pt polybenzimidazole (PBI)-H3PO4\\Pt, (H-2, Ar) fuel cell at 135degreesC. A mixture of NO/H-2/Ar was used as the working mixture at one electrode and a mixture of H-2/Ar was used as reference...... and counter gas at the other electrode. Products of NO reduction (N-2 and H2O) were analyzed by an on-line mass spectrometer. At high NO+H-2+Ar flow rate (17 mL/min; 17 and 354 mL/min, respectively, at atmospheric pressure) the maximum rate enhancement ratio was 4.65. At low NO+H-2+Ar flow rate (17 mL/min; 17...

  9. Impacts of halogen additions on mercury oxidation, in a slipstream selective catalyst reduction (SCR), reactor when burning sub-bituminous coal.

    Science.gov (United States)

    Cao, Yan; Gao, Zhengyang; Zhu, Jiashun; Wang, Quanhai; Huang, Yaji; Chiu, Chengchung; Parker, Bruce; Chu, Paul; Pant, Wei-Ping

    2008-01-01

    This paper presents a comparison of impacts of halogen species on the elemental mercury (Hg(0)) oxidation in a real coal-derived flue gas atmosphere. It is reported there is a higher percentage of Hg(0) in the flue gas when burning sub-bituminous coal (herein Powder River Basin (PRB) coal) and lignite, even with the use of selective catalytic reduction (SCR). The higher Hg(0)concentration in the flue gas makes it difficult to use the wet-FGD process for the mercury emission control in coal-fired utility boilers. Investigation of enhanced Hg(0) oxidation by addition of hydrogen halogens (HF, HCl, HBr, and HI) was conducted in a slipstream reactor with and without SCR catalysts when burning PRB coal. Two commercial SCR catalysts were evaluated. SCR catalyst no. 1 showed higher efficiencies of both NO reduction and Hg(0) oxidation than those of SCR catalyst no. 2. NH3 addition seemed to inhibit the Hg(0) oxidation, which indicated competitive processes between NH3 reduction and Hg(0) oxidation on the surface of SCR catalysts. The hydrogen halogens, in the order of impact on Hg(0) oxidation, were HBr, HI, and HCl or HF. Addition of HBr at approximately 3 ppm could achieve 80% Hg(0) oxidation. Addition of HI at approximately 5 ppm could achieve 40% Hg(0) oxidation. In comparison to the empty reactor, 40% Hg(0) oxidation could be achieved when HCl addition was up to 300 ppm. The enhanced Hg(0) oxidation by addition of HBr and HI seemed not to be correlated to the catalytic effects by both evaluated SCR catalysts. The effectiveness of conversion of hydrogen halogens to halogen molecules or interhalogens seemed to be attributed to their impacts on Hg(0) oxidation.

  10. Design and implementation of mixing chambers to improve thermal decomposition of urea for NOX abatement

    KAUST Repository

    Lee, Junggil

    2012-10-01

    Urea-selective catalytic reduction (SCR) has been reported as the most promising technique for adherence to NOX emissions regulations. In the urea-SCR process, NH3 is generated by urea thermal decomposition and hydrolysis and is then used as a reductant of NOX in the SCR catalyst. Therefore, improving the NOX conversion efficiency of urea-SCR requires enhancement of thermal decomposition upstream of the SCR catalyst. In the present work, two types of mixing chambers were designed and fabricated to improve urea thermal decomposition, and experiments with and without a mixing chamber were carried out to analyze thermal-decomposition characteristics of urea in the exhaust pipe with respect to inlet velocity (4-12μm/s) and temperature (350°C-500°C). Urea thermal decomposition is greatly enhanced at higher gas temperatures. At an inlet velocity of 6μm/s in the A-type mixing chamber, NH3 concentrations generated along the exhaust pipe were about 171% and 157% greater than those without the mixing chamber for inlet temperatures of 400°C and 500°C, respectively. In the case of the B-type mixing chamber, NH3 concentrations generated at inlet temperatures of 400°C and 500°C were about 147% and 179% greater than those without the mixing chamber, respectively. Note that the implementation of mixing chambers significantly enhanced conversion of urea to NH3 because it increased the residence time of urea in the exhaust pipe and improved mixing between urea and exhaust gas. © 2012, Mary Ann Liebert, Inc.

  11. Electrochemically reduced titanocene dichloride as a catalyst of reductive dehalogenation of organic halides

    International Nuclear Information System (INIS)

    Magdesieva, Tatiana V.; Graczyk, Magdalena; Vallat, Alain; Nikitin, Oleg M.; Demyanov, Petr I.; Butin, Kim P.; Vorotyntsev, Mikhail A.

    2006-01-01

    We have studied a reaction between the reduced form of titanocene dichloride (Cp 2 TiCl 2 ) and a group of organic halides: benzyl derivatives (4-X-C 6 H 4 CH 2 Cl, X = H, NO 2 , CH 3 ; 4-X-C 6 H 4 CH 2 Br, X = H, NO 2 , PhC(O); 4-X-C 6 H 4 CH 2 SCN, X = H, NO 2 ) as well as three aryl halides (4-NO 2 C 6 H 4 Hal, Hal = Cl, Br; 4-CH 3 O-C 6 H 4 Cl). It has been shown that the electrochemical reduction of Cp 2 TiCl 2 in the presence of these benzyl halides leads to a catalytic cycle resulting in the reductive dehalogenation of these organic substrates to yield mostly corresponding toluene derivatives as the main product. No dehalogenation has been observed for aryl derivatives. Based on electrochemical data and digital simulation, possible schemes of the catalytic process have been outlined. For non-substituted benzyl halides halogen atom abstraction is a key step. For the reaction of nitrobenzyl halides the complexation of Ti(III) species with the nitro group takes place, with the electron transfer from Ti(III) to this group (owing to its highest coefficient in LUMO of the nitro benzyl halide) followed by an intramolecular dissociative electron redistribution in the course of the heterolytic C-Hal bond cleavage. The results for reduced titanocene dichloride centers immobilized inside a polymer film showed that the catalytic reductive dehalogenation of the p-nitrobenzyl chloride does occur but with a low efficiency because of the partial deactivation of the film due to the blocking of the electron charge transport between the electrode and catalytic centers

  12. Electro catalyst of platinum prepared by CVD for the oxygen reduction reaction

    International Nuclear Information System (INIS)

    Garcia C, M.A.; Fernandez V, S.M.; Vargas G, J.R.

    2004-01-01

    In this work it is reported the preparation and characterization of platinum films obtained by the technique of chemical vapor deposition at low pressure, better well-known as LPCVD for their initials in English (Low Pressure Chemical Vapor Deposition). The technique has several industrial applications and in this work it is explored their possible use to prepare applicable electrocatalysts in fuel cells. The films were characterized by XRD, SEM, EDS and they were proven for to determine their acting in the Oxygen reduction reaction (Orr) in sulfuric acid 0.5 M, the results show that the material presents good activity for the reaction in study. (Author)

  13. Wavelength Effect on Photocatalytic Reduction of CO(2) by Ag/TiO(2) Catalyst

    Czech Academy of Sciences Publication Activity Database

    Kočí, K.; Zatloukalová, K.; Obalová, L.; Krejčíková, Simona; Lacný, Z.; Čapek, L.; Hospodková, Alice; Šolcová, Olga

    2011-01-01

    Roč. 32, 5/SI/ (2011), s. 812-815 ISSN 0253-9837. [6th International Conference on Environmental Catalysis (6th ICEC). Beijing, 12.09.2010-15.09.2010] R&D Projects: GA ČR GA104/09/0694 Institutional research plan: CEZ:AV0Z40720504; CEZ:AV0Z10100521 Keywords : silver doping * titania * carbon dioxide reduction * photocatalysis * wavelength Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 1.171, year: 2011

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

    Directory of Open Access Journals (Sweden)

    H. Jiang

    2017-08-01

    Full Text Available 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

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

    Science.gov (United States)

    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

  16. Experience from performance testing of low NOx burners for refinery heaters; Tests de performance avec des bruleurs de raffinerie a basse emission de NOx

    Energy Technology Data Exchange (ETDEWEB)

    Boden, J.C. [Refining Technology, BP Oil International, Sunbury (United Kingdom)

    2001-07-01

    Developments in low NOx burner technology have resulted in major reductions in NOx emissions from refinery process heaters. However, the techniques used in low NOx burners to reduce NOx emissions can potentially affect other key aspects of burner performance, particularly flame stability and completeness of combustion. BP has evaluated many of the currently available low and ultra-low NOx burners, both natural and forced draught, in its purpose-built test furnace. This extensive test programme has shown that to be a reliable predictor of actual performance a test rig must recreate accurately the real furnace conditions, particularly with respect to furnace and hearth temperatures. The testing has demonstrated the NOx emissions to be expected in practice from different generic types of burner, conventional, low NOx and ultra-low NOx, and has highlighted the sets of conditions most likely to lead to combustion performance problems. (authors)

  17. Towards ‘greener’ catalyst manufacture: Reduction of wastewater from the preparation of Cu/ZnO/Al2O3 methanol synthesis catalysts

    NARCIS (Netherlands)

    Prieto, G.; de Jong, K.P.; de Jongh, P.E.

    2013-01-01

    The generation of large volumes of nitrate-containing wastewater is a major issue in the industrial production of solid catalysts such as Cu/ZnO/Al2O3 employed in methanol synthesis. Extensive washing with water is needed to remove nitrate (and sodium) residues in the as-precipitated metal

  18. Molecular Cobalt Catalysts for O 2 Reduction: Low-Overpotential Production of H 2 O 2 and Comparison with Iron-Based Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Yu-Heng [Department; Pegis, Michael L. [Department; Mayer, James M. [Department; Stahl, Shannon S. [Department

    2017-11-07

    A series of mononuclear pseudo-macrocyclic cobalt complexes have been investigated as catalysts for O2 reduction. Each of these complexes, with CoIII/II reduction potentials that span nearly 400 mV, mediate highly selective two- electron reduction of O2 to H2O2 (93–99%) using decamethylferrocene (Fc*) as the reductant and acetic acid as the proton source. Kinetic studies reveal that the rate exhibits a first- order dependence on [Co] and [AcOH], but no dependence on [O2] or [Fc*]. A linear correlation is observed between log(TOF) vs. E1/2(CoIII/II) for the different cobalt complexes (TOF = turnover frequency). The thermodynamic potential for+ O2 reduction to H2O2 was estimated by measuring the H /H2 open-circuit potential under the reaction conditions. This value provides the basis for direct assessment of the thermodynamic efficiency of the different catalysts and shows that H2O2 is formed with overpotentials as low as 90 mV. These results are compared with a recently reported series of Fe-porphyrin complexes, which catalyze four-electron reduction of O2 to H2O. The data show that the TOFs of the Co complexes exhibit a shallower dependence on E1/2(MIII/II) than the Fe complexes. This behavior, which underlies the low overpotential, is rationalized on the basis of the catalytic rate law.

  19. MECHANISTIC STUDIES AND DESIGN OF HIGHLY ACTIVE CUPRATE CATALYSTS FOR THE DIRECT DECOMPOSITION AND SELECTIVE REDUCTION OF NITRIC OXIDE AND HYDROCARBONS TO NITROGEN FOR ABATEMENT OF STACK EMISSIONS

    Energy Technology Data Exchange (ETDEWEB)

    None

    1998-04-30

    A flow trough type catalytic reactor system was adequately modified for NO related catalytic and adsorption measurements, including the on-line connection of a digital chemiluminescent NO-NO{sub x} analyzer to the reactor outlet system. Moreover, we have largely completed the installation of an FTIR coupled catalytic system containing a HTEC cell for high temperature DRIFT studies. Three different barium cuprate samples, Ba{sub 2}CuO{sub 3}, BaCuO{sub 2}, and Ba{sub 2}Cu{sub 3}O{sub 5} were synthesized and characterized by powder XRD for catalytic tests. Prior to catalytic studies over these cuprates, a new, liquid indium based supported molten metal catalyst (In-SMMC) was tested in the reduction of NO by various reductants. In the presence of excess O{sub 2} and H{sub 2}O, the In-SMMC proved to be more active for the selective catalytic reduction (SCR) of NO to N{sub 2} by ethanol than most other catalysts. Using C{sub 1}-C{sub 3} alcohols as reductants, self sustained periodic oscillations observed in the NO{sub x} concentrations of reactor effluents indicated the first time that radical intermediates can be involved in the SCR of NO by alcohols. Further, In-SMMC is the only effective and water tolerant SCR catalyst reported thus far which contains SiO{sub 2} support. Thus, this novel catalyst opens up a promising new alternative for developing an effective and durable catalyst for NO{sub x} abatement in stack emission.

  20. Electrochemically reduced titanocene dichloride as a catalyst of reductive dehalogenation of organic halides

    Energy Technology Data Exchange (ETDEWEB)

    Magdesieva, Tatiana V. [Department Chemistry, M.V. Lomonosov Moscow State University, Moscow 119992 (Russian Federation)]. E-mail: tvm@org.chem.msu.ru; Graczyk, Magdalena [LSEO-UMR 5188 CNRS, Universite de Bourgogne, Dijon (France); Vallat, Alain [LSEO-UMR 5188 CNRS, Universite de Bourgogne, Dijon (France); Nikitin, Oleg M. [Department Chemistry, M.V. Lomonosov Moscow State University, Moscow 119992 (Russian Federation); Demyanov, Petr I. [Department Chemistry, M.V. Lomonosov Moscow State University, Moscow 119992 (Russian Federation); Butin, Kim P. [Department Chemistry, M.V. Lomonosov Moscow State University, Moscow 119992 (Russian Federation); Vorotyntsev, Mikhail A. [LSEO-UMR 5188 CNRS, Universite de Bourgogne, Dijon (France)]. E-mail: MV@u-bourgogne.fr

    2006-11-12

    We have studied a reaction between the reduced form of titanocene dichloride (Cp{sub 2}TiCl{sub 2}) and a group of organic halides: benzyl derivatives (4-X-C{sub 6}H{sub 4}CH{sub 2}Cl, X = H, NO{sub 2}, CH{sub 3}; 4-X-C{sub 6}H{sub 4}CH{sub 2}Br, X = H, NO{sub 2}, PhC(O); 4-X-C{sub 6}H{sub 4}CH{sub 2}SCN, X = H, NO{sub 2}) as well as three aryl halides (4-NO{sub 2}C{sub 6}H{sub 4}Hal, Hal = Cl, Br; 4-CH{sub 3}O-C{sub 6}H{sub 4}Cl). It has been shown that the electrochemical reduction of Cp{sub 2}TiCl{sub 2} in the presence of these benzyl halides leads to a catalytic cycle resulting in the reductive dehalogenation of these organic substrates to yield mostly corresponding toluene derivatives as the main product. No dehalogenation has been observed for aryl derivatives. Based on electrochemical data and digital simulation, possible schemes of the catalytic process have been outlined. For non-substituted benzyl halides halogen atom abstraction is a key step. For the reaction of nitrobenzyl halides the complexation of Ti(III) species with the nitro group takes place, with the electron transfer from Ti(III) to this group (owing to its highest coefficient in LUMO of the nitro benzyl halide) followed by an intramolecular dissociative electron redistribution in the course of the heterolytic C-Hal bond cleavage. The results for reduced titanocene dichloride centers immobilized inside a polymer film showed that the catalytic reductive dehalogenation of the p-nitrobenzyl chloride does occur but with a low efficiency because of the partial deactivation of the film due to the blocking of the electron charge transport between the electrode and catalytic centers.

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

    Directory of Open Access Journals (Sweden)

    Ralf Moos

    2013-04-01

    Full Text Available 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.

  2. Metal-Carbon-CNF Composites Obtained by Catalytic Pyrolysis of Urban Plastic Residues as Electro-Catalysts for the Reduction of CO2

    Directory of Open Access Journals (Sweden)

    Jesica Castelo-Quibén

    2018-05-01

    Full Text Available Metal–carbon–carbon nanofibers composites obtained by catalytic pyrolysis of urban plastic residues have been prepared using Fe, Co or Ni as pyrolitic catalysts. The composite materials have been fully characterized from a textural and chemical point of view. The proportion of carbon nanofibers and the final content of carbon phases depend on the used pyrolitic metal with Ni being the most active pyrolitic catalysts. The composites show the electro-catalyst activity in the CO2 reduction to hydrocarbons, favoring all the formation of C1 to C4 hydrocarbons. The tendency of this activity is in accordance with the apparent faradaic efficiencies and the linear sweep voltammetries. The cobalt-based composite shows high selectivity to C3 hydrocarbons within this group of compounds.

  3. High-performance oxygen reduction catalysts in both alkaline and acidic fuel cells based on pre-treating carbon material and iron precursor

    Energy Technology Data Exchange (ETDEWEB)

    Song, Ping; Barkholtz, Heather M.; Wang, Ying; Xu, Weilin; Liu, Dijia; Zhuang, Lin

    2017-12-01

    We demonstrate a new and simple method for pre-treating the carbon material and iron precursor to prepare oxygen reduction reaction (ORR) catalysts, which can produce super-high performance and stability in alkaline solution, with high performance in acid solution. This strategy using cheap materials is simply controllable. Moreover, it has achieved smaller uniform nanoparticles to exhibit high stability, and the synergetic effect of Fe and N offered much higher performance in ORR than commercial Pt/C, with high maximum power density in alkaline and acid fuel cell test. So it can make this kind of catalysts be the most promising alternatives of Pt-based catalysts with best performance/price.

  4. Re-examination of the Pt Particle Size Effect on the Oxygen Reduction Reaction for Ultrathin Uniform Pt/C Catalyst Layers without Influence from Nafion

    International Nuclear Information System (INIS)

    Shinozaki, Kazuma; Morimoto, Yu; Pivovar, Bryan S.; Kocha, Shyam S.

    2016-01-01

    Highlights: • Pt particle size effect on ORR was re-evaluated for Pt/C catalysts. • Nafion-free activity of Pt/C catalysts was evaluated using thin-film RDE methods. • Ultrathin-uniform catalyst layers were employed to obtain accurate activity values. • Specific activity increased steeply from 2 to 10 nm and less steeply at over 10 nm. • Re-evaluated effect agrees with a particle model assuming terrace active sites. - Abstract: The platinum ‘particle size effect’ on the oxygen reduction reaction (ORR) has been re-evaluated using commercial Pt/C catalysts (2–10 nm Pt particle) and polycrystalline Pt (poly-Pt) in 0.1 M HClO 4 with a rotating disk electrode method. Nafion-free catalyst layers were employed to obtain specific activities (SA) that were not perturbed (suppressed) by sulfonate anion adsorption/blocking. By using ultrathin uniform catalyst layers, O 2 diffusion limitation was minimized as confirmed from the high SAs of our supported catalysts that were comparable to unsupported sputtered Pt having controlled sizes. The specific activity (SA) steeply increased for the particle sizes in the range ∼2–10 nm (0.8–1.8 mA/cm 2 Pt at 0.9 V vs. RHE) and plateaued over ∼10 nm to 2.7 mA/cm 2 Pt for bulk poly-Pt. On the basis of the activity trend for the range of particle sizes studied, it appears that the effect of carbon support on activity is negligible. The experimental results and the concomitant profile of SA vs. particle size was found to be in an agreement to a truncated octahedral particle model that assumes active terrace sites.

  5. Application of numerical modeling of selective NOx reduction by hydrocarbon under diesel transient conditions in consideration of hydrocarbon adsorption and desorption process

    International Nuclear Information System (INIS)

    Watanabe, Y.; Asano, A.; Banno, K.; Yokota, K.; Sugiura, M.

    2001-01-01

    A model of NO x selective reduction by hydrocarbon (HC) was developed, which takes into account the adsorption and desorption of HC. The model was applied for predicting the performance of a De-NO x catalytic reactor, working under transient conditions such as a legislative driving cycle. Diesel fuel was used as a supplemental reductant. The behavior of HC and NO x reactions and HC adsorption and desorption has been simulated successfully by our numerical approach under the transient conditions of the simulated Japanese 10-15 driving cycle. Our model is expected to optimize the design of selective diesel NO x reduction systems using a diesel fuel as a supplemental reductant

  6. A review of carbon-based and non-carbon-based catalyst supports for the selective catalytic reduction of nitric oxide.

    Science.gov (United States)

    Anthonysamy, Shahreen Binti Izwan; Afandi, Syahidah Binti; Khavarian, Mehrnoush; Mohamed, Abdul Rahman Bin

    2018-01-01

    Various types of carbon-based and non-carbon-based catalyst supports for nitric oxide (NO) removal through selective catalytic reduction (SCR) with ammonia are examined in this review. A number of carbon-based materials, such as carbon nanotubes (CNTs), activated carbon (AC), and graphene (GR) and non-carbon-based materials, such as Zeolite Socony Mobil-5 (ZSM-5), TiO 2 , and Al 2 O 3 supported materials, were identified as the most up-to-date and recently used catalysts for the removal of NO gas. The main focus of this review is the study of catalyst preparation methods, as this is highly correlated to the behaviour of NO removal. The general mechanisms involved in the system, the Langmuir-Hinshelwood or Eley-Riedeal mechanism, are also discussed. Characterisation analysis affecting the surface and chemical structure of the catalyst is also detailed in this work. Finally, a few major conclusions are drawn and future directions for work on the advancement of the SCR-NH 3 catalyst are suggested.

  7. Rudimentary simple, single step fabrication of nano-flakes like AgCd alloy electro-catalyst for oxygen reduction reaction in alkaline fuel cell

    International Nuclear Information System (INIS)

    Bhandary, Nimai; Basu, Suddhasatwa; Ingole, Pravin P.

    2016-01-01

    In this work, for the first time, we report rudimentary simple, single step fabrication of an electro-catalyst based on AgCd alloy nanoparticles with flakes like geometry which shows highly efficient activity towards oxygen reduction reaction (ORR). A simple potentiostatic deposition method has been employed for co-depositing AgCd alloy nanostructures with flakes like shapes along with dendrites on the surface of carbon fibre paper. The chemico-physical properties of the catalyst are investigated by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDXS). Electro-catalytic activity of AgCd alloy based electro-catalyst towards ORR is studied in alkaline medium by cyclic voltammetry and rotating ring disk electrode (RRDE) technique. Electrochemical in-situ FTIR measurements are also performed to identify the species generated during ORR process. Based on the results from electro-catalysis experiment, it is concluded that nano-alloyed AgCd electrodeposited on carbon paper shows excellent activity for ORR, following four electron pathways with H_2O_2 yield less than 15%. The combination of low cost of Ag and Cd, fast and facile method of its fabrication and higher activity towards ORR makes the AgCd electro-catalyst an attractive catalyst of choice for alkaline fuel cell.

  8. Enhanced photocatalytic CO2 reduction to CH4 over separated dual co-catalysts Au and RuO2

    Science.gov (United States)

    Dong, Chunyang; Hu, Songchang; Xing, Mingyang; Zhang, Jinlong

    2018-04-01

    A spatially separated, dual co-catalyst photocatalytic system was constructed by the stepwise introduction of RuO2 and Au nanoparticles (NPs) at the internal and external surfaces of a three dimensional, hierarchically ordered TiO2-SiO2 (HTSO) framework (the final photocatalyst was denoted as Au/HRTSO). Characterization by HR-TEM, EDS-mapping, XRD and XPS confirmed the existence and spatially separated locations of Au and RuO2. In CO2 photocatalytic reduction (CO2PR), Au/HRTSO (0.8%) shows the optimal performance in both the activity and selectivity towards CH4; the CH4 yield is almost twice that of the singular Au/HTSO or HRTSO (0.8%, weight percentage of RuO2) counterparts. Generally, Au NPs at the external surface act as electron trapping agents and RuO2 NPs at the inner surface act as hole collectors. This advanced spatial configuration could promote charge separation and transfer efficiency, leading to enhanced CO2PR performance in both the yield and selectivity toward CH4 under simulated solar light irradiation.

  9. Al- or Si-decorated graphene oxide: A favorable metal-free catalyst for the N2O reduction

    Science.gov (United States)

    Esrafili, Mehdi D.; Sharifi, Fahimeh; Nematollahi, Parisa

    2016-11-01

    The structural and catalytic properties of Al- or Si-decorated graphene oxide (Al-/Si-GO) are studied by means of density functional theory calculations. The relatively large adsorption energy together with the small Alsbnd O or Sisbnd O binding distances indicate that the epoxy groups over the GO surface can strongly stabilize the single Al or Si atom. Hence, Al-GO and Si-GO are stable enough to be utilized in catalytic reduction of N2O by CO molecule. It is found that the adsorption and decomposition of N2O molecule over Si-GO is more favorable than over Al-GO, due to its larger adsorption energy (Eads) and charge transfer (qCT) values. On the other hand, the CO molecule is physically adsorbed over both surfaces, with relatively small Eads and qCT values. Therefore, at the presence of N2O and CO molecules as the reaction gas, the Al or Si atom of the surface should be dominantly covered by N2O molecule. Our results indicate that the N2O decomposition process can take place with a negligible activation energy over Al-/Si-GO surface, where the N2 molecule can be easily released from the surface. Then, the activated oxygen atom (Oads) which remains over the surface reacts with the CO molecule to form the CO2 molecule via the reaction Oads + CO → CO2. Based on the calculated activation energies, it is suggested that both Al-GO and Si-GO can be used as an efficient metal-free catalyst for the reduction of N2O molecule at ambient conditions.

  10. Iridium-decorated palladium-platinum core-shell catalysts for oxygen reduction reaction in proton exchange membrane fuel cell.

    Science.gov (United States)

    Wang, Chen-Hao; Hsu, Hsin-Cheng; Wang, Kai-Ching

    2014-08-01

    Carbon-supported Pt, Pd, Pd-Pt core-shell (Pt(shell)-Pd(core)/C) and Ir-decorated Pd-Pt core-shell (Ir-decorated Pt(shell)-Pd(core)/C) catalysts were synthesized, and their physical properties, electrochemical behaviors, oxygen reduction reaction (ORR) characteristics and proton exchange membrane fuel cell (PEMFC) performances were investigated herein. From the XRD patterns and TEM images, Ir-decorated Pt(shell)-Pd(core)/C has been confirmed that Pt was deposited on the Pd nanoparticle which had the core-shell structure. Ir-decorated Pt(shell)-Pd(core)/C has more positive OH reduction peak than Pt/C, which is beneficial to weaken the binding energy of Pt-OH during the ORR. Thus, Ir-decorated Pt(shell)-Pd(core)/C has higher ORR activity than Pt/C. The maximum power density of H2-O2 PEMFC using Ir-decorated Pt(shell)-Pd(core)/C is 792.2 mW cm(-2) at 70°C, which is 24% higher than that using Pt/C. The single-cell accelerated degradation test of PEMFC using Ir-decorated Pt(shell)-Pd(core)/C shows good durability by the potential cycling of 40,000 cycles. This study concludes that Ir-decorated Pt(shell)-Pd(core)/C has the low Pt content, but it can facilitate the low-cost and high-efficient PEMFC. Copyright © 2013 Elsevier Inc. All rights reserved.

  11. Fe3C-based oxygen reduction catalysts: synthesis, hollow spherical structures and applications in fuel cells

    DEFF Research Database (Denmark)

    Hu, Yang; Jensen, Jens Oluf; Zhang, Wei

    2015-01-01

    We present a detailed study of a novel Fe3C-based spherical catalyst with respect to synthetic parameters, nanostructure formation, ORR active sites and fuel cell demonstration. The catalyst is synthesized by high temperature autoclave pyrolysis using decomposing precursors. Below 500 °C, melamine...

  12. Reductive dehalogenation of aryl halides over palladium catalysts deposited on SBA-15 type molecular sieve modified with amine donor groups

    Czech Academy of Sciences Publication Activity Database

    Štěpnička, P.; Semler, M.; Demel, J.; Zukal, Arnošt; Čejka, Jiří

    2011-01-01

    Roč. 341, č. 1-2 (2011), s. 97-102 ISSN 1381-1169 R&D Projects: GA ČR GA104/09/0561 Institutional research plan: CEZ:AV0Z40400503 Keywords : heterogeneous catalysts * supported catalysts * palladium Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.947, year: 2011

  13. The Effect of Acidic and Redox Properties of V2O5/CeO2-ZrO2 Catalysts in Selective Catalytic Reduction of NO by NH3

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Riisager, Anders; Fehrmann, Rasmus

    2009-01-01

    V2O5 supported ZrO2 and CeO2–ZrO2 catalysts were prepared and characterized by N2 physisorption, XRPD, TPR, and NH3-TPD methods. The influence of calcination temperature from 400 to 600 °C on crystallinity, acidic and redox properties were studied and compared with the catalytic activity...... in the selective catalytic reduction (SCR) of NO with ammonia. The surface area of the catalysts decreased gradually with increasing calcination temperature. The SCR activity of V2O5/ZrO2 catalysts was found to be related with the support crystallinity, whereas V2O5/CeO2–ZrO2 catalysts were also dependent...... on acidic and redox properties of the catalyst. The V2O5/CeO2–ZrO2 catalysts showed high activity and selectivity for reduction of NO with NH3....

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

    Energy Technology Data Exchange (ETDEWEB)

    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

  15. A novel differential electrochemical mass spectrometry method to determine the product distribution from parasitic Methanol oxidation reaction on oxygen reduction reaction catalysts

    Science.gov (United States)

    Jurzinsky, Tilman; Kurzhals, Philipp; Cremers, Carsten

    2018-06-01

    The oxygen reduction reaction is in research focus since several decades due to its importance for the overall fuel cell performance. In direct methanol fuel cells, the crossover of methanol and its subsequent parasitic oxidation are main issues when it comes to preventing fuel cell performance losses. In this work, we present a novel differential electrochemical mass spectrometry method to evaluate oxygen reduction reaction catalysts on their tolerance to methanol being present at the cathode. Besides this, the setup allows to measure under more realistic fuel cell conditions than typical rotating disc electrode measurements, because the oxygen reduction reaction is evaluated in gaseous phase and a gas diffusion electrode is used as working electrode. Due to the new method, it was possible to investigate the oxygen reduction reaction on two commonly used catalysts (Pt/C and Pt3Co/C) in absence and presence of methanol. It was found, that Pt3Co/C is less prone to parasitic current losses due to methanol oxidation reaction. By connecting a mass spectrometer to the electrochemical cell, the new method allows to determine the products formed on the catalysts due to parasitic methanol electrooxidation.

  16. Bio-inspired CO2 reduction by a rhenium tricarbonyl bipyridine-based catalyst appended to amino acids and peptidic platforms: incorporating proton relays and hydrogen-bonding functional groups.

    Science.gov (United States)

    Chabolla, S A; Machan, C W; Yin, J; Dellamary, E A; Sahu, S; Gianneschi, N C; Gilson, M K; Tezcan, F A; Kubiak, C P

    2017-06-02

    Herein, we report a new approach to bio-inspired catalyst design. The molecular catalyst employed in these studies is based on the robust and selective Re(bpy)(CO) 3 Cl-type (bpy = 2,2'-bipyridine) homogeneous catalysts, which have been extensively studied for their ability to reduce CO 2 electrochemically or photochemically in the presence of a photosensitizer. These catalysts can be highly active photocatalysts in their own right. In this work, the bipyridine ligand was modified with amino acids and synthetic peptides. These results build on earlier findings wherein the bipyridine ligand was functionalized with amide groups to promote dimer formation and CO 2 reduction by an alternate bimolecular mechanism at lower overpotential (ca. 250 mV) than the more commonly observed unimolecular process. The bio-inspired catalysts were designed to allow for the incorporation of proton relays to support reduction of CO 2 to CO and H 2 O. The coupling of amino acids tyrosine and phenylalanine led to the formation of two structurally similar Re catalyst/peptide catalysts for comparison of proton transport during catalysis. This article reports the synthesis and characterization of novel catalyst/peptide hybrids by molecular dynamics (MD simulations of structural dynamics), NMR studies of solution phase structures, and electrochemical studies to measure the activities of new bio-inspired catalysts in the reduction of CO 2.

  17. Uniformly active phase loaded selective catalytic reduction catalysts (V_2O_5/TNTs) with superior alkaline resistance performance

    International Nuclear Information System (INIS)

    Wang, Haiqiang; Wang, Penglu; Chen, Xiongbo; Wu, Zhongbiao

    2017-01-01

    Highlights: • VOSO_4 exhibited better synergistic effect with titanate nanotubes than NH_4VO_3. • Ion-exchange reaction occurs between VOSO_4 and titanate nanotubes. • Ion-exchange resulting in uniformly vanadium distribution on titanate nanotubes. • VOSO_4-based catalyst exhibited impressive SCR activity and alkaline resistance. - Abstract: In this work, protonated titanate nanotubes was performed as a potential useful support and different vanadium precursors (NH_4VO_3 and VOSO_4) were used to synthesize deNO_x catalysts. The results showed that VOSO_4 exhibited better synergistic effect with titanate nanotubes than NH_4VO_3, which was caused by the ion-exchange reaction. Then high loading content of vanadium, uniformly active phase distribution, better dispersion of vanadium, more acid sites, better V"5"+/V"4"+ redox cycles and superior oxygen mobility were achieved. Besides, VOSO_4-based titanate nanotubes catalysts also showed enhanced alkaline resistance than particles (P25) based catalysts. It was strongly associated with its abundant acid sites, large surface area, flexible redox cycles and oxygen transfer ability. For the loading on protonated titanate nanotubes, active metal with cation groups was better precursors than anion ones. V_2O_5/TNTs catalyst was a promising substitute for the commercial vanadium catalysts and the work conducted herein provided a useful idea to design uniformly active phase loaded catalyst.

  18. An investigation of the activity and stability of Pd and Pd-Zr modified Y-zeolite catalysts for the removal of PAH, CO, CH4 and NOx emissions

    International Nuclear Information System (INIS)

    Klingstedt, F.; Kalantar Neyestanaki, A.; Lindfors, L.-E.; Salmi, T.; Heikkila, T.; Laine, E.

    2003-01-01

    Pd-Y- and Pd-Zr-Y-zeolite catalysts were prepared by the ion-exchange of parent NH 3 -Y-zeolite, thermally pre-treated Y-zeolite and hydrothermally pre-treated Y-zeolite. The activity of the catalysts was studied in conversion of gas mixtures simulating the flue gases from the combustion of biofuels and natural gas driven vehicles (NGVs) at temperature ranges of 120-800C. The effect of sulphur-poisoning was examined by the addition of 5ppm SO 2 into the feed gas mixtures. High activity in the removal of the model pollutants was obtained over the fresh catalysts. De-activation was observed as a result of catalyst ageing in the reactants' flow (800C, 6h) or steam treatment (850C, 12vol.% H 2 O, 16h). The de-activation was attributed to the de-alumination as well as to the migration of Pd 2+ cations. The catalysts were characterised by XRD, SEM-EDXA, N 2 -physisorption, O 2 /SO 2 /NH 3 /naphthalene-TPD, XRF and DCP

  19. Building Selectivity for NO Sensing in a NOx Mixture with Sonochemically Prepared CuO Structures

    Directory of Open Access Journals (Sweden)

    Max R. Mullen

    2015-12-01

    Full Text Available Several technologies are available for decreasing nitrogen oxide (NOx emissions from combustion sources, including selective catalytic reduction methods. In this process, ammonia reacts with nitric oxide (NO and nitrogen dioxide (NO2. As the stoichiometry of the two reactions is different, electrochemical sensor systems that can distinguish between NO and NO2 in a mixture of these two gases are of interest. Since NO and NO2 can be brought to equilibrium, depending on the temperature and the surfaces that they are in contact with, the detection of NO and NO2 independently is a difficult problem and has not been solved to date. In this study, we explore a high surface area sonochemically prepared CuO as the resistive sensing medium. CuO is a poor catalyst for NOx equilibration, and requires temperatures of 500 C to bring about equilibration. Thus, at 300 C, NO and NO2 retain their levels after interaction with CuO surface. In addition, NO adsorbs more strongly on the CuO over NO2. Using these two concepts, we can detect NO with minimal interference from NO2, if the latter gas concentration does not exceed 20% in a NOx mixture over a range of 100–800 ppm. Since this range constitutes most of the range of total NOx concentrations in diesel and other lean burn engines, this sensor should find application in selective detection of NO in this combustion application. A limitation of this sensor is the interference with CO, but with combustion in excess air, this problem should be alleviated.

  20. Reduction of light cycle oil in catalytic cracking of bitumen-derived crude HGOs through catalyst selection

    Energy Technology Data Exchange (ETDEWEB)

    Ding, Fuchen; Xu, Chunming [State Key Laboratory of Heavy Oil Processing, China University of Petroleum Beijing, 102200 (China); Ng, Siauw H. [National Centre for Upgrading Technology, 1 Oil Patch Drive, Suite A202, Devon, Alberta (Canada); Yui, Sok [Syncrude Research Centre, 9421-17 Avenue, Edmonton, Alberta (Canada)

    2007-09-15

    In an attempt to reduce the production of light cycle oil (LCO), a non-premium fluid catalytic cracking (FCC) product in North America, a large-pore catalyst containing rare-earth-exchanged Y (REY) zeolite, was used to crack two Canadian bitumen-derived crude heavy gas oils (HGOs) hydrotreated to different extents. For comparison, a regular equilibrium FCC catalyst with ultra-stable Y (USY) zeolite and a conventional western Canadian crude HGO were also included in the study. Cracking experiments were conducted in a fixed-bed microactivity test (MAT) reactor at 510 C, 30 s oil injection time, and varying catalyst-to-oil ratios for different conversions. The results show that pre-cracking of heavy molecules with wide-pore matrix, followed by zeolite cracking, enhanced conversion at the expense of light and heavy cycle oils at a constant catalyst-to-oil ratio, giving improved product selectivities (e.g., higher gasoline and lower dry gas, LCO, and coke yields, in general, at a given conversion). To systematically assess the benefits of employing the specialty catalyst over the regular catalyst in cracking Canadian HGOs, individual product yields were compared at common bases, including constant catalyst-to-oil ratios, conversions, and coke yields for three feeds, and at maximum gasoline yield for one feed. In most cases, the preferred choice of large-pore zeolite-rich catalyst over its counterpart was evident. The observed cracking phenomena were explained based on properties of catalysts and characterization data of feedstocks, including their hydrocarbon type analyses by gas chromatograph with a mass-selective detector (GC-MSD). (author)

  1. Iron(II) phthalocyanine covalently functionalized graphene as a highly efficient non-precious-metal catalyst for the oxygen reduction reaction in alkaline media

    International Nuclear Information System (INIS)

    Liu, Ying; Wu, Yan-Ying; Lv, Guo-Jun; Pu, Tao; He, Xing-Quan; Cui, Li-Li

    2013-01-01

    Graphical abstract: The fabricated FePc-Gr catalyst for ORR exhibited high activity, favoring a direct 4-electron process, good stability and selectivity, all of which should be attributed to its high conductivity, the synergistic effect between FePc and graphene, as well as the formation of stable FePc-Gr composite through covalent bonding and π–π interaction. - Abstract: A novel iron(II) phthalocyanine covalently modified graphene (FePc-Gr) was synthesized by reduction of the product obtained through an amidation reaction between carboxyl-functionalized graphene oxide (CFGO) and iron(II) tetra-aminophthalocyanine (FeTAPc). The FePc-Gr hybird was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectroscopy (RS) and X-ray photoelectron spectroscopy (XPS), respectively. The electrocatalytic properties of FePc-Gr toward the oxygen reduction reaction (ORR) were evaluated using cyclic voltammetry (CV) and linear sweep voltammetry methods. The peak potential of the ORR on the FePc-Gr catalyst was found to be about −0.12 V vs. SCE in 0.1 M NaOH solution, which was 180 and 360 mV more positive than that on FeTAPc and bare GCE, respectively. The rotating disk electrode (RDE) and rotating ring disk electrode (RRDE) measurements revealed that the ORR mechanism was nearly via a direct four-electron pathway to water on FePc-Gr. The current still remained 83.5% of its initial after chronoamperometric test for 10,000 s. Nevertheless, Pt/C catalyst only retained 40.5% of its initial current. The peak potential and peak current changed slightly when 3 M methanol was introduced. So the FePc-Gr composite catalyst for ORR exhibited high activity, good stability and methanol-tolerance, which could be used as a promising Pt-free catalyst for ORR in alkaline direct methanol fuel cell (DMFC)

  2. High-performance Platinum-free oxygen reduction reaction and hydrogen oxidation reaction catalyst in polymer electrolyte membrane fuel cell.

    Science.gov (United States)

    Chandran, Priji; Ghosh, Arpita; Ramaprabhu, Sundara

    2018-02-26

    The integration of polymer electrolyte membrane fuel cell (PEMFC) stack into vehicles necessitates the replacement of high-priced platinum (Pt)-based electrocatalyst, which contributes to about 45% of the cost of the stack. The implementation of high-performance and durable Pt metal-free catalyst for both oxygen reduction reaction (ORR) and hydrogen oxidation reaction (HOR) could significantly enable large-scale commercialization of fuel cell-powered vehicles. Towards this goal, a simple, scalable, single-step synthesis method was adopted to develop palladium-cobalt alloy supported on nitrogen-doped reduced graphene oxide (Pd 3 Co/NG) nanocomposite. Rotating ring-disk electrode (RRDE) studies for the electrochemical activity towards ORR indicates that ORR proceeds via nearly four-electron mechanism. Besides, the mass activity of Pd 3 Co/NG shows an enhancement of 1.6 times compared to that of Pd/NG. The full fuel cell measurements were carried out using Pd 3 Co/NG at the anode, cathode in conjunction with Pt/C and simultaneously at both anode and cathode. A maximum power density of 68 mW/cm 2 is accomplished from the simultaneous use of Pd 3 Co/NG as both anode and cathode electrocatalyst with individual loading of 0.5 mg/cm 2 at 60 °C without any backpressure. To the best of our knowledge, the present study is the first of its kind of a fully non-Pt based PEM full cell.

  3. Enhanced Combustion Low NOx Pulverized Coal Burner

    Energy Technology Data Exchange (ETDEWEB)

    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

  4. A Platinum Monolayer Core-Shell Catalyst with a Ternary Alloy Nanoparticle Core and Enhanced Stability for the Oxygen Reduction Reaction

    Directory of Open Access Journals (Sweden)

    Haoxiong Nan

    2015-01-01

    Full Text Available We synthesize a platinum monolayer core-shell catalyst with a ternary alloy nanoparticle core of Pd, Ir, and Ni. A Pt monolayer is deposited on carbon-supported PdIrNi nanoparticles using an underpotential deposition method, in which a copper monolayer is applied to the ternary nanoparticles; this is followed by the galvanic displacement of Cu with Pt to generate a Pt monolayer on the surface of the core. The core-shell Pd1Ir1Ni2@Pt/C catalyst exhibits excellent oxygen reduction reaction activity, yielding a mass activity significantly higher than that of Pt monolayer catalysts containing PdIr or PdNi nanoparticles as cores and four times higher than that of a commercial Pt/C electrocatalyst. In 0.1 M HClO4, the half-wave potential reaches 0.91 V, about 30 mV higher than that of Pt/C. We verify the structure and composition of the carbon-supported PdIrNi nanoparticles using X-ray powder diffraction, X-ray photoelectron spectroscopy, thermogravimetry, transmission electron microscopy, and energy dispersive X-ray spectrometry, and we perform a stability test that confirms the excellent stability of our core-shell catalyst. We suggest that the porous structure resulting from the dissolution of Ni in the alloy nanoparticles may be the main reason for the catalyst’s enhanced performance.

  5. Synthesis and kinetics investigation of meso-microporous Cu-SAPO-34 catalysts for the selective catalytic reduction of NO with ammonia.

    Science.gov (United States)

    Liu, Jixing; Yu, Fuhong; Liu, Jian; Cui, Lifeng; Zhao, Zhen; Wei, Yuechang; Sun, Qianyao

    2016-10-01

    A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH 3 -SCR performance at low temperature. Their structure and physic chemical properties were characterized by means of X-ray diffraction patterns (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), N 2 sorption-desorption, nuclear magnetic resonance (NMR), Inductively Coupled Plasma-Atomic Emission spectrometer (ICP-AES), X-ray absorption spectroscopy (XPS), Temperature-programmed desorption of ammonia (NH 3 -TPD), Ultraviolet visible diffuse reflectance spectroscopy (UV-Vis DRS) and Temperature programmed reduction (TPR). The analysis results indicate that the high activities of Cu-SAPO-34 catalysts could be attributed to the enhancement of redox property, the formation of mesopores and the more acid sites. Furthermore, the kinetic results verify that the formation of mesopores remarkably reduces diffusion resistance and then improves the accessibility of reactants to catalytically active sites. The 1.0-Cu-SAPO-34 catalyst exhibited the high NO conversion (>90%) among the wide activity temperature window in the range of 150-425°C. Copyright © 2016. Published by Elsevier B.V.

  6. In situ DRIFTS investigation of NH3-SCR reaction over CeO2/zirconium phosphate catalyst

    Science.gov (United States)

    Zhang, Qiulin; Fan, Jie; Ning, Ping; Song, Zhongxian; Liu, Xin; Wang, Lanying; Wang, Jing; Wang, Huimin; Long, Kaixian

    2018-03-01

    A series of ceria modified zirconium phosphate catalysts were synthesized for selective catalytic reduction of NO with ammonia (NH3-SCR). Over 98% NOx conversion and 98% N2 selectivity were obtained by the CeO2/ZrP catalyst with 20 wt.% CeO2 loading at 250-425 °C. The interaction between CeO2 and zirconium phosphate enhanced the redox abilities and surface acidities of the catalysts, resulting in the improvement of NH3-SCR activity. The in situ DRIFTS results indicated that the NH3-SCR reaction over the catalysts followed both Eley-Rideal and Langmuir-Hinshelwood mechanisms. The amide (sbnd NH2) groups and the NH4+ bonded to Brønsted acid sites were the important intermediates of Eley-Rideal mechanism.

  7. Carbon-doped boron nitride nanosheet as a promising catalyst for N2O reduction by CO or SO2 molecule: A comparative DFT study

    Science.gov (United States)

    Esrafili, Mehdi D.; Saeidi, Nasibeh

    2018-06-01

    We report for the first time, the catalytic activity of the experimentally available carbon-doped boron nitride nanosheet (C-BNNS) towards the reduction of N2O in the presence of CO or SO2 molecule. According to our density functional theory calculations, C-doping can introduce high spin density into BN monolayer which is mainly localized over the C and its neighboring N atoms. The Hirshfeld charge density analysis reveals that the electron-rich C-BNNS acts as an electron donating support to activate N2O molecule which is an important step in the reduction of N2O. The N2O reduction reaction starts with the dissociative adsorption of N2O over the C-BNNS surface, yielding the N2 molecule and an activated oxygen moiety (Oads) adsorbed over the C atom. The reaction then proceeds via the elimination of Oads by a CO or SO2 molecule. The obtained low activation energies clearly indicate that the metal-free C-BNNS surface can be regarded as a highly active catalyst for the reduction of N2O. The results of this study may open new avenues in searching low cost and highly active BN-based catalysts for low temperature reduction of N2O.

  8. Regeneration and sulfur poisoning behavior of In/H-BEA catalyst for NO{sub x} reduction by CH{sub 4}

    Energy Technology Data Exchange (ETDEWEB)

    Pan, Hua; Jian, Yanfei; Yu, Yanke, E-mail: yankeyu@xjtu.edu.cn; He, Chi, E-mail: chi_he@xjtu.edu.cn; Shen, Zhenxing; Liu, Hongxia

    2017-04-15

    Highlights: • Sulfur poisoning mechanism of In/H-BEA was investigated for CH{sub 4}-SCR by in situ DRIFT. • H{sub 2} reduction could reduce In{sub 2}(SO{sub 4}){sub 3} to InO{sup +} via In{sub 2}(SO{sub 4}){sub 3} → In{sub 2}O{sub 3} → In(OH){sub 2}{sup +} → InO{sup +}. • The optimal regeneration parameters of H{sub 2} reduction was 400 °C and 60 min. - Abstract: Sulfur poisoning and regeneration behavior of In/H-BEA catalyst were carried out in NO{sub x} reduction by CH{sub 4}. In/H-BEA catalyst exhibited a poor resistance to sulfur dioxide after addition of 200 ppm SO{sub 2} and 10 vol.% H{sub 2}O into NO reduction with CH{sub 4} at 450 °C for 45 h. Sulfur poisoning of In/H-BEA was attributed to the inhibition of NO{sub x} 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 CH{sub 4}. H{sub 2} reduction is a promising technology for regeneration of In/H-BEA deactivated by SO{sub 2} for removing NO{sub x} from lean-burn and diesel exhausts. Indium sulfate could be reduced by H{sub 2} to InO{sup +} with In{sub 2}O{sub 3} and In(OH){sub 2}{sup +} as the intermediates. The optimal parameters of H{sub 2} reduction was regeneration temperature of 400 °C and regeneration time of 60 min which completely recovered the catalytic activity of In/H-BEA.

  9. Combined effects Na and SO{sub 2} in flue gas on Mn-Ce/TiO{sub 2} catalyst for low temperature selective catalytic reduction of NO by NH{sub 3} simulated by Na{sub 2}SO{sub 4} doping

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Aiyi [Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023 (China); Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023 (China); Yu, Danqing [School of Chemical Engineering and Technology, Wuhan University of Science and Technology, Wuhan 430081 (China); Yang, Liu [Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023 (China); Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023 (China); Sheng, Zhongyi, E-mail: 09377@njnu.edu.cn [Department of Environmental Science and Engineering, Nanjing Normal University, Nanjing 210023 (China); Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, Nanjing 210023 (China)

    2016-08-15

    Highlights: • Sodium sulfate (Na{sub 2}SO{sub 4}) was deposited on Mn-Ce/TiO{sub 2} catalyst to simulate the co-existing of sodium and SO{sub 2} in the flue gas. • Na{sub 2}SO{sub 4} had strong and fluctuant influence on Mn-Ce/TiO{sub 2} catalyst’s performance in SCR of NOx with NH{sub 3}, due to the combined effect of the deactivation of sodium salts and the enhanced performance of ceria with surface sulfation. • The changes of the surface chemical species and acid sites on the Na{sub 2}SO{sub 4} deposited catalysts could be considered as the main reasons for the fluctuation changes with the catalytic activity. - Abstract: A series of Mn-Ce/TiO{sub 2} catalysts were synthesized through an impregnation method and used for low temperature selective catalytic reduction (SCR) of NOx with ammonia (NH{sub 3}). Na{sub 2}SO{sub 4} was added into the catalyst to simulate the combined effects of alkali metal and SO{sub 2} in the flue gas. Experimental results showed that Na{sub 2}SO{sub 4} had strong and fluctuant influence on the activity of Mn-Ce/TiO{sub 2}, because the effect of Na{sub 2}SO{sub 4} included pore occlusion and sulfation effect simultaneously. When Na{sub 2}SO{sub 4} loading content increased from 0 to 1 wt.%, the SCR activities of Na{sub 2}SO{sub 4}-doped catalysts decreased greatly. With further increasing amount of Na{sub 2}SO{sub 4}, however, the catalytic activity increased gradually. XRD results showed that Na{sub 2}SO{sub 4} doping could induce the crystallization of MnOx phases, which were also confirmed by TEM and SEM results. BET results showed that the surface areas decreased and a new bimodal mesoporous structure formed gradually with the increasing amount of Na{sub 2}SO{sub 4}. XPS results indicated that part of Ce{sup 4+} and Mn{sup 3+} were transferred to Ce{sup 3+} and Mn{sup 4+} due to the sulfation after Na{sub 2}SO{sub 4} deposition on the surface of the catalysts. When the doped amounts of Na{sub 2}SO{sub 4} increased, NH{sub 3

  10. Selective catalytic reduction system and process for control of NO.sub.x emissions in a sulfur-containing gas stream

    Science.gov (United States)

    Sobolevskiy, Anatoly

    2015-08-11

    An exhaust gas treatment process, apparatus, and system for reducing the concentration of NOx, CO and hydrocarbons in a gas stream, such as an exhaust stream (29), via selective catalytic reduction with ammonia is provided. The process, apparatus and system include a catalytic bed (32) having a reducing only catalyst portion (34) and a downstream reducing-plus-oxidizing portion (36). Each portion (34, 36) includes an amount of tungsten. The reducing-plus-oxidizing catalyst portion (36) advantageously includes a greater amount of tungsten than the reducing catalyst portion (36) to markedly limit ammonia salt formation.

  11. Reduction and re-oxidation of Cu/Al{sub 2}O{sub 3} catalysts investigated with quick-scanning XANES and EXAFS

    Energy Technology Data Exchange (ETDEWEB)

    Stoetzel, J; Luetzenkirchen-Hecht, D; Frahm, R [Department of Physics, University of Wuppertal, Gaussstr. 20, D-42097 Wuppertal (Germany); Kimmerle, B; Baiker, A [Department of Chemistry and Applied Biosciences, ETH Zuerich, CH-8093 Zuerich (Switzerland); Nachtegaal, M [Paul Scherrer Institut, CH-5232 Villigen (Switzerland); Beier, M J; Grunwaldt, J-D, E-mail: j.stoetzel@uni-wuppertal.d, E-mail: jdg@kt.dtu.d [Department of Chemical and Biochemical Engineering, Technical University of Denmark, Building 229, DK-2800 Kgs. Lyngby (Denmark)

    2009-11-15

    In the present study the structure of copper catalysts on alumina support were investigated in situ and time resolved during reduction and re-oxidation at different temperatures with the quick-scanning EXAFS (QEXAFS) technique. Different impregnation times (2 min and 90 min) were chosen for the preparation which resulted in different copper species that show a strong variation in the reduction/re-oxidation behaviour. These dynamic changes as well as possible intermediate phases during the gas atmospheres changes were followed with up to 20 EXAFS spectra per second at the copper K-edge covering an energy range of 450 eV. The high time resolution provided new insights into the dynamics of the catalysts e.g. revealing Cu(I) as intermediate state during re-oxidation. Latest advances in the data acquisition hardware are leading to an improved data quality of spectra collected at the SuperXAS beamline. Thus, not only accurate analysis of the catalysts via XANES but also by EXAFS was possible. This is also due to the recent upgrade to monitor the Bragg angle directly with an encoder during the experiments.

  12. Environmental Assessment for the Commercial Demonstration of the Low NOx Burner/Separated Over-Fire Air (LNB/SOFA) Integration System Emission Reduction Technology, Finney County, Kansas

    Energy Technology Data Exchange (ETDEWEB)

    n/a

    2003-03-11

    The U.S. Department of Energy (DOE) proposes to provide partial funding to the Sunflower Electric Power Corporation (Sunflower), to demonstrate the commercial application of Low-NO{sub x} Burner/Separated Over-Fire Air (LNB/SOFA) integration system to achieve NO{sub x} emission reduction to the level of 0.15 to 0.22 pounds per million British thermal units (lb/MM Btu). The proposed project station is Sunflower's 360 MW coal-fired generation station, Holcomb Unit No. 1 (Holcomb Station). The station, fueled by coal from Wyoming's Powder River Basin, is located near Garden City, in Finney County, Kansas. The period of performance is expected to last approximately 2 years. The Holcomb Station, Sunflower LNB/SOFA integrated system would be modified in three distinct phases to demonstrate the synergistic effect of layering NO{sub x} control technologies. Once modified, the station would demonstrate that a unit equipped with an existing low-NO{sub x} burner system can be retrofitted with a new separated over-fire air (SOFA) system, coal flow measurement and control, and enhanced combustion monitoring to achieve about 45 percent reduction in nitrogen oxides (NO{sub x}) emissions. The proposed project would demonstrate a technology alternative to Selective Catalytic Reduction (SCR) systems. While SCR does generally achieve high reductions in NO{sub x} emissions (from about 0.8 lb/MM to 0.12 lb/MM Btu), it does so at higher capital and operating cost, requires the extensive use of critical construction labor, requires longer periods of unit outage for deployment, and generally requires longer periods of time to complete shakedown and full-scale operation. Cost of the proposed project technology would be on the order of 15-25 percent of that for SCR, with consequential benefits derived from reductions in construction manpower requirements and periods of power outages. This proposed technology demonstration would generally be applicable to boilers using opposed

  13. Synthesis of palladium nanoparticles with leaf extract of Chrysophyllum cainito (Star apple) and their applications as efficient catalyst for C-C coupling and reduction reactions

    Science.gov (United States)

    Majumdar, Rakhi; Tantayanon, Supawan; Bag, Braja Gopal

    2017-10-01

    A simple green chemical method for the one-step synthesis of palladium nanoparticles (PdNPs) has been described by reducing palladium (II) chloride with the leaf extract of Chrysophyllum cainito in aqueous medium. The synthesis of the palladium nanoparticles completed within 2-3 h at room temperature, whereas on heat treatment (70-80 °C), the synthesis of colloidal PdNPs completed almost instantly. The stabilized PdNPs have been characterized in detail by spectroscopic, electron microscopic and light scattering measurements. The synthesized PdNPs have been utilized as a green catalyst for C-C coupling reactions under aerobic and phosphine-free conditions in aqueous medium. In addition, the synthesized PdNPs have also been utilized as a catalyst for a very efficient sodium borohydride reduction of 3- and 4-nitrophenols. The synthesized PdNPs can retain their catalytic activity for several months.

  14. Reducción catalítica selectiva de NOx usando nanopartículas de ferritas Cu1-XCoXFe2O4 como catalizador

    Directory of Open Access Journals (Sweden)

    Sarah Briceño1*

    2009-12-01

    Full Text Available Nanostructured catalysts AB2O4 spinel type oxides (A = Co and B = Cu were prepared by the sol-gel self-combustion method using citric acid as precursor. They were characterized by X-ray diffraction (XRD, Scanning Electron Microscopy (SEM, Transmission Electron Microscopy (TEM and Catalytic activity tests, which have proven to be effective for selective catalytic reduction of NOx using hydrocarbon as a reducing agent (SCR-HC in a temperature range 250 - 450 ° C, reaching up to 40% conversion of NO and 100% selectivity towards the formation of N2

  15. Selective reduction of nitric oxide over Cu/ZSM-5: The role of oxygen in suppressing catalyst deactivation by carbonaceous deposits

    Energy Technology Data Exchange (ETDEWEB)

    d' Itri, Julie L; Sachtler, Wolfgang M.H. [V.N. Ipatieff Laboratory, Center for Catalysis and Surface Science, Departments of Chemical Engineering and Chemistry, Northwestern University, Evanston, IL (United States)

    1993-06-15

    The role of oxygen in the selective reduction of nitrogen monoxide by either propane or propene over 'excessively' ion-exchanged Cu/ZSM-5 has been studied. In a wide temperature region and in the absence of additives such as steam, propane is a more effective reductant than propene; with propane and in the presence of oxygen reduction of nitric oxide to nitrogen approaches 100% above 600 K. The difference in effectiveness is due to the different degree of catalyst deactivation by carbonaceous deposits: more carbonaceous material is deposited from propene than from propane. Temperature-programmed oxidation shows that above 600 K the rate of oxidation of carbonaceous deposits by oxygen is significant. The amount of such carbonaceous deposits is, therefore, lower when catalytic tests above 600 K are done in the presence of oxygen. At very high temperatures, the in situ volatilization of the deposits by reaction with oxygen keeps the catalyst surface clean in the steady state of nitric oxide reduction.

  16. Palladium nanoparticles encapsulated in core-shell silica: A structured hydrogenation catalyst with enhanced activity for reduction of oxyanion water pollutants

    KAUST Repository

    Wang, Yin; Liu, Jinyong; Wang, Peng; Werth, Charles; Strathmann, Timothy J.

    2014-01-01

    Noble metal nanoparticles have been applied to mediate catalytic removal of toxic oxyanions and halogenated hydrocarbons in contaminated water using H2 as a clean and sustainable reductant. However, activity loss by nanoparticle aggregation and difficulty of nanoparticle recovery are two major challenges to widespread technology adoption. Herein, we report the synthesis of a core-shell-structured catalyst with encapsulated Pd nanoparticles and its enhanced catalytic activity in reduction of bromate (BrO3-), a regulated carcinogenic oxyanion produced during drinking water disinfection process, using 1 atm H2 at room temperature. The catalyst material consists of a nonporous silica core decorated with preformed octahedral Pd nanoparticles that were further encapsulated within an ordered mesoporous silica shell (i.e., SiO2@Pd@mSiO2). Well-defined mesopores (2.3 nm) provide a physical barrier to prevent Pd nanoparticle (6 nm) movement, aggregation, and detachment from the support into water. Compared to freely suspended Pd nanoparticles and SiO2@Pd, encapsulation in the mesoporous silica shell significantly enhanced Pd catalytic activity (by a factor of 10) under circumneutral pH conditions that are most relevant to water purification applications. Mechanistic investigation of material surface properties combined with Langmuir-Hinshelwood modeling of kinetic data suggest that mesoporous silica shell enhances activity by promoting BrO3- adsorption near the Pd active sites. The dual function of the mesoporous shell, enhancing Pd catalyst activity and preventing aggregation of active nanoparticles, suggests a promising general strategy of using metal nanoparticle catalysts for water purification and related aqueous-phase applications.

  17. Palladium nanoparticles encapsulated in core-shell silica: A structured hydrogenation catalyst with enhanced activity for reduction of oxyanion water pollutants

    KAUST Repository

    Wang, Yin

    2014-10-03

    Noble metal nanoparticles have been applied to mediate catalytic removal of toxic oxyanions and halogenated hydrocarbons in contaminated water using H2 as a clean and sustainable reductant. However, activity loss by nanoparticle aggregation and difficulty of nanoparticle recovery are two major challenges to widespread technology adoption. Herein, we report the synthesis of a core-shell-structured catalyst with encapsulated Pd nanoparticles and its enhanced catalytic activity in reduction of bromate (BrO3-), a regulated carcinogenic oxyanion produced during drinking water disinfection process, using 1 atm H2 at room temperature. The catalyst material consists of a nonporous silica core decorated with preformed octahedral Pd nanoparticles that were further encapsulated within an ordered mesoporous silica shell (i.e., SiO2@Pd@mSiO2). Well-defined mesopores (2.3 nm) provide a physical barrier to prevent Pd nanoparticle (6 nm) movement, aggregation, and detachment from the support into water. Compared to freely suspended Pd nanoparticles and SiO2@Pd, encapsulation in the mesoporous silica shell significantly enhanced Pd catalytic activity (by a factor of 10) under circumneutral pH conditions that are most relevant to water purification applications. Mechanistic investigation of material surface properties combined with Langmuir-Hinshelwood modeling of kinetic data suggest that mesoporous silica shell enhances activity by promoting BrO3- adsorption near the Pd active sites. The dual function of the mesoporous shell, enhancing Pd catalyst activity and preventing aggregation of active nanoparticles, suggests a promising general strategy of using metal nanoparticle catalysts for water purification and related aqueous-phase applications.

  18. A general strategy for the in situ decoration of porous Mn-Co bi-metal oxides on metal mesh/foam for high performance de-NOx monolith catalysts.

    Science.gov (United States)

    Cai, Sixiang; Liu, Jie; Zha, Kaiwen; Li, Hongrui; Shi, Liyi; Zhang, Dengsong

    2017-05-04

    Owing to their advantages of strong mechanical stability, plasticity, thermal conductivity and mass transfer ability, metal foam or meshes are considered promising monolith supports for de-NO x application. In this work, we developed a facile method for the decoration of porous Mn-Co bi-metal oxides on Fe meshes. The block-like structure was derived from in situ coating, and simultaneous nucleation and growth of the Mn-Co hydroxide precursor, while the porous Mn-Co oxides were formed via the calcination process. Moreover, the decoration of the high-purity Co 2 MnO 4 spinel could lead to enhanced reducibility and adsorption behaviors, which are crucial to the catalytic process. Of note is the fact that the Fe mesh used in the synthesis procedure could be substituted by various metal supports including Ti mesh, Cu foam and Ni foam. Driven by the above motivations, metal supports decorated with Mn-Co oxides were evaluated as monolith de-NO x catalysts for the first time. Inspiringly, these catalysts demonstrate outstanding low-temperature catalytic activity, desirable stability and excellent H 2 O resistance. This work might open up a new path for the design and development of high performance de-NO x monolith catalysts.

  19. Automotive Catalyst State Diagnosis Using Microwaves

    Directory of Open Access Journals (Sweden)

    Moos Ralf

    2015-01-01

    Full Text Available The state of catalysts plays a key role in automotive exhaust gas aftertreatment. The soot or ash loading of Diesel particulate filters, the oxygen loading degree in three-way catalysts, the amount of stored ammonia in SCR catalysts, or the NOx loading degree in NOx storage catalysts are important parameters that are today determined indirectly and in a model-based manner with gas sensors installed upstream and/or downstream of the catalysts. This contribution gives an overview on a novel approach to determine the catalyst state directly by a microwave-based technique. The method exploits the fact that the catalyst housing acts as a microwave cavity resonator. As “sensing” elements, one or two simple antennas are mounted inside the catalyst canning. The electrical properties of the catalyst device (ceramic honeycomb plus coating and storage material can be measured. Preferably, the resonance characteristics, e.g., the resonance frequencies, of selected cavity modes are observed. The information on the catalyst interior obtained in such a contactless manner is very well correlated with the catalyst state as will be demonstrated for different exhaust gas aftertreatment systems.

  20. Selective catalytic reduction of NO{sub x} with NH{sub 3} over iron-cerium-tungsten mixed oxide catalyst prepared by different methods

    Energy Technology Data Exchange (ETDEWEB)

    Xiong, Zhi-bo, E-mail: xzb328@163.com [School of Energy and Power Engineering, University of Shanghai for Science & Technology, Shanghai 200093 (China); Collaborative Innovation Research Institute, University of Shanghai for Science & Technology, Shanghai 200093 (China); Shanghai Power Equipment Research Institute, Shanghai 200240 (China); Liu, Jing; Zhou, Fei; Liu, Dun-yu; Lu, Wei [School of Energy and Power Engineering, University of Shanghai for Science & Technology, Shanghai 200093 (China); Jin, Jing [School of Energy and Power Engineering, University of Shanghai for Science & Technology, Shanghai 200093 (China); Collaborative Innovation Research Institute, University of Shanghai for Science & Technology, Shanghai 200093 (China); Ding, Shi-fa [Shanghai Power Equipment Research Institute, Shanghai 200240 (China)

    2017-06-01

    Highlights: • Iron-cerium-tungsten mixed oxide catalysts were prepared through three different methods. • The effect of preparation methods on the NH{sub 3}-SCR activity and the surface structure properties of catalyst were investigated. • Iron-cerium-tungsten mixed oxide prepared through microwave irradiation assistant critic acid sol-gel shows higher NH{sub 3}-SCR activity. - Abstract: A series of magnetic Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z} catalysts were synthesized by three different methods(Co-precipitation(Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-CP), Hydrothermal treatment assistant critic acid sol-gel method(Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-HT) and Microwave irradiation assistant critic acid sol-gel method(Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-MW)), and the catalytic activity was evaluated for selective catalytic reduction of NO with NH{sub 3}. The catalyst was characterized by XRD, N{sub 2} adsorption-desorption, XPS, H{sub 2}-TPR and NH{sub 3}-TPD. Among the tested catalysts, Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-MW shows the highest NO{sub x} conversion over per gram in unit time with NO{sub x} conversion of 60.8% at 350 °C under a high gas hourly space velocity of 1,200,000 ml/(g h). Different from Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-CP catalyst, there exists a large of iron oxide crystallite(γ-Fe{sub 2}O{sub 3} and α-Fe{sub 2}O{sub 3}) scattered in Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z} catalysts prepared through hydrothermal treatment or microwave irradiation assistant critic acid sol-gel method, and higher iron atomic concentration on their surface. And Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-MW shows higher surface absorbed oxygen concentration and better dispersion compared with Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-HT catalyst. These features were favorable for the high catalytic performance of NO reduction with NH{sub 3} over Fe{sub 0.85}Ce{sub 0.10}W{sub 0.05}O{sub z}-MW catalyst.

  1. Pilot test and optimization of plasma based deNOx

    DEFF Research Database (Denmark)

    Stamate, Eugen; Chen, Weifeng; Michelsen, Poul

    . Experiments are in good agreement with numerical simulations. An optimized oxidation scheme for NOx reduction processes with time dependent combustion, such as the biomass power plants, was developed. Ozone production by micro-hollow and capillary discharges at atmospheric pressures was investigated......The NOx reduction of flue gas by plasma generated ozone was investigated in pilot test experiments at two industrial power plants running on natural gas (Ringsted) and biomass (Haslev). Reduction rates higher than 95% have been achieved for a molar ratio O3:NOx of 1.56. Fourier transform infrared...... and ultraviolet absorption spectroscopy were used for spatial measurements of stable molecules and radicals along the reduction reactor. Reactions of O3 injected in the flue gas in the reduction reactor were also modeled including the influence of the flue gas temperature, water droplets and SOx and HCl content...

  2. Non-sensitized selective photochemical reduction of CO2 to CO under visible light with an iron molecular catalyst.

    Science.gov (United States)

    Rao, Heng; Bonin, Julien; Robert, Marc

    2017-03-02

    A substituted tetraphenyl iron porphyrin, bearing positively charged trimethylammonio groups at the para position of each phenyl ring, demonstrates its ability as a homogeneous molecular catalyst to selectively reduce CO 2 to CO under visible light irradiation in organic media without the assistance of a sensitizer and no competitive hydrogen evolution for several days.

  3. Dual redox catalysts for oxygen reduction and evolution reactions: towards a redox flow Li-O2 battery.

    Science.gov (United States)

    Zhu, Yun Guang; Jia, Chuankun; Yang, Jing; Pan, Feng; Huang, Qizhao; Wang, Qing

    2015-06-11

    A redox flow lithium-oxygen battery (RFLOB) by using soluble redox catalysts with good performance was demonstrated for large-scale energy storage. The new device enables the reversible formation and decomposition of Li2O2 via redox targeting reactions in a gas diffusion tank, spatially separated from the electrode, which obviates the passivation and pore clogging of the cathode.

  4. Surfactant-controlled synthesis of Pd/Ce0.6Zr0.4O2 catalyst for NO reduction by CO with excess oxygen

    International Nuclear Information System (INIS)

    Chen, L.F.; Gonzalez, G.; Wang, J.A.; Norena, L.E.; Toledo, A.; Castillo, S.; Moran-Pineda, M.

    2005-01-01

    For the first time, this work reports a surfactant-controlled synthetic method to obtain a nanophase of mesoporous ceria-zirconia solid solution containing cationic defects in the crystalline structure. The incorporation of a cationic surfactant (myristyltrimethylammonium bromide) into the ceria-zirconia solid network not only controlled the pore diameter distribution but also induced creation of the lattice defect. Ceria-zirconia solid solution showed crystal microstrain and structural distortion that varied with the calcination temperature. Compared to pure ceria, the addition of zirconium to the ceria promoted the bulk oxygen reducibility and enhanced the thermal stability of the solid. Hydrogen could be stored into or released from the PdO/Ce 0.6 Zr 0.4 O 2 catalyst during the TPR procedure, which is associated to the formation/decomposition of a PdH x phase, due to the hydrogen dissociation catalyzed by metallic Pd. At cool start of reaction, NO reduction by CO with excess oxygen over the Pd/Ce 0.6 Zr 0.4 O 2 catalyst showed selectivity around 100% to N 2 . A competition between NO reduction by CO and CO oxidation by O 2 was observed: at reaction temperatures below 200 deg. C, NO inhibited CO oxidation activity; however, at reaction temperatures above 200 deg. C, high activity of CO oxidation resulted in an inhibition effect on NO reduction

  5. Utilization of Common Automotive Three-Way NO{sub x} Reduction Catalyst for Managing Off- Gas from Thermal Treatment of High-Nitrate Waste - 13094

    Energy Technology Data Exchange (ETDEWEB)

    Foster, Adam L.; Ki Song, P.E. [Studsvik, Inc. 5605 Glenridge Drive Suite 705, Atlanta, GA 30342 (United States)

    2013-07-01

    Studsvik's Thermal Organic Reduction (THOR) steam reforming process has been tested and proven to effectively treat radioactive and hazardous wastes streams with high nitrate contents to produce dry, stable mineral products, while providing high conversion (>98%) of nitrates and nitrites directly to nitrogen gas. However, increased NO{sub x} reduction may be desired for some waste streams under certain regulatory frameworks. In order to enhance the NO{sub x} reduction performance of the THOR process, a common Three-Way catalytic NO{sub x} reduction unit was installed in the process gas piping of a recently completed Engineering Scale Technology Demonstration (ESTD). The catalytic DeNO{sub x} unit was located downstream of the main THOR process vessel, and it was designed to catalyze the reduction of residual NO{sub x} to nitrogen gas via the oxidation of the hydrogen, carbon monoxide, and volatile organic compounds that are inherent to the THOR process gas. There was no need for auxiliary injection of a reducing gas, such as ammonia. The unit consisted of four monolith type catalyst sections positioned in series with a gas mixing section located between each catalyst section. The process gas was monitored for NO{sub x} concentration upstream and downstream of the catalytic DeNO{sub x} unit. Conversion efficiencies ranged from 91% to 97% across the catalytic unit, depending on the composition of the inlet gas. Higher concentrations of hydrogen and carbon monoxide in the THOR process gas increased the NO{sub x} reduction capability of the catalytic DeNO{sub x} unit. The NO{sub x} destruction performance of THOR process in combination with the Three-Way catalytic unit resulted in overall system NO{sub x} reduction efficiencies of greater than 99.9% with an average NO{sub x} reduction efficiency of 99.94% for the entire demonstration program. This allowed the NO{sub x} concentration in the ESTD exhaust gas to be maintained at less than 40 parts per million (ppm

  6. DEVELOPMENT OF A NOVEL RADIATIVELY/CONDUCTIVELY STABILIZED BURNER FOR SIGNIFICANT REDUCTION OF NOx EMISSIONS AND FOR ADVANCING THE MODELING AND UNDERSTANDING OF PULVERIZED COAL COMBUSTION AND EMISSIONS

    Energy Technology Data Exchange (ETDEWEB)

    Noam Lior; Stuart W. Churchill

    2003-10-01

    the Gordon Conference on Modern Development in Thermodynamics. The results obtained are very encouraging for the development of the RCSC as a commercial burner for significant reduction of NO{sub x} emissions, and highly warrants further study and development.

  7. Performance and selectivity of PtxSn/C electro-catalysts for ethanol oxidation prepared by reduction with different formic acid concentrations

    International Nuclear Information System (INIS)

    Zignani, Sabrina C.; Baglio, Vincenzo; Linares, José J.; Monforte, Giuseppe; Gonzalez, Ernesto R.; Aricò, Antonino S.

    2012-01-01

    Carbon supported Pt–Sn catalysts were prepared by reduction of Pt and Sn precursors with formic acid and characterized in terms of structure, morphology and surface properties. The electrocatalytic activity for ethanol oxidation was studied in a direct ethanol fuel cell (DEFC) at 70 °C and 90 °C. Electrochemical and physico-chemical data indicated that a proper balance of Pt and Sn species in the near surface region was necessary to maximize the reaction rate. The best atomic surface composition, in terms of electrochemical performance, was Pt:Sn 65:35 corresponding to a bulk composition 75:25 namely Pt 3 Sn 1 /C. The reaction products of ethanol electro-oxidation in single cell and their distribution as a function of the nature of catalyst were determined. Essentially, acetaldehyde and acetic acid were detected as the main reaction products; whereas, a lower content of CO 2 was formed. The selectivity toward acetic acid vs. acetaldehyde increased with the increase of the Sn content and decreased by decreasing the concentration of the reducing agent used in the catalyst preparation. According to the recent literature, these results have been interpreted on the basis of ethanol adsorption characteristics and ligand effects occurring for Sn-rich electrocatalysts.

  8. High Performance and Cost-Effective Direct Methanol Fuel Cells: Fe-N-C Methanol-Tolerant Oxygen Reduction Reaction Catalysts.

    Science.gov (United States)

    Sebastián, David; Serov, Alexey; Artyushkova, Kateryna; Gordon, Jonathan; Atanassov, Plamen; Aricò, Antonino S; Baglio, Vincenzo

    2016-08-09

    Direct methanol fuel cells (DMFCs) offer great advantages for the supply of power with high efficiency and large energy density. The search for a cost-effective, active, stable and methanol-tolerant catalyst for the oxygen reduction reaction (ORR) is still a great challenge. In this work, platinum group metal-free (PGM-free) catalysts based on Fe-N-C are investigated in acidic medium. Post-treatment of the catalyst improves the ORR activity compared with previously published PGM-free formulations and shows an excellent tolerance to the presence of methanol. The feasibility for application in DMFC under a wide range of operating conditions is demonstrated, with a maximum power density of approximately 50 mW cm(-2) and a negligible methanol crossover effect on the performance. A review of the most recent PGM-free cathode formulations for DMFC indicates that this formulation leads to the highest performance at a low membrane-electrode assembly (MEA) cost. Moreover, a 100 h durability test in DMFC shows suitable applicability, with a similar performance-time behavior compared to common MEAs based on Pt cathodes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. Identifying active surface phases for metal oxide electrocatalysts: a study of manganese oxide bi-functional catalysts for oxygen reduction and water oxidation catalysis

    DEFF Research Database (Denmark)

    Su, Hai-Yan; Gorlin, Yelena; Man, Isabela Costinela

    2012-01-01

    Progress in the field of electrocatalysis is often hampered by the difficulty in identifying the active site on an electrode surface. Herein we combine theoretical analysis and electrochemical methods to identify the active surfaces in a manganese oxide bi-functional catalyst for the oxygen...... reduction reaction (ORR) and the oxygen evolution reaction (OER). First, we electrochemically characterize the nanostructured α-Mn2O3 and find that it undergoes oxidation in two potential regions: initially, between 0.5 V and 0.8 V, a potential region relevant to the ORR and, subsequently, between 0.8 V...

  10. Enhanced catalytic activity over MIL-100(Fe) loaded ceria catalysts for the selective catalytic reduction of NO{sub x} with NH{sub 3} at low temperature

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Peng [School of Environmental Science and Technology, Dalian University of Technology, Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), Dalian 116024 (China); Sun, Hong [School of Environmental & Chemical Engineering, Dalian Jiaotong University, Dalian 116028 (China); Quan, Xie, E-mail: quanxie@dlut.edu.cn [School of Environmental Science and Technology, Dalian University of Technology, Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), Dalian 116024 (China); Chen, Shuo [School of Environmental Science and Technology, Dalian University of Technology, Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), Dalian 116024 (China)

    2016-01-15

    Highlights: • Nano-ceria was successfully encapsulated into MIL-100(Fe) for the SCR of NO{sub x}. • The incorporated ceria in MIL-100(Fe) showed high content of chemisorbed oxygen. • The added ceria into MIL-100(Fe) improved the formation of adsorbed NO{sub 2} species. • The addition of ceria into MIL-100(Fe) enhanced SCR activity at low temperature. - Abstract: The development of catalysts for selective catalytic reduction (SCR) reactions that are highly active at low temperatures and show good resistance to SO{sub 2} and H{sub 2}O 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-CeO{sub 2}/MIL-100(Fe) catalyst shows improved catalytic activity both at low temperatures and throughout a wide temperature window. The temperature window for 90% NO{sub x} 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 NO{sub 2} species responsible for fast SCR reactions.

  11. High Specific and Mass Activity for the Oxygen Reduction Reaction for Thin Film Catalysts of Sputtered Pt3Y

    DEFF Research Database (Denmark)

    Lindahl, Niklas; Zamburlini, Eleonora; Feng, Ligang

    2017-01-01

    Fuel cells have the potential to play an important role in sustainable energy systems, provided that catalysts with higher activity and stability are developed. In this work, it is found that thin alloy films of single-target cosputtered platinum-yttrium exhibit up to seven times higher specific...... additional chemical or thermal treatment. The films show an improvement in stability over the same materials in nanoparticulate form. Physical characterization shows that the thin films form a platinum overlayer supported on an underlying alloy. The high activity is likely related to compressive strain...... in that overlayer. As sputtering can be used to mass-produce fuel cell electrodes, the results open new possibilities for the preparation of platinum-rare earth metal alloy catalysts in commercial devices....

  12. LOW NOX BURNER DEVELOPMENT

    Energy Technology Data Exchange (ETDEWEB)

    KRISHNA,C.R.; BUTCHER,T.

    2004-09-30

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

  13. Nanoparticular metal oxide/anatase catalysts

    DEFF Research Database (Denmark)

    2010-01-01

    The present invention concerns a method of preparation of nanoparticular metal oxide catalysts having a narrow particle size distribution. In particular, the invention concerns preparation of nanoparticular metal oxide catalyst precursors comprising combustible crystallization seeds upon which...... the catalyst metai oxide is co-precipitated with the carrier metal oxide, which crystallization seeds are removed by combustion in a final calcining step. The present invention also concerns processes wherein the nanoparticular metal oxide catalysts of the invention are used, such as SCR (deNOx) reactions...

  14. Effect of cationic molecules on the oxygen reduction reaction on fuel cell grade Pt/C (20 wt%) catalyst in potassium hydroxide (aq, 1 mol dm(-3)).

    Science.gov (United States)

    Ong, Ai Lien; Inglis, Kenneth K; Whelligan, Daniel K; Murphy, Sam; Varcoe, John R

    2015-05-14

    This study investigates the effect of 1 mmol dm(-3) concentrations of a selection of small cationic molecules on the performance of a fuel cell grade oxygen reduction reaction (ORR) catalyst (Johnson Matthey HiSPEC 3000, 20 mass% Pt/C) in aqueous KOH (1 mol dm(-3)). The cationic molecules studied include quaternary ammonium (including those based on bicyclic systems) and imidazolium types as well as a phosphonium example: these serve as fully solubilised models for the commonly encountered head-groups in alkaline anion-exchange membranes (AAEM) and anion-exchange ionomers (AEI) that are being developed for application in alkaline polymer electrolyte fuel cells (APEFCs), batteries and electrolysers. Both cyclic and hydrodynamic linear sweep rotating disk electrode voltammetry techniques were used. The resulting voltammograms and subsequently derived data (e.g. apparent electrochemical active surface areas, Tafel plots, and number of [reduction] electrons transferred per O2) were compared. The results show that the imidazolium examples produced the highest level of interference towards the ORR on the Pt/C catalyst under the experimental conditions used.

  15. Technical characterisation of different catalysts for the selective reduction of nitrogen oxides in fluegas. Reaktionstechnische Charakterisierung unterschiedlicher Katalysatoren zur selektiven Reduktion von Stickoxiden in Rauchgasen

    Energy Technology Data Exchange (ETDEWEB)

    Dembele, C.

    1993-11-26

    In the context of this work, experimental investigations were made on the kinetics of the selective catalytic reduction of nitrogen monoxide with ammonia on catalysts of industrial origin. The aim of the work was to examine the effect of NO, NH[sub 3], H[sub 2]O and SO[sub 2] concentrations and the temperature on the speed of material quantity change of NO. The measurements with water proved difficult, as with high water contents, there was a drift of the measured values of NO concentration, the cause of which could not be cleared up. By repeated calibration of the NO concentrations to be set in the waste gas during a series of measurements, success was achieved in compensating for this drift and in obtaining reproducible results. The addition of SO[sub 2] to the reaction mixture brings the simulated fluegas closer to real powerstation fluegas. In determining the NO and NH[sub 3] concentration, the 'quenching' effect occurred and the calibration of the chemi-luminescence equipment frequently had to be repeated. The limited partial step of the reduction of NO is the transports of the educts into the pores of the catalyst grain to the active centres. (orig./EF)

  16. Gas Turbines: ''low NOx'' technologies at EGT

    International Nuclear Information System (INIS)

    Anon.

    1996-01-01

    For more than 15 years, European Gas Turbines (EGT - GEC Alsthom Group) has gained an important know-how culture and can use its rich feedback experience in the domain of gas turbine emissions. The EGT gas turbine units equipped with denitrogenation technologies cover the 4 to 226 MW power range and cumulate more than 1.7 hours of functioning in the different existing installations in the world. This paper describes the economical and environmental interests of gas turbines for power production and the combustion technologies developed by EGT to reduce the NOx emissions. The selective catalytic reduction technique is the only available secondary technique with can allow NOx and CO emissions lower than 10 ppm. Other technologies involving diluent injection (water, water-fuel mixture, vapor..) are also described and were developed in several countries to reduce the emission of these pollutants. (J.S.)

  17. Use of lanthanide catalysts in air electrodes

    International Nuclear Information System (INIS)

    Souza Parente, L.T. de

    1982-01-01

    A review on the lanthanide catalysts suitable for the reduction catalysis of oxygen in air electrodes is presented. The kinds of lanthanide indicated to be used as catalysts of oxygen reduction are shown. (A.R.H.) [pt

  18. NOx Emission Reduction by Oscillating Combustion

    Energy Technology Data Exchange (ETDEWEB)

    John C. Wagner

    2004-03-31

    High-temperature, natural gas-fired furnaces, especially those fired with preheated air, produce large quantities of NO{sub x} per ton of material processed. Regulations on emissions from industrial furnaces are becoming increasingly more stringent. In addition, competition is forcing operators to make their furnaces more productive and/or efficient. Switching from preheated air to industrial oxygen can increase efficiency and reduce NO{sub x}, but oxygen is significantly more costly than air and may not be compatible with the material being heated. What was needed, and what was developed during this project, is a technology that reduces NO{sub x} emissions while increasing furnace efficiency for both air- and oxy-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. Heat transfer from the flame to the load increases due to the more luminous fuel-rich zones, a longer overall flame length, and the breakup of the thermal boundary layer. The increased heat transfer shortens heat up times, thereby increasing furnace productivity, and reduces the heat going up the stack, thereby increasing efficiency. The fuel-rich and fuel-lean zones also produce substantially less NO{sub x} than firing at a constant excess air level. The longer flames and higher heat transfer rate reduces overall peak flame temperature and thus reduces additional NO{sub x} formation from the eventual mixing of the zones and burnout of combustibles from the rich zones. This project involved the development of hardware to implement oscillating combustion on an industrial scale, the laboratory testing of oscillating combustion on various types of industrial burners, and the field testing of oscillating combustion on several types of industrial furnace. Before laboratory testing began, a market study was conducted, based on the attributes of oscillating combustion and on the results of an earlier project at GTI and Air Liquide, to determine which applications for oscillating combustion would show the greatest probability for technical success and greatest probability for market acceptability. The market study indicated that furnaces in the steel, glass, and metal melting industries would perform well in both categories. These findings guided the selection of burners for laboratory testing and, with the results of the laboratory testing, guided the selection of field test sites.

  19. NOx Emission Reduction by Oscillating combustion

    Energy Technology Data Exchange (ETDEWEB)

    Institute of Gas Technology

    2004-01-30

    High-temperature, natural gas-fired furnaces, especially those fired with preheated air, produce large quantities of NO{sub x} per ton of material processed. Regulations on emissions from industrial furnaces are becoming increasingly more stringent. In addition, competition is forcing operators to make their furnaces more productive and/or efficient. Switching from preheated air to industrial oxygen can increase efficiency and reduce NO{sub x}, but oxygen is significantly more costly than air and may not be compatible with the material being heated. What was needed, and what was developed during this project, is a technology that reduces NO{sub x} emissions while increasing furnace efficiency for both air- and oxy-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. Heat transfer from the flame to the load increases due to the more luminous fuel-rich zones, a longer overall flame length, and the breakup of the thermal boundary layer. The increased heat transfer shortens heat up times, thereby increasing furnace productivity, and reduces the heat going up the stack, thereby increasing efficiency. The fuel-rich and fuel-lean zones also produce substantially less NO{sub x} than firing at a constant excess air level. The longer flames and higher heat transfer rate reduces overall peak flame temperature and thus reduces additional NO{sub x} formation from the eventual mixing of the zones and burnout of combustibles from the rich zones. This project involved the development of hardware to implement oscillating combustion on an industrial scale, the laboratory testing of oscillating combustion on various types of industrial burners, and the field testing of oscillating combustion on several types of industrial furnace. Before laboratory testing began, a market study was conducted, based on the attributes of oscillating combustion and on the results of an earlier project at GTI and Air Liquide, to determine which applications for oscillating combustion would show the greatest probability for technical success and greatest probability for market acceptability. The market study indicated that furnaces in the steel, glass, and metal melting industries would perform well in both categories. These findings guided the selection of burners for laboratory testing and, with the results of the laboratory testing, guided the selection of field test sites.

  20. Thermal Reduction of NOx with Recycled Plastics.

    Science.gov (United States)

    Oluwoye, Ibukun; Dlugogorski, Bogdan Z; Gore, Jeff; Vyazovkin, Sergey; Boyron, Olivier; Altarawneh, Mohammednoor

    2017-07-05

    This study develops technology for mitigation of NO x formed in thermal processes using recycled plastics such as polyethylene (PE). Experiments involve sample characterization, and thermogravimetric decomposition of PE under controlled atmospheres, with NO x concentration relevant to industrial applications. TGA-Fourier transform infrared (FTIR) spectroscopy and NO x chemiluminescence serve to obtain the removal efficiency of NO x by fragments of pyrolyzing PE. Typical NO x removal efficiency amounts to 80%. We apply the isoconversional method to derive the kinetic parameters, and observe an increasing dependency of activation energy on the reaction progress. The activation energies of the process span 135 kJ/mol to 226 kJ/mol, and 188 kJ/mol to 268 kJ/mol, for neat and recycled PE, respectively, and the so-called compensation effect accounts for the natural logarithmic pre-exponential ln (A/min -1 ) factors of ca. 19-35 and 28-41, in the same order, depending on the PE conversion in the experimental interval of between 5 and 95%. The observed delay in thermal events of recycled PE reflects different types of PE in the plastic, as measurements of intrinsic viscosity indicate that, the recycled PE comprises longer linear chains. The present evaluation of isoconversional activation energies affords accurate kinetic modeling of both isothermal and nonisothermal decomposition of PE in NO x -doped atmosphere. Subsequent investigations will focus on the effect of mass transfer and the presence of oxygen, as reburning of NO x in large-scale combustors take place at higher temperatures than those included in the current study.

  1. KINETICS AND MECHANISMS OF NOx - CHAR REDUCTION

    Energy Technology Data Exchange (ETDEWEB)

    Suuberg, E.M.

    1998-06-19

    This study was undertaken in order to improve understanding of several aspects of the NO-carbon reaction. This reaction is of practical importance in combustion systems, but its close examination also provides some fundamental insight into oxidizing gas-carbon reactions. As part of this study, a comprehensive literature review of earlier work on this reaction has been published (Aarna and Suuberg, Fuel, 1997, 76, 475-491). It has been thought for some time that the kinetics of the NO-carbon reaction are unusual, in that they often show a two-regime Arrhenius behavior. It has, however, turned out during this work that NO is not alone in this regard. In this laboratory, we also uncovered evidence of two kinetic regime behavior in CO{sub 2} gasification. In another laboratory, a former colleague has identified the same behavior in N{sub 2}O. The low temperature reaction regime always shows an activation energy which is lower than that in the high temperature regime, leaving little doubt that a shift in mechanism, as opposed to transport limitations, dictates the behavior. The activation energy of the low temperature regime of these reactions is typically less than 100 kJ/mol, and the activation energy of the high temperature regime is generally considerably in excess of this value. In this study, we have resolved some apparent inconsistencies in the explanation of the low temperature regime, whose rate has generally been ascribed to desorption-controlled processes. Part of the problem in characterization of the different temperature regimes is that they overlap to a high degree. It is difficult to probe the low temperature regime experimentally, because of slow relaxation of the surface oxides in that regime. Using careful experimental techniques, we were able to demonstrate that the low temperature regime is indeed characterized by zero order in NO, as it must be. A separate study is being carried out to model the behavior in this regime in NO and in other gases, and the results will be presented shortly.

  2. NOx emission reduction from gas turbines

    International Nuclear Information System (INIS)

    Groppi, G.; Lietti, L.; Forzatti, P.

    2001-01-01

    NO x emissions from gas turbines are a serious environmental concern. Primary control technologies significantly reduce NO x formation, which however is still too high to match increasingly strict emission laws. Catalytic processes can provide lower NO x emissions both as primary and secondary control methods, but their economics should be carefully addressed [it

  3. Oxidation catalyst

    Science.gov (United States)

    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.

  4. Reburning technology - a means to reduce NOx emissions

    International Nuclear Information System (INIS)

    Kremer, H.; Lorra, M.

    1999-01-01

    Nitrogen oxide emission control technologies can be classified as either combustion modifications to minimize the NO production or post-combustion flue gas treatment to reduce the NO concentration afterwards. The techniques for minimizing NOx Production includes the use of low-NOx burners, overfire air (staged combustion) and boiler combustion optimization. Procedures for flue gas treatment can be subdivided into selective catalytic reduction (SCR) or selective non-catalytic reduction (SNCR). The re burning process is a selective non-catalytic technology which is applicable to a wide variety of boilers and can be implemented within a relatively short period of time. The NOx reduction potential of this technique is in the range of 50 % up to 70 %. (author)

  5. Photo-driven electron transfer from the highly reducing excited state of naphthalene diimide radical anion to a CO 2 reduction catalyst within a molecular triad

    Energy Technology Data Exchange (ETDEWEB)

    Martinez, Jose F. [Department of Chemistry and Argonne-Northwestern Solar Energy Research (ANSER) Center; Northwestern University; Evanston; USA; La Porte, Nathan T. [Department of Chemistry and Argonne-Northwestern Solar Energy Research (ANSER) Center; Northwestern University; Evanston; USA; Mauck, Catherine M. [Department of Chemistry and Argonne-Northwestern Solar Energy Research (ANSER) Center; Northwestern University; Evanston; USA; Wasielewski, Michael R. [Department of Chemistry and Argonne-Northwestern Solar Energy Research (ANSER) Center; Northwestern University; Evanston; USA

    2017-01-01

    The naphthalene-1,4:5,8-bis(dicarboximide) radical anion (NDI-˙), which is easily produced by mild chemical or electrochemical reduction (-0.5 Vvs.SCE), can be photoexcited at wavelengths as long as 785 nm, and has an excited state (NDI-˙*) oxidation potential of -2.1 Vvs.SCE, making it a very attractive choice for artificial photosynthetic systems that require powerful photoreductants, such as CO2 reduction catalysts. However, once an electron is transferred from NDI-˙* to an acceptor directly bound to it, a combination of strong electronic coupling and favorable free energy change frequently make the back electron transfer rapid. To mitigate this effect, we have designed a molecular triad system comprising an NDI-˙ chromophoric donor, a 9,10-diphenylanthracene (DPA) intermediate acceptor, and a Re(dmb)(CO)3carbon dioxide reduction catalyst, where dmb is 4,4'-dimethyl-2,2'-bipyridine, as the terminal acceptor. Photoexcitation of NDI-˙ to NDI-˙* is followed by ultrafast reduction of DPA to DPA-˙, which then rapidly reduces the metal complex. The overall time constant for the forward electron transfer to reduce the metal complex is τ = 20.8 ps, while the time constant for back-electron transfer is six orders of magnitude longer, τ = 43.4 μs. Achieving long-lived, highly reduced states of these metal complexes is a necessary condition for their use as catalysts. The extremely long lifetime of the reduced metal complex is attributed to careful tuning of the redox potentials of the chromophore and intermediate acceptor. The NDI-˙–DPA fragment presents many attractive features for incorporation into other photoinduced electron transfer assemblies directed at the long-lived photosensitization of difficult-to-reduce catalytic centers.

  6. A concise guide to sustainable PEMFCs: recent advances in improving both oxygen reduction catalysts and proton exchange membranes.

    Science.gov (United States)

    Scofield, Megan E; Liu, Haiqing; Wong, Stanislaus S

    2015-08-21

    The rising interest in fuel cell vehicle technology (FCV) has engendered a growing need and realization to develop rational chemical strategies to create highly efficient, durable, and cost-effective fuel cells. Specifically, technical limitations associated with the major constituent components of the basic proton exchange membrane fuel cell (PEMFC), namely the cathode catalyst and the proton exchange membrane (PEM), have proven to be particularly demanding to overcome. Therefore, research trends within the community in recent years have focused on (i) accelerating the sluggish kinetics of the catalyst at the cathode and (ii) minimizing overall Pt content, while simultaneously (a) maximizing activity and durability as well as (b) increasing membrane proton conductivity without causing any concomitant loss in either stability or as a result of damage due to flooding. In this light, as an example, high temperature PEMFCs offer a promising avenue to improve the overall efficiency and marketability of fuel cell technology. In this Critical Review, recent advances in optimizing both cathode materials and PEMs as well as the future and peculiar challenges associated with each of these systems will be discussed.

  7. Hierarchical hybrid of Ni{sub 3}N/N-doped reduced graphene oxide nanocomposite as a noble metal free catalyst for oxygen reduction reaction

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Qi; Li, Yingjun; Li, Yetong [College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021 (China); Huang, Keke [State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012 (China); Wang, Qin, E-mail: qinwang@imu.edu.cn [College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021 (China); Inner Mongolia Key Lab. of Nanoscience and Nanotechnology, Inner Mongolia University, Hohhot 010021 (China); Zhang, Jun, E-mail: cejzhang@imu.edu.cn [College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021 (China); Inner Mongolia Key Lab. of Nanoscience and Nanotechnology, Inner Mongolia University, Hohhot 010021 (China)

    2017-04-01

    Highlights: • Hybrid of Ni{sub 3}N/N-RGO catalysts are synthesized by using a two-step method. • The catalysts manifest superior catalytic activity towards the ORR. • High activities are attributed to enhanced electron density and synergistic effects. - Abstract: Novel nickel nitride (Ni{sub 3}N) nanoparticles supported on nitrogen-doped reduced graphene oxide nanosheets (N-RGOs) are synthesized via a facile strategy including hydrothermal and subsequent calcination methods, in which the reduced graphene oxide nanosheets (RGOs) are simultaneously doped with nitrogen species. By varying the content of the RGOs, a series of Ni{sub 3}N/N-RGO nanocomposites are obtained. The Ni{sub 3}N/N-RGO-30% hybrid nanocomposite exhibits superior catalytic activity towards oxygen reduction reaction (ORR) under alkaline condition (0.1 M KOH). Furthermore, this hybrid catalyst also demonstrates high tolerance to methanol poisoning. The RGO containing rich N confers the nanocomposite with large specific surface area and high electronic conduction ability, which can enhance the catalytic efficiency of Ni{sub 3}N nanoparticles. The enhanced catalytic activity can be attributed to the synergistic effect between Ni{sub 3}N and nitrogen doped reduced graphene oxide. In addition, the sufficient contact between Ni{sub 3}N nanoparticles and the N-RGO nanosheets simultaneously promotes good nanoparticle dispersion and provides a consecutive activity sites to accelerate electron transport continuously, which further enhance the ORR performance. The Ni{sub 3}N/N-RGO may be further an ideal candidate as efficient and inexpensive noble metal-free ORR electrocatalyst in fuel cells.

  8. Post combustion methods for control of NOx emission

    Energy Technology Data Exchange (ETDEWEB)

    Rosenberg, H S; Curran, L M; Slack, A V; Ando, J; Oxley, J H

    1980-01-01

    Review of stack gas treatment methods for the control of NOx emissions. Particular emphasis is placed on status of development and factors affecting the performance of the processes. Catalytic, noncatalytic, and scrubbing processes are compared on a uniform engineering basis. Most of the active process development work is taking place in Japan. The three leading stack gas treatment techniques for NOx control are catalytic reduction with ammonia, noncatalytic reduction with ammonia, and direct scrubbing of NO with simultaneous absorption of SO2. The wet processes are much less developed than the dry processes.

  9. Optimization of the fluid catalytic cracking unit performance by application of a high motor Octane catalyst and reduction of gasoline vapour pressure

    International Nuclear Information System (INIS)

    Chavdarov, I.; Stratiev, D.; Shishkova, I.; Dinkov, R.; Petkov, P.

    2013-01-01

    Full text: The fluid catalytic cracking (FCC) gasoline is the main contributor to the refinery gasoline pool in the LUKOIL Neftohim Burgas (LNB) refinery. Next in quantity contributor in the refinery gasoline pool is the reformate. The FCC gasoline sensitivity (MON-RON) is about 12 points. The reformer gasoline sensitivity is 11 points. The high sensitivity of the main contributors to the LNB refinery gasoline pool leads to a shortage in the motor octane number. For that reason a selection of an FCC catalyst that is capable of increasing the motor octane number of the FCC gasoline was performed. The application of this catalyst in the LNB FCC unit has led to an increase of the motor octane number of the FCC gasoline by 0.5 points, which enabled the refinery to increase the production of automotive gasolines by 1.3 % and to increase the share of premium automotive gasoline by 5 %. This had an effect of improvement of the refinery economics by a six figure number of US $ per year. The optimization of the FCC gasoline Reid Vapor Pressure (RVP) during the winter season, consisting in a reduction of the RVP from 60 to 50 kPa and an increase of the FCC C 4 olefins yield, has led to an augmentation of high motor octane number alkylate production. As a result the refinery economics was improved by a five figure number of US $ per year. key words: FCC gasoline motor octane number, gasoline RVP, FCC operation profitability

  10. N/S/B-doped graphitized carbon encased Fe species as a highly active and durable catalyst towards oxygen reduction reaction.

    Science.gov (United States)

    Li, Guang-Lan; Cheng, Guang-Chun; Chen, Wen-Wen; Liu, Cai-Di; Yuan, Li-Fang; Yang, Bei-Bei; Hao, Ce

    2018-03-15

    Exploring cost-effective, high-performance and durable non-precious metal catalysts is of great significance for the acceleration of sluggish oxygen reduction reaction (ORR). Here, we report an intriguing heteroatom-doped graphitized carbon encased Fe species composite by introducing N, S and B sequentially. The experimental approach was designed ingeniously for that the FeCl 3 ·6H 2 O could catalyze thiourea to synthesize N, S co-doped carbon materials which would further react with H 3 BO 3 and NH 3 (emerged at the heat-treatment process) to prepare N, S and B co-doped carbon materials (Fe-N/S/B-C). The Fe-N/S/B-C exhibits an impressive ORR activity for its half-wave potential of -0.1 V, which is 36 mV or 19 mV higher than that of the corresponding single or dual doped counterparts (Fe-N-C or Fe-N/S-C) and 31 mV positive than that of Pt/C catalyst, respectively. Further chronoamperometric measurement and accelerated aging test confirm the excellent electrochemical durability of Fe-N/S/B-C with the stable core-shell structure. The remarkable ORR performance and facile preparation method enable Fe-N/S/B-C as a potential candidate in electrochemical energy devices. Copyright © 2017 Elsevier Inc. All rights reserved.

  11. Selective catalytic reduction of NO{sub x} in lean-burn engine exhaust over a Pt/V/MCM-41 catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Jeon, Jong Yeol; Kim, Hee Young [Division of Advanced Chemical Technology, Korea Reasearch Institute of Chemical Technology, P.O. Box 107, Yusong, Taejon 305-600 (Korea, Republic of); Woo, Seong Ihl [Department of Chemical and Biomolecular Engineering, Center for Ultramicrochemical Process Systems, Korea Advanced Institute of Science and Technology, 373-1, Kusong-dong, Yusong-gu, Taejon, 305-701 (Korea, Republic of)

    2003-09-08

    The activities of Pt supported on various metal-substituted MCM-41 (V-, Ti-, Fe-, Al-, Ga-, La-, Co-, Mo-, Ce-, and Zr-MCM-41) and V-impregnated MCM-41 were investigated for the reduction of NO by C{sub 3}H{sub 6}. Among these catalysts, Pt supported on V-impregnated MCM-41 showed the best activity. The maximum conversion of NO into N{sub 2}+N{sub 2}O over this Pt/V/MCM-41 catalyst (Pt=1wt.%, V=3.8wt.%) was 73%, and this maximum conversion was sustained over a temperature range of 70C from 270 to 340C. The high activity of Pt/V/MCM-41 over a broad temperature range resulted from two additional reactions besides the reaction occurring on usual supported Pt, the reaction of NO with surface carbonaceous materials, and the reaction of NO occurring on support V-impregnated MCM-41. The former additional reaction showed an oscillation characteristic, a phenomenon in which the concentrations of parts of reactant and product gases oscillate continuously. At low temperature, some water vapor injected into the reactant gas mixture promoted the reaction occurring on usual supported Pt, whereas at high temperature, it suppressed the additional reaction related to carbonaceous materials. Five-hundred parts per million of SO{sub 2} added to the reactant gas mixture only slightly decreased the NO conversion of Pt/V/MCM-41.

  12. Low NOx combustion technologies for high-temperature natural gas combustion

    International Nuclear Information System (INIS)

    Flamme, Michael

    1999-01-01

    Because of the high process temperature which is required for some processes like glass melting and the high temperature to which the combustion air is preheated, NOx emission are extremely high. Even at these high temperatures, NOx emissions could be reduced drastically by using advanced combustion techniques such as staged combustion or flame-less oxidation, as experimental work has shown. In the case of oxy-fuel combustion, the NOx emission are also very high if conventional burners are used. The new combustion techniques achieve similar NOx reductions. (author)

  13. Systematic Investigations of the Oxygen Reduction Reaction on Pt Based Catalysts Comparing Transient and Steady State Performance

    DEFF Research Database (Denmark)

    Deng, Yujia

    . Above 0.6 VRHE, OHad begins to form on the surface and at0.95 VRHE a monolayer completes. Above 0.95 VRHE, OHad can be oxidized to Oad and at 1.1VRHE a monolayer of Oad is formed. When the potential increases further above 1.1 VRHE, Pt-oxidestarts to form. The ORR can only proceed on free Pt sites...... the electrode potential is held. A combination of a site blockingmechanism and an increase in viscosity at the polarized electrode surface is proposed toexplain this extraordinary behavior in H3PO4.Atomic layer deposition of Pt onto an Au substrate is employed as model catalyst toinvestigate how ligand...

  14. Mg-Cu-Al layered double hydroxides based catalysts for the reduction of nitrates in aqueous solutions

    Directory of Open Access Journals (Sweden)

    Vulić Tatjana J.

    2010-01-01

    Full Text Available The secondary waste and bacterial contamination in physico-chemical and biological separation processes used today for nitrate removal from ground water make novel catalytic technologies that convert nitrates to unharmful gaseous nitrogen, very attractive for scientific research. The Mg-Cu-Al layered double hydroxide (LDH based catalysts with different Mg/Al ratio were investigated in water denitrification reaction in the presence of hydrogen and with solely copper as an active phase. Since LDHs have ion exchange properties and their derived mixed oxides possess memory effect (restoration of layered structure after thermal decomposition, their adsorption capacity for nitrates was also measured in the same model system. All studied samples showed nitrate removal from 23% to 62% following the decrease in Al content, as well as the substantial adsorption capacity ranging from 18% to 38%. These results underlie the necessity to take into account the effects of the adsorption in all future investigations.

  15. SEMS operating as a proven system for screening real-world NOx and NH3 emissions

    NARCIS (Netherlands)

    Vermeulen, R.J.; Goethem, S. van; Baarbe, H.L.; Zuidgeest, L.W.M.; Spreen, J.S.; Vonk, W.A.

    2014-01-01

    NOx emissions of heavy-duty and light-duty diesel vehicles depend strongly on the driving conditions. The introduction of combined emission reduction technologies in Euro VI vehicles have demonstrated that NOx emissions become less predictable when the data is based on relatively short test cycles.

  16. 40 CFR 76.5 - NOX emission limitations for Group 1 boilers.

    Science.gov (United States)

    2010-07-01

    ... 40 Protection of Environment 16 2010-07-01 2010-07-01 false NOX emission limitations for Group 1 boilers. 76.5 Section 76.5 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) ACID RAIN NITROGEN OXIDES EMISSION REDUCTION PROGRAM § 76.5 NOX emission limitations...

  17. 40 CFR 76.6 - NOX emission limitations for Group 2 boilers.

    Science.gov (United States)

    2010-07-01

    ... 40 Protection of Environment 16 2010-07-01 2010-07-01 false NOX emission limitations for Group 2 boilers. 76.6 Section 76.6 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) ACID RAIN NITROGEN OXIDES EMISSION REDUCTION PROGRAM § 76.6 NOX emission limitations...

  18. 40 CFR 76.7 - Revised NOX emission limitations for Group 1, Phase II boilers.

    Science.gov (United States)

    2010-07-01

    ... 40 Protection of Environment 16 2010-07-01 2010-07-01 false Revised NOX emission limitations for Group 1, Phase II boilers. 76.7 Section 76.7 Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) ACID RAIN NITROGEN OXIDES EMISSION REDUCTION PROGRAM § 76.7 Revised NOX...

  19. Electrochemical investigations of Co3Fe-RGO as a bifunctional catalyst for oxygen reduction and evolution reactions in alkaline media

    Science.gov (United States)

    Kumar, Surender; Kumar, Divyaratan; Kishore, Brij; Ranganatha, Sudhakar; Munichandraiah, Nookala; Venkataramanan, Natarajan S.

    2017-10-01

    Nanoparticles of Co3Fe alloy is prepared on reduced graphene oxide (RGO) sheets by modified polyol method. Synthesized alloy particles are characterized by various physicochemical techniques. TEM and SEM pictures showed homogeneously dispersed alloy nanoparticles on the RGO sheets. Electrochemistry of alloy nanoparticles is investigated in alkaline medium. The result shows that oxygen evaluation reaction (OER) activity of Co3Fe-RGO is higher than Pt-black particles. RDE studies in alkaline medium shows that oxygen reduction reaction (ORR) follow four electron pathway. It is suggest that Co3Fe-RGO is an efficient non-precious catalyst for oxygen (ORR/OER) reactions in alkaline electrolyte for PEMFC applications.

  20. High-Throughput Screening as a Supplemental Tool for the Development of Advanced Emission Control Catalysts: Methodological Approaches and Data Processing

    Directory of Open Access Journals (Sweden)

    Andreas Sundermann

    2016-01-01

    Full Text Available A high-throughput (HT screening platform developed at hte with the application focus on automotive catalysis is described. hte HT units are configured for performing steady-state testing, as well as dynamic tests with fast feed switches, such as lean/rich excursions for the evaluation of NOx storage capacity and efficiency of lean NOx traps (LNT, ammonia storage capacity for selective catalytic reduction (SCR, evaluation of oxygen storage capacity (OSC, as well as lambda sweep tests for screening of three-way catalysts (TWC. Even though catalysts are screened on a rather small scale (~100 mg powder, experience showed that dosing rather complex gas mixtures in concentrations close to that found in real exhaust for the given application is mandatory to generate relevant data. The objective of this work is to give additional insight into HT technology. In the industrial research laboratory, HT screening has matured to become a reliable approach for rapid screening of both reaction parameter spaces, as well as material properties relevant for exhaust gas catalyst development. Due to the speed of optimized screening involving 48 parallel reactors, automated handling of primary data is an imported requirement. Software for data reduction, like estimation of light-of