Combined UHV/high-pressure catalysis setup for depth-resolved near-surface spectroscopic characterization and catalytic testing of model catalysts

NASA Astrophysics Data System (ADS)

Mayr, Lukas; Rameshan, Raffael; Klötzer, Bernhard; Penner, Simon; Rameshan, Christoph

2014-05-01

An ultra-high vacuum (UHV) setup for "real" and "inverse" model catalyst preparation, depth-resolved near-surface spectroscopic characterization, and quantification of catalytic activity and selectivity under technologically relevant conditions is described. Due to the all-quartz reactor attached directly to the UHV-chamber, transfer of the catalyst for in situ testing without intermediate contact to the ambient is possible. The design of the UHV-compatible re-circulating batch reactor setup allows the study of reaction kinetics under close to technically relevant catalytic conditions up to 1273 K without contact to metallic surfaces except those of the catalyst itself. With the attached differentially pumped exchangeable evaporators and the quartz-microbalance thickness monitoring equipment, a reproducible, versatile, and standardised sample preparation is possible. For three-dimensional near-surface sample characterization, the system is equipped with a hemispherical analyser for X-ray photoelectron spectroscopy (XPS), electron-beam or X-ray-excited Auger-electron spectroscopy, and low-energy ion scattering measurements. Due the dedicated geometry of the X-ray gun (54.7°, "magic angle") and the rotatable sample holder, depth analysis by angle-resolved XPS measurements can be performed. Thus, by the combination of characterisation methods with different information depths, a detailed three-dimensional picture of the electronic and geometric structure of the model catalyst can be obtained. To demonstrate the capability of the described system, comparative results for depth-resolved sample characterization and catalytic testing in methanol steam reforming on PdGa and PdZn near-surface intermetallic phases are shown.

Performance and emissions of a catalytic reactor with propane, diesel, and Jet A fuels

NASA Technical Reports Server (NTRS)

Anderson, D. N.

1977-01-01

Tests were made to determine the performance and emissions of a catalytic reactor operated with propane, No. 2 diesel, and Jet A fuels. A 12-cm diameter and 16-cm long catalytic reactor using a proprietary noble metal catalyst was operated at an inlet temperature of 800 K, a pressure of 300,000 Pa and reference velocities of 10 to 15 m/s. No significant differences between the performance of the three fuels were observed when 98.5 percent purity propane was used. The combustion efficiency for 99.8-percent purity propane tested later was significantly lower, however. The diesel fuel contained 135 ppm of bound nitrogen and consequently produced the highest NOx emissions of the three fuels. As much as 85 percent of the bound nitrogen was converted to NOx. Steady-state emissions goals based on half the most stringent proposed automotive standards were met when the reactor was operated at an adiabatic combustion temperature higher than 1350 K with all fuels except the 99.8-percent purity propane. With that fuel, a minimum temperature of 1480 K was required.

Vapor Phase Catalytic Ammonia Reduction

NASA Technical Reports Server (NTRS)

Flynn, Michael T.; Harper, Lynn D. (Technical Monitor)

1994-01-01

This paper discusses the development of a Vapor Phase Catalytic Ammonia Reduction (VPCAR) teststand and the results of an experimental program designed to evaluate the potential of the technology as a water purification process. In the experimental program the technology is evaluated based upon product water purity, water recovery rate, and power consumption. The experimental work demonstrates that the technology produces high purity product water and attains high water recovery rates at a relatively high specific power consumption. The experimental program was conducted in 3 phases. In phase I an Igepon(TM) soap and water mixture was used to evaluate the performance of an innovative Wiped-Film Rotating-Disk evaporator and associated demister. In phase II a phenol-water solution was used to evaluate the performance of the high temperature catalytic oxidation reactor. In phase III a urine analog was used to evaluate the performance of the combined distillation/oxidation functions of the processor.

Continuous-flow processes for the catalytic partial hydrogenation reaction of alkynes

PubMed Central

Moreno-Marrodan, Carmen; Liguori, Francesca

2017-01-01

The catalytic partial hydrogenation of substituted alkynes to alkenes is a process of high importance in the manufacture of several market chemicals. The present paper shortly reviews the heterogeneous catalytic systems engineered for this reaction under continuous flow and in the liquid phase. The main contributions appeared in the literature from 1997 up to August 2016 are discussed in terms of reactor design. A comparison with batch and industrial processes is provided whenever possible. PMID:28503209

Catalytic combustion of coal-derived liquids

NASA Technical Reports Server (NTRS)

Bulzan, D. L.; Tacina, R. R.

1981-01-01

A noble metal catalytic reactor was tested with three grades of SRC 2 coal derived liquids, naphtha, middle distillate, and a blend of three parts middle distillate to one part heavy distillate. A petroleum derived number 2 diesel fuel was also tested to provide a direct comparison. The catalytic reactor was tested at inlet temperatures from 600 to 800 K, reference velocities from 10 to 20 m/s, lean fuel air ratios, and a pressure of 3 x 10 to the 5th power Pa. Compared to the diesel, the naphtha gave slightly better combustion efficiency, the middle distillate was almost identical, and the middle heavy blend was slightly poorer. The coal derived liquid fuels contained from 0.58 to 0.95 percent nitrogen by weight. Conversion of fuel nitrogen to NOx was approximately 75 percent for all three grades of the coal derived liquids.

Katie Gaston | NREL

Science.gov Websites

gasification. The new catalytic riser reactor system can be used for ex situ vapor-phase upgrading or steam , and Wood: 1. Parametric Study and Comparison with Literature," Industrial & Engineering

Development of a high-temperature durable catalyst for use in catalytic combustors for advanced automotive gas turbine engines

NASA Astrophysics Data System (ADS)

Tong, H.; Snow, G. C.; Chu, E. K.; Chang, R. L. S.; Angwin, M. J.; Pessagno, S. L.

1981-09-01

Durable catalytic reactors for advanced gas turbine engines were developed. Objectives were: to evaluate furnace aging as a cost effective catalytic reactor screening test, measure reactor degradation as a function of furnace aging, demonstrate 1,000 hours of combustion durability, and define a catalytic reactor system with a high probability of successful integration into an automotive gas turbine engine. Fourteen different catalytic reactor concepts were evaluated, leading to the selection of one for a durability combustion test with diesel fuel for combustion conditions. Eight additional catalytic reactors were evaluated and one of these was successfully combustion tested on propane fuel. This durability reactor used graded cell honeycombs and a combination of noble metal and metal oxide catalysts. The reactor was catalytically active and structurally sound at the end of the durability test.

Development of a high-temperature durable catalyst for use in catalytic combustors for advanced automotive gas turbine engines

NASA Technical Reports Server (NTRS)

Tong, H.; Snow, G. C.; Chu, E. K.; Chang, R. L. S.; Angwin, M. J.; Pessagno, S. L.

1981-01-01

Durable catalytic reactors for advanced gas turbine engines were developed. Objectives were: to evaluate furnace aging as a cost effective catalytic reactor screening test, measure reactor degradation as a function of furnace aging, demonstrate 1,000 hours of combustion durability, and define a catalytic reactor system with a high probability of successful integration into an automotive gas turbine engine. Fourteen different catalytic reactor concepts were evaluated, leading to the selection of one for a durability combustion test with diesel fuel for combustion conditions. Eight additional catalytic reactors were evaluated and one of these was successfully combustion tested on propane fuel. This durability reactor used graded cell honeycombs and a combination of noble metal and metal oxide catalysts. The reactor was catalytically active and structurally sound at the end of the durability test.

Mixed ionic and electronic conducting ceramic membranes for hydrocarbon processing

DOEpatents

Van Calcar, Pamela; Mackay, Richard; Sammells, Anthony F.

2002-01-01

The invention relates to mixed phase materials for the preparation of catalytic membranes which exhibit ionic and electronic conduction and which exhibit improved mechanical strength compared to single phase ionic and electronic conducting materials. The mixed phase materials are useful for forming gas impermeable membranes either as dense ceramic membranes or as dense thin films coated onto porous substrates. The membranes and materials of this invention are useful in catalytic membrane reactors in a variety of applications including synthesis gas production. One or more crystalline second phases are present in the mixed phase material at a level sufficient to enhance the mechanical strength of the mixture to provide membranes for practical application in CMRs.

Solid state proton and electron mediating membrane and use in catalytic membrane reactors

DOEpatents

White, J.H.; Schwartz, M.; Sammells, A.F.

1998-10-13

This invention provides catalytic proton and electron mediating membranes useful in catalytic reactors. The membranes have an oxidation and a reduction surface and comprise a single-phase mixed metal oxide material of the formula: AB{sub 1{minus}x}B{prime}{sub x}O{sub 3{minus}y} wherein A is selected from Ca, Sr or Ba ions; B is selected from Ce, Tb, Pr, or Th ions; B{prime} is selected from Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Al, Ga, or In ions, or combinations thereof; and x is greater than or equal to 0.02 and less than or equal to 0.5. The membranes can further comprise a catalyst on either the oxidation or reduction surface, or both. Membranes include those which are fabricated by combining powders of metal oxides or metal carbonates of metal A ion, metal B ion and metal B{prime} ion such that the stoichiometric ratio A:B:B{prime} is 1:1{minus}x:x where 0.2{<=}{times}0.5, repeatedly calcining and milling the combined powders until a single-phase material is obtained and pressing and sintering the single phase material to obtain a membrane. 6 figs.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Camacho-Bunquin, Jeffrey; Shou, Heng; Marshall, Christopher L.

An integrated atomic layer deposition synthesis-catalysis (I-ALD-CAT) tool was developed. It combines an ALD manifold in-line with a plug-flow reactor system for the synthesis of supported catalytic materials by ALD and immediate evaluation of catalyst reactivity using gas-phase probe reactions. The I-ALD-CAT delivery system consists of 12 different metal ALD precursor channels, 4 oxidizing or reducing agents, and 4 catalytic reaction feeds to either of the two plug-flow reactors. The system can employ reactor pressures and temperatures in the range of 10{sup −3} to 1 bar and 300–1000 K, respectively. The instrument is also equipped with a gas chromatograph andmore » a mass spectrometer unit for the detection and quantification of volatile species from ALD and catalytic reactions. In this report, we demonstrate the use of the I-ALD-CAT tool for the synthesis of platinum active sites and Al{sub 2}O{sub 3} overcoats, and evaluation of catalyst propylene hydrogenation activity.« less

Oxidative coupling of methane using inorganic membrane reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ma, Y.H.; Moser, W.R.; Dixon, A.G.

1995-12-31

The goal of this research is to improve the oxidative coupling of methane in a catalytic inorganic membrane reactor. A specific target is to achieve conversion of methane to C{sub 2} hydrocarbons at very high selectivity and relatively higher yields than in fixed bed reactors by controlling the oxygen supply through the membrane. A membrane reactor has the advantage of precisely controlling the rate of delivery of oxygen to the catalyst. This facility permits balancing the rate of oxidation and reduction of the catalyst. In addition, membrane reactors minimize the concentration of gas phase oxygen thus reducing non selective gasmore » phase reactions, which are believed to be a main route for formation of CO{sub x} products. Such gas phase reactions are a cause for decreased selectivity in oxidative coupling of methane in conventional flow reactors. Membrane reactors could also produce higher product yields by providing better distribution of the reactant gases over the catalyst than the conventional plug flow reactors. Modeling work which aimed at predicting the observed experimental trends in porous membrane reactors was also undertaken in this research program.« less

Coal hydrogenation and deashing in ebullated bed catalytic reactor

DOEpatents

Huibers, Derk T. A.; Johanson, Edwin S.

1983-01-01

An improved process for hydrogenation of coal containing ash with agglomeration and removal of ash from an ebullated bed catalytic reactor to produce deashed hydrocarbon liquid and gas products. In the process, a flowable coal-oil slurry is reacted with hydrogen in an ebullated catalyst bed reaction zone at elevated temperature and pressure conditions. The upward velocity and viscosity of the reactor liquid are controlled so that a substantial portion of the ash released from the coal is agglomerated to form larger particles in the upper portion of the reactor above the catalyst bed, from which the agglomerated ash is separately withdrawn along with adhering reaction zone liquid. The resulting hydrogenated hydrocarbon effluent material product is phase separated to remove vapor fractions, after which any ash remaining in the liquid fraction can be removed to produce substantially ash-free coal-derived liquid products.

Method and apparatus for monitoring a hydrocarbon-selective catalytic reduction device

DOEpatents

Schmieg, Steven J; Viola, Michael B; Cheng, Shi-Wai S; Mulawa, Patricia A; Hilden, David L; Sloane, Thompson M; Lee, Jong H

2014-05-06

A method for monitoring a hydrocarbon-selective catalytic reactor device of an exhaust aftertreatment system of an internal combustion engine operating lean of stoichiometry includes injecting a reductant into an exhaust gas feedstream upstream of the hydrocarbon-selective catalytic reactor device at a predetermined mass flowrate of the reductant, and determining a space velocity associated with a predetermined forward portion of the hydrocarbon-selective catalytic reactor device. When the space velocity exceeds a predetermined threshold space velocity, a temperature differential across the predetermined forward portion of the hydrocarbon-selective catalytic reactor device is determined, and a threshold temperature as a function of the space velocity and the mass flowrate of the reductant is determined. If the temperature differential across the predetermined forward portion of the hydrocarbon-selective catalytic reactor device is below the threshold temperature, operation of the engine is controlled to regenerate the hydrocarbon-selective catalytic reactor device.

Computer model of catalytic combustion/Stirling engine heater head

NASA Technical Reports Server (NTRS)

Chu, E. K.; Chang, R. L.; Tong, H.

1981-01-01

The basic Acurex HET code was modified to analyze specific problems for Stirling engine heater head applications. Specifically, the code can model: an adiabatic catalytic monolith reactor, an externally cooled catalytic cylindrical reactor/flat plate reactor, a coannular tube radiatively cooled reactor, and a monolithic reactor radiating to upstream and downstream heat exchangers.

Carbon Dioxide Reduction Systems

NASA Technical Reports Server (NTRS)

Burghardt, Stanley I.; Chandler, Horace W.; Taylor, T. I.; Walden, George

1961-01-01

The Methoxy system for regenerating oxygen from carbon dioxide was studied. Experiments indicate that the reaction between carbon dioxide and hydrogen can be carried out with ease in an efficient manner and with excellent heat conservation. A small reactor capable of handling the C02 expired by three men has been built and operated. The decomposition of methane by therma1,arc and catalytic processes was studied. Both the arc and catalytic processes gave encouraging results with over 90 percent of the methane being decomposed to carbon and hydrogen in some of the catalytic processes. Control of the carbon deposition in both the catalytic and arc processes is of great importance to prevent catalyst deactivation and short circuiting of electrical equipment. Sensitive analytical techniques have been developed for all of the components present in the reactor effluent streams.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Agblevor, Foster A.; Elliott, Douglas C.; Santosa, Daniel M.

Pinyon juniper biomass feedstocks, which cover a large acreage of rangeland in the western United States, are being eradicated and, therefore, considered as a convenient biomass feedstock for biofuel production. Pinyon juniper whole biomass (wood, bark, and leaves) were pyrolyzed in a pilot-scale bubbling fluidized-bed reactor at 450 °C, and the noncondensable gases were recycled to fluidize the reactor. Red mud was used as the in situ catalyst for the pyrolysis of the pinyon juniper biomass. The pyrolysis products were condensed in three stages, and products were analyzed for physicochemical properties. The condenser oil formed two phases with the aqueousmore » fraction, whereas the electrostatic precipitator oils formed a single phase. The oil pH was 3.3; the higher heating value (HHV) was 28 MJ/kg; and the viscosity was less than 100 cP. There was a direct correlation between the viscosity of the oils and the alcohol/ether content of the oils, and this was also related to the aging rate of the oils. The catalytic pyrolysis oils were hydrotreated in a continuous single-stage benchtop hydrotreater to produce hydrocarbon fuels with a density of 0.80$-$0.82 cm 3/g. The hydrotreater ran continuously for over 300 h with no significant catalyst deactivation or coke formation. This is the first time that such a long single-stage hydrotreatment has been demonstrated on biomass catalytic pyrolysis oils.« less

Microchannel Reactor System for Catalytic Hydrogenation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Adeniyi Lawal; Woo Lee; Ron Besser

2010-12-22

We successfully demonstrated a novel process intensification concept enabled by the development of microchannel reactors, for energy efficient catalytic hydrogenation reactions at moderate temperature, and pressure, and low solvent levels. We designed, fabricated, evaluated, and optimized a laboratory-scale microchannel reactor system for hydrogenation of onitroanisole and a proprietary BMS molecule. In the second phase of the program, as a prelude to full-scale commercialization, we designed and developed a fully-automated skid-mounted multichannel microreactor pilot plant system for multiphase reactions. The system is capable of processing 1 – 10 kg/h of liquid substrate, and an industrially relevant immiscible liquid-liquid was successfully demonstratedmore » on the system. Our microreactor-based pilot plant is one-of-akind. We anticipate that this process intensification concept, if successfully demonstrated, will provide a paradigm-changing basis for replacing existing energy inefficient, cost ineffective, environmentally detrimental slurry semi-batch reactor-based manufacturing practiced in the pharmaceutical and fine chemicals industries.« less

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

PubMed

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.

Solid state proton and electron mediating membrane and use in catalytic membrane reactors

DOEpatents

White, James H.; Schwartz, Michael; Sammells, Anthony F.

1998-01-01

This invention provides catalytic proton and electron mediating membranes useful in catalytic reactors. The membranes have an oxidation and a reduction surface and comprise a single-phase mixed metal oxide material of the formula: AB.sub.1-x B'.sub.x O.sub.3-y wherein A is selected from Ca, Sr or Ba ions; B is selected from Ce, Tb, Pr, or Th ions; B' is selected from Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Al, Ga, or In ions, or combinations thereof; and x is greater than or equal to 0.02 and less than or equal to 0.5. The membranes can further comprise a catalyst on either the oxidation or reduction surface, or both. Membranes include those which are fabricated-by combining powders of metal oxides or metal carbonates of metal A ion, metal B ion and metal B' ion such that the stoichiometric ratio A:B:B' is 1:1-x:x where 0.2.ltoreq..times.0.5, repeatedly calcining and milling the combined powders until a single-phase material is obtained and pressing and sintering the singlephase material to obtain a membrane.

Conversion of NO with a catalytic packed-bed dielectric barrier discharge reactor

NASA Astrophysics Data System (ADS)

Xu, CAO; Weixuan, ZHAO; Renxi, ZHANG; Huiqi, HOU; Shanping, CHEN; Ruina, ZHANG

2017-11-01

This paper discusses the conversion of nitric oxide (NO) with a low-temperature plasma induced by a catalytic packed-bed dielectric barrier discharge (DBD) reactor. Alumina oxide (Al2O3), glass (SiO2) and zirconium oxide (ZrO2), three different spherical packed materials of the same size, were each present in the DBD reactor. The NO conversion under varying input voltage and specific energy density, and the effects of catalysts (titanium dioxide (TiO2) and manganese oxide (MnO x ) coated on Al2O3) on NO conversion were investigated. The experimental results showed that NO conversion was greatly enhanced in the presence of packed materials in the reactor, and the catalytic packed bed of MnO x /Al2O3 showed better performance than that of TiO2/Al2O3. The surface and crystal structures of the materials and catalysts were characterized through scanning electron microscopy analysis. The final products were clearly observed by a Fourier transform infrared spectrometer and provided a better understanding of NO conversion.

Apparatus for the investigation of high-temperature, high-pressure gas-phase heterogeneous catalytic and photo-catalytic materials.

PubMed

Alvino, Jason F; Bennett, Trystan; Kler, Rantej; Hudson, Rohan J; Aupoil, Julien; Nann, Thomas; Golovko, Vladimir B; Andersson, Gunther G; Metha, Gregory F

2017-05-01

A high-temperature, high-pressure, pulsed-gas sampling and detection system has been developed for testing new catalytic and photocatalytic materials for the production of solar fuels. The reactor is fitted with a sapphire window to allow the irradiation of photocatalytic samples from a lamp or solar simulator light source. The reactor has a volume of only 3.80 ml allowing for the investigation of very small quantities of a catalytic material, down to 1 mg. The stainless steel construction allows the cell to be heated to 350 °C and can withstand pressures up to 27 bar, limited only by the sapphire window. High-pressure sampling is made possible by a computer controlled pulsed valve that delivers precise gas flow, enabling catalytic reactions to be monitored across a wide range of pressures. A residual gas analyser mass spectrometer forms a part of the detection system, which is able to provide a rapid, real-time analysis of the gas composition within the photocatalytic reaction chamber. This apparatus is ideal for investigating a number of industrially relevant reactions including photocatalytic water splitting and CO 2 reduction. Initial catalytic results using Pt-doped and Ru nanoparticle-doped TiO 2 as benchmark experiments are presented.

Dehydrogenation of liquid fuel in microchannel catalytic reactor

DOEpatents

Toseland, Bernard Allen; Pez, Guido Peter; Puri, Pushpinder Singh

2010-08-03

The present invention is an improved process for the storage and delivery of hydrogen by the reversible hydrogenation/dehydrogenation of an organic compound wherein the organic compound is initially in its hydrogenated state. The improvement in the route to generating hydrogen is in the dehydrogenation step and recovery of the dehydrogenated organic compound resides in the following steps: introducing a hydrogenated organic compound to a microchannel reactor incorporating a dehydrogenation catalyst; effecting dehydrogenation of said hydrogenated organic compound under conditions whereby said hydrogenated organic compound is present as a liquid phase; generating a reaction product comprised of a liquid phase dehydrogenated organic compound and gaseous hydrogen; separating the liquid phase dehydrogenated organic compound from gaseous hydrogen; and, recovering the hydrogen and liquid phase dehydrogenated organic compound.

Dehydrogenation of liquid fuel in microchannel catalytic reactor

DOEpatents

Toseland, Bernard Allen [Allentown, PA; Pez, Guido Peter [Allentown, PA; Puri, Pushpinder Singh [Emmaus, PA

2009-02-03

The present invention is an improved process for the storage and delivery of hydrogen by the reversible hydrogenation/dehydrogenation of an organic compound wherein the organic compound is initially in its hydrogenated state. The improvement in the route to generating hydrogen is in the dehydrogenation step and recovery of the dehydrogenated organic compound resides in the following steps: introducing a hydrogenated organic compound to a microchannel reactor incorporating a dehydrogenation catalyst; effecting dehydrogenation of said hydrogenated organic compound under conditions whereby said hydrogenated organic compound is present as a liquid phase; generating a reaction product comprised of a liquid phase dehydrogenated organic compound and gaseous hydrogen; separating the liquid phase dehydrogenated organic compound from gaseous hydrogen; and, recovering the hydrogen and liquid phase dehydrogenated organic compound.

Method and apparatus for a catalytic firebox reactor

DOEpatents

Smith, Lance L.; Etemad, Shahrokh; Ulkarim, Hasan; Castaldi, Marco J.; Pfefferle, William C.

2001-01-01

A catalytic firebox reactor employing an exothermic catalytic reaction channel and multiple cooling conduits for creating a partially reacted fuel/oxidant mixture. An oxidation catalyst is deposited on the walls forming the boundary between the multiple cooling conduits and the exothermic catalytic reaction channel, on the side of the walls facing the exothermic catalytic reaction channel. This configuration allows the oxidation catalyst to be backside cooled by any fluid passing through the cooling conduits. The heat of reaction is added to both the fluid in the exothermic catalytic reaction channel and the fluid passing through the cooling conduits. After discharge of the fluids from the exothermic catalytic reaction channel, the fluids mix to create a single combined flow. A further innovation in the reactor incorporates geometric changes in the exothermic catalytic reaction channel to provide streamwise variation of the velocity of the fluids in the reactor.

Method of producing gaseous products using a downflow reactor

DOEpatents

Cortright, Randy D; Rozmiarek, Robert T; Hornemann, Charles C

2014-09-16

Reactor systems and methods are provided for the catalytic conversion of liquid feedstocks to synthesis gases and other noncondensable gaseous products. The reactor systems include a heat exchange reactor configured to allow the liquid feedstock and gas product to flow concurrently in a downflow direction. The reactor systems and methods are particularly useful for producing hydrogen and light hydrocarbons from biomass-derived oxygenated hydrocarbons using aqueous phase reforming. The generated gases may find used as a fuel source for energy generation via PEM fuel cells, solid-oxide fuel cells, internal combustion engines, or gas turbine gensets, or used in other chemical processes to produce additional products. The gaseous products may also be collected for later use or distribution.

Conversion of wood residues to diesel fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuester, J.L.

1981-01-01

The basic approach is indirect liquefaction, i.e., thermal gasification followed by catalytic liquefaction. The indirect approach results in separation of the oxygen in the biomass feedstock, i.e., oxygenated compounds do not appear in the liquid hydrocarbon fuel product. The general conversion scheme is shown. The process is capable of accepting a wide variety of feedstocks. Potential products include medium quality gas, normal propanol, paraffinic fuel and/or high octane gasoline. A flow diagram of the continuous laboratory unit is shown. A fluidized bed pyrolysis system is used for gasification. Capacity is about 10 lbs/h of feedstock. The pyrolyzer can be fluidizedmore » with recycle pyrolysis gas, steam or recycle liquefaction system off gas or some combination thereof. Tars are removed in a wet scrubber. Unseparated pyrolysis gases are utilized as feed to a modified Fischer-Tropsch reactor. The liquid condensate from the reactor consists of a normal propanol-water phase and a paraffinic hydrocarbon phase. The reactor can be operated to optimize for either product. If a high octane gasoline is desired, the paraffinic fuel is passed through a conventional catalytic reformer. The normal propanol could be used as a fuel extender if blended with the hydrocarbon fuel products. Off gases from the downstream reactors are of high quality due to the accumulation of low molecular weight paraffins.« less

Catalytic Ignition and Upstream Reaction Propagation in a Platinum Tube

NASA Technical Reports Server (NTRS)

Struk, P. M.; Dietrich, D. L.; Mellish, B. P.; Miller, F. J.; T'ien, J. S.

2007-01-01

A challenge for catalytic combustion in monolithic reactors at elevated temperatures is the start-up or "light-off" from a cold initial condition. In this work, we demonstrate a concept called "back-end catalytic ignition that potentially can be utilized in the light-off of catalytic monoliths. An external downstream flame or Joule heating raises the temperature of a small portion of the catalyst near the outlet initiating a localized catalytic reaction that propagates upstream heating the entire channel. This work uses a transient numerical model to demonstrate "back-end" ignition within a single channel which can characterize the overall performance of a monolith. The paper presents comparisons to an experiment using a single non-adiabatic channel but the concept can be extended to the adiabatic monolith case. In the model, the time scales associated with solid heat-up are typically several orders of magnitude larger than the gas-phase and chemical kinetic time-scales. Therefore, the model assumes a quasi-steady gas-phase with respect to a transient solid. The gas phase is one-dimensional. Appropriate correlations, however, account for heat and mass transfer in a direction perpendicular to the flow. The thermally-thin solid includes axial conduction. The gas phase, however, does not include axial conduction due to the high Peclet number flows. The model includes both detailed gas-phase and catalytic surface reactions. The experiment utilizes a pure platinum circular channel oriented horizontally though which a CO/O2 mixture (equivalence ratios ranging from 0.6 to 0.9) flows at 2 m/s.

Simple and rapid hydrogenation of p-nitrophenol with aqueous formic acid in catalytic flow reactors

PubMed Central

Kawasaki, Shin-ichiro; Suzuki, Akira

2013-01-01

Summary The inner surface of a metallic tube (i.d. 0.5 mm) was coated with a palladium (Pd)-based thin metallic layer by flow electroless plating. Simultaneous plating of Pd and silver (Ag) from their electroless-plating solution produced a mixed distributed bimetallic layer. Preferential acid leaching of Ag from the Pd–Ag layer produced a porous Pd surface. Hydrogenation of p-nitrophenol was examined in the presence of formic acid simply by passing the reaction solution through the catalytic tubular reactors. p-Aminophenol was the sole product of hydrogenation. No side reaction occurred. Reaction conversion with respect to p-nitrophenol was dependent on the catalyst layer type, the temperature, pH, amount of formic acid, and the residence time. A porous and oxidized Pd (PdO) surface gave the best reaction conversion among the catalytic reactors examined. p-Nitrophenol was converted quantitatively to p-aminophenol within 15 s of residence time in the porous PdO reactor at 40 °C. Evolution of carbon dioxide (CO2) was observed during the reaction, although hydrogen (H2) was not found in the gas phase. Dehydrogenation of formic acid did not occur to any practical degree in the absence of p-nitrophenol. Consequently, the nitro group was reduced via hydrogen transfer from formic acid to p-nitrophenol and not by hydrogen generated by dehydrogenation of formic acid. PMID:23843908

Research and proposal on selective catalytic reduction reactor optimization for industrial boiler.

PubMed

Yang, Yiming; Li, Jian; He, Hong

2017-08-24

The advanced computational fluid dynamics (CFD) software STAR-CCM+ was used to simulate a denitrification (De-NOx) project for a boiler in this paper, and the simulation result was verified based on a physical model. Two selective catalytic reduction (SCR) reactors were developed: reactor 1 was optimized and reactor 2 was developed based on reactor 1. Various indicators, including gas flow field, ammonia concentration distribution, temperature distribution, gas incident angle, and system pressure drop were analyzed. The analysis indicated that reactor 2 was of outstanding performance and could simplify developing greatly. Ammonia injection grid (AIG), the core component of the reactor, was studied; three AIGs were developed and their performances were compared and analyzed. The result indicated that AIG 3 was of the best performance. The technical indicators were proposed for SCR reactor based on the study. Flow filed distribution, gas incident angle, and temperature distribution are subjected to SCR reactor shape to a great extent, and reactor 2 proposed in this paper was of outstanding performance; ammonia concentration distribution is subjected to ammonia injection grid (AIG) shape, and AIG 3 could meet the technical indicator of ammonia concentration without mounting ammonia mixer. The developments above on the reactor and the AIG are both of great application value and social efficiency.

An experimental study of catalytic and non-catalytic reaction in heat recirculating reactors and applications to power generation

NASA Astrophysics Data System (ADS)

Ahn, Jeongmin

An experimental study of the performance of a Swiss roll heat exchanger and reactor was conducted, with emphasis on the extinction limits and comparison of results with and without Pt catalyst. At Re<40, the catalyst was required to sustain reaction; with the catalyst self-sustaining reaction could be obtained at Re less than 1. Both lean and rich extinction limits were extended with the catalyst, though rich limits were extended much further. At low Re, the lean extinction limit was rich of stoichiometric and rich limit had equivalence ratios 80 in some cases. Non-catalytic reaction generally occurred in a flameless mode near the center of the reactor. With or without catalyst, for sufficiently robust conditions, a visible flame would propagate out of the center, but this flame could only be re-centered with catalyst. Gas chromatography indicated that at low Re, CO and non-C3 H8 hydrocarbons did not form. For higher Re, catalytic limits were slightly broader but had much lower limit temperatures. At sufficiently high Re, catalytic and gas-phase limits merged. Experiments with titanium Swiss rolls have demonstrated reducing wall thermal conductivity and thickness leads to lower heat losses and therefore increases operating temperatures and extends flammability limits. By use of Pt catalysts, reaction of propane-air mixtures at temperatures 54°C was sustained. Such low temperatures suggest that polymers may be employed as a reactor material. A polyimide reactor was built and survived prolonged testing at temperatures up to 500°C. Polymer reactors may prove more practical for microscale devices due to their lower thermal conductivity and ease of manufacturing. Since the ultimate goal of current efforts is to develop combustion driven power generation devices at MEMS like scales, a thermally self-sustaining miniature power generation device was developed utilizing a single-chamber solid-oxide-fuel-cell (SOFC) placed in a Swiss roll. With the single-chamber design, fuel/oxygen crossover due to cracking of seals via thermal cycling is irrelevant and coking on the anode is practically eliminated. SOFC power densities up to 420mW/cm2 were observed at low Re. These results suggest that single-chamber SOFC's integrated with heat-recirculating reactors may be a viable approach for small-scale power generation devices.

Catalytic Reactor for Inerting of Aircraft Fuel Tanks

DTIC Science & Technology

1974-06-01

Aluminum Panels After Triphase Corrosion Test 79 35 Inerting System Flows in Various Flight Modes 82 36 High Flow Reactor Parametric Data 84 37 System...AD/A-000 939 CATALYTIC REACTOR FOR INERTING OF AIRCRAFT FUEL TANKS George H. McDonald, et al AiResearch Manufacturing Company Prepared for: Air Force...190th Street 2b. GROUP Torrance, California .. REPORT TITLE CATALYTIC REACTOR FOR INERTING OF AIRCRAFT FUEL TANKS . OESCRIP TIVE NOTEs (Thpe of refpoft

Heat production in depth up to 2500m via in situ combustion of methane using a counter-current heat-exchange reactor

NASA Astrophysics Data System (ADS)

Schicks, Judith Maria; Spangenberg, Erik; Giese, Ronny; Heeschen, Katja; Priegnitz, Mike; Luzi-Helbing, Manja; Thaler, Jan; Abendroth, Sven; Klump, Jens

2014-05-01

In situ combustion is a well-known method used for exploitation of unconventional oil deposits such as heavy oil/bitumen reservoirs where the required heat is produced directly within the oil reservoir by combustion of a small percentage of the oil. A new application of in situ combustion for the production of methane from hydrate-bearing sediments was tested at pilot plant scale within the first phase of the German national gas hydrate project SUGAR. The applied method of in situ combustion was a flameless, catalytic oxidation of CH4 in a counter-current heat-exchange reactor with no direct contact between the catalytic reaction zone and the reservoir. The catalyst permitted a flameless combustion of CH4 with air to CO2 and H2O below the auto-ignition temperature of CH4 in air (868 K) and outside the flammability limits. This led to a double secured application of the reactor. The relatively low reaction temperature allowed the use of cost-effective standard materials for the reactor and prevented NOx formation. Preliminary results were promising and showed that only 15% of the produced CH4 was needed to be catalytically burned to provide enough heat to dissociate the hydrates in the environment and release CH4. The location of the heat source right within the hydrate-bearing sediment is a major advantage for the gas production from natural gas hydrates as the heat is generated where it is needed without loss of energy due to transportation. As part of the second period of the SUGAR project the reactor prototype of the first project phase was developed further to a borehole tool. The dimensions of this counter-current heat-exchange reactor are about 540 cm in length and 9 cm in diameter. It is designed for applications up to depths of 2500 m. A functionality test and a pressure test of the reactor were successfully carried out in October 2013 at the continental deep drilling site (KTB) in Windischeschenbach, Germany, in 600 m depth and 2000 m depth, respectively. In this study we present technical details of the reactor, the catalyst and potential fields of application beside the production of natural gas from hydrate bearing sediments.

Reactor for tracking catalyst nanoparticles in liquid at high temperature under a high-pressure gas phase with X-ray absorption spectroscopy.

PubMed

Nguyen, Luan; Tao, Franklin Feng

2018-02-01

Structure of catalyst nanoparticles dispersed in liquid phase at high temperature under gas phase of reactant(s) at higher pressure (≥5 bars) is important for fundamental understanding of catalytic reactions performed on these catalyst nanoparticles. Most structural characterizations of a catalyst performing catalysis in liquid at high temperature under gas phase at high pressure were performed in an ex situ condition in terms of characterizations before or after catalysis since, from technical point of view, access to the catalyst nanoparticles during catalysis in liquid phase at high temperature under high pressure reactant gas is challenging. Here we designed a reactor which allows us to perform structural characterization using X-ray absorption spectroscopy including X-ray absorption near edge structure spectroscopy and extended X-ray absorption fine structure spectroscopy to study catalyst nanoparticles under harsh catalysis conditions in terms of liquid up to 350 °C under gas phase with a pressure up to 50 bars. This reactor remains nanoparticles of a catalyst homogeneously dispersed in liquid during catalysis and X-ray absorption spectroscopy characterization.

Oxygen transport membrane system and method for transferring heat to catalytic/process reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kelly, Sean M.; Kromer, Brian R.; Litwin, Michael M.

A method and apparatus for producing heat used in a synthesis gas production process is provided. The disclosed method and apparatus include a plurality of tubular oxygen transport membrane elements adapted to separate oxygen from an oxygen containing stream contacting the retentate side of the membrane elements. The permeated oxygen is combusted with a hydrogen containing synthesis gas stream contacting the permeate side of the tubular oxygen transport membrane elements thereby generating a reaction product stream and radiant heat. The present method and apparatus also includes at least one catalytic reactor containing a catalyst to promote the steam reforming reactionmore » wherein the catalytic reactor is surrounded by the plurality of tubular oxygen transport membrane elements. The view factor between the catalytic reactor and the plurality of tubular oxygen transport membrane elements radiating heat to the catalytic reactor is greater than or equal to 0.5« less

Oxygen transport membrane system and method for transferring heat to catalytic/process reactors

DOEpatents

Kelly, Sean M; Kromer, Brian R; Litwin, Michael M; Rosen, Lee J; Christie, Gervase Maxwell; Wilson, Jamie R; Kosowski, Lawrence W; Robinson, Charles

2014-01-07

A method and apparatus for producing heat used in a synthesis gas production is provided. The disclosed method and apparatus include a plurality of tubular oxygen transport membrane elements adapted to separate oxygen from an oxygen containing stream contacting the retentate side of the membrane elements. The permeated oxygen is combusted with a hydrogen containing synthesis gas stream contacting the permeate side of the tubular oxygen transport membrane elements thereby generating a reaction product stream and radiant heat. The present method and apparatus also includes at least one catalytic reactor containing a catalyst to promote the stream reforming reaction wherein the catalytic reactor is surrounded by the plurality of tubular oxygen transport membrane elements. The view factor between the catalytic reactor and the plurality of tubular oxygen transport membrane elements radiating heat to the catalytic reactor is greater than or equal to 0.5.

Catalytic conversion of syngas to mixed alcohols over Zn-Mn promoted Cu-Fe based catalyst

DOE PAGES

Lu, Yongwu; Yu, Fei; Hu, Jin; ...

2012-04-12

Zn-Mn promoted Cu-Fe based catalyst was synthesized by the co-precipitation method. Mixed alcohols synthesis from syngas was studied in a half-inch tubular reactor system after the catalyst was reduced. Zn-Mn promoted Cu-Fe based catalyst was characterized by SEM-EDS, TEM, XRD, and XPS. The liquid phase products (alcohol phase and hydrocarbon phase) were analyzed by GC-MS and the gas phase products were analyzed by GC. The results showed that Zn-Mn promoted Cu-Fe based catalyst had high catalytic activity and high alcohol selectivity. The maximal CO conversion rate was 72%, and the yield of alcohol and hydrocarbons were also very high. Cumore » (111) was the active site for mixed alcohols synthesis, Fe 2C (101) was the active site for olefin and paraffin synthesis. The reaction mechanism of mixed alcohols synthesis from syngas over Zn-Mn promoted Cu-Fe based catalyst was proposed. Here, Zn-Mn promoted Cu-Fe based catalyst can be regarded as a potential candidate for catalytic conversion of biomass-derived syngas to mixed alcohols.« less

ENERGY EFFICIENT VAPOR PHASE OXIDATION OF METHANOL USING OZONE AND CATALYTIC REACTOR

EPA Science Inventory

The pulp and paper industry releases more than 144 million tons of Volatile Organic Compounds (VOCs) per year. A big portion of this effluent, 66+% is released to air making it the fourth highest contributor of VOC emissions to the atmosphere by industry sector [1]. The current...

Clean catalytic combustor program

NASA Technical Reports Server (NTRS)

Ekstedt, E. E.; Lyon, T. F.; Sabla, P. E.; Dodds, W. J.

1983-01-01

A combustor program was conducted to evolve and to identify the technology needed for, and to establish the credibility of, using combustors with catalytic reactors in modern high-pressure-ratio aircraft turbine engines. Two selected catalytic combustor concepts were designed, fabricated, and evaluated. The combustors were sized for use in the NASA/General Electric Energy Efficient Engine (E3). One of the combustor designs was a basic parallel-staged double-annular combustor. The second design was also a parallel-staged combustor but employed reverse flow cannular catalytic reactors. Subcomponent tests of fuel injection systems and of catalytic reactors for use in the combustion system were also conducted. Very low-level pollutant emissions and excellent combustor performance were achieved. However, it was obvious from these tests that extensive development of fuel/air preparation systems and considerable advancement in the steady-state operating temperature capability of catalytic reactor materials will be required prior to the consideration of catalytic combustion systems for use in high-pressure-ratio aircraft turbine engines.

Hydrodynamics of Packed Bed Reactor in Low Gravity

NASA Technical Reports Server (NTRS)

Motil, Brian J.; Nahra, Henry K.; Balakotaiah, Vemuri

2005-01-01

Packed bed reactors are well known for their vast and diverse applications in the chemical industry; from gas absorption, to stripping, to catalytic conversion. Use of this type of reactor in terrestrial applications has been rather extensive because of its simplicity and relative ease of operation. Developing similar reactors for use in microgravity is critical to many space-based advanced life support systems. However, the hydrodynamics of two-phase flow packed bed reactors in this new environment and the effects of one physiochemical process on another has not been adequately assessed. Surface tension or capillary forces play a much greater role which results in a shifting in flow regime transitions and pressure drop. Results from low gravity experiments related to flow regimes and two-phase pressure drop models are presented in this paper along with a description of plans for a flight experiment on the International Space Station (ISS). Understanding the packed bed hydrodynamics and its effects on mass transfer processes in microgravity is crucial for the design of packed bed chemical or biological reactors to be used for water reclamation and other life support processes involving water purification.

Use of a Ceramic Membrane to Improve the Performance of Two-Separate-Phase Biocatalytic Membrane Reactor.

PubMed

Ranieri, Giuseppe; Mazzei, Rosalinda; Wu, Zhentao; Li, Kang; Giorno, Lidietta

2016-03-14

Biocatalytic membrane reactors (BMR) combining reaction and separation within the same unit have many advantages over conventional reactor designs. Ceramic membranes are an attractive alternative to polymeric membranes in membrane biotechnology due to their high chemical, thermal and mechanical resistance. Another important use is their potential application in a biphasic membrane system, where support solvent resistance is highly needed. In this work, the preparation of asymmetric ceramic hollow fibre membranes and their use in a two-separate-phase biocatalytic membrane reactor will be described. The asymmetric ceramic hollow fibre membranes were prepared using a combined phase inversion and sintering technique. The prepared fibres were then used as support for lipase covalent immobilization in order to develop a two-separate-phase biocatalytic membrane reactor. A functionalization method was proposed in order to increase the density of the reactive hydroxyl groups on the surface of ceramic membranes, which were then amino-activated and treated with a crosslinker. The performance and the stability of the immobilized lipase were investigated as a function of the amount of the immobilized biocatalytst. Results showed that it is possible to immobilize lipase on a ceramic membrane without altering its catalytic performance (initial residual specific activity 93%), which remains constant after 6 reaction cycles.

Utilization of the Recycle Reactor in Determining Kinetics of Gas-Solid Catalytic Reactions.

ERIC Educational Resources Information Center

Paspek, Stephen C.; And Others

1980-01-01

Describes a laboratory scale reactor that determines the kinetics of a gas-solid catalytic reaction. The external recycle reactor construction is detailed with accompanying diagrams. Experimental details, application of the reactor to CO oxidation kinetics, interphase gradients, and intraphase gradients are discussed. (CS)

Catalytic multi-stage process for hydroconversion and refining hydrocarbon feeds

DOEpatents

Comolli, Alfred G.; Lee, Lap-Keung

2001-01-01

A multi-stage catalytic hydrogenation and hydroconversion process for heavy hydrocarbon feed materials such as coal, heavy petroleum fractions, and plastic waste materials. In the process, the feedstock is reacted in a first-stage, back-mixed catalytic reactor with a highly dispersed iron-based catalyst having a powder, gel or liquid form. The reactor effluent is pressure-reduced, vapors and light distillate fractions are removed overhead, and the heavier liquid fraction is fed to a second stage back-mixed catalytic reactor. The first and second stage catalytic reactors are operated at 700-850.degree. F. temperature, 1000-3500 psig hydrogen partial pressure and 20-80 lb./hr per ft.sup.3 reactor space velocity. The vapor and light distillates liquid fractions removed from both the first and second stage reactor effluent streams are combined and passed to an in-line, fixed-bed catalytic hydrotreater for heteroatom removal and for producing high quality naphtha and mid-distillate or a full-range distillate product. The remaining separator bottoms liquid fractions are distilled at successive atmospheric and vacuum pressures, low and intermediate-boiling hydrocarbon liquid products are withdrawn, and heavier distillate fractions are recycled and further upgraded to provide additional low-boiling hydrocarbon liquid products. This catalytic multistage hydrogenation process provides improved flexibility for hydroprocessing the various carbonaceous feedstocks and adjusting to desired product structures and for improved economy of operations.

Highly efficient catalytic systems based on Pd-coated microbeads

NASA Astrophysics Data System (ADS)

Lim, Jin Hyun; Cho, Ahyoung; Lee, Seung Hwan; Park, Bumkyo; Kang, Dong Woo; Koo, Chong Min; Yu, Taekyung; Park, Bum Jun

2018-01-01

The efficiency of two prototype catalysis systems using palladium (Pd)-coated microparticles was investigated with regard to the recovery and recyclability of the catalytic particles. One such system was the interface-adsorption method, in which polymer particles coated with Pd nanoparticles strongly and irreversibly attach to the oil-water interface. Due to the irreversible adsorption of the catalytic particles to the interface, particle loss was completely prevented while mixing the aqueous solution and while collecting the products. The other system was based on the magnetic field-associated particle recovery method. The use of polymeric microparticles containing Pd nanoparticles and magnetite nanoparticles accelerated the sedimentation of the particles in the aqueous phase by applying a strong magnetic field, consequently suppressing drainage of the particles from the reactor along the product stream. Upon multiple runs of the catalytic reactions, it was found that conversion does not change significantly, demonstrating the excellent recyclability and performance efficiency in the catalytic processes.

VAPOR PHASE OXIDATION OF DIMETHYL SULFIDE WITH OZONE OVER V2O5/TIO2 CATALYST

EPA Science Inventory

Removal of volatile and odorous compounds emissions from the pulp and paper industry usually creates secondary pollution for scrubbing and adsorption processes or sulfur poising for catalytic incineration. Product studies performed in a flow reactor packed with 10 % V2O5/TiO2 cat...

Bubbling bed catalytic hydropyrolysis process utilizing larger catalyst particles and smaller biomass particles featuring an anti-slugging reactor

DOEpatents

Marker, Terry L; Felix, Larry G; Linck, Martin B; Roberts, Michael J

2014-09-23

This invention relates to a process for thermochemically transforming biomass or other oxygenated feedstocks into high quality liquid hydrocarbon fuels. In particular, a catalytic hydropyrolysis reactor, containing a deep bed of fluidized catalyst particles is utilized to accept particles of biomass or other oxygenated feedstocks that are significantly smaller than the particles of catalyst in the fluidized bed. The reactor features an insert or other structure disposed within the reactor vessel that inhibits slugging of the bed and thereby minimizes attrition of the catalyst. Within the bed, the biomass feedstock is converted into a vapor-phase product, containing hydrocarbon molecules and other process vapors, and an entrained solid char product, which is separated from the vapor stream after the vapor stream has been exhausted from the top of the reactor. When the product vapor stream is cooled to ambient temperatures, a significant proportion of the hydrocarbons in the product vapor stream can be recovered as a liquid stream of hydrophobic hydrocarbons, with properties consistent with those of gasoline, kerosene, and diesel fuel. Separate streams of gasoline, kerosene, and diesel fuel may also be obtained, either via selective condensation of each type of fuel, or via later distillation of the combined hydrocarbon liquid.

Bubbling bed catalytic hydropyrolysis process utilizinig larger catalyst particles and small biomass particles featuring an anti-slugging reactor

DOEpatents

Marker, Terry L.; Felix, Larry G.; Linck, Martin B.; Roberts, Michael J.

2016-12-06

This invention relates to a process for thermochemically transforming biomass or other oxygenated feedstocks into high quality liquid hydrocarbon fuels. In particular, a catalytic hydropyrolysis reactor, containing a deep bed of fluidized catalyst particles is utilized to accept particles of biomass or other oxygenated feedstocks that are significantly smaller than the particles of catalyst in the fluidized bed. The reactor features an insert or other structure disposed within the reactor vessel that inhibits slugging of the bed and thereby minimizes attrition of the catalyst. Within the bed, the biomass feedstock is converted into a vapor-phase product, containing hydrocarbon molecules and other process vapors, and an entrained solid char product, which is separated from the vapor stream after the vapor stream has been exhausted from the top of the reactor. When the product vapor stream is cooled to ambient temperatures, a significant proportion of the hydrocarbons in the product vapor stream can be recovered as a liquid stream of hydrophobic hydrocarbons, with properties consistent with those of gasoline, kerosene, and diesel fuel. Separate streams of gasoline, kerosene, and diesel fuel may also be obtained, either via selective condensation of each type of fuel, or via later distillation of the combined hydrocarbon liquid.

Catalytic reactor for promoting a chemical reaction on a fluid passing therethrough

NASA Technical Reports Server (NTRS)

Roychoudhury, Subir (Inventor); Pfefferle, William C. (Inventor)

2001-01-01

A catalytic reactor with an auxiliary heating structure for raising the temperature of a fluid passing therethrough whereby the catalytic reaction is promoted. The invention is a apparatus employing multiple electrical heating elements electrically isolated from one another by insulators that are an integral part of the flow path. The invention provides step heating of a fluid as the fluid passes through the reactor.

Cellular graphene aerogel combines ultralow weight and high mechanical strength: A highly efficient reactor for catalytic hydrogenation

PubMed Central

Zhang, Bingxing; Zhang, Jianling; Sang, Xinxin; Liu, Chengcheng; Luo, Tian; Peng, Li; Han, Buxing; Tan, Xiuniang; Ma, Xue; Wang, Dong; Zhao, Ning

2016-01-01

The construction of three-dimensional graphene aerogels (GAs) is of great importance owing to their outstanding properties for various applications. Up to now, the combination of ultralow weight and super mechanical strength for GA remains a great challenge. Here we demonstrate the fabrication of cellular GAs by a facile, easily controlled and versatile route, i.e. the chemical reduction of graphene oxide assemblies at oil-water interface under a mild condition (70 °C). The GA is ultralight (with density <3 mg cm−3) yet mechanically resilient because the walls of the cell closely pack in a highly ordered manner to maximize mechanical strength. The GA has been utilized as an appealing reactor for catalytic hydrogenation, which exhibited great advantages such as large oil absorption capability, exceptional catalytic activity, ease of product separation and high stability. PMID:27174450

Cellular graphene aerogel combines ultralow weight and high mechanical strength: A highly efficient reactor for catalytic hydrogenation

NASA Astrophysics Data System (ADS)

Zhang, Bingxing; Zhang, Jianling; Sang, Xinxin; Liu, Chengcheng; Luo, Tian; Peng, Li; Han, Buxing; Tan, Xiuniang; Ma, Xue; Wang, Dong; Zhao, Ning

2016-05-01

The construction of three-dimensional graphene aerogels (GAs) is of great importance owing to their outstanding properties for various applications. Up to now, the combination of ultralow weight and super mechanical strength for GA remains a great challenge. Here we demonstrate the fabrication of cellular GAs by a facile, easily controlled and versatile route, i.e. the chemical reduction of graphene oxide assemblies at oil-water interface under a mild condition (70 °C). The GA is ultralight (with density <3 mg cm-3) yet mechanically resilient because the walls of the cell closely pack in a highly ordered manner to maximize mechanical strength. The GA has been utilized as an appealing reactor for catalytic hydrogenation, which exhibited great advantages such as large oil absorption capability, exceptional catalytic activity, ease of product separation and high stability.

Advanced catalytic combustors for low pollutant emissions, phase 1

NASA Technical Reports Server (NTRS)

Dodds, W. J.

1979-01-01

The feasibility of employing the known attractive and distinguishing features of catalytic combustion technology to reduce nitric oxide emissions from gas turbine engines during subsonic, stratospheric cruise operation was investigated. Six conceptual combustor designs employing catalytic combustion were defined and evaluated for their potential to meet specific emissions and performance goals. Based on these evaluations, two parallel-staged, fixed-geometry designs were identified as the most promising concepts. Additional design studies were conducted to produce detailed preliminary designs of these two combustors. Results indicate that cruise nitric oxide emissions can be reduced by an order of magnitude relative to current technology levels by the use of catalytic combustion. Also, these combustors have the potential for operating over the EPA landing-takeoff cycle and at cruise with a low pressure drop, high combustion efficiency and with a very low overall level of emission pollutants. The use of catalytic combustion, however, requires advanced technology generation in order to obtain the time-temperature catalytic reactor performance and durability required for practical aircraft engine combustors.

Laser-assisted isotope separation of tritium

DOEpatents

Herman, Irving P.; Marling, Jack B.

1983-01-01

Methods for laser-assisted isotope separation of tritium, using infrared multiple photon dissociation of tritium-bearing products in the gas phase. One such process involves the steps of (1) catalytic exchange of a deuterium-bearing molecule XYD with tritiated water DTO from sources such as a heavy water fission reactor, to produce the tritium-bearing working molecules XYT and (2) photoselective dissociation of XYT to form a tritium-rich product. By an analogous procedure, tritium is separated from tritium-bearing materials that contain predominately hydrogen such as a light water coolant from fission or fusion reactors.

SYNTHESIZING ALCOHOLS AND KETONES BY PHOTOINDUCED CATALYTIC PARTIAL-OXIDATION OF HYDROCARBONS IN TI02 FILM REACTORS PREPARED BY THREE DIFFERENT METHODS

EPA Science Inventory

The partial oxidation of cyclohexane to cyclohexanol and cyclohexanone on UV irradiated titanium dioxide films in the presence of molecular oxygen at ambient temperatures and pressures was studied. Three different coating methodologies (dip coating using titanium isopropoxide an...

Catalytic wet air oxidation of bisphenol A solution in a batch-recycle trickle-bed reactor over titanate nanotube-based catalysts.

PubMed

Kaplan, Renata; Erjavec, Boštjan; Senila, Marin; Pintar, Albin

2014-10-01

Catalytic wet air oxidation (CWAO) is classified as an advanced oxidation process, which proved to be highly efficient for the removal of emerging organic pollutant bisphenol A (BPA) from water. In this study, BPA was successfully removed in a batch-recycle trickle-bed reactor over bare titanate nanotube-based catalysts at very short space time of 0.6 min gCAT g(-1). The as-prepared titanate nanotubes, which underwent heat treatment at 600 °C, showed high activity for the removal of aqueous BPA. Liquid-phase recycling (5- or 10-fold recycle) enabled complete BPA conversion already at 200 °C, together with high conversion of total organic carbon (TOC), i.e., 73 and 98 %, respectively. The catalyst was chemically stable in the given range of operating conditions for 189 h on stream.

[Synergetic effects of silicon carbide and molecular sieve loaded catalyst on microwave assisted catalytic oxidation of toluene].

PubMed

Wang, Xiao-Hui; Bo, Long-Li; Liu, Hai-Nan; Zhang, Hao; Sun, Jian-Yu; Yang, Li; Cai, Li-Dong

2013-06-01

Molecular sieve loaded catalyst was prepared by impregnation method, microwave-absorbing material silicon carbide and the catalyst were investigated for catalytic oxidation of toluene by microwave irradiation. Research work examined effects of silicon carbide and molecular sieve loading Cu-V catalyst's mixture ratio as well as mixed approach changes on degradation of toluene, and characteristics of catalyst were measured through scanning electron microscope, specific surface area test and X-ray diffraction analysis. The result showed that the fixed bed reactor had advantages of both thermal storage property and low-temperature catalytic oxidation when 20% silicon carbide was filled at the bottom of the reactor, and this could effectively improve the utilization of microwave energy as well as catalytic oxidation efficiency of toluene. Under microwave power of 75 W and 47 W, complete-combustion temperatures of molecular sieve loaded Cu-V catalyst and Cu-V-Ce catalyst to toluene were 325 degrees C and 160 degrees C, respectively. Characteristics of the catalysts showed that mixture of rare-earth element Ce increased the dispersion of active components in the surface of catalyst, micropore structure of catalyst effectively guaranteed high adsorption capacity for toluene, while amorphous phase of Cu and V oxides increased the activity of catalyst greatly.

Catalytic pyrolysis of Alcea pallida stems in a fixed-bed reactor for production of liquid bio-fuels.

PubMed

Aysu, Tevfik

2015-09-01

Pyrolysis of Alcea pallida stems was performed in a fixed-bed tubular reactor with and without catalyst at three different temperatures. The effects of pyrolysis parameters including temperature and catalyst on the product yields were investigated. It was found that higher temperature resulted in lower liquid (bio-oil) and solid (bio-char) yields and higher gas yields. Catalysts had different effects on product yields and composition of bio-oils. Liquid yields were increased in the presence of zinc chloride and alumina but decreased with calcium hydroxide, tincal and ulexite. The highest bio-oil yield (39.35%) by weight including aqueous phase was produced with alumina catalyst at 500 °C. The yields of bio-char, bio-oil and gas produced, as well as the compositions of the resulting bio-oils were determined by elemental analysis, TGA, FT-IR and GC-MS. 160 different compounds were identified by GC-MS in the bio-oils obtained at 500 °C. Copyright © 2015 Elsevier Ltd. All rights reserved.

Active disturbance rejection controller for chemical reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Both, Roxana; Dulf, Eva H.; Muresan, Cristina I., E-mail: roxana.both@aut.utcluj.ro

2015-03-10

In the petrochemical industry, the synthesis of 2 ethyl-hexanol-oxo-alcohols (plasticizers alcohol) is of high importance, being achieved through hydrogenation of 2 ethyl-hexenal inside catalytic trickle bed three-phase reactors. For this type of processes the use of advanced control strategies is suitable due to their nonlinear behavior and extreme sensitivity to load changes and other disturbances. Due to the complexity of the mathematical model an approach was to use a simple linear model of the process in combination with an advanced control algorithm which takes into account the model uncertainties, the disturbances and command signal limitations like robust control. However themore » resulting controller is complex, involving cost effective hardware. This paper proposes a simple integer-order control scheme using a linear model of the process, based on active disturbance rejection method. By treating the model dynamics as a common disturbance and actively rejecting it, active disturbance rejection control (ADRC) can achieve the desired response. Simulation results are provided to demonstrate the effectiveness of the proposed method.« less

Catalytic decomposition of toxic chemicals over metal-promoted carbon nanotubes.

PubMed

Li, Lili; Han, Changxiu; Han, Xinyu; Zhou, Yixiao; Yang, Li; Zhang, Baogui; Hu, Jianli

2011-01-15

Effective decomposition of toxic gaseous compounds is important for pollution control at many chemical manufacturing plants. This study explores catalytic decomposition of phosphine (PH(3)) using novel metal-promoted carbon nanotubes (CNTs). The cerium-promoted Co/CNTs catalysts (CoCe/CNTs) are synthesized by means of coimpregnation method and reduced by three different methods (H(2), KBH(4), NaH(2)PO(2)·H(2)O/KBH(4)). The morphology, structure, and composition of the catalysts are characterized using a number of analytical instrumentations including high-resolution transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, BET surface area measurement, and inductively coupled plasma. The activity of the catalysts in PH(3) decomposition reaction is measured and correlated with their surface and structural properties. The characterization results show that the CoCe/CNTs catalyst reduced by H(2) possesses small particles and is shown thermally stable in PH(3) decomposition reaction. The activities of these catalysts are compared and are shown in the following sequence: CoCe/CNTs > Co/CNTs > CoCeBP/CNTs> CoCeB/CNTs. The difference in reduction method results in the formation of different active phases during the PH(3) decomposition reaction. After a catalytic activity test, only the CoP phase is formed on CoCe/CNTs and Co/CNTs catalysts, whereas multiphases CoP, Co(2)P, and Co phases are formed on CoCeBP/CNTs and CoCeB/CNTs. Results show that the CoP phase is formed predominantly on the CoCe/CNTs and Co/CNTs catalysts and is found to likely be the most active phase for this reaction. Furthermore, the CoCe/CNTs catalyst exhibits not only highest activity but also long-term stability in PH(3) decomposition reaction. When operated in a fixed-bed reactor at 360 °C, single-pass PH(3) conversion of about 99.8% can be achieved.

Fiber-Optical Sensors: Basics and Applications in Multiphase Reactors

PubMed Central

Li, Xiangyang; Yang, Chao; Yang, Shifang; Li, Guozheng

2012-01-01

This work presents a brief introduction on the basics of fiber-optical sensors and an overview focused on the applications to measurements in multiphase reactors. The most commonly principle utilized is laser back scattering, which is also the foundation for almost all current probes used in multiphase reactors. The fiber-optical probe techniques in two-phase reactors are more developed than those in three-phase reactors. There are many studies on the measurement of gas holdup using fiber-optical probes in three-phase fluidized beds, but negative interference of particles on probe function was less studied. The interactions between solids and probe tips were less studied because glass beads etc. were always used as the solid phase. The vision probes may be the most promising for simultaneous measurements of gas dispersion and solids suspension in three-phase reactors. Thus, the following techniques of the fiber-optical probes in multiphase reactors should be developed further: (1) online measuring techniques under nearly industrial operating conditions; (2) corresponding signal data processing techniques; (3) joint application with other measuring techniques.

Two component-three dimensional catalysis

DOEpatents

Schwartz, Michael; White, James H.; Sammells, Anthony F.

2002-01-01

This invention relates to catalytic reactor membranes having a gas-impermeable membrane for transport of oxygen anions. The membrane has an oxidation surface and a reduction surface. The membrane is coated on its oxidation surface with an adherent catalyst layer and is optionally coated on its reduction surface with a catalyst that promotes reduction of an oxygen-containing species (e.g., O.sub.2, NO.sub.2, SO.sub.2, etc.) to generate oxygen anions on the membrane. The reactor has an oxidation zone and a reduction zone separated by the membrane. A component of an oxygen containing gas in the reduction zone is reduced at the membrane and a reduced species in a reactant gas in the oxidation zone of the reactor is oxidized. The reactor optionally contains a three-dimensional catalyst in the oxidation zone. The adherent catalyst layer and the three-dimensional catalyst are selected to promote a desired oxidation reaction, particularly a partial oxidation of a hydrocarbon.

High aspect ratio catalytic reactor and catalyst inserts therefor

DOEpatents

Lin, Jiefeng; Kelly, Sean M.

2018-04-10

The present invention relates to high efficient tubular catalytic steam reforming reactor configured from about 0.2 inch to about 2 inch inside diameter high temperature metal alloy tube or pipe and loaded with a plurality of rolled catalyst inserts comprising metallic monoliths. The catalyst insert substrate is formed from a single metal foil without a central supporting structure in the form of a spiral monolith. The single metal foil is treated to have 3-dimensional surface features that provide mechanical support and establish open gas channels between each of the rolled layers. This unique geometry accelerates gas mixing and heat transfer and provides a high catalytic active surface area. The small diameter, high aspect ratio tubular catalytic steam reforming reactors loaded with rolled catalyst inserts can be arranged in a multi-pass non-vertical parallel configuration thermally coupled with a heat source to carry out steam reforming of hydrocarbon-containing feeds. The rolled catalyst inserts are self-supported on the reactor wall and enable efficient heat transfer from the reactor wall to the reactor interior, and lower pressure drop than known particulate catalysts. The heat source can be oxygen transport membrane reactors.

Piloted rich-catalytic lean-burn hybrid combustor

DOEpatents

Newburry, Donald Maurice

2002-01-01

A catalytic combustor assembly which includes, an air source, a fuel delivery means, a catalytic reactor assembly, a mixing chamber, and a means for igniting a fuel/air mixture. The catalytic reactor assembly is in fluid communication with the air source and fuel delivery means and has a fuel/air plenum which is coated with a catalytic material. The fuel/air plenum has cooling air conduits passing therethrough which have an upstream end. The upstream end of the cooling conduits is in fluid communication with the air source but not the fuel delivery means.

Porous media for catalytic renewable energy conversion

NASA Astrophysics Data System (ADS)

Hotz, Nico

2012-05-01

A novel flow-based method is presented to place catalytic nanoparticles into a reactor by sol-gelation of a porous ceramic consisting of copper-based nanoparticles, silica sand, ceramic binder, and a gelation agent. This method allows for the placement of a liquid precursor containing the catalyst into the final reactor geometry without the need of impregnating or coating of a substrate with the catalytic material. The so generated foam-like porous ceramic shows properties highly appropriate for use as catalytic reactor material, e.g., reasonable pressure drop due to its porosity, high thermal and catalytic stability, and excellent catalytic behavior. The catalytic activity of micro-reactors containing this foam-like ceramic is tested in terms of their ability to convert alcoholic biofuel (e.g. methanol) to a hydrogen-rich gas mixture with low concentrations of carbon monoxide (up to 75% hydrogen content and less than 0.2% CO, for the case of methanol). This gas mixture is subsequently used in a low-temperature fuel cell, converting the hydrogen directly to electricity. A low concentration of CO is crucial to avoid poisoning of the fuel cell catalyst. Since conventional Polymer Electrolyte Membrane (PEM) fuel cells require CO concentrations far below 100 ppm and since most methods to reduce the mole fraction of CO (such as Preferential Oxidation or PROX) have CO conversions of up to 99%, the alcohol fuel reformer has to achieve initial CO mole fractions significantly below 1%. The catalyst and the porous ceramic reactor of the present study can successfully fulfill this requirement.

A catalytic chiral gel microfluidic reactor assembled via dynamic covalent chemistry† †Electronic supplementary information (ESI) available: Experimental details, additional characterization and catalytic data. See DOI: 10.1039/c5sc00314h Click here for additional data file.

PubMed Central

Liu, Haoliang; Feng, Juan; Chen, Liuping

2015-01-01

A novel dynamic covalent gel strategy is reported to immobilize an asymmetric catalyst within the channels of a microfluidic flow reactor. A layer of a catalytically active Mn–salen dynamic covalent imine gel matrix was coated onto a functionalized capillary. Mn–salen active moiety was incorporated into dynamic covalent imine gel matrix via the reaction of a chiral Mn–salen dialdehyde unit with a tetraamine linker. The catalytic activity of the capillary reactor has been demonstrated in enantioselective kinetic resolution of secondary alcohols. PMID:28706652

Solid state oxygen anion and electron mediating membrane and catalytic membrane reactors containing them

DOEpatents

Schwartz, Michael; White, James H.; Sammells, Anthony F.

2005-09-27

This invention relates to gas-impermeable, solid state materials fabricated into membranes for use in catalytic membrane reactors. This invention particularly relates to solid state oxygen anion- and electron-mediating membranes for use in catalytic membrane reactors for promoting partial or full oxidation of different chemical species, for decomposition of oxygen-containing species, and for separation of oxygen from other gases. Solid state materials for use in the membranes of this invention include mixed metal oxide compounds having the brownmillerite crystal structure.

Solid state oxygen anion and electron mediating membrane and catalytic membrane reactors containing them

DOEpatents

Schwartz, Michael; White, James H.; Sammels, Anthony F.

2000-01-01

This invention relates to gas-impermeable, solid state materials fabricated into membranes for use in catalytic membrane reactors. This invention particularly relates to solid state oxygen anion- and electron-mediating membranes for use in catalytic membrane reactors for promoting partial or full oxidation of different chemical species, for decomposition of oxygen-containing species, and for separation of oxygen from other gases. Solid state materials for use in the membranes of this invention include mixed metal oxide compounds having the brownmillerite crystal structure.

Pd-Ag Membrane Coupled to a Two-Zone Fluidized Bed Reactor (TZFBR) for Propane Dehydrogenation on a Pt-Sn/MgAl2O4 Catalyst

PubMed Central

Medrano, José-Antonio; Julián, Ignacio; Herguido, Javier; Menéndez, Miguel

2013-01-01

Several reactor configurations have been tested for catalytic propane dehydrogenation employing Pt-Sn/MgAl2O4 as a catalyst. Pd-Ag alloy membranes coupled to the multifunctional Two-Zone Fluidized Bed Reactor (TZFBR) provide an improvement in propane conversion by hydrogen removal from the reaction bed through the inorganic membrane in addition to in situ catalyst regeneration. Twofold process intensification is thereby achieved when compared to the use of traditional fluidized bed reactors (FBR), where coke formation and thermodynamic equilibrium represent important process limitations. Experiments were carried out at 500–575 °C and with catalyst mass to molar flow of fed propane ratios between 15.1 and 35.2 g min mmol−1, employing three different reactor configurations: FBR, TZFBR and TZFBR + Membrane (TZFBR + MB). The results in the FBR showed catalyst deactivation, which was faster at high temperatures. In contrast, by employing the TZFBR with the optimum regenerative agent flow (diluted oxygen), the process activity was sustained throughout the time on stream. The TZFBR + MB showed promising results in catalytic propane dehydrogenation, displacing the reaction towards higher propylene production and giving the best results among the different reactor configurations studied. Furthermore, the results obtained in this study were better than those reported on conventional reactors. PMID:24958620

Method of producing pyrolysis gases from carbon-containing materials

DOEpatents

Mudge, Lyle K.; Brown, Michael D.; Wilcox, Wayne A.; Baker, Eddie G.

1989-01-01

A gasification process of improved efficiency is disclosed. A dual bed reactor system is used in which carbon-containing feedstock materials are first treated in a gasification reactor to form pyrolysis gases. The pyrolysis gases are then directed into a catalytic reactor for the destruction of residual tars/oils in the gases. Temperatures are maintained within the catalytic reactor at a level sufficient to crack the tars/oils in the gases, while avoiding thermal breakdown of the catalysts. In order to minimize problems associated with the deposition of carbon-containing materials on the catalysts during cracking, a gaseous oxidizing agent preferably consisting of air, oxygen, steam, and/or mixtures thereof is introduced into the catalytic reactor at a high flow rate in a direction perpendicular to the longitudinal axis of the reactor. This oxidizes any carbon deposits on the catalysts, which would normally cause catalyst deactivation.

Catalytic biomass conversion methods, catalysts, and methods of making the same

DOEpatents

Delgass, William Nicholas; Agrawal, Rakesh; Ribeiro, Fabio Henrique; Saha, Basudeb; Yohe, Sara Lynn; Abu-Omar, Mahdi M; Parsell, Trenton; Dietrich, Paul James; Klein, Ian Michael

2017-10-10

Described herein are processes for one-step delignification and hydrodeoxygenation of lignin fraction a biomass feedstock. The lignin feedstock is derived from by-products of paper production and biorefineries. Additionally described is a process for converting biomass-derived oxygenates to lower oxygen-content compounds and/or hydrocarbons in the liquid or vapor phase in a reactor system containing hydrogen and a catalyst comprised of a hydrogenation function and/or an oxophilic function and/or an acid function. Finally, also described herein is a process for converting biomass-derived oxygenates to lower oxygen-content compounds and/or hydrocarbons in the liquid or vapor phase in a reactor system containing hydrogen and a catalyst comprised of a hydrogenation function and/or an oxophilic function and/or an acid function.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Byong-chul Kim; Sushil Gupta; David French

Iron minerals in coke can catalyze its gasification and may affect coke behavior in the blast furnace. The catalytic behavior of iron depends largely upon the nature of the iron-bearing minerals. To determine the mineralogical changes that iron could undergo in the blast furnace, cokes made from three coals containing iron present in different mineral forms (clays, carbonates, and pyrite) were examined. All coke samples were heat-treated in a horizontal furnace at 1373, 1573, and 1773 K and then gasified with CO{sub 2} at 1173 K in a fixed bed reactor (FBR). Coke mineralogy was characterized using quantitative X-ray diffractionmore » (XRD) analysis of coke mineral matter prepared by low-temperature ashing (LTA) and field emission scanning electron microscopy combined with energy dispersive X-ray analysis (FESEM/EDS). The mineralogy of the three cokes was most notably distinguished by differing proportions of iron-bearing phases. During heat treatment and subsequent gasification, iron-containing minerals transformed to a range of minerals but predominantly iron-silicides and iron oxides, the relative amounts of which varied with heat treatment temperature and gasification conditions. The relationship between initial apparent reaction rate and the amount of catalytic iron minerals - pyrrhotite, metallic iron, and iron oxides - was linear and independent of heat treatment temperature at total catalyst levels below 1 wt %. The study showed that the coke reactivity decreased with increasing temperature of heat treatment due to decreased levels of catalytic iron minerals (largely due to formation of iron silicides) as well as increased ordering of the carbon structure. The study also showed that the importance of catalytic mineral matter in determining reactivity declines as gasification proceeds. 37 refs., 13 figs., 7 tabs.« less

In Situ Monitoring of Ni-based Catalysts during the Synthesis of Propylene Carbonate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ramin, Michael; Reimann, Sven; Grunwaldt, Jan-Dierk

2007-02-02

Three different nickel complexes were catalytically tested in the synthesis of propylene carbonate by carbon dioxide insertion. XAS measurements of the as prepared catalysts confirmed the differences in the structure which led to the varying catalytic activity. The structure of one of the active nickel-based catalysts was followed in situ by X-ray absorption spectroscopy using a specially designed batch reactor cell. The novel batch reactor allows in situ studies in dense carbon dioxide at elevated temperature and high pressure (up to 200 bar) even at the low energy of the nickel K-edge. Hence, important information on the fate of themore » ligands and structural changes under reaction conditions could be gained providing new insight into the reaction mechanism.« less

Efficient H2O2/CH3COOH oxidative desulfurization/denitrification of liquid fuels in sonochemical flow-reactors.

PubMed

Calcio Gaudino, Emanuela; Carnaroglio, Diego; Boffa, Luisa; Cravotto, Giancarlo; Moreira, Elizabeth M; Nunes, Matheus A G; Dressler, Valderi L; Flores, Erico M M

2014-01-01

The oxidative desulfurization/denitrification of liquid fuels has been widely investigated as an alternative or complement to common catalytic hydrorefining. In this process, all oxidation reactions occur in the heterogeneous phase (the oil and the polar phase containing the oxidant) and therefore the optimization of mass and heat transfer is of crucial importance to enhancing the oxidation rate. This goal can be achieved by performing the reaction in suitable ultrasound (US) reactors. In fact, flow and loop US reactors stand out above classic batch US reactors thanks to their greater efficiency and flexibility as well as lower energy consumption. This paper describes an efficient sonochemical oxidation with H2O2/CH3COOH at flow rates ranging from 60 to 800 ml/min of both a model compound, dibenzotiophene (DBT), and of a mild hydro-treated diesel feedstock. Four different commercially available US loop reactors (single and multi-probe) were tested, two of which were developed in the authors' laboratory. Full DBT oxidation and efficient diesel feedstock desulfurization/denitrification were observed after the separation of the polar oxidized S/N-containing compounds (S≤5 ppmw, N≤1 ppmw). Our studies confirm that high-throughput US applications benefit greatly from flow-reactors. Copyright © 2013 Elsevier B.V. All rights reserved.

Coal liquefaction process utilizing coal/CO.sub.2 slurry feedstream

DOEpatents

Comolli, Alfred G.; McLean, Joseph B.

1989-01-01

A coal hydrogenation and liquefaction process in which particulate coal feed is pressurized to an intermediate pressure of at least 500 psig and slurried with CO.sub.2 liquid to provide a flowable coal/CO.sub.2 slurry feedstream, which is further pressurized to at least 1000 psig and fed into a catalytic reactor. The coal particle size is 50-375 mesh (U.S. Sieve Series) and provides 50-80 W % coal in the coal/CO.sub.2 slurry feedstream. Catalytic reaction conditions are maintained at 650.degree.-850.degree. F. temperature, 1000-4000 psig hydrogen partial pressure and coal feed rate of 10-100 lb coal/hr ft.sup.3 reactor volume to produce hydrocarbon gas and liquid products. The hydrogen and CO.sub.2 are recovered from the reactor effluent gaseous fraction, hydrogen is recycled to the catalytic reactor, and CO.sub.2 is liquefied and recycled to the coal slurrying step. If desired, two catalytic reaction stages close coupled together in series relation can be used. The process advantageously minimizes the recycle and processing of excess hydrocarbon liquid previously needed for slurrying the coal feed to the reactor(s).

Complex Wall Boundary Conditions for Modeling Combustion in Catalytic Channels

NASA Astrophysics Data System (ADS)

Zhu, Huayang; Jackson, Gregory

2000-11-01

Monolith catalytic reactors for exothermic oxidation are being used in automobile exhaust clean-up and ultra-low emissions combustion systems. The reactors present a unique coupling between mass, heat, and momentum transport in a channel flow configuration. The use of porous catalytic coatings along the channel wall presents a complex boundary condition when modeled with the two-dimensional channel flow. This current work presents a 2-D transient model for predicting the performance of catalytic combustion systems for methane oxidation on Pd catalysts. The model solves the 2-D compressible transport equations for momentum, species, and energy, which are solved with a porous washcoat model for the wall boundary conditions. A time-splitting algorithm is used to separate the stiff chemical reactions from the convective/diffusive equations for the channel flow. A detailed surface chemistry mechanism is incorporated for the catalytic wall model and is used to predict transient ignition and steady-state conversion of CH4-air flows in the catalytic reactor.

Super-hydrophobic yolk-shell nanostructure with enhanced catalytic performance in the reduction of hydrophobic nitroaromatic compounds.

PubMed

Shi, Song; Wang, Min; Chen, Chen; Gao, Jin; Ma, Hong; Ma, Jiping; Xu, Jie

2013-10-25

A self-templating method to fabricate a super-hydrophobic yolk-shell nano-reactor was reported. Metal nanoparticles were encapsulated in the porous super-hydrophobic shell. This super-hydrophobic catalyst showed excellent performance in the reduction of nitroaromatic compounds in aqueous phase and a positive correlation was found between the reaction rate and the hydrophobicity of the substrate.

Synthesis gas method and apparatus

DOEpatents

Kelly, Sean M.; Kromer, Brian R.; Litwin, Michael M.; Rosen, Lee J.; Christie, Gervase Maxwell; Wilson, Jamie; Kosowski, Lawrence W; Robinson, Charles

2015-11-06

A method and apparatus for producing a synthesis gas product having one or more oxygen transport membrane elements thermally coupled to one or more catalytic reactors such that heat generated from the oxygen transport membrane element supplies endothermic heating requirements for steam methane reforming reactions occurring within the catalytic reactor through radiation and convention heat transfer. A hydrogen containing stream containing no more than 20 percent methane is combusted within the oxygen transport membrane element to produce the heat and a heated combustion product stream. The heated combustion product stream is combined with a reactant stream to form a combined stream that is subjected to the reforming within the catalytic reactor. The apparatus may include modules in which tubular membrane elements surround a central reactor tube.

Synthesis gas method and apparatus

DOEpatents

Kelly, Sean M.; Kromer, Brian R.; Litwin, Michael M.; Rosen, Lee J.; Christie, Gervase Maxwell; Wilson, Jamie R.; Kosowski, Lawrence W.; Robinson, Charles

2013-01-08

A method and apparatus for producing a synthesis gas product having one or more oxygen transport membrane elements thermally coupled to one or more catalytic reactors such that heat generated from the oxygen transport membrane element supplies endothermic heating requirements for steam methane reforming reactions occurring within the catalytic reactor through radiation and convention heat transfer. A hydrogen containing stream containing no more than 20 percent methane is combusted within the oxygen transport membrane element to produce the heat and a heated combustion product stream. The heated combustion product stream is combined with a reactant stream to form a combined stream that is subjected to the reforming within the catalytic reactor. The apparatus may include modules in which tubular membrane elements surround a central reactor tube.

Pyrolysis of aseptic packages (tetrapak) in a laboratory screw type reactor and secondary thermal/catalytic tar decomposition.

PubMed

Haydary, J; Susa, D; Dudáš, J

2013-05-01

Pyrolysis of aseptic packages (tetrapak cartons) in a laboratory apparatus using a flow screw type reactor and a secondary catalytic reactor for tar cracking was studied. The pyrolysis experiments were realized at temperatures ranging from 650 °C to 850 °C aimed at maximizing of the amount of the gas product and reducing its tar content. Distribution of tetrapak into the product yields at different conditions was obtained. The presence of H2, CO, CH4, CO2 and light hydrocarbons, HCx, in the gas product was observed. The Aluminum foil was easily separated from the solid product. The rest part of char was characterized by proximate and elemental analysis and calorimetric measurements. The total organic carbon in the tar product was estimated by elemental analysis of tars. Two types of catalysts (dolomite and red clay marked AFRC) were used for catalytic thermal tar decomposition. Three series of experiments (without catalyst in a secondary cracking reactor, with dolomite and with AFRC) at temperatures of 650, 700, 750, 800 and 850 °C were carried out. Both types of catalysts have significantly affected the content of tars and other components in pyrolytic gases. The effect of catalyst on the tetrapack distribution into the product yield on the composition of gas and on the total organic carbon in the tar product is presented in this work. Copyright © 2013 Elsevier Ltd. All rights reserved.

Treatment of ammonia by catalytic wet oxidation process over platinum-rhodium bimetallic catalyst in a trickle-bed reactor: effect of pH.

PubMed

Hung, Chang-Mao; Lin, Wei-Bang; Ho, Ching-Lin; Shen, Yun-Hwei; Hsia, Shao-Yi

2010-08-01

This work adopted aqueous solutions of ammonia for use in catalytic liquid-phase reduction in a trickle-bed reactor with a platinum-rhodium bimetallic catalyst, prepared by the co-precipitation of chloroplatinic acid (H2PtCl6) and rhodium nitrate [Rh(NO3)3]. The experimental results demonstrated that a minimal amount of ammonia was removed from the solution by wet oxidation in the absence of any catalyst, while approximately 97.0% of the ammonia was removed by wet oxidation over the platinum-rhodium bimetallic catalyst at 230 degrees C with an oxygen partial pressure of 2.0 MPa. The oxidation of ammonia has been studied as a function of pH, and the main reaction products were determined. A synergistic effect is manifest in the platinum-rhodium bimetallic structure, in which the material has the greatest capacity to reduce ammonia. The reaction pathway linked the oxidizing ammonia to nitric oxide, nitrogen, and water.

Process of forming catalytic surfaces for wet oxidation reactions

NASA Technical Reports Server (NTRS)

Jagow, R. B. (Inventor)

1977-01-01

A wet oxidation process was developed for oxidizing waste materials, comprising dissolved ruthenium salt in a reactant feed stream containing the waste materials. The feed stream is introduced into a reactor, and the reactor contents are then raised to an elevated temperature to effect deposition of a catalytic surface of ruthenium black on the interior walls of the reactor. The feed stream is then maintained in the reactor for a period of time sufficient to effect at least partial oxidation of the waste materials.

Catalytic oxidation of waste materials

NASA Technical Reports Server (NTRS)

Jagow, R. B.

1977-01-01

Aqueous stream of human waste is mixed with soluble ruthenium salts and is introduced into reactor at temperature where ruthenium black catalyst forms on internal surfaces of reactor. This provides catalytically active surface to convert oxidizable wastes into breakdown products such as water and carbon dioxide.

hcp-Co nanowires grown on metallic foams as catalysts for the Fischer-Tropsch synthesis.

PubMed

Soulantica, Katerina; Harmel, Justine; Peres, Laurent; Estrader, Marta; Berliet, Adrien; Maury, Sylvie; Fécant, Antoine; Chaudret, Bruno; Serp, Philippe

2018-06-12

The possibility to control the structural characteristics of the active phase of supported catalysts offers the opportunity to improve catalyst performance, especially in structure sensitive catalytic reactions. In parallel, heat management is of critical importance for the catalytic performance in highly endo- or exothermic reactions. The Fisher-Tropsch synthesis (FTS) is a structure sensitive exothermic reaction, which enables catalytic transformation of syngas to high quality liquid fuels. We have elaborated monolithic cobalt based heterogeneous catalysts through a wet chemistry approach that allows control over nanocrystal shape and crystallographic phase, while at the same time enables heat management. Copper and nickel foams have been employed as supports for the epitaxial growth of hcp-Co nanowires, directly from a solution containing a coordination compound of cobalt and stabilizing ligands. The Co/Cufoam catalyst has been tested for the Fischer-Tropsch synthesis in fixed bed reactor, showing stability, and significantly superior activity and selectivity towards C5+ compared to a Co/SiO2-Al2O3 reference catalyst under the same conditions. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Effect of the carrier gas flow rate on the microstructure evolution and the generation of the charged nanoparticles during silicon chemical vapor deposition.

PubMed

Youn, Woong-Kyu; Kim, Chan-Soo; Hwang, Nong-Moon

2013-10-01

The generation of charged nanoparticles in the gas phase has been continually reported in many chemical vapor deposition processes. Charged silicon nanoparticles in the gas phase were measured using a differential mobility analyzer connected to an atmospheric-pressure chemical vapor deposition reactor at various nitrogen carrier gas flow rates (300-1000 standard cubic centimeter per minute) under typical conditions for silicon deposition at the reactor temperature of 900 degrees C. The carrier gas flow rate affected not only the growth behavior of nanostructures but also the number concentration and size distribution of both negatively and positively charged nanoparticles. As the carrier gas flow rate decreased, the growth behavior changed from films to nanowires, which grew without catalytic metal nanoparticles on a quartz substrate.

Contact structure for use in catalytic distillation

DOEpatents

Jones, Jr., Edward M.

1984-01-01

A method for conducting catalytic chemical reactions and fractionation of the reaction mixture comprising feeding reactants into a distillation column reactor contracting said reactant in liquid phase with a fixed bed catalyst in the form of a contact catalyst structure consisting of closed porous containers containing the catatlyst for the reaction and a clip means to hold and support said containers, which are disposed above, i.e., on the distillation trays in the tower. The trays have weir means to provide a liquid level on the trays to substantially cover the containers. In other words, the trays function in their ordinary manner with the addition thereto of the catalyst. The reaction mixture is concurrently fractionated in the column.

Estimation of transient heat flux density during the heat supply of a catalytic wall steam methane reformer

NASA Astrophysics Data System (ADS)

Settar, Abdelhakim; Abboudi, Saïd; Madani, Brahim; Nebbali, Rachid

2018-02-01

Due to the endothermic nature of the steam methane reforming reaction, the process is often limited by the heat transfer behavior in the reactors. Poor thermal behavior sometimes leads to slow reaction kinetics, which is characterized by the presence of cold spots in the catalytic zones. Within this framework, the present work consists on a numerical investigation, in conjunction with an experimental one, on the one-dimensional heat transfer phenomenon during the heat supply of a catalytic-wall reactor, which is designed for hydrogen production. The studied reactor is inserted in an electric furnace where the heat requirement of the endothermic reaction is supplied by electric heating system. During the heat supply, an unknown heat flux density, received by the reactive flow, is estimated using inverse methods. In the basis of the catalytic-wall reactor model, an experimental setup is engineered in situ to measure the temperature distribution. Then after, the measurements are injected in the numerical heat flux estimation procedure, which is based on the Function Specification Method (FSM). The measured and estimated temperatures are confronted and the heat flux density which crosses the reactor wall is determined.

Enantioselective syntheses of aeruginosin 298-A and its analogues using a catalytic asymmetric phase-transfer reaction and epoxidation.

PubMed

Ohshima, Takashi; Gnanadesikan, Vijay; Shibuguchi, Tomoyuki; Fukuta, Yuhei; Nemoto, Tetsuhiro; Shibasaki, Masakatsu

2003-09-17

We developed a versatile synthetic process for aeruginosin 298-A as well as several attractive analogues, in which all stereocenters were controlled by a catalytic asymmetric phase-transfer reaction and epoxidation. Furthermore, drastic counteranion effects in phase-transfer catalysis were observed for the first time, making it possible to three-dimensionally fine-tune the catalyst (ketal part, aromatic part, and counteranion).

MERCURY OXIDATION PROMOTED BY A SELECTIVE CATALYTIC REDUCTION CATALYST UNDER SIMULATED POWDER RIVER BASIN COAL COMBUSTION CONDITIONS

EPA Science Inventory

A bench-scale reactor consisting of a natural gas burner and an electrically heated reactor housing a selective catalytic reduction (SCR) catalyst was constructed for studying elemental mercury oxidation under SCR conditions. A low sulfur Power River Basin (PRB) coal combustion ...

Transient Numerical Modeling of Catalytic Channels

NASA Technical Reports Server (NTRS)

Struk, Peter M.; Dietrich, Daniel L.; Miller, Fletcher J.; T'ien, James S.

2007-01-01

This paper presents a transient model of catalytic combustion suitable for isolated channels and monolith reactors. The model is a lumped two-phase (gas and solid) model where the gas phase is quasi-steady relative to the transient solid. Axial diffusion is neglected in the gas phase; lateral diffusion, however, is accounted for using transfer coefficients. The solid phase includes axial heat conduction and external heat loss due to convection and radiation. The combustion process utilizes detailed gas and surface reaction models. The gas-phase model becomes a system of stiff ordinary differential equations while the solid phase reduces, after discretization, into a system of stiff ordinary differential-algebraic equations. The time evolution of the system came from alternating integrations of the quasi-steady gas and transient solid. This work outlines the numerical model and presents some sensitivity studies on important parameters including internal transfer coefficients, catalytic surface site density, and external heat-loss (if applicable). The model is compared to two experiments using CO fuel: (1) steady-state conversion through an isothermal platinum (Pt) tube and (2) transient propagation of a catalytic reaction inside a small Pt tube. The model requires internal mass-transfer resistance to match the experiments at lower residence times. Under mass-transport limited conditions, the model reasonably predicted exit conversion using global mass-transfer coefficients. Near light-off, the model results did not match the experiment precisely even after adjustment of mass-transfer coefficients. Agreement improved for the first case after adjusting the surface kinetics such that the net rate of CO adsorption increased compared to O2. The CO / O2 surface mechanism came from a sub-set of reactions in a popular CH4 / O2 mechanism. For the second case, predictions improved for lean conditions with increased external heat loss or adjustment of the kinetics as in the first case. Finally, the results show that different initial surface-species distribution leads to different steady-states under certain conditions. These results demonstrate the utility of a lumped two-phase model of a transient catalytic combustor with detailed chemistry.

Increasing the reliability of the shutdown of 500 - 750-kV overhead lines equipped with shunt reactors in an unsuccessful three-phase automatic repeated closure cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuz'micheva, K. I.; Merzlyakov, A. S.; Fokin, G. G.

2013-05-15

The reasons for circuit-breaker failures during repeated disconnection of 500 - 750 kV overhead lines with shunt reactors in a cycle of unsuccessful three-phase automatic reconnection (TARC) are analyzed. Recommendations are made for increasing the operating reliability of power transmission lines with shunt reactors when there is unsuccessful reconnection.

The Sugar Model: Catalytic Flow Reactor Dynamics of Pyruvaldehyde Synthesis from Triose Catalyzed by Poly-L-Lysine Contained in a Dialyzer

NASA Technical Reports Server (NTRS)

Weber, Arthur L.; DeVincenzi, Donald (Technical Monitor)

2000-01-01

The formation of pyruvaldehyde from triose sugars was catalyzed by poly-L-lysine contained in a small dialyzer (100 MWCO) suspended in a much larger triose substrate reservoir. The polylysine confined in the dialyzer functioned as a catalytic flow reactor that constantly brought in triose from the substrate reservoir by diffusion to offset the drop in triose concentration within the reactor caused by its conversion to pyruvaldehyde. A 400 mM solution of poly-L-lysine contained in a 0.35 ml dialyzer placed in a 120 ml solution of triose substrate (pH 5.5, 40 C) generated pyruvaldehyde 11 -times faster than an a control reaction without the catalytic dialyzer. However, since the catalytic dialyzer's volume was 343-times smaller than the control reaction, the synthetic intensity (rate/volume) of pyruvaldehyde synthesis within the catalytic dialyzer was 3400-times greater than that of the control reaction and substrate solution. A similar result was obtained using a dialyzer with a 500 MWCO value. Acting as a catalytic flow reactor the polylysine catalytic dialyzer synthesized about 3.5 molecules of pyruvaldehyde per lysine residue in 7 days -- an amount of triose equal to twice the weight of the catalyst. At 7 days the catalytic activity of polylysine was 16% of its initial value, a result indicating catalyst-poisoning caused by reaction of pyruvaldehyde with the e-amino groups of polylysine. The dialyzer method of catalyst containment was selected it provides a simple, flexible, and easily manipulated experimental system for studying the dynamics and evolutionary development of confined autocatalytic processes related to the origin of life under anaerobic conditions.

Rapid starting methanol reactor system

DOEpatents

Chludzinski, Paul J.; Dantowitz, Philip; McElroy, James F.

1984-01-01

The invention relates to a methanol-to-hydrogen cracking reactor for use with a fuel cell vehicular power plant. The system is particularly designed for rapid start-up of the catalytic methanol cracking reactor after an extended shut-down period, i.e., after the vehicular fuel cell power plant has been inoperative overnight. Rapid system start-up is accomplished by a combination of direct and indirect heating of the cracking catalyst. Initially, liquid methanol is burned with a stoichiometric or slightly lean air mixture in the combustion chamber of the reactor assembly. The hot combustion gas travels down a flue gas chamber in heat exchange relationship with the catalytic cracking chamber transferring heat across the catalyst chamber wall to heat the catalyst indirectly. The combustion gas is then diverted back through the catalyst bed to heat the catalyst pellets directly. When the cracking reactor temperature reaches operating temperature, methanol combustion is stopped and a hot gas valve is switched to route the flue gas overboard, with methanol being fed directly to the catalytic cracking reactor. Thereafter, the burner operates on excess hydrogen from the fuel cells.

Catalytic effect of different reactor materials under subcritical water conditions: decarboxylation of cysteic acid into taurine

NASA Astrophysics Data System (ADS)

Faisal, M.

2018-03-01

In order to understand the influence of reactor materials on the catalytic effect for a particular reaction, the decomposition of cysteic acid from Ni/Fe-based alloy reactors under subcritical water conditions was examined. Experiments were carried out in three batch reactors made of Inconel 625, Hastelloy C-22 and SUS 316 over temperatures of 200 to 300 °C. The highest amount of eluted metals was found for SUS 316. The results demonstrated that reactor materials contribute to the resulting product. Under the tested conditions, cysteic acid decomposes readily with SUS 316. However, the Ni-based materials (Inconel 625 and Hastelloy C-22) show better resistance to metal elution. It was found that among the materials used in this work, SUS 316 gave the highest reaction rate constant of 0.1934 s‑1. The same results were obtained at temperatures of 260 and 300 °C. Investigation of the Arrhenius activation energy revealed that the highest activation energy was for Hastelloy C-22 (109 kJ/mol), followed by Inconel 625 (90 kJ/mol) and SUS 316 (70 kJ/mol). The decomposition rate of cysteic acid was found to follow the results for the trend of the eluted metals. Therefore, it can be concluded that the decomposition of cysteic acid was catalyzed by the elution of heavy metals from the surface of the reactor. The highest amount of taurine from the decarboxylation of cysteic acid was obtained from SUS 316.

In situ IR and X-ray high spatial-resolution microspectroscopy measurements of multistep organic transformation in flow microreactor catalyzed by Au nanoclusters.

PubMed

Gross, Elad; Shu, Xing-Zhong; Alayoglu, Selim; Bechtel, Hans A; Martin, Michael C; Toste, F Dean; Somorjai, Gabor A

2014-03-05

Analysis of catalytic organic transformations in flow reactors and detection of short-lived intermediates are essential for optimization of these complex reactions. In this study, spectral mapping of a multistep catalytic reaction in a flow microreactor was performed with a spatial resolution of 15 μm, employing micrometer-sized synchrotron-based IR and X-ray beams. Two nanometer sized Au nanoclusters were supported on mesoporous SiO2, packed in a flow microreactor, and activated toward the cascade reaction of pyran formation. High catalytic conversion and tunable products selectivity were achieved under continuous flow conditions. In situ synchrotron-sourced IR microspectroscopy detected the evolution of the reactant, vinyl ether, into the primary product, allenic aldehyde, which then catalytically transformed into acetal, the secondary product. By tuning the residence time of the reactants in a flow microreactor a detailed analysis of the reaction kinetics was performed. An in situ micrometer X-ray absorption spectroscopy scan along the flow reactor correlated locally enhanced catalytic conversion, as detected by IR microspectroscopy, to areas with high concentration of Au(III), the catalytically active species. These results demonstrate the fundamental understanding of the mechanism of catalytic reactions which can be achieved by the detailed mapping of organic transformations in flow reactors.

Hydrogenation with monolith reactor under conditions of immiscible liquid phases

DOEpatents

Nordquist, Andrew Francis; Wilhelm, Frederick Carl; Waller, Francis Joseph; Machado, Reinaldo Mario

2002-01-01

The present invention relates to an improved for the hydrogenation of an immiscible mixture of an organic reactant in water. The immiscible mixture can result from the generation of water by the hydrogenation reaction itself or, by the addition of, water to the reactant prior to contact with the catalyst. The improvement resides in effecting the hydrogenation reaction in a monolith catalytic reactor from 100 to 800 cpi, at a superficial velocity of from 0.1 to 2 m/second in the absence of a cosolvent for the immiscible mixture. In a preferred embodiment, the hydrogenation is carried out using a monolith support which has a polymer network/carbon coating onto which a transition metal is deposited.

Evaluation of catalytic combustion of actual coal-derived gas

NASA Technical Reports Server (NTRS)

Blanton, J. C.; Shisler, R. A.

1982-01-01

The combustion characteristics of a Pt-Pl catalytic reactor burning coal-derived, low-Btu gas were investigated. A large matrix of test conditions was explored involving variations in fuel/air inlet temperature and velocity, reactor pressure, and combustor exit temperature. Other data recorded included fuel gas composition, reactor temperatures, and exhaust emissions. Operating experience with the reactor was satisfactory. Combustion efficiencies were quite high (over 95 percent) over most of the operating range. Emissions of NOx were quite high (up to 500 ppm V and greater), owing to the high ammonia content of the fuel gas.

Contact structure for use in catalytic distillation

DOEpatents

Jones, E.M. Jr.

1984-03-27

A method is described for conducting catalytic chemical reactions and fractionation of the reaction mixture comprising feeding reactants into a distillation column reactor, contracting said reactant in liquid phase with a fixed bed catalyst in the form of a contact catalyst structure consisting of closed porous containers containing the catalyst for the reaction and a clip means to hold and support said containers, which are disposed above, i.e., on the distillation trays in the tower. The trays have weir means to provide a liquid level on the trays to substantially cover the containers. In other words, the trays function in their ordinary manner with the addition thereto of the catalyst. The reaction mixture is concurrently fractionated in the column. 7 figs.

Contact structure for use in catalytic distillation

DOEpatents

Jones, Jr., Edward M.

1985-01-01

A method and apparatus for conducting catalytic chemical reactions and fractionation of the reaction mixture, comprising and feeding reactants into a distillation column reactor contracting said reactant in a liquid phase with a fixed bed catalyst in the form of a contact catalyst structure, consisting of closed porous containers containing the catalyst for the reaction and a clip means to hold and support said containers, which are disposed above, i.e., on the distillation trays in the tower. The trays have weir means to provide a liquid level on the trays to substantially cover the containers. In other words, the trays function in their ordinary manner with the addition thereto of the catalyst. The reaction mixture is concurrently fractionated in the column.

Contact structure for use in catalytic distillation

DOEpatents

Jones, E.M. Jr.

1985-08-20

A method and apparatus are disclosed for conducting catalytic chemical reactions and fractionation of the reaction mixture, comprising and feeding reactants into a distillation column reactor contracting said reactant in a liquid phase with a fixed bed catalyst in the form of a contact catalyst structure, consisting of closed porous containers containing the catalyst for the reaction and a clip means to hold and support said containers, which are disposed above, i.e., on the distillation trays in the tower. The trays have weir means to provide a liquid level on the trays to substantially cover the containers. In other words, the trays function in their ordinary manner with the addition thereto of the catalyst. The reaction mixture is concurrently fractionated in the column. 7 figs.

Space and time-resolved probing of heterogeneous catalysis reactions using lab-on-a-chip

NASA Astrophysics Data System (ADS)

Navin, Chelliah V.; Krishna, Katla Sai; Theegala, Chandra S.; Kumar, Challa S. S. R.

2016-03-01

Probing catalytic reactions on a catalyst surface in real time is a major challenge. Herein, we demonstrate the utility of a continuous flow millifluidic chip reactor coated with a nanostructured gold catalyst as an effective platform for in situ investigation of the kinetics of catalytic reactions by taking 5-(hydroxymethyl)furfural (HMF) to 2,5-furandicarboxylic acid (FDCA) conversion as a model reaction. The idea conceptualized in this paper can not only dramatically change the ability to probe the time-resolved kinetics of heterogeneous catalysis reactions but also used for investigating other chemical and biological catalytic processes, thereby making this a broad platform for probing reactions as they occur within continuous flow reactors.Probing catalytic reactions on a catalyst surface in real time is a major challenge. Herein, we demonstrate the utility of a continuous flow millifluidic chip reactor coated with a nanostructured gold catalyst as an effective platform for in situ investigation of the kinetics of catalytic reactions by taking 5-(hydroxymethyl)furfural (HMF) to 2,5-furandicarboxylic acid (FDCA) conversion as a model reaction. The idea conceptualized in this paper can not only dramatically change the ability to probe the time-resolved kinetics of heterogeneous catalysis reactions but also used for investigating other chemical and biological catalytic processes, thereby making this a broad platform for probing reactions as they occur within continuous flow reactors. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr06752a

Catalytic fast pyrolysis of white oak wood in-situ using a bubbling fluidized bed reactor

USDA-ARS?s Scientific Manuscript database

Catalytic fast pyrolysis was performed on white oak wood using two zeolite-type catalysts as bed material in a bubbling fluidized bed reactor. The two catalysts chosen, based on a previous screening study, were Ca2+ exchanged Y54 (Ca-Y54) and a proprietary ß-zeolite type catalyst (catalyst M) both ...

Nanoscale effects of silica particle supports on the formation and properties of TiO2 nanocatalysts

NASA Astrophysics Data System (ADS)

Li, Aize; Jin, Yuhui; Muggli, Darrin; Pierce, David T.; Aranwela, Hemantha; Marasinghe, Gaya K.; Knutson, Theodore; Brockman, Greg; Zhao, Julia Xiaojun

2013-06-01

Small TiO2 crystals in the anatase phase are in high demand as photocatalysts. Stable TiO2 crystals in the anatase phase were obtained using a silica nanoparticle as a support. The focus of this study was to investigate the nanoscale effect of the silica support on the formation and properties of small anatase crystals. The experiments were carried out using powder X-ray diffraction, differential thermal analysis, transmission electron microscopy, and energy dispersion spectroscopy. The results showed that the size of the silica support played a crucial role in crystallization of TiO2 and regulation of TiO2 properties, including phase transition, crystal size, thermodynamic property and catalytic activity. A nanoscale curvature model of the spherical silica support was proposed to explain these size effects. Finally, the developed TiO2 catalysts were applied to the oxidation of methanol using a high-throughput photochemical reactor. The size effect of the silica supports on the TiO2 catalytic efficiency was demonstrated using this system.

Catalytic Ignition and Upstream Reaction Propagation in Monolith Reactors

NASA Technical Reports Server (NTRS)

Struk, Peter M.; Dietrich, Daniel L.; Miller, Fletcher J.; T'ien, James S.

2007-01-01

Using numerical simulations, this work demonstrates a concept called back-end ignition for lighting-off and pre-heating a catalytic monolith in a power generation system. In this concept, a downstream heat source (e.g. a flame) or resistive heating in the downstream portion of the monolith initiates a localized catalytic reaction which subsequently propagates upstream and heats the entire monolith. The simulations used a transient numerical model of a single catalytic channel which characterizes the behavior of the entire monolith. The model treats both the gas and solid phases and includes detailed homogeneous and heterogeneous reactions. An important parameter in the model for back-end ignition is upstream heat conduction along the solid. The simulations used both dry and wet CO chemistry as a model fuel for the proof-of-concept calculations; the presence of water vapor can trigger homogenous reactions, provided that gas-phase temperatures are adequately high and there is sufficient fuel remaining after surface reactions. With sufficiently high inlet equivalence ratio, back-end ignition occurs using the thermophysical properties of both a ceramic and metal monolith (coated with platinum in both cases), with the heat-up times significantly faster for the metal monolith. For lower equivalence ratios, back-end ignition occurs without upstream propagation. Once light-off and propagation occur, the inlet equivalence ratio could be reduced significantly while still maintaining an ignited monolith as demonstrated by calculations using complete monolith heating.

Ceramic oxygen transport membrane array reactor and reforming method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kelly, Sean M.; Christie, Gervase Maxwell; Robinson, Charles

2016-11-08

The invention relates to a commercially viable modular ceramic oxygen transport membrane reforming reactor configured using repeating assemblies of oxygen transport membrane tubes and catalytic reforming reactors.

The ISS Water Processor Catalytic Reactor as a Post Processor for Advanced Water Reclamation Systems

NASA Technical Reports Server (NTRS)

Nalette, Tim; Snowdon, Doug; Pickering, Karen D.; Callahan, Michael

2007-01-01

Advanced water processors being developed for NASA s Exploration Initiative rely on phase change technologies and/or biological processes as the primary means of water reclamation. As a result of the phase change, volatile compounds will also be transported into the distillate product stream. The catalytic reactor assembly used in the International Space Station (ISS) water processor assembly, referred to as Volatile Removal Assembly (VRA), has demonstrated high efficiency oxidation of many of these volatile contaminants, such as low molecular weight alcohols and acetic acid, and is considered a viable post treatment system for all advanced water processors. To support this investigation, two ersatz solutions were defined to be used for further evaluation of the VRA. The first solution was developed as part of an internal research and development project at Hamilton Sundstrand (HS) and is based primarily on ISS experience related to the development of the VRA. The second ersatz solution was defined by NASA in support of a study contract to Hamilton Sundstrand to evaluate the VRA as a potential post processor for the Cascade Distillation system being developed by Honeywell. This second ersatz solution contains several low molecular weight alcohols, organic acids, and several inorganic species. A range of residence times, oxygen concentrations and operating temperatures have been studied with both ersatz solutions to provide addition performance capability of the VRA catalyst.

Development of the Monolith Froth Reactor for Catalytic Wet Oxidation of CELSS Model Wastes

NASA Technical Reports Server (NTRS)

Fisher, John W.; Abraham, Martin

1993-01-01

The aqueous phase oxidation of acetic acid, used as a model compound for the treatment of CELSS (Controlled Ecological Life Support System) waste, was carried out in the monolith froth reactor which utilizes two-phase flow in the monolith channels. The catalytic oxidation of acetic acid was carried out over a Pt/Al2O3 catalyst at temperatures and pressures below the critical point of water. The effect of externally controllable parameters (temperature, liquid flow rate, distributor plate orifice size, pitch, and catalyst distance from the distributor plate) on the rate of acetic acid oxidation was investigated. Results indicate reaction rate increased with increasing temperature and exhibited a maximum with respect to liquid flow rate. The apparent activation energy calculated from reaction rate data was 99.7 kJ/mol. This value is similar to values reported for the oxidation of acetic acid in other systems and is comparable to intrinsic values calculated for oxidation reactions. The kinetic data were modeled using simple power law kinetics. The effect of "froth" feed system characteristics was also investigated. Results indicate that the reaction rate exhibits a maximum with respect to distributor plate orifice size, pitch, and catalyst distance from the distributor plate. Fundamental results obtained were used to extrapolate where the complete removal of acetic acid would be obtained and for the design and operation of a full scale CELSS treatment system.

Fuel-rich catalytic combustion: A soot-free technique for in situ hydrogen-like enrichment

NASA Technical Reports Server (NTRS)

Brabbs, T. A.; Olson, S. L.

1985-01-01

An experimental program on the catalytic oxidation of iso-octane demonstrated the feasibility of the two-stage combustion system for reducing particulate emissions. With a fuel-rich (phi = 4.8 to 7.8) catalytic combustion preburner as the first stage the combustion process was soot free at reactor outlet temperatures of 1200 K or less. Although soot was not measured directly, its absence was indicated. Reaction products collected at two positions downstream of the catalyst bed were analyzed on a gas chromatograph. Comparison of these products indicated that pyrolysis of the larger molecules continued along the drift tube and that benzene formation was a gas-phase reaction. The effective hydrogen-carbon ratio calculated from the reaction products increased by 20 to 68 percent over the range of equivalence ratios tested. The catalytic partial oxidation process also yielded a large number of smaller-containing molecules. The fraction of fuel carbon in compounds having two or fewer carbon atoms ranged from 30 percent at 1100 K to 80 percent at 1200 K.

Degradation of volatile organic compounds in the gas phase by heterogeneous photocatalysis with titanium dioxide/ultraviolet light.

PubMed

Rochetto, Ursula Luana; Tomaz, Edson

2015-07-01

This work presents an overview over heterogeneous photocatalysis performed in gas phase towards the degradation of o-xylene, n-hexane, n-octane, n-decane, methylcyclohexane and 2,2,4-trimethylpentane. The experimental set-up composed by a titanium plug flow reactor vessel contained a quartz tube with a 100 W UV lamp placed at center position from 1.7 cm to the quartz wall. A titanium dioxide film was immobilized on the internal walls of the reactor and used as catalyst. All measurements were taken after reaching steady state condition and evaluated at the inlet and outlet of the system. Conversion rates were studied in a wide range of residence times yielding to a 90% or above conversion as from 20 seconds of residence time. During experiments the temperature of reactor's wall was monitored and remained between 52 and 62 °C. Temperature influence over degradation rates was negligible once a control experiment performed at 15 °C did not modify outgoing results. Humidity effect was also evaluated showing an ideal working range of 10-80% with abrupt conversion decay outside the range. By varying inlet concentration between 60 and 110 ppmv the VOC degradation curves remained unchanged. Loss over catalytic activity was only observed for o-xylene after 30 minutes of reaction, the catalyst was reactivated with a solution of hydrogen peroxide and UV light followed by additional deposition of the catalytic layer. The kinetic study suggests a first order reaction rate. The study of effective and economically viable techniques on the treatment of volatile organic compounds (VOCs) has being highlighted as an important parameter on the environmental research. The heterogeneous photocatalysis in gas phase was proved to be an effective process for the degradation of the nonaromatic VOCs tested, yielding high conversion values for the optimized systems.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Haydary, J., E-mail: juma.haydary@stuba.sk; Susa, D.; Dudáš, J.

Highlights: ► Pyrolysis of aseptic packages was carried out in a laboratory flow reactor. ► Distribution of tetrapak into the product yields was obtained. ► Composition of the pyrolysis products was estimated. ► Secondary thermal and catalytic decomposition of tars was studied. ► Two types of catalysts (dolomite and red clay marked AFRC) were used. - Abstract: Pyrolysis of aseptic packages (tetrapak cartons) in a laboratory apparatus using a flow screw type reactor and a secondary catalytic reactor for tar cracking was studied. The pyrolysis experiments were realized at temperatures ranging from 650 °C to 850 °C aimed at maximizingmore » of the amount of the gas product and reducing its tar content. Distribution of tetrapak into the product yields at different conditions was obtained. The presence of H{sub 2}, CO, CH{sub 4}, CO{sub 2} and light hydrocarbons, HCx, in the gas product was observed. The Aluminum foil was easily separated from the solid product. The rest part of char was characterized by proximate and elemental analysis and calorimetric measurements. The total organic carbon in the tar product was estimated by elemental analysis of tars. Two types of catalysts (dolomite and red clay marked AFRC) were used for catalytic thermal tar decomposition. Three series of experiments (without catalyst in a secondary cracking reactor, with dolomite and with AFRC) at temperatures of 650, 700, 750, 800 and 850 °C were carried out. Both types of catalysts have significantly affected the content of tars and other components in pyrolytic gases. The effect of catalyst on the tetrapack distribution into the product yield on the composition of gas and on the total organic carbon in the tar product is presented in this work.« less

The transport phase of pyrolytic oil exiting a fast fluidized bed reactor

NASA Astrophysics Data System (ADS)

Daugaard, Daren Einar

An unresolved and debated aspect in the fast pyrolysis of biomass is whether the bio-oil exits as a vapor or as an aerosol from the pyrolytic reactor. The determination of the bio-oil transport phase will have direct and significant impact on the design of fast pyrolysis systems. Optimization of both the removal of particulate matter and collection of bio-oil will require this information. In addition, the success of catalytic reforming of bio-oil to high-value chemicals will depend upon this transport phase. A variety of experimental techniques were used to identify the transport phase. Some tests were as simple as examining the catch of an inline filter while others attempted to deduce whether vapor or aerosol predominated by examining the pressure drop across a flow restriction. In supplementary testing, the effect of char on aerosol formation and the potential impact of cracking during direct contact filtering are evaluated. The study indicates that for pyrolysis of red oak approximately 90 wt-% of the collected bio-oil existed as a liquid aerosol. Conversely, the pyrolysis of corn starch produced bio-oil predominately in the vapor phase at the exit of the reactor. Furthermore, it was determined that the addition of char promotes the production of aerosols during pyrolysis of corn starch. Direct contact filtering of the product stream did not collect any liquids and the bio-oil yield was not significantly reduced indicating measurable cracking or coking did not occur.

[Kinetics of catalytic wet air oxidation of phenol in trickle bed reactor].

PubMed

Li, Guang-ming; Zhao, Jian-fu; Wang, Hua; Zhao, Xiu-hua; Zhou, Yang-yuan

2004-05-01

By using a trickle bed reactor which was designed by the authors, the catalytic wet air oxidation reaction of phenol on CuO/gamma-Al2O3 catalyst was studied. The results showed that in mild operation conditions (at temperature of 180 degrees C, pressure of 3 MPa, liquid feed rate of 1.668 L x h(-1) and oxygen feed rate of 160 L x h(-1)), the removal of phenol can be over 90%. The curve of phenol conversion is similar to "S" like autocatalytic reaction, and is accordance with chain reaction of free radical. The kinetic model of pseudo homogenous reactor fits the catalytic wet air oxidation reaction of phenol. The effects of initial concentration of phenol, liquid feed rate and temperature for reaction also were investigated.

Catalytic reactor for automobile

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vroman, W.R.

1977-05-03

A catalytic reactor of oval cross section consists of a generally cylindrical catalytic substrate clamped between paired housing shells and spaced from them by a mesh support that extends around the oval periphery of the substrate and slightly overlaps the latter's axially opposite end to provide locating projections. The support and housing are preferably interlocked by one or more pairs of inwardly opening channels of the housing having portions of the mesh support confined inside, each pair being spaced axially by a rib of the housing projecting into the mesh support. The housing has axially endwise converging cam portions adjacentmore » and axially endwise of the opposite ends of the substrate to engage the locating projections and center the assembled substrate and mesh support within the housing during manufacture of the reactor.« less

Effect of inlet temperature on the performance of a catalytic reactor. [air pollution control

NASA Technical Reports Server (NTRS)

Anderson, D. N.

1978-01-01

A 12 cm diameter by 15 cm long catalytic reactor was tested with No. 2 diesel fuel in a combustion test rig at inlet temperatures of 700, 800, 900, and 1000 K. Other test conditions included pressures of 3 and 6 x 10 to the 5th power Pa, reference velocities of 10, 15, and 20 m/s, and adiabatic combustion temperatures in the range 1100 to 1400 K. The combustion efficiency was calculated from measurements of carbon monoxide and unburned hydrocarbon emissions. Nitrogen oxide emissions and reactor pressure drop were also measured. At a reference velocity of 10 m/s, the CO and unburned hydrocarbons emissions, and, therefore, the combustion efficiency, were independent of inlet temperature. At an inlet temperature of 1000 K, they were independent of reference velocity. Nitrogen oxides emissions resulted from conversion of the small amount (135 ppm) of fuel-bound nitrogen in the fuel. Up to 90 percent conversion was observed with no apparent effect of any of the test variables. For typical gas turbine operating conditions, all three pollutants were below levels which would permit the most stringent proposed automotive emissions standards to be met.

Complexity and Challenges in Noncontact High Temperature Measurements in Microwave-Assisted Catalytic Reactors

PubMed Central

2017-01-01

The complexity and challenges in noncontact temperature measurements inside microwave-heated catalytic reactors are presented in this paper. A custom-designed microwave cavity has been used to focus the microwave field on the catalyst and enable monitoring of the temperature field in 2D. A methodology to study the temperature distribution in the catalytic bed by using a thermal camera in combination with a thermocouple for a heterogeneous catalytic reaction (methane dry reforming) under microwave heating has been demonstrated. The effects of various variables that affect the accuracy of temperature recordings are discussed in detail. The necessity of having at least one contact sensor, such as a thermocouple, or some other microwave transparent sensor, is recommended to keep track of the temperature changes occurring in the catalytic bed during the reaction under microwave heating. PMID:29170599

Low-temperature catalytic gasification of food processing wastes. 1995 topical report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Elliott, D.C.; Hart, T.R.

The catalytic gasification system described in this report has undergone continuing development and refining work at Pacific Northwest National Laboratory (PNNL) for over 16 years. The original experiments, performed for the Gas Research Institute, were aimed at developing kinetics information for steam gasification of biomass in the presence of catalysts. From the fundamental research evolved the concept of a pressurized, catalytic gasification system for converting wet biomass feedstocks to fuel gas. Extensive batch reactor testing and limited continuous stirred-tank reactor tests provided useful design information for evaluating the preliminary economics of the process. This report is a follow-on to previousmore » interim reports which reviewed the results of the studies conducted with batch and continuous-feed reactor systems from 1989 to 1994, including much work with food processing wastes. The discussion here provides details of experiments on food processing waste feedstock materials, exclusively, that were conducted in batch and continuous- flow reactors.« less

CFD Simulation of flow pattern in a bubble column reactor for forming aerobic granules and its development.

PubMed

Fan, Wenwen; Yuan, LinJiang; Li, Yonglin

2018-06-22

The flow pattern is considered to play an important role in the formation of aerobic granular sludge in a bubble column reactor; therefore, it is necessary to understand the behavior of the flow in the reactor. A three-dimensional computational fluid dynamics (CFD) simulation for bubble column reactor was established to visualize the flow patterns of two-phase air-liquid flow and three-phase air-liquid-sludge flow under different ratios of height to diameter (H/D ratio) and superficial gas upflow velocities (SGVs). Moreover, a simulation of the three-phase flow pattern at the same SGV and different characteristics of the sludge was performed in this study. The results show that not only SGV but also properties of sludge involve the transformation of flow behaviors and relative velocity between liquid and sludge. For the original activated sludge floc to cultivate aerobic granules, the flow pattern has nothing to do with sludge, but is influenced by SGV, and the vortices is occurred and the relative velocity is increased with an increase in SGV; the two-phase flow can simplify the three-phase flow that predicts the flow pattern development in bubble column reactor (BCR) for aerobic granulation. For the aerobic granules, the liquid flow behavior developed from the symmetrical circular flow to numbers and small-size vortices with an increase in the sludge diameter, the relative velocity is amount up to u r  = 5.0, it is 29.4 times of original floc sludge.

Polymer network/carbon layer on monolith support and monolith catalytic reactor

DOEpatents

Nordquist, Andrew Francis; Wilhelm, Frederick Carl; Waller, Francis Joseph; Machado, Reinaldo Mario

2003-08-26

The present invention relates to an improved monolith catalytic reactor and a monolith support. The improvement in the support resides in a polymer network/carbon coating applied to the surface of a porous substrate and a catalytic metal, preferably a transition metal catalyst applied to the surface of the polymer network/carbon coating. The monolith support has from 100 to 800 cells per square inch and a polymer network/carbon coating with surface area of from 0.1 to 15 m.sup.2 /gram as measured by adsorption of N.sub.2 or Kr using the BET method.

Method and apparatus for controlling accidental releases of tritium

DOEpatents

Galloway, T.R.

1980-04-01

An improvement is described in a tritium control system based on a catalytic oxidation reactor wherein accidental releases of tritium into room air are controlled by flooding the catalytic oxidation reactor with hydrogen when the tritium concentration in the room air exceeds a specified limit. The sudden flooding with hydrogen heats the catalyst to a high temperature within seconds, thereby greatly increasing the catalytic oxidation rate of tritium to tritiated water vapor. Thus, the catalyst is heated only when needed. In addition to the heating effect, the hydrogen flow also swamps the tritium and further reduces the tritium release. 1 fig.

Method and apparatus for controlling accidental releases of tritium

DOEpatents

Galloway, Terry R. [Berkeley, CA

1980-04-01

An improvement in a tritium control system based on a catalytic oxidation reactor wherein accidental releases of tritium into room air are controlled by flooding the catalytic oxidation reactor with hydrogen when the tritium concentration in the room air exceeds a specified limit. The sudden flooding with hydrogen heats the catalyst to a high temperature within seconds, thereby greatly increasing the catalytic oxidation rate of tritium to tritiated water vapor. Thus, the catalyst is heated only when needed. In addition to the heating effect, the hydrogen flow also swamps the tritium and further reduces the tritium release.

Chemically-modified cellulose paper as a microstructured catalytic reactor.

PubMed

Koga, Hirotaka; Kitaoka, Takuya; Isogai, Akira

2015-01-15

We discuss the successful use of chemically-modified cellulose paper as a microstructured catalytic reactor for the production of useful chemicals. The chemical modification of cellulose paper was achieved using a silane-coupling technique. Amine-modified paper was directly used as a base catalyst for the Knoevenagel condensation reaction. Methacrylate-modified paper was used for the immobilization of lipase and then in nonaqueous transesterification processes. These catalytic paper materials offer high reaction efficiencies and have excellent practical properties. We suggest that the paper-specific interconnected microstructure with pulp fiber networks provides fast mixing of the reactants and efficient transport of the reactants to the catalytically-active sites. This concept is expected to be a promising route to green and sustainable chemistry.

Kinetics studies of d-glucose hydrogenation over activated charcoal supported platinum catalyst

NASA Astrophysics Data System (ADS)

Ahmed, Muthanna J.

2012-02-01

The kinetics of the catalytic hydrogenation of d-glucose to produce d-sorbitol was studied in a three-phase laboratory scale reactor. The hydrogenation reactions were performed on activated charcoal supported platinum catalyst in the temperature range 25-65°C and in a constant pressure of 1 atm. The kinetic data were modeled by zero, first and second-order reaction equations. In the operating regimes studied, the results show that the hydrogenation reaction was of a first order with respect to d-glucose concentration. Also the activation energy of the reaction was determined, and found to be 12.33 kJ mole-1. A set of experiment was carried out to test the deactivation of the catalyst, and the results show that the deactivation is slow with the ability of using the catalyst for several times with a small decrease in product yield.

In Situ and ex Situ Catalytic Pyrolysis of Pine in a Bench-Scale Fluidized Bed Reactor System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Iisa, Kristiina; French, Richard J.; Orton, Kellene A.

In situ and ex situ catalytic pyrolysis were compared in a system with two 2-in. bubbling fluidized bed reactors. Pine was pyrolyzed in the system with a catalyst, HZSM-5 with a silica-to-alumina ratio of 30, placed either in the first (pyrolysis) reactor or the second (upgrading) reactor. Both the pyrolysis and upgrading temperatures were 500 degrees C, and the weight hourly space velocity was 1.1 h -1. Five catalytic cycles were completed in each experiment. The catalytic cycles were continued until oxygenates in the vapors became dominant. The catalyst was then oxidized, after which a new catalytic cycle was begun.more » The in situ configuration gave slightly higher oil yield but also higher oxygen content than the ex situ configuration, which indicates that the catalyst deactivated faster in the in situ configuration than the ex situ configuration. Analysis of the spent catalysts confirmed higher accumulation of metals in the in situ experiment. In all experiments, the organic oil mass yields varied between 14 and 17% and the carbon efficiencies between 20 and 25%. The organic oxygen concentrations in the oils were 16-18%, which represented a 45% reduction compared to corresponding noncatalytic pyrolysis oils prepared in the same fluidized bed reactor system. GC/MS analysis showed the oils to contain one- to four-ring aromatic hydrocarbons and a variety of oxygenates (phenols, furans, benzofurans, methoxyphenols, naphthalenols, indenols). Lastly, high fractions of oxygen were rejected as water, CO, and CO 2, which indicates the importance of dehydration, decarbonylation, and decarboxylation reactions. Light gases were the major sources of carbon losses, followed by char and coke.« less

In Situ and ex Situ Catalytic Pyrolysis of Pine in a Bench-Scale Fluidized Bed Reactor System

DOE PAGES

Iisa, Kristiina; French, Richard J.; Orton, Kellene A.; ...

2016-02-03

In situ and ex situ catalytic pyrolysis were compared in a system with two 2-in. bubbling fluidized bed reactors. Pine was pyrolyzed in the system with a catalyst, HZSM-5 with a silica-to-alumina ratio of 30, placed either in the first (pyrolysis) reactor or the second (upgrading) reactor. Both the pyrolysis and upgrading temperatures were 500 degrees C, and the weight hourly space velocity was 1.1 h -1. Five catalytic cycles were completed in each experiment. The catalytic cycles were continued until oxygenates in the vapors became dominant. The catalyst was then oxidized, after which a new catalytic cycle was begun.more » The in situ configuration gave slightly higher oil yield but also higher oxygen content than the ex situ configuration, which indicates that the catalyst deactivated faster in the in situ configuration than the ex situ configuration. Analysis of the spent catalysts confirmed higher accumulation of metals in the in situ experiment. In all experiments, the organic oil mass yields varied between 14 and 17% and the carbon efficiencies between 20 and 25%. The organic oxygen concentrations in the oils were 16-18%, which represented a 45% reduction compared to corresponding noncatalytic pyrolysis oils prepared in the same fluidized bed reactor system. GC/MS analysis showed the oils to contain one- to four-ring aromatic hydrocarbons and a variety of oxygenates (phenols, furans, benzofurans, methoxyphenols, naphthalenols, indenols). Lastly, high fractions of oxygen were rejected as water, CO, and CO 2, which indicates the importance of dehydration, decarbonylation, and decarboxylation reactions. Light gases were the major sources of carbon losses, followed by char and coke.« less

Cloud iron speciation: Experimental simulations

NASA Astrophysics Data System (ADS)

Sofikitis, A. M.; Colin, J. L.; Desboeufs, K. V.; Losno, R.

2003-04-01

The aim of our contribution is to identify major processes controlling iron speciation in the atmospheric aqueous phase. Fe is known to participate in a variety of redox reactions in cloud chemistry, as well as controlling free radical production in the troposphere. Iron cycling is slower than cycles with other catalytic transition metals (Cu, Mn). The residence time of each iron species is around ten minutes, this allows analytical separation and determination of each iron redox species and therefore its ratio. As the only source of trace metals in aqueous atmospheric phase is due to the solubilization of aerosols, we present here dissolution rate measurements obtained by laboratory experiments with an open flow reactor. This reactor enables us to reproduce the dissolution of a particle in aqueous atmospheric water. The dissolution rate and the speciation of iron are dependent on the mineralogy of the solid phase. Our experiments included Goethite, hematite and vermiculite, which are typical mineral constituents of dust particles. Comparisons were made with natural loess which is a blend of various crystalline and amorphous phases. We will present results of crustal origin particles dissolution experiments where kinetic parameters are determined, including iron speciation. Major functions of variation are pH and photochemistry in the aqueous weathering solution.

Apple juice clarification by immobilized pectolytic enzymes in packed or fluidized bed reactors.

PubMed

Diano, Nadia; Grimaldi, Tiziana; Bianco, Mariangela; Rossi, Sergio; Gabrovska, Katya; Yordanova, Galya; Godjevargova, Tzonka; Grano, Valentina; Nicolucci, Carla; Mita, Luigi; Bencivenga, Umberto; Canciglia, Paolo; Mita, Damiano G

2008-12-10

The catalytic behavior of a mixture of pectic enzymes, covalently immobilized on different supports (glass microspheres, nylon 6/6 pellets, and PAN beads), was analyzed with a pectin aqueous solution that simulates apple juice. The following parameters were investigated: the rate constant at which pectin hydrolysis is conducted, the time (tau(50)) in which the reduction of 50% of the initial viscosity is reached, and the time (tau(comp,dep)) required to obtain complete depectinization. The best catalytic system was proven to be PAN beads, and their pH and temperature behavior were determined. The yields of two bed reactors, packed or fluidized, using the catalytic PAN beads, were compared to the circulation flow rate of real apple juice. The experimental conditions were as follows: pH 4.0, T = 50 degrees C, and beads volume = 20 cm(3). The initial pectin concentration was the one that was present in our apple juice sample. No differences were observed at low circulation rates, while at higher recirculation rates, the time required to obtain complete pectin hydrolysis into the fluidized reactor was found to be 0.25 times smaller than in the packed bed reactor: 131 min for the packed reactors and 41 min for the fluidized reactors.

Catalytic distillation process

DOEpatents

Smith, Jr., Lawrence A.

1982-01-01

A method for conducting chemical reactions and fractionation of the reaction mixture comprising feeding reactants to a distillation column reactor into a feed zone and concurrently contacting the reactants with a fixed bed catalytic packing to concurrently carry out the reaction and fractionate the reaction mixture. For example, a method for preparing methyl tertiary butyl ether in high purity from a mixed feed stream of isobutene and normal butene comprising feeding the mixed feed stream to a distillation column reactor into a feed zone at the lower end of a distillation reaction zone, and methanol into the upper end of said distillation reaction zone, which is packed with a properly supported cationic ion exchange resin, contacting the C.sub.4 feed and methanol with the catalytic distillation packing to react methanol and isobutene, and concurrently fractionating the ether from the column below the catalytic zone and removing normal butene overhead above the catalytic zone.

Catalytic distillation process

DOEpatents

Smith, L.A. Jr.

1982-06-22

A method is described for conducting chemical reactions and fractionation of the reaction mixture comprising feeding reactants to a distillation column reactor into a feed zone and concurrently contacting the reactants with a fixed bed catalytic packing to concurrently carry out the reaction and fractionate the reaction mixture. For example, a method for preparing methyl tertiary butyl ether in high purity from a mixed feed stream of isobutene and normal butene comprising feeding the mixed feed stream to a distillation column reactor into a feed zone at the lower end of a distillation reaction zone, and methanol into the upper end of said distillation reaction zone, which is packed with a properly supported cationic ion exchange resin, contacting the C[sub 4] feed and methanol with the catalytic distillation packing to react methanol and isobutene, and concurrently fractionating the ether from the column below the catalytic zone and removing normal butene overhead above the catalytic zone.

Recovery of useful chemicals from palm oil mill wastewater

NASA Astrophysics Data System (ADS)

Ratanaporn, Yuangsawad; Duangkamol, Na-Ranong; Teruoki, Tago; Takao, Masuda

2017-11-01

A two-step process consisting of pyrolysis of dried sludge and catalytic upgrading of pyrolysed liquid was proposed. Wastewater from a palm oil mill was separated to solid cake and liquid by filtration. The solid cake was dried and pyrolysed at 773 K. Liquid product obtained from the pyrolysis had two immiscible aqueous and oil phases (PL-A and PL-O). Identification of chemicals in PL-A and PL-O indicated that both phases contained various chemicals with unsaturated bonds, such as carboxylic acids and alcohols, however, most of the chemicals could not be identified. Catalytic upgrading of PL-A and PL-O over ZrO2·FeOx were separately performed using a fixed bed reactor at various conditions, T = 513-723 K and mass of catalyst to feed rate = 0.25-10 h. The main components in the liquid products of PL-A upgrading were methanol and acetone whereas they were acetone and phenol in the case of PL-O upgrading. More than 15% of carbon in raw material was deposited on the catalyst. To reduce the carbon deposition, the used catalyst was treated with air at 823 K. This simple treatment could reasonably regenerate the catalyst only for the case of PL-A catalytic upgrading.

Reforming Biomass Derived Pyrolysis Bio-oil Aqueous Phase to Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mukarakate, Calvin; Evans, Robert J.; Deutch, Steve

Fast pyrolysis and catalytic fast pyrolysis (CFP) of biomass produce a liquid product stream comprised of various classes of organic compounds having different molecule size and polarity. This liquid, either spontaneously in the case of catalytic fast pyrolysis or by water addition for the non-catalytic process separates into a non-polar organic-rich fraction and a highly polar water-rich fraction. The organic fraction can be used as a blendstock or feedstock for further processing in a refinery while, in the CFP process design, the aqueous phase is currently sent to wastewater treatment, which results in a loss of residual biogenic carbon presentmore » in this stream. Our work focuses on the catalytic conversion of the biogenic carbon in pyrolysis aqueous phase streams to produce hydrocarbons using a vertical micro-reactor coupled to a molecular beam mass spectrometer (MBMS). Furthermore, the MBMS provides real-time analysis of products while also tracking catalyst deactivation. The catalyst used in this work was HZSM-5, which upgraded the oxygenated organics in the aqueous fraction to fuels comprising small olefins and aromatic hydrocarbons. During processing the aqueous bio-oil fraction the HZSM-5 catalyst exhibited higher activity and coke resistance than those observed in similar experiments using biomass or whole bio-oils. Reduced coking is likely due to ejection of coke precursors from the catalyst pores that was enhanced by excess process water available for steam stripping. The water reacted with coke precursors to form phenol, methylated phenols, naphthol, and methylated naphthols. Conversion data shows that up to 40 wt% of the carbon in the feed stream is recovered as hydrocarbons.« less

Reforming Biomass Derived Pyrolysis Bio-oil Aqueous Phase to Fuels

DOE PAGES

Mukarakate, Calvin; Evans, Robert J.; Deutch, Steve; ...

2017-01-07

Fast pyrolysis and catalytic fast pyrolysis (CFP) of biomass produce a liquid product stream comprised of various classes of organic compounds having different molecule size and polarity. This liquid, either spontaneously in the case of catalytic fast pyrolysis or by water addition for the non-catalytic process separates into a non-polar organic-rich fraction and a highly polar water-rich fraction. The organic fraction can be used as a blendstock or feedstock for further processing in a refinery while, in the CFP process design, the aqueous phase is currently sent to wastewater treatment, which results in a loss of residual biogenic carbon presentmore » in this stream. Our work focuses on the catalytic conversion of the biogenic carbon in pyrolysis aqueous phase streams to produce hydrocarbons using a vertical micro-reactor coupled to a molecular beam mass spectrometer (MBMS). Furthermore, the MBMS provides real-time analysis of products while also tracking catalyst deactivation. The catalyst used in this work was HZSM-5, which upgraded the oxygenated organics in the aqueous fraction to fuels comprising small olefins and aromatic hydrocarbons. During processing the aqueous bio-oil fraction the HZSM-5 catalyst exhibited higher activity and coke resistance than those observed in similar experiments using biomass or whole bio-oils. Reduced coking is likely due to ejection of coke precursors from the catalyst pores that was enhanced by excess process water available for steam stripping. The water reacted with coke precursors to form phenol, methylated phenols, naphthol, and methylated naphthols. Conversion data shows that up to 40 wt% of the carbon in the feed stream is recovered as hydrocarbons.« less

Development of the Monolith Froth Reactor for Catalytic Wet Oxidation of CELSS Model Wastes

NASA Technical Reports Server (NTRS)

Abraham, Martin; Fisher, John W.

1995-01-01

The aqueous phase oxidation of acetic acid, used as a model compound for the treatment of CELSS (Controlled Ecological Life Support System) waste, was carried out in the monolith froth reactor which utilizes two-phase flow in the monolith channels. The catalytic oxidation of acetic acid was carried out over a Pt/Al2O3 catalyst, prepared at The University of Tulsa, at temperatures and pressures below the critical point of water. The effect of externally controllable parameters (temperature, liquid flow rate, distributor plate orifice size, pitch, and catalyst distance from the distributor plate) on the rate of acetic acid oxidation was investigated. Results indicate reaction rate increased with increasing temperature and exhibited a maximum with respect to liquid flow rate. The apparent activation energy calculated from reaction rate data was 99.7 kJ/mol. This value is similar to values reported for the oxidation of acetic acid in other systems and is comparable to intrinsic values calculated for oxidation reactions. The kinetic data were modeled using simple power law kinetics. The effect of "froth" feed system characteristics was also investigated. Results indicate that the reaction rate exhibits a maximum with respect to distributor plate orifice size, pitch, and catalyst distance from the distributor plate. Fundamental results obtained were used to extrapolate where the complete removal of acetic acid would be obtained and for the design and operation of a full scale CELSS treatment system.

Syngas Production from CO2 Reforming and CO2-steam Reforming of Methane over Ni/Ce-SBA-15 Catalyst

NASA Astrophysics Data System (ADS)

Tan, J. S.; Danh, H. T.; Singh, S.; Truong, Q. D.; Setiabudi, H. D.; Vo, D.-V. N.

2017-06-01

This study compares the catalytic performance of mesoporous 10 Ni/Ce-SBA-15 catalyst for CO2 reforming and CO2-steam reforming of methane reactions in syngas production. The catalytic performance of 10 Ni/Ce-SBA-15 catalyst for CO2 reforming and CO2-steam reforming of methane was evaluated in a temperature-controlled tubular fixed-bed reactor at stoichiometric feed composition, 1023 K and atmospheric pressure for 12 h on-stream with gas hourly space velocity (GHSV) of 36 L gcat -1 h-1. The 10 Ni/Ce-SBA-15 catalyst possessed a high specific BET surface area and average pore volume of 595.04 m2 g-1. The XRD measurement revealed the presence of NiO phase with crystallite dimension of about 13.60 nm whilst H2-TPR result indicates that NiO phase was completely reduced to metallic Ni0 phase at temperature beyond 800 K and the reduction temperature relied on different degrees of metal-support interaction associated with the location and size of NiO particles. The catalytic reactivity was significantly enhanced with increasing H2O/CO2 feed ratio. Interestingly, the H2/CO ratio for CO2-steam reforming of methane varied between 1 and 3 indicated the occurrence of parallel reactions, i.e., CH4 steam reforming giving a H2/CO of 3 whilst reverse water-gas shift (RWGS) reaction consuming H2 to produce CO gaseous product.

Catalyst Residence Time Distributions in Riser Reactors for Catalytic Fast Pyrolysis. Part 2: Pilot-Scale Simulations and Operational Parameter Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Foust, Thomas D.; Ziegler, Jack L.; Pannala, Sreekanth

2017-02-21

Here, wsing the validated simulation model developed in part one of this study for biomass catalytic fast pyrolysis (CFP), we assess the functional utility of using this validated model to assist in the development of CFP processes in fluidized catalytic cracking (FCC) reactors to a commercially viable state. Specifically, we examine the effects of mass flow rates, boundary conditions (BCs), pyrolysis vapor molecular weight variation, and the impact of the chemical cracking kinetics on the catalyst residence times. The factors that had the largest impact on the catalyst residence time included the feed stock molecular weight and the degree ofmore » chemical cracking as controlled by the catalyst activity. Lastly, because FCC reactors have primarily been developed and utilized for petroleum cracking, we perform a comparison analysis of CFP with petroleum and show the operating regimes are fundamentally different.« less

Effect of UV on De-NOx performance and microbial community of a hybrid catalytic membrane biofilm reactor

NASA Astrophysics Data System (ADS)

Chen, Zhouyang; Huang, Zhensha; He, Yiming; Xiao, Xiaoliang; Wei, Zaishan

2018-02-01

The hybrid membrane catalytic biofilm reactor provides a new way of flue gas denitration. However, the effects of UV on denitrification performance, microbial community and microbial nitrogen metabolism are still unknown. In this study, the effects of UV on deNO x performance, nitrification and denitrification, microbial community and microbial nitrogen metabolism of a bench scale N-TiO2/PSF hybrid catalytic membrane biofilm reactor (HCMBR) were evaluated. The change from nature light to UV in the HCMBR leads to the fall of NO removal efficiency of HCMBR from 92.8% to 81.8%. UV affected the microbial community structure, but did not change microbial nitrogen metabolism, as shown by metagenomics sequencing method. Some dominant phyla, such as Gammaproteobacteria, Bacteroidetes, Firmicutes, Actinobacteria, and Alphaproteobacteria, increased in abundance, whereas others, such as Proteobacteria and Betaproteobacteria, decreased. There were nitrification, denitrification, nitrogen fixation, and organic nitrogen metabolism in the HCMBR.

Immobilizing Highly Catalytically Active Pt Nanoparticles inside the Pores of Metal-Organic Framework: A Double Solvents Approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aijaz, Arshad; Karkamkar, Abhijeet J.; Choi, Young Joon

2012-08-29

Ultrafine Pt nanoparticles were successfully immobilized inside the pores of a metal-organic framework MIL-101 without deposition of Pt nanoparticles on the external surfaces of framework by using a 'double solvents' method. The resulting Pt@MIL-101 composites with different Pt loadings represent the first highly active MOF-immobilized metal nanocatalysts for catalytic reactions in all three phases: liquid-phase ammonia borane hydrolysis; solid-phase ammonia borane thermal dehy-drogenation and gas-phase CO oxidation. The observed excellent catalytic performances are at-tributed to the small Pt nanoparticles within the pores of MIL-101. 'We are thankful to AIST and METI for financial support. TA & AK are thankful formore » support from the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. PNNL is operated by Battelle.'« less

Real-Time Monitoring of Heterogeneous Catalysis with Mass Spectrometry

ERIC Educational Resources Information Center

Young, Mark A.

2009-01-01

Heterogeneous, gas-solid processes constitute an important class of catalytic reactions that play a key role in a variety of applications, such as industrial processing and environmental controls. Heterogeneous catalytic chemistry can be demonstrated in a simple heated flow reactor containing a fragment of the catalytic converter from a vehicular…

Catalytic two-stage coal hydrogenation and hydroconversion process

DOEpatents

MacArthur, James B.; McLean, Joseph B.; Comolli, Alfred G.

1989-01-01

A process for two-stage catalytic hydrogenation and liquefaction of coal to produce increased yields of low-boiling hydrocarbon liquid and gas products. In the process, the particulate coal is slurried with a process-derived liquid solvent and fed at temperature below about 650.degree. F. into a first stage catalytic reaction zone operated at conditions which promote controlled rate liquefaction of the coal, while simultaneously hydrogenating the hydrocarbon recycle oils at conditions favoring hydrogenation reactions. The first stage reactor is maintained at 650.degree.-800.degree. F. temperature, 1000-4000 psig hydrogen partial pressure, and 10-60 lb coal/hr/ft.sup.3 reactor space velocity. The partially hydrogenated material from the first stage reaction zone is passed directly to the close-coupled second stage catalytic reaction zone maintained at a temperature at least about 25.degree. F. higher than for the first stage reactor and within a range of 750.degree.-875.degree. F. temperature for further hydrogenation and thermal hydroconversion reactions. By this process, the coal feed is successively catalytically hydrogenated and hydroconverted at selected conditions, which results in significantly increased yields of desirable low-boiling hydrocarbon liquid products and minimal production of undesirable residuum and unconverted coal and hydrocarbon gases, with use of less energy to obtain the low molecular weight products, while catalyst life is substantially increased.

Catalytic and thermal cracking processes of waste cooking oil for bio-gasoline synthesis

NASA Astrophysics Data System (ADS)

Dewanto, Muhammad Andry Rizki; Januartrika, Aulia Azka; Dewajani, Heny; Budiman, Arief

2017-03-01

Non-renewable energy resources such as fossil fuels, and coal were depleted as the increase of global energy demand. Moreover, environmental aspect becomes a major concern which recommends people to utilize bio-based resources. Waste cooking oil is one of the economical sources for biofuel production and become the most used raw material for biodiesel production. However, the products formed during frying, can affect the trans-esterification reaction and the biodiesel properties. Therefore, it needs to convert low-quality cooking oil directly into biofuel by both thermal and catalytic cracking processes. Thermal and catalytic cracking sometimes are regarded as prospective bio-energy conversion processes. This research was carried out in the packed bed reactor equipped with 2 stages preheater with temperature of reactor was variated in the range of 450-550°C. At the same temperature, catalytic cracking had been involved in this experiment, using activated ZSM-5 catalyst with 1 cm in length. The organic liquid product was recovered by three stages of double pipe condensers. The composition of cracking products were analyzed using GC-MS instrument and the caloric contents were analyzed using Bomb calorimeter. The results reveal that ZSM-5 was highly selective toward aromatic and long aliphatic compounds formation. The percentage recovery of organic liquid product from the cracking process varies start from 8.31% and the optimal results was 54.08%. The highest heating value of liquid product was resulted from catalytic cracking process at temperature of 450°C with value of 10880.48 cal/gr and the highest product yield with 54.08% recovery was achieved from thermal cracking process with temperature of 450°C.

[Study on the start-up of anaerobic ammonium oxidation process in biological activated carbon reactor].

PubMed

Lai, Wei-Yi; Zhou, Wei-Li; He, Sheng-Bing

2013-08-01

In order to shorten the start-up time of anaerobic ammonium oxidation (ANAMMOX) reactor, biological activated cabon reactor was applied. Three lab scale UASB reactors were seeded with anaerobic sludge, fed with synthetic wastewater containing ammonia and nitrite, and supplemented with granular activated carbon on day 0, 33 and 56, respectively. The nitrogen removal performance of the first reactor, into which GAC was added on day 0, showed no significant improvement in 90 days. After being suspended for about one month, the secondary start-up of this reactor succeeded in another 33 days (totally 123 days). 49 d and 85 d were taken for the other two reactors started up by the addition of GAC on day 33 and 56, respectively. After the reactors were started up, the average removal rates of total nitrogen were 89.8%, 86.7% and 86.7%, respectively. The start-up process could be divided into four stages, namely, the bacterial autolysis phase, the lag phase, the improve phase and the stationary phase, and the best time for adding GAC carrier was right after the start of the lag phase.

Gas chemical studies using corona discharge reactors

NASA Astrophysics Data System (ADS)

Schulze, P.; Stankiewicz, A.; Aicher, M.; Mattner, M.; Ulrich, A.

2010-12-01

Corona discharges with voltages up to 60 kV (DC) were studied with the aim to induce chemical reactions in flue gases at atmospheric pressure. Various plasma reactors with different geometries of multi-needle arrays were tested. The power input was optimised by studying the electrical parameters of the set-up systematically. Both, solid and liquid electrodes were used in combination with the needle arrays. A precise positioning of the corona needles allowed operation without a ballast resistor. Formation rates for CO and the sum of NO2 and O3 are reported and discussed. Three catalytic anode-coatings were tested for their potential to decompose carbon dioxide.

Renewable Wood Pulp Paper Reactor with Hierarchical Micro/Nanopores for Continuous-Flow Nanocatalysis.

PubMed

Koga, Hirotaka; Namba, Naoko; Takahashi, Tsukasa; Nogi, Masaya; Nishina, Yuta

2017-06-22

Continuous-flow nanocatalysis based on metal nanoparticle catalyst-anchored flow reactors has recently provided an excellent platform for effective chemical manufacturing. However, there has been limited progress in porous structure design and recycling systems for metal nanoparticle-anchored flow reactors to create more efficient and sustainable catalytic processes. In this study, traditional paper is used for a highly efficient, recyclable, and even renewable flow reactor by tailoring the ultrastructures of wood pulp. The "paper reactor" offers hierarchically interconnected micro- and nanoscale pores, which can act as convective-flow and rapid-diffusion channels, respectively, for efficient access of reactants to metal nanoparticle catalysts. In continuous-flow, aqueous, room-temperature catalytic reduction of 4-nitrophenol to 4-aminophenol, a gold nanoparticle (AuNP)-anchored paper reactor with hierarchical micro/nanopores provided higher reaction efficiency than state-of-the-art AuNP-anchored flow reactors. Inspired by traditional paper materials, successful recycling and renewal of AuNP-anchored paper reactors were also demonstrated while high reaction efficiency was maintained. © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

On-line Analysis of Catalytic Reaction Products Using a High-Pressure Tandem Micro-reactor GC/MS.

PubMed

Watanabe, Atsushi; Kim, Young-Min; Hosaka, Akihiko; Watanabe, Chuichi; Teramae, Norio; Ohtani, Hajime; Kim, Seungdo; Park, Young-Kwon; Wang, Kaige; Freeman, Robert R

2017-01-01

When a GC/MS system is coupled with a pressurized reactor, the separation efficiency and the retention time are directly affected by the reactor pressure. To keep the GC column flow rate constant irrespective of the reaction pressure, a restrictor capillary tube and an open split interface are attached between the GC injection port and the head of a GC separation column. The capability of the attached modules is demonstrated for the on-line GC/MS analysis of catalytic reaction products of a bio-oil model sample (guaiacol), produced under a pressure of 1 to 3 MPa.

Process Development for Hydrothermal Liquefaction of Algae Feedstocks in a Continuous-Flow Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Elliott, Douglas C.; Hart, Todd R.; Schmidt, Andrew J.

Wet algae slurries can be converted into an upgradeable biocrude by hydrothermal liquefaction (HTL). High levels of carbon conversion to gravity-separable biocrude product were accomplished at relatively low temperature (350 °C) in a continuous-flow, pressurized (sub-critical liquid water) environment (20 MPa). As opposed to earlier work in batch reactors reported by others, direct oil recovery was achieved without the use of a solvent and biomass trace components were removed by processing steps so that they did not cause process difficulties. High conversions were obtained even with high slurry concentrations of up to 35 wt% of dry solids. Catalytic hydrotreating wasmore » effectively applied for hydrodeoxygenation, hydrodenitrogenation, and hydrodesulfurization of the biocrude to form liquid hydrocarbon fuel. Catalytic hydrothermal gasification was effectively applied for HTL byproduct water cleanup and fuel gas production from water soluble organics, allowing the water to be considered for recycle of nutrients to the algae growth ponds. As a result, high conversion of algae to liquid hydrocarbon and gas products was found with low levels of organic contamination in the byproduct water. All three process steps were accomplished in bench-scale, continuous-flow reactor systems such that design data for process scale-up was generated.« less

Effect of Catalytic Cylinders on Autothermal Reforming of Methane for Hydrogen Production in a Microchamber Reactor

PubMed Central

Yan, Yunfei; Guo, Hongliang; Zhang, Li; Zhu, Junchen; Yang, Zhongqing; Tang, Qiang; Ji, Xin

2014-01-01

A new multicylinder microchamber reactor is designed on autothermal reforming of methane for hydrogen production, and its performance and thermal behavior, that is, based on the reaction mechanism, is numerically investigated by varying the cylinder radius, cylinder spacing, and cylinder layout. The results show that larger cylinder radius can promote reforming reaction; the mass fraction of methane decreased from 26% to 21% with cylinder radius from 0.25 mm to 0.75 mm; compact cylinder spacing corresponds to more catalytic surface and the time to steady state is decreased from 40 s to 20 s; alteration of staggered and aligned cylinder layout at constant inlet flow rates does not result in significant difference in reactor performance and it can be neglected. The results provide an indication and optimize performance of reactor; it achieves higher conversion compared with other reforming reactors. PMID:25097877

Kinetic study on the catalytic performance of Rh/TiO/sub 2/ reduced at different temperatures in the CO-H/sub 2/ reaction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fujitsu, H.; Ikeyama, N.; Mochida, I.

1986-08-01

Catalytic CO-H/sub 2/ reaction on Rh/TiO/sub 2/ reduced at 200, 400, and 500/sup 0/C (Cat-200, -400, -500) for 2 h was kinetically studied at 250/sup 0/C using a circulating reactor and Fourier transform-infrared (FT-IR) spectroscopy to determine how Cat-400 exhibited the highest activity. The rate equation distinguished the best catalyst with zero and first orders in CO and H/sub 2/, respectively, from other catalysts with negative order in CO. The adsorption ability of the catalyst at 200/sup 0/C was comparable to that of Cat-200, and two to three times larger than that of Cat-500, although the ability of Cat-200 wasmore » much larger at room temperature. Carbon monoxide adsorbed on the catalysts reversibly as well as irreversibly. IR spectroscopy revealed that the major form of irreversibly adsorbed CO was linear on Cat-200, whereas similar amounts of linear and bridge forms were observed on Cat-400 and Cat-500. These latter forms were highly reactive against hydrogen molecules when no carbon monoxide was present in the gas phase. Based on these results, the highest activity of Cat-400 is ascribed to rhodium metal modified by properly reduced TiO/sub 2/ to show the appropriate adsorption ability of carbon monoxide which least retards the activation of hydrogen according to first-order kinetics. Typical strong metal-support interaction decreases the catalytic activity by decreasing the active sites and strengthening the CO adsorption too much.« less

Combustion engine system

NASA Technical Reports Server (NTRS)

Houseman, John (Inventor); Voecks, Gerald E. (Inventor)

1986-01-01

A flow through catalytic reactor which selectively catalytically decomposes methanol into a soot free hydrogen rich product gas utilizing engine exhaust at temperatures of 200 to 650 C to provide the heat for vaporizing and decomposing the methanol is described. The reactor is combined with either a spark ignited or compression ignited internal combustion engine or a gas turbine to provide a combustion engine system. The system may be fueled entirely by the hydrogen rich gas produced in the methanol decomposition reactor or the system may be operated on mixed fuels for transient power gain and for cold start of the engine system. The reactor includes a decomposition zone formed by a plurality of elongated cylinders which contain a body of vapor permeable, methanol decomposition catalyst preferably a shift catalyst such as copper-zinc.

Balancing Near-Field Enhancement, Absorption, and Scattering for Effective Antenna-Reactor Plasmonic Photocatalysis.

PubMed

Li, Kun; Hogan, Nathaniel J; Kale, Matthew J; Halas, Naomi J; Nordlander, Peter; Christopher, Phillip

2017-06-14

Efficient photocatalysis requires multifunctional materials that absorb photons and generate energetic charge carriers at catalytic active sites to facilitate a desired chemical reaction. Antenna-reactor complexes are an emerging multifunctional photocatalytic structure where the strong, localized near field of the plasmonic metal nanoparticle (e.g., Ag) is coupled to the catalytic properties of the nonplasmonic metal nanoparticle (e.g., Pt) to enable chemical transformations. With an eye toward sustainable solar driven photocatalysis, we investigate how the structure of antenna-reactor complexes governs their photocatalytic activity in the light-limited regime, where all photons need to be effectively utilized. By synthesizing core@shell/satellite (Ag@SiO 2 /Pt) antenna-reactor complexes with varying Ag nanoparticle diameters and performing photocatalytic CO oxidation, we observed plasmon-enhanced photocatalysis only for antenna-reactor complexes with antenna components of intermediate sizes (25 and 50 nm). Optimal photocatalytic performance was shown to be determined by a balance between maximized local field enhancements at the catalytically active Pt surface, minimized collective scattering of photons out of the catalyst bed by the complexes, and minimal light absorption in the Ag nanoparticle antenna. These results elucidate the critical aspects of local field enhancement, light scattering, and absorption in plasmonic photocatalyst design, especially under light-limited illumination conditions.

Renewable Wood Pulp Paper Reactor with Hierarchical Micro/Nanopores for Continuous‐Flow Nanocatalysis

PubMed Central

Namba, Naoko; Takahashi, Tsukasa; Nogi, Masaya; Nishina, Yuta

2017-01-01

Abstract Continuous‐flow nanocatalysis based on metal nanoparticle catalyst‐anchored flow reactors has recently provided an excellent platform for effective chemical manufacturing. However, there has been limited progress in porous structure design and recycling systems for metal nanoparticle‐anchored flow reactors to create more efficient and sustainable catalytic processes. In this study, traditional paper is used for a highly efficient, recyclable, and even renewable flow reactor by tailoring the ultrastructures of wood pulp. The “paper reactor” offers hierarchically interconnected micro‐ and nanoscale pores, which can act as convective‐flow and rapid‐diffusion channels, respectively, for efficient access of reactants to metal nanoparticle catalysts. In continuous‐flow, aqueous, room‐temperature catalytic reduction of 4‐nitrophenol to 4‐aminophenol, a gold nanoparticle (AuNP)‐anchored paper reactor with hierarchical micro/nanopores provided higher reaction efficiency than state‐of‐the‐art AuNP‐anchored flow reactors. Inspired by traditional paper materials, successful recycling and renewal of AuNP‐anchored paper reactors were also demonstrated while high reaction efficiency was maintained. PMID:28394501

Biomass Conversion to Produce Hydrocarbon Liquid Fuel Via Hot-vapor Filtered Fast Pyrolysis and Catalytic Hydrotreating.

PubMed

Wang, Huamin; Elliott, Douglas C; French, Richard J; Deutch, Steve; Iisa, Kristiina

2016-12-25

Lignocellulosic biomass conversion to produce biofuels has received significant attention because of the quest for a replacement for fossil fuels. Among the various thermochemical and biochemical routes, fast pyrolysis followed by catalytic hydrotreating is considered to be a promising near-term opportunity. This paper reports on experimental methods used 1) at the National Renewable Energy Laboratory (NREL) for fast pyrolysis of lignocellulosic biomass to produce bio-oils in a fluidized-bed reactor and 2) at Pacific Northwest National Laboratory (PNNL) for catalytic hydrotreating of bio-oils in a two-stage, fixed-bed, continuous-flow catalytic reactor. The configurations of the reactor systems, the operating procedures, and the processing and analysis of feedstocks, bio-oils, and biofuels are described in detail in this paper. We also demonstrate hot-vapor filtration during fast pyrolysis to remove fine char particles and inorganic contaminants from bio-oil. Representative results showed successful conversion of biomass feedstocks to fuel-range hydrocarbon biofuels and, specifically, the effect of hot-vapor filtration on bio-oil production and upgrading. The protocols provided in this report could help to generate rigorous and reliable data for biomass pyrolysis and bio-oil hydrotreating research.

Biomass Conversion to Produce Hydrocarbon Liquid Fuel Via Hot-vapor Filtered Fast Pyrolysis and Catalytic Hydrotreating

PubMed Central

Wang, Huamin; Elliott, Douglas C.; French, Richard J.; Deutch, Steve; Iisa, Kristiina

2016-01-01

Lignocellulosic biomass conversion to produce biofuels has received significant attention because of the quest for a replacement for fossil fuels. Among the various thermochemical and biochemical routes, fast pyrolysis followed by catalytic hydrotreating is considered to be a promising near-term opportunity. This paper reports on experimental methods used 1) at the National Renewable Energy Laboratory (NREL) for fast pyrolysis of lignocellulosic biomass to produce bio-oils in a fluidized-bed reactor and 2) at Pacific Northwest National Laboratory (PNNL) for catalytic hydrotreating of bio-oils in a two-stage, fixed-bed, continuous-flow catalytic reactor. The configurations of the reactor systems, the operating procedures, and the processing and analysis of feedstocks, bio-oils, and biofuels are described in detail in this paper. We also demonstrate hot-vapor filtration during fast pyrolysis to remove fine char particles and inorganic contaminants from bio-oil. Representative results showed successful conversion of biomass feedstocks to fuel-range hydrocarbon biofuels and, specifically, the effect of hot-vapor filtration on bio-oil production and upgrading. The protocols provided in this report could help to generate rigorous and reliable data for biomass pyrolysis and bio-oil hydrotreating research. PMID:28060311

Method and apparatus for decoupled thermo-catalytic pollution control

DOEpatents

Tabatabaie-Raissi, Ali; Muradov, Nazim Z.; Martin, Eric

2006-07-11

A new method for design and scale-up of thermocatalytic processes is disclosed. The method is based on optimizing process energetics by decoupling of the process energetics from the DRE for target contaminants. The technique is applicable to high temperature thermocatalytic reactor design and scale-up. The method is based on the implementation of polymeric and other low-pressure drop support for thermocatalytic media as well as the multifunctional catalytic media in conjunction with a novel rotating fluidized particle bed reactor.

Packed-bed catalytic cracking of oak derived pyrolytic vapors

USDA-ARS?s Scientific Manuscript database

Catalytic upgrading of pyrolysis vapors derived from oak was carried out using a fixed-bed catalytic column at 425 deg C. The vapors were drawn by splitting a fraction from the full stream of vapors produced at 500 deg C in a 5 kg/hr bench-scale fast pyrolysis reactor system downstream the cyclone s...

Largely enhanced photocatalytic activity of Au/XS2/Au (X = Re, Mo) antenna-reactor hybrids: charge and energy transfer.

PubMed

Chen, Kai; Ding, Si-Jing; Luo, Zhi-Jun; Pan, Gui-Ming; Wang, Jia-Hong; Liu, Jia; Zhou, Li; Wang, Qu-Quan

2018-02-22

An antenna-reactor hybrid coupling plasmonic antenna with catalytic nanoparticles is a new strategy to optimize photocatalytic activity. Herein, we have rationally proposed a Au/XS 2 /Au (X = Re, Mo) antenna reactor, which has a large Au core as the antenna and small satellite Au nanoparticles as the reactor separated by an ultrathin two-dimensional transition-metal dichalcogenide XS 2 shell (∼2.6 nm). Due to efficient charge transfer across the XS 2 shell as well as energy transfer via coupling of the Au antenna and Au reactor, the photocatalytic activity has been largely enhanced: Au/ReS 2 /Au exhibits a 3.59-fold enhancement, whereas Au/MoS 2 /Au exhibits a 2.66-fold enhancement as compared to that of the sum of the three individual components. The different enhancement in the Au/ReS 2 /Au and Au/MoS 2 /Au antenna-reactor hybrid is related to the competition and cooperation of charge and energy transfer. These results indicate the great potential of the Au/XS 2 /Au antenna-reactor hybrid for the development of highly efficient plasmonic photocatalysts.

Spatially and temporally resolved gas distributions around heterogeneous catalysts using infrared planar laser-induced fluorescence

PubMed Central

Zetterberg, Johan; Blomberg, Sara; Gustafson, Johan; Evertsson, Jonas; Zhou, Jianfeng; Adams, Emma C.; Carlsson, Per-Anders; Aldén, Marcus; Lundgren, Edvin

2015-01-01

Visualizing and measuring the gas distribution in close proximity to a working catalyst is crucial for understanding how the catalytic activity depends on the structure of the catalyst. However, existing methods are not able to fully determine the gas distribution during a catalytic process. Here we report on how the distribution of a gas during a catalytic reaction can be imaged in situ with high spatial (400 μm) and temporal (15 μs) resolution using infrared planar laser-induced fluorescence. The technique is demonstrated by monitoring, in real-time, the distribution of carbon dioxide during catalytic oxidation of carbon monoxide above powder catalysts. Furthermore, we demonstrate the versatility and potential of the technique in catalysis research by providing a proof-of-principle demonstration of how the activity of several catalysts can be measured simultaneously, either in the same reactor chamber, or in parallel, in different reactor tubes. PMID:25953006

Dehydration of glycerol over niobia-supported silicotungstic acid catalysts.

PubMed

Lee, Young Yi; Ok, Hye Jeong; Moon, Dong Ju; Kim, Jong Ho; Park, Nam Cook; Kim, Young Chul

2013-01-01

Liquid-phase dehydration of glycerol to acrolein over nanosized niobia-supported silicotungstic acid catalysts was performed to investigate the effect of the silicotungstic acid loading on the catalytic performance of the catalysts. The catalysts were prepared by following an impregnation method with different HSiW loadings in the range of 10-50 wt%. The prepared catalysts were characterized by N2 physisorption, XRD, FT-IR, TPD of ammonia, and TGA. Dehydration of glycerol was conducted in an autoclave reactor under the conditions of controlled reaction temperatures under corresponding pressure. Increasing HSiW loading rapidly increased the acidity of HSiW/Nb205 catalyst and rate of glycerol conversion, but acrolein selectivity decreased due to enhanced deactivation of the catalyst by carbon deposit. Consequently, it was confirmed that catalytic activity for the dehydration of glycerol to acrolein was dependant on the acidity of catalyst and can be controlled by HSiW loading.

High-throughput investigation of catalysts for JP-8 fuel cracking to liquefied petroleum gas.

PubMed

Bedenbaugh, John E; Kim, Sungtak; Sasmaz, Erdem; Lauterbach, Jochen

2013-09-09

Portable power technologies for military applications necessitate the production of fuels similar to LPG from existing feedstocks. Catalytic cracking of military jet fuel to form a mixture of C₂-C₄ hydrocarbons was investigated using high-throughput experimentation. Cracking experiments were performed in a gas-phase, 16-sample high-throughput reactor. Zeolite ZSM-5 catalysts with low Si/Al ratios (≤25) demonstrated the highest production of C₂-C₄ hydrocarbons at moderate reaction temperatures (623-823 K). ZSM-5 catalysts were optimized for JP-8 cracking activity to LPG through varying reaction temperature and framework Si/Al ratio. The reducing atmosphere required during catalytic cracking resulted in coking of the catalyst and a commensurate decrease in conversion rate. Rare earth metal promoters for ZSM-5 catalysts were screened to reduce coking deactivation rates, while noble metal promoters reduced onset temperatures for coke burnoff regeneration.

Degradation pathway of malachite green in a novel dual-tank photoelectrochemical catalytic reactor.

PubMed

Diao, Zenghui; Li, Mingyu; Zeng, Fanyin; Song, Lin; Qiu, Rongliang

2013-09-15

A novel dual-tank photoelectrochemical catalytic reactor was designed to investigate the degradation pathway of malachite green. A thermally formed TiO₂/Ti thin film electrode was used as photoanode, graphite was used as cathode, and a saturated calomel electrode was employed as the reference electrode in the reactor. In the reactor, the anode and cathode tanks were connected by a cation exchange membrane. Results showed that the decolorization ratio of malachite green in the anode and cathode was 98.5 and 96.5% after 120 min, respectively. Malachite green in the two anode and cathode tanks was oxidized, achieving the bipolar double effect. Malachite green in both the anode and cathode tanks exhibited similar catalytic degradation pathways. The double bond of the malachite green molecule was attacked by strong oxidative hydroxyl radicals, after which the organic compound was degraded by the two pathways into 4,4-bis(dimethylamino) benzophenone, 4-(dimethylamino) benzophenone, 4-(dimethylamino) phenol, and other intermediate products. Eventually, malachite green was degraded into oxalic acid as a small molecular organic acid, which was degraded by processes such as demethylation, deamination, nitration, substitution, addition, and other reactions. Copyright © 2013 Elsevier B.V. All rights reserved.

Selective Conversion of Lignin-Derivable 4-Alkylguaiacols to 4-Alkylcyclohexanols over Noble and Non-Noble-Metal Catalysts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schutyser, Wouter; Van den Bossche, Gil; Raaffels, Anton

2016-10-03

Recent lignin-first catalytic lignocellulosic biorefineries produce large quantities of two potential platform chemicals, 4-n-propylguaiacol (PG) and 4-n-propylsyringol. Because conversion into 4-n-propylcyclohexanol (PCol), a precursor for novel polymer building blocks, presents a promising valorization route, reductive demethoxylation of PG was examined here in the liquid-phase over three commercial hydrogenation catalysts, viz. 5 wt % Ru/C, 5 wt % Pd/C and 65 wt % Ni/SiO2-Al2O3, at elevated temperatures ranging from 200 to 300 degrees C under hydrogen atmosphere. Kinetic profiles suggest two parallel conversion pathways: Pathway I involves PG hydrogenation to 4-n-propyl-2-methoxycyclohexanol (PMCol), followed by its demethoxylation to PCol, whereas Pathway IImore » constitutes PG hydrodemethoxylation to 4-n-propylphenol (PPh), followed by its hydrogenation into PCol. The slowest step in the catalytic formation of PCol is the reductive methoxy removal from PMCol. Moreover, under the applied reaction conditions, PCol may react further into hydrocarbons. The following criteria are therefore essential to reach a high PCol yield: (i) catalytic pathway II is preferred as this route does not involve stable intermediates; (ii) reactivity of PMCol should be higher than that of PCol, and (iii) the overall carbon balance should be high. Both the catalyst type and the reaction conditions have a substantial impact on the PCol yield. Only the commercial Ni catalyst meets the three criteria, provided the reaction is performed at 250 degrees C in hexadecane. Additional advantages of this solvent choice are a high boiling point (low operational pressure in closed reactor systems), high solubility of PG and derived products, high thermal, reductive stability, and easy derivability from fatty biomass feedstock. This Ni catalyst also showed an excellent stability in recycling runs and is capable of converting highly concentrated (up to 20 wt %) PG in hexadecane. Ru and Pd on carbon showed a low PCol yield, as they are not conform the three criteria. Low hydrogen pressure favors Pathway II, resulting in a very high PCol yield of 85% at 10 bar. Catalytic conversion of guaiacol, 4-methyl- and 4-ethylguaiacol in comparable circumstances showed similarly high yields of the corresponding cyclohexanols.« less

Catalytic Oxidation of Vanillyl Alcohol Using FeMCM-41 Nanoporous Tubular Reactor

NASA Astrophysics Data System (ADS)

Elamathi, P.; Kolli, Murali Krishna; Chandrasekar, G.

Iron containing nanoporous MCM-41 (FeMCM-41) with different Si/Fe ratios of 50, 100 and 150 was synthesized by hydrothermal synthesis process. The materials obtained from hydrothermal synthesis were characterized by various physico chemical techniques such as XRD, N2 adsorption, DR UV-vis, EPR and FTIR spectroscopy. XRD analyses of FeMCM-41 materials confirmed the presence of well-ordered crystalline structure. N2 isotherm of FeMCM-41 materials showed type IV adsorption isotherm. EPR and DR UV-vis analysis of FeMCM-41 samples indicates the presence of high tetrahedral coordination at the Si/Fe ratios of 100 and 150. The catalytic performance of FeMCM-41 nano tubular reactor was tested in the liquid phase oxidation of vanillyl alcohol into vanillin using H2O2 (50wt% in water). The reaction products were analyzed by gas chromatography in DB-5 capillary column with flame ionization detector. The products were confirmed by 1H NMR, 13C NMR and LC-Mass spectroscopy. The maximum conversion of vanillyl alcohol (85%) and selectivity towards vanillin (82%) were observed using the catalyst FeMCM-41(100) in 30min at 60∘C. The influence of reaction temperature, reaction time, reactants molar ratio, Si/Fe ratio and amount of catalyst were investigated.

Polymer nanocomposite membranes with hierarchically structured catalysts for high throughput dehalogenation

NASA Astrophysics Data System (ADS)

Crock, Christopher A.

Halogenated organics are categorized as primary pollutants by the Environmental Protection Agency. Trichloroethylene (TCE), which had broad industrial use in the past, shows persistence in the environment because of its chemical stability. The large scale use and poor control of TCE resulted in its prolonged release into the environment before the carcinogenic risk associated with TCE was fully understood. TCE pollution stemmed from industrial effluents and improper disposal of solvent waste. Membrane reactors are promising technology for treating TCE polluted groundwater because of the high throughput, relatively low cost of membrane fabrication and facile retrofitting of existing membrane based water treatment facilities with catalytic membrane reactors. Compared to catalytic fluidized or fixed bed reactors, catalytic membrane reactors feature minimal diffusional limitation. Additionally, embedding catalyst within the membrane avoids the need for catalyst recovery and can prevent aggregation of catalytic nanoparticles. In this work, Pd/xGnP, Pd-Au/xGnP, and commercial Pd/Al2O3 nanoparticles were employed in batch and flow-through membrane reactors to catalyze the dehalogenation of TCE in the presence of dissolved H2. Bimetallic Pd-Au/xGnP catalysts were shown to be more active than monometallic Pd/xGnP or commercial Pd/Al 2O3 catalysts. In addition to synthesizing nanocomposite membranes for high-throughput TCE dehalogenation, the membrane based dehalogenation process was designed to minimize the detrimental impact of common catalyst poisons (S2-, HS-, and H2S -) by concurrent oxidation of sulfide species to gypsum in the presence of Ca2+ and removal of gypsum through membrane filtration. The engineered membrane dehalogenation process demonstrated that bimetallic Pd-Au/xGnP catalysts resisted deactivation by residual sulfide species after oxidation, and showed complete removal of gypsum during membrane filtration.

Catalytic combustion of residual fuels

NASA Technical Reports Server (NTRS)

Bulzan, D. L.; Tacina, R. R.

1981-01-01

A noble metal catalytic reactor was tested using two grades of petroleum derived residual fuels at specified inlet air temperatures, pressures, and reference velocities. Combustion efficiencies greater than 99.5 percent were obtained. Steady state operation of the catalytic reactor required inlet air temperatures of at least 800 K. At lower inlet air temperatures, upstream burning in the premixing zone occurred which was probably caused by fuel deposition and accumulation on the premixing zone walls. Increasing the inlet air temperature prevented this occurrence. Both residual fuels contained about 0.5 percent nitrogen by weight. NO sub x emissions ranged from 50 to 110 ppm by volume at 15 percent excess O2. Conversion of fuel-bound nitrogen to NO sub x ranged from 25 to 50 percent.

The catalytic activity of CoMo/USY on deoxygenation reaction of anisole in a batch reactor

NASA Astrophysics Data System (ADS)

Nugrahaningtyas, K. D.; Putri, I. F.; Heraldy, E.; Hidayat, Y.

2018-04-01

The catalytic hydrodeoxigenation of the bio oil model compounds (biomass pyrolysis results) typically uses sulphide catalysts. In this study, we studied the activity of non-sulphide catalyst, the effect of temperature and reaction time on anisole deoxygenation. The catalytic activity was performed in a batch reactor, using N2 gas at 1 bar of pressure. The product was analyzed by gas chromatography (GC) and gas chromatography-mass spectrometry (GC-MS). The result showed that the Co-Mo/USY catalyst perform a highest activity and produce pentamethylbenzene, an oxygen free products, when reaction time is 2 hours. The Co-Mo/USY catalysts has the value of the total yield of the product increased with time increase drastically.

Pre-biotic stage of life origin under non-photosynthetic conditions

NASA Technical Reports Server (NTRS)

Bartsev, S. I.; Mezhevikin, V. V.

2005-01-01

Spontaneous assembling of a simplest bacterial cell even if all necessary molecules are present in a solution seems to be extremely rare event and from the scientific standpoint has to be considered as impossible. Therefore, a predecessor of a living cell has to be very simple for providing its self-assembling and at the same time it should be able of progressive increase in complexity. Now phase-separated particles, first of all micelles, are put forward as possible predecessors of living cell. According to the offered working concept only phase-separated particles possessing autocatalytic properties can be considered as predecessors of living cells. The first stage of evolution of these phase-separated autocatalytic systems is the appearance of pre-biotic metabolism providing synthesis of amphiphiles for formation of capsules of these systems. This synthesis is maintained by the energy of a base reaction being a component of a planet-chemical cycle. Catalytic system providing functioning of pre-biotic metabolism is based on multivariate oligomeric autocatalyst, which reproduces itself from monomers, penetrating the particles from the outside. Since the autocatalyst realizes random polymerization then a collection of other oligomers possessing different catalytic functions is produced. In the paper the functioning of multivariate oligomeric autocatalyst in flow reactor is analyzed. c2005 Published by Elsevier Ltd on behalf of COSPAR.

Catalytic decomposition of methanol for onboard hydrogen generation

NASA Technical Reports Server (NTRS)

Brabbs, T.

1978-01-01

The steam reformation of an equimolar mixture of methanol and water on a copper chromite catalyst was studied at three furnace temperatures and at feed space velocities from 800 to 2600 per hour. The hydrogen space velocity could be related to the reactor temperature by the equation Sv = A exp (-omega T), where A and omega are constants determined for each value of alpha and T is temperature. At a methanol conversion of 0.87 and a reactor temperature of 589 K, the extrapolated value of the hydrogen space velocity was 9400 per hour. This velocity was used to estimate the size of an onboard hydrogen reactor for automotive applications. Such a reactor would need only about 0.8 liter of catalyst to produce 7630 STP liters (1.5 lb) of hydrogen per hour. This quantity of catalyst would fit into nine tubes 17.8 centimeters along and 2.54 centimeters in inside diameter, which is smaller than most mufflers. The reactor products would contain 12 to 13 percent more chemical energy than the incoming methanol and water.

Steam Reformer With Fibrous Catalytic Combustor

NASA Technical Reports Server (NTRS)

Voecks, Gerald E.

1987-01-01

Proposed steam-reforming reactor derives heat from internal combustion on fibrous catalyst. Supplies of fuel and air to combustor controlled to meet demand for heat for steam-reforming reaction. Enables use of less expensive reactor-tube material by limiting temperature to value safe for material yet not so low as to reduce reactor efficiency.

Non-catalytic steam hydrolysis of fats. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deibert, M.C.

1992-08-28

Hydrolysis of fats and oils produces fatty acid and glycerol. The catalyzed, liquid phase Colgate-Emry process, state-of-the-art, produces impure products that require extensive energy investment for their purification to commercial grade. Non-catalytic steam hydrolysis may produce products more easily purified. A bench-scale hydrolyzer was designed and constructed to contact descending liquid fat or oil with rising superheated steam. Each of the five stages in the reactor was designed similar to a distillation column stage to promote intimate liquid-gas contact. Degree of hydrolysis achieved in continuous tests using tallow feed were 15% at 280C and 35% at 300C at a tallow-to-steammore » mass feed ratio of 4.2. At a feed ratio of 9.2, the degree of hydrolysis was 21% at 300C. Decomposition was strongly evident at 325C but not at lower temperatures. Soybean oil rapidly polymerized under reaction conditions. Batch tests at 320C produced degrees of hydrolyses of between 44% and 63% using tallow and palm oil feeds. Over 95% fatty acids were present in a clean, readily separated organic portion of the overhead product from most tests. The test reactor had serious hydraulic resistance to liquid down-flow which limited operation to very long liquid residence times. These times are in excess of those that tallow and palm oil are stable at the reaction temperature. Little glycerol and extensive light organics were produced indicating that unexplained competing reactions to hydrolysis occurred in the experimental system. Further tests using an improved reactor will be required.« less

Non-catalytic steam hydrolysis of fats

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deibert, M.C.

1992-08-28

Hydrolysis of fats and oils produces fatty acid and glycerol. The catalyzed, liquid phase Colgate-Emry process, state-of-the-art, produces impure products that require extensive energy investment for their purification to commercial grade. Non-catalytic steam hydrolysis may produce products more easily purified. A bench-scale hydrolyzer was designed and constructed to contact descending liquid fat or oil with rising superheated steam. Each of the five stages in the reactor was designed similar to a distillation column stage to promote intimate liquid-gas contact. Degree of hydrolysis achieved in continuous tests using tallow feed were 15% at 280C and 35% at 300C at a tallow-to-steammore » mass feed ratio of 4.2. At a feed ratio of 9.2, the degree of hydrolysis was 21% at 300C. Decomposition was strongly evident at 325C but not at lower temperatures. Soybean oil rapidly polymerized under reaction conditions. Batch tests at 320C produced degrees of hydrolyses of between 44% and 63% using tallow and palm oil feeds. Over 95% fatty acids were present in a clean, readily separated organic portion of the overhead product from most tests. The test reactor had serious hydraulic resistance to liquid down-flow which limited operation to very long liquid residence times. These times are in excess of those that tallow and palm oil are stable at the reaction temperature. Little glycerol and extensive light organics were produced indicating that unexplained competing reactions to hydrolysis occurred in the experimental system. Further tests using an improved reactor will be required.« less

Polypropylene Production Optimization in Fluidized Bed Catalytic Reactor (FBCR): Statistical Modeling and Pilot Scale Experimental Validation

PubMed Central

Khan, Mohammad Jakir Hossain; Hussain, Mohd Azlan; Mujtaba, Iqbal Mohammed

2014-01-01

Propylene is one type of plastic that is widely used in our everyday life. This study focuses on the identification and justification of the optimum process parameters for polypropylene production in a novel pilot plant based fluidized bed reactor. This first-of-its-kind statistical modeling with experimental validation for the process parameters of polypropylene production was conducted by applying ANNOVA (Analysis of variance) method to Response Surface Methodology (RSM). Three important process variables i.e., reaction temperature, system pressure and hydrogen percentage were considered as the important input factors for the polypropylene production in the analysis performed. In order to examine the effect of process parameters and their interactions, the ANOVA method was utilized among a range of other statistical diagnostic tools such as the correlation between actual and predicted values, the residuals and predicted response, outlier t plot, 3D response surface and contour analysis plots. The statistical analysis showed that the proposed quadratic model had a good fit with the experimental results. At optimum conditions with temperature of 75°C, system pressure of 25 bar and hydrogen percentage of 2%, the highest polypropylene production obtained is 5.82% per pass. Hence it is concluded that the developed experimental design and proposed model can be successfully employed with over a 95% confidence level for optimum polypropylene production in a fluidized bed catalytic reactor (FBCR). PMID:28788576

Catalytic biomass pyrolysis process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dayton, David C.; Gupta, Raghubir P.; Turk, Brian S.

Described herein are processes for converting a biomass starting material (such as lignocellulosic materials) into a low oxygen containing, stable liquid intermediate that can be refined to make liquid hydrocarbon fuels. More specifically, the process can be a catalytic biomass pyrolysis process wherein an oxygen removing catalyst is employed in the reactor while the biomass is subjected to pyrolysis conditions. The stream exiting the pyrolysis reactor comprises bio-oil having a low oxygen content, and such stream may be subjected to further steps, such as separation and/or condensation to isolate the bio-oil.

Performance of rotary kiln reactor for the elephant grass pyrolysis.

PubMed

De Conto, D; Silvestre, W P; Baldasso, C; Godinho, M

2016-10-01

The influence of process conditions (rotary speed/temperature) on the performance of a rotary kiln reactor for non-catalytic pyrolysis of a perennial grass (elephant grass) was investigated. The product yields, the production of non-condensable gases as well as the biochar properties were evaluated. The maximum H2 yield was close to that observed for catalytic pyrolysis processes, while the bio-oil yield was higher than reported for pyrolysis of other biomass in rotary kiln reactors. A H2/CO ratio suitable for Fischer-Tropsch synthesis (FTS) was obtained. The biochars presented an alkaline pH (above 10) and interesting contents of nutrients, as well as low electrical conductivity, indicating a high potential as soil amendment. Copyright © 2016 Elsevier Ltd. All rights reserved.

Catalytic reactor

DOEpatents

Aaron, Timothy Mark [East Amherst, NY; Shah, Minish Mahendra [East Amherst, NY; Jibb, Richard John [Amherst, NY

2009-03-10

A catalytic reactor is provided with one or more reaction zones each formed of set(s) of reaction tubes containing a catalyst to promote chemical reaction within a feed stream. The reaction tubes are of helical configuration and are arranged in a substantially coaxial relationship to form a coil-like structure. Heat exchangers and steam generators can be formed by similar tube arrangements. In such manner, the reaction zone(s) and hence, the reactor is compact and the pressure drop through components is minimized. The resultant compact form has improved heat transfer characteristics and is far easier to thermally insulate than prior art compact reactor designs. Various chemical reactions are contemplated within such coil-like structures such that as steam methane reforming followed by water-gas shift. The coil-like structures can be housed within annular chambers of a cylindrical housing that also provide flow paths for various heat exchange fluids to heat and cool components.

Biomass conversion to produce hydrocarbon liquid fuel via hot-vapor filtered fast pyrolysis and catalytic hydrotreating

DOE PAGES

Wang, Huamin; Elliott, Douglas C.; French, Richard J.; ...

2016-12-25

Lignocellulosic biomass conversion to produce biofuels has received significant attention because of the quest for a replacement for fossil fuels. Among the various thermochemical and biochemical routes, fast pyrolysis followed by catalytic hydrotreating is considered to be a promising near-term opportunity. This paper reports on experimental methods used 1) at the National Renewable Energy Laboratory (NREL) for fast pyrolysis of lignocellulosic biomass to produce bio-oils in a fluidized-bed reactor and 2) at Pacific Northwest National Laboratory (PNNL) for catalytic hydrotreating of bio-oils in a two-stage, fixed-bed, continuous-flow catalytic reactor. The configurations of the reactor systems, the operating procedures, and themore » processing and analysis of feedstocks, bio-oils, and biofuels are described in detail in this paper. We also demonstrate hot-vapor filtration during fast pyrolysis to remove fine char particles and inorganic contaminants from bio-oil. Representative results showed successful conversion of biomass feedstocks to fuel-range hydrocarbon biofuels and, specifically, the effect of hot-vapor filtration on bio-oil production and upgrading. As a result, the protocols provided in this report could help to generate rigorous and reliable data for biomass pyrolysis and bio-oil hydrotreating research.« less

Biomass conversion to produce hydrocarbon liquid fuel via hot-vapor filtered fast pyrolysis and catalytic hydrotreating

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Huamin; Elliott, Douglas C.; French, Richard J.

Lignocellulosic biomass conversion to produce biofuels has received significant attention because of the quest for a replacement for fossil fuels. Among the various thermochemical and biochemical routes, fast pyrolysis followed by catalytic hydrotreating is considered to be a promising near-term opportunity. This paper reports on experimental methods used 1) at the National Renewable Energy Laboratory (NREL) for fast pyrolysis of lignocellulosic biomass to produce bio-oils in a fluidized-bed reactor and 2) at Pacific Northwest National Laboratory (PNNL) for catalytic hydrotreating of bio-oils in a two-stage, fixed-bed, continuous-flow catalytic reactor. The configurations of the reactor systems, the operating procedures, and themore » processing and analysis of feedstocks, bio-oils, and biofuels are described in detail in this paper. We also demonstrate hot-vapor filtration during fast pyrolysis to remove fine char particles and inorganic contaminants from bio-oil. Representative results showed successful conversion of biomass feedstocks to fuel-range hydrocarbon biofuels and, specifically, the effect of hot-vapor filtration on bio-oil production and upgrading. As a result, the protocols provided in this report could help to generate rigorous and reliable data for biomass pyrolysis and bio-oil hydrotreating research.« less

Gas hydrate dissociation via in situ combustion of methane - lab studies and field tests

NASA Astrophysics Data System (ADS)

Luzi-Helbing, Manja; Schicks, Judith M.; Spangenberg, Erik; Giese, Ronny

2013-04-01

In general, three different methods for gas hydrate production are known: thermal stimulation, pressure reduction, and chemical stimulation. In the framework of the German joint project SUGAR (Submarine Gas Hydrate Reservoirs: exploration, extraction and transport) a countercurrent heat exchange reactor was developed at GFZ which has been designed to decompose gas hydrates in sediments via thermal stimulation. The heat is produced by the catalytic oxidation of methane. The advantage of this method is that the heat is generated in place i.e. within the borehole on the same level like the hydrate-bearing sediments. The system is closed which means that there is no contact between the products or catalyst and the environment. The power output and the temperature of the reactor are regulated via the volume flow of the feed gases air and methane. Therefore, the catalytic reaction runs temperature-controlled, autothermic and safe. So far, a lab-scale prototype of the reactor (outer diameter 40 mm, length 457 mm) was successfully tested in a large reservoir simulator (LARS) which was set up at GFZ. Pt, Pd and Ir on ZrO2 as carrier material turned out to be a robust and reliable catalyst. This work presents results of the latest reactor test for which LARS was filled with sand, and ca. 80 % of the pore space was saturated with methane hydrate. To form hydrates the pore pressure and the confining pressure were kept at 8 MPa and 12 MPa, respectively, and the temperature was set to 278 K. During the start sequence the reactor was ignited at room temperature with hydrogen. By the time the reactor temperature reached ca. 523 K (ca. 15 min after hydrogen ignition) the fuel flow was changed to methane. After 9 hours all temperature sensors which are spatially distributed in LARS showed a temperature above the equilibrium temperature of 282 K at 8 MPa. All in all, the reactor was run for 12 h at 723 K. The data analysis showed that 15 % of the methane gas released from hydrates would have to be used for the catalytic combustion of methane. However, only a part of the hydrate-bound methane gas could be produced during the experiment. The residual gas remained in the pore space. Currently the pilot-scale reactor is developed to a borehole tool with an outer diameter of 90 mm and ca. 5 m length. The first field test is planned for summer 2013 at the continental deep drilling KTB in Windischeschenbach, Germany. In future, we aim for a field test in hydrate-bearing sediments.

Multiscale Evaluation of Catalytic Upgrading of Biomass Pyrolysis Vapors on Ni- and Ga-Modified ZSM-5

DOE PAGES

Yung, Matthew M.; Stanton, Alexander R.; Iisa, Kristiina; ...

2016-10-07

Metal-impregnated (Ni or Ga) ZSM-5 catalysts were studied for biomass pyrolysis vapor upgrading to produce hydrocarbons using three reactors constituting a 100 000x change in the amount of catalyst used in experiments. Catalysts were screened for pyrolysis vapor phase upgrading activity in two small-scale reactors: (i) a Pyroprobe with a 10 mg catalyst in a fixed bed and (ii) a fixed-bed reactor with 500 mg of catalyst. The best performing catalysts were then validated with a larger scale fluidized-bed reactor (using ~1 kg of catalyst) that produced measurable quantities of bio-oil for analysis and evaluation of mass balances. Despite somemore » inherent differences across the reactor systems (such as residence time, reactor type, analytical techniques, mode of catalyst and biomass feed) there was good agreement of reaction results for production of aromatic hydrocarbons, light gases, and coke deposition. Relative to ZSM-5, Ni or Ga addition to ZSM-5 increased production of fully deoxygenated aromatic hydrocarbons and light gases. In the fluidized bed reactor, Ga/ZSM-5 slightly enhanced carbon efficiency to condensed oil, which includes oxygenates in addition to aromatic hydrocarbons, and reduced oil oxygen content compared to ZSM-5. Ni/ZSM-5, while giving the highest yield of fully deoxygenated aromatic hydrocarbons, gave lower overall carbon efficiency to oil but with the lowest oxygen content. Reaction product analysis coupled with fresh and spent catalyst characterization indicated that the improved performance of Ni/ZSM-5 is related to decreasing deactivation by coking, which keeps the active acid sites accessible for the deoxygenation and aromatization reactions that produce fully deoxygenated aromatic hydrocarbons. The addition of Ga enhances the dehydrogenation activity of the catalyst, which leads to enhanced olefin formation and higher fully deoxygenated aromatic hydrocarbon yields compared to unmodified ZSM-5. Catalyst characterization by ammonia temperature programmed desorption, surface area measurements, and postreaction temperature-programmed oxidation (TPO) also showed that the metal-modified zeolites retained a greater percentage of their initial acidity and surface area, which was consistent between the reactor scales. These results demonstrate that the trends observed with smaller (milligram to gram) catalyst reactors are applicable to larger, more industrially relevant (kg) scales to help guide catalyst research toward application.« less

Methane and hydrogen sulfide emissions in UASB reactors treating domestic wastewater.

PubMed

Souza, C L; Chernicharo, C A L; Melo, G C B

2012-01-01

The release of CH(4) and H(2)S in UASB reactors was evaluated with the aim to quantify the emissions from the liquid surfaces (three-phase separator and settler compartment) and also from the reactor's discharge hydraulic structures. The studies were carried out in two pilot- (360 L) and one demo-scale (14 m(3)) UASB reactors treating domestic wastewater. As expected, the release rates were much higher across the gas/liquid interfaces of the three-phase separators (5.4-9.7 kg CH(4) m(-2) d(-1) and 23.0-35.8 g S m(-2) d(-1)) as compared with the quiescent settler surfaces (11.0-17.8 g CH(4) m(-2) d(-1) and 0.21 to 0.37 g S m(-2) d(-1)). The decrease of dissolved methane and dissolved hydrogen sulfide was very large in the discharging hydraulic structures very close to the reactor (>60 and >80%, respectively), largely due to the loss to the atmosphere, indicating that the concentration of these compounds will probably fall to values close to zero in the near downstream structures. The emission factors due to the release of dissolved methane in the discharge structure amounted to around 0.040 g CH(4) g COD(infl)(-1) and 0.060 g CH(4) g COD(rem)(-1), representing around 60% of the methane collected in the three-phase separator.

Kinetics of gas phase formic acid decomposition on platinum single crystal and polycrystalline surfaces

NASA Astrophysics Data System (ADS)

Detwiler, Michael D.; Milligan, Cory A.; Zemlyanov, Dmitry Y.; Delgass, W. Nicholas; Ribeiro, Fabio H.

2016-06-01

Formic acid dehydrogenation turnover rates (TORs) were measured on Pt(111), Pt(100), and polycrystalline Pt foil surfaces at a total pressure of 800 Torr between 413 and 513 K in a batch reactor connected to an ultra-high vacuum (UHV) system. The TORs, apparent activation energies, and reaction orders are not sensitive to the structure of the Pt surface, within the precision of the measurements. CO introduced into the batch reactor depressed the formic acid dehydrogenation TOR and increased the reaction's apparent activation energies on Pt(111) and Pt(100), consistent with behavior predicted by the Temkin equation. Two reaction mechanisms were explored which explain the formic acid decomposition mechanism on Pt, both of which include dissociative adsorption of formic acid, rate limiting formate decomposition, and quasi-equilibrated hydrogen recombination and CO adsorption. No evidence was found that catalytic supports used in previous studies altered the reaction kinetics or mechanism.

Generating Breathable Air Through Dissociation of N2O

NASA Technical Reports Server (NTRS)

Zubrin, Robert; Frankie, Brian

2006-01-01

A nitrous oxide-based oxygen-supply system (NOBOSS) is an apparatus in which a breathable mixture comprising 2/3 volume parts of N2 and 1/3 volume part of O2 is generated through dissociation of N2O. The NOBOSS concept can be adapted to a variety of applications in which there are requirements for relatively compact, lightweight systems to supply breathable air. These could include air-supply systems for firefighters, divers, astronauts, and workers who must be protected against biological and chemical hazards. A NOBOSS stands in contrast to compressed-gas and cryogenic air-supply systems. Compressed-gas systems necessarily include massive tanks that can hold only relatively small amounts of gases. Alternatively, gases can be stored compactly in greater quantities and at low pressures when they are liquefied, but then cryogenic equipment is needed to maintain them in liquid form. Overcoming the disadvantages of both compressed-gas and cryogenic systems, the NOBOSS exploits the fact that N2O can be stored in liquid form at room temperature and moderate pressure. The mass of N2O that can be stored in a tank of a given mass is about 20 times the mass of compressed air that can be stored in a tank of equal mass. In a NOBOSS, N2O is exothermically dissociated to N2 and O2 in a main catalytic reactor. In order to ensure the dissociation of N2O to the maximum possible extent, the temperature of the reactor must be kept above 400 C. At the same time, to minimize concentrations of nitrogen oxides (which are toxic), it is necessary to keep the reactor temperature at or below 540 C. To keep the temperature within the required range throughout the reactor and, in particular, to prevent the formation of hot spots that would be generated by local concentrations of the exothermic dissociation reaction, the N2O is introduced into the reactor through an injector tube that features carefully spaced holes to distribute the input flow of N2O widely throughout the reactor. A NOBOSS includes one or more "destroyer" subsystems for removing any nitrogen oxides that remain downstream of the main N2O-dissociation reactor. A destroyer includes a carbon bed in series with a catalytic reactor, and is in thermal contact with the main N2O-dissociation reactor. The gas mixture that leaves the main reactor first goes through a carbon bed, which adsorbs all of the trace NO and most of the trace NO2. The gas mixture then goes through the destroyer catalytic reactor, wherein most or all of the remaining NO2 is dissociated. A NOBOSS can be designed to regulate its reactor temperature across a range of flow rates. One such system includes three destroyer loops; these loops act, in combination with a heat sink, to remove heat from the main N2O-dissociation reactor. In this system, the N2O and product gases play an additional role as coolants; thus, as needed, the coolant flow increases in proportion to the rate of generation of heat, helping to keep the main-reactor temperature below 540 C.

Bio-oil from fast pyrolysis of lignin: Effects of process and upgrading parameters.

PubMed

Fan, Liangliang; Zhang, Yaning; Liu, Shiyu; Zhou, Nan; Chen, Paul; Cheng, Yanling; Addy, Min; Lu, Qian; Omar, Muhammad Mubashar; Liu, Yuhuan; Wang, Yunpu; Dai, Leilei; Anderson, Erik; Peng, Peng; Lei, Hanwu; Ruan, Roger

2017-10-01

Effects of process parameters on the yield and chemical profile of bio-oil from fast pyrolysis of lignin and the processes for lignin-derived bio-oil upgrading were reviewed. Various process parameters including pyrolysis temperature, reactor types, lignin characteristics, residence time, and feeding rate were discussed and the optimal parameter conditions for improved bio-oil yield and quality were concluded. In terms of lignin-derived bio-oil upgrading, three routes including pretreatment of lignin, catalytic upgrading, and co-pyrolysis of hydrogen-rich materials have been investigated. Zeolite cracking and hydrodeoxygenation (HDO) treatment are two main methods for catalytic upgrading of lignin-derived bio-oil. Factors affecting zeolite activity and the main zeolite catalytic mechanisms for lignin conversion were analyzed. Noble metal-based catalysts and metal sulfide catalysts are normally used as the HDO catalysts and the conversion mechanisms associated with a series of reactions have been proposed. Copyright © 2017 Elsevier Ltd. All rights reserved.

Fabrication and testing of low-temperature catalytically active washcoat materials for next-generation vehicle catalytic converters.

DOT National Transportation Integrated Search

2014-01-01

With funds from this grant, Youngstown State University has purchased a : Quantachrome iQ Chemisorption Analyzer and built a Chemical Reactor with Gas : Chromatographer for catalyst characterization. PI has been involved in the purchase and : install...

In-situ upgrading of biomass pyrolysis vapors: catalyst screening on a fixed bed reactor.

PubMed

Stefanidis, S D; Kalogiannis, K G; Iliopoulou, E F; Lappas, A A; Pilavachi, P A

2011-09-01

In-situ catalytic upgrading of biomass fast pyrolysis vapors was performed in a fixed bed bench-scale reactor at 500°C, for catalyst screening purposes. The catalytic materials tested include a commercial equilibrium FCC catalyst (E-cat), various commercial ZSM-5 formulations, magnesium oxide and alumina materials with varying specific surface areas, nickel monoxide, zirconia/titania, tetragonal zirconia, titania and silica alumina. The bio-oil was characterized measuring its water content, the carbon-hydrogen-oxygen (by difference) content and the chemical composition of its organic fraction. Each catalytic material displayed different catalytic effects. High surface area alumina catalysts displayed the highest selectivity towards hydrocarbons, yielding however low organic liquid products. Zirconia/titania exhibited good selectivity towards desired compounds, yielding higher organic liquid product than the alumina catalysts. The ZSM-5 formulation with the highest surface area displayed the most balanced performance having a moderate selectivity towards hydrocarbons, reducing undesirable compounds and producing organic liquid products at acceptable yields. Copyright © 2011 Elsevier Ltd. All rights reserved.

Vanadium and tungsten release from V-based selective catalytic reduction diesel aftertreatment

NASA Astrophysics Data System (ADS)

Liu, Z. Gerald; Ottinger, Nathan A.; Cremeens, Christopher M.

2015-03-01

Vanadium-based selective catalytic reduction (V-SCR) catalysts are currently used for the reduction of nitrogen oxides (NOx) in worldwide diesel applications including Euro IV, V, and VI as well as U.S. nonroad Tier 4 Final. Although V-SCR catalysts are attractive because of their high NOx conversion, low cost, resistance to sulfur poisoning, and ability to reduce hydrocarbon emissions, there is concern that V-SCR washcoat material (e.g., vanadium and tungsten) and its derivatives may be released into the atmosphere, potentially harming human health and the environment. In this study, vanadium and tungsten release measurements are made with both a reactor- and engine-based approach in order to determine the potential release of these metals from diesel exhaust aftertreatment systems that contain a V-SCR catalyst. Results for a commercially available V-SCR reveal that both V and W release begin at 500 °C, and both reactor- and engine-based methods are capable of measuring qualitatively similar release. Emissions with the engine-based method are higher at all temperatures evaluated, likely due to this method's ability to capture particle-phase and vapor-phase emissions which become particle-bound after their evolution from the catalyst surface. Certification relevant data (NRTC and NRSC) from a nonroad engine is used to understand probable emissions from V-SCR aftertreatment architectures. Finally, results from a V-SCR catalyst formulated for improved thermal durability illustrate that it is possible to increase the maximum temperature for V-SCR catalysts. This comprehensive understanding of the temperature dependence of vanadium and tungsten volatility can be used to further analyze the full impact of diesel aftertreatment on exhaust emissions and their impact on human health and environmental toxicity.

Novel Anaerobic Wastewater Treatment System for Energy Generation at Forward Operating Bases

DTIC Science & Technology

2016-08-01

AnMBR) technology with clinoptilolite ion exchange and GreenBox™ ammonia electrolysis. The system generates both methane and hydrogen fuels...experimental setup. ................................................ 21 Figure 10. Methane phase semi batch experimental setup, a total of three reactors were...set up for PS + solid, Bioc and ADS methane phase reactors. .................... 21 Figure 11. Dried PS solid for the control, Bioc blend for the

Phased Development of Accident Tolerant Fue

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bragg-Sitton, Shannon M.; Carmack, W. Jon

2016-09-01

The United States Department of Energy (U.S. DOE) Advanced Fuels Campaign (AFC) has adopted a three-phase approach for the development and eventual commercialization of enhanced, accident tolerant fuel (ATF) for light water reactors (LWRs). Extending from 2012 to 2016, AFC is currently coming to the end of Phase 1 research that has entailed Feasibility Assessment and Prioritization for a large number of proposed fuel systems (fuel and cladding) that could provide improved performance under accident conditions. Phase 1 activities will culminate with a prioritization of concepts for both near-term and long-term development based on the available experimental data and modelingmore » predictions. This process will provide guidance to DOE on what concepts should be prioritized for investment in Phase 2 Development/Qualification activities based on technical performance improvements and probability of meeting the aggressive schedule to insert a lead fuel rod (LFR) in a commercial power reactor by 2022. While Phase 1 activities include small-scale fabrication work, materials characterization, and limited irradiation of samples, Phase 2 will require development teams to expand to industrial fabrication methods, conduct irradiation tests under more prototypic reactor conditions (i.e. in contact with reactor primary coolant at LWR conditions and in-pile transient testing), conduct additional characterization and post-irradiation examination, and develop a fuel performance code for the candidate ATF. Phase 2 will culminate in the insertion of an LFR (or lead fuel assembly) in a commercial power reactor. The Phase 3 Commercialization work will extend past 2022. Following post-irradiation examination of LFRs, partial-core reloads will be demonstrated. The commercialization phase will further entail the establishment of commercial fabrication capabilities and the transition of LWR cores to the new fuel. The three development phases described roughly correspond to the technology readiness levels (TRL) defined for nuclear fuel development. TRL 1–3 corresponds to the “proof-of-concept” stage (Phase 1), TRL 4–6 to “proof-of-principle” (Phase 2), and TRL 7–9 to “proof-of-performance” (Phase 3). This paper will provide an overview of the anticipated activities within each phase of development and will provide an update on the current ATF development status.« less

A new three-phase heterocrystal catalysts and their superior treatment efficiency for tetracycline

NASA Astrophysics Data System (ADS)

Wang, Feng-Rui; Sun, Hui-Ping; Wang, Yan; Liu, Jin-Ku; Fang, Yi; Wang, Jian-Dong

An easy recyclable and interesting Ag3PO4@Pt@TiO2 (APTP) three-phase heterocrystal chains were self-assembled by the cohesive action and chemical construction of polyvinylpyrrolidone (PVP). We found that a new electron-hole transmission path has been built via the rematch of the band structure of Ag3PO4, Pt and TiO2 which extends the light absorption and promoted the electron-hole separation to treat the antibiotic residues in the water. Based on the thorough investigations, a new catalytic material was provided for antibiotics degradation. The catalytic activity of APTP toward the degradation of tetracycline solution was enhanced by 166.67% and the stability increased remarkably compared with pure Ag3PO4 through the integration of different functional components.

Removal of hazardous gaseous pollutants from industrial flue gases by a novel multi-stage fluidized bed desulfurizer.

PubMed

Mohanty, C R; Adapala, Sivaji; Meikap, B C

2009-06-15

Sulfur dioxide and other sulfur compounds are generated as primary pollutants from the major industries such as sulfuric acid plants, cupper smelters, catalytic cracking units, etc. and cause acid rain. To remove the SO(2) from waste flue gas a three-stage counter-current multi-stage fluidized bed adsorber was developed as desulfurization equipment and operated in continuous bubbling fluidization regime for the two-phase system. This paper represents the desulfurization of gas mixtures by chemical sorption of sulfur dioxide on porous granular calcium oxide particles in the reactor at ambient temperature. The advantages of the multi-stage fluidized bed reactor are of high mass transfer and high gas-solid residence time that can enhance the removal of acid gas at low temperature by dry method. Experiments were carried out in the bubbling fluidization regime supported by visual observation. The effects of the operating parameters such as sorbent (lime) flow rate, superficial gas velocity, and the weir height on SO(2) removal efficiency in the multistage fluidized bed are reported. The results have indicated that the removal efficiency of the sulfur dioxide was found to be 65% at high solid flow rate (2.0 kg/h) corresponding to lower gas velocity (0.265 m/s), wier height of 70 mm and SO(2) concentration of 500 ppm at room temperature.

Sludge settling processes in SBR-related sewage treatment plants according to the Biocos method.

PubMed

Meusel, S; Englert, R

2004-01-01

This paper describes the investigations in a sedimentation and circulation reactor (SU-reactor) of a three-phase Biocos plant. The aim of these investigations was the determination of the temporal and depth-dependent distribution of suspended solid contents, as well as describing the sludge sedimentation curves. The calculated results reveal peculiarities of the Biocos method with regard to sedimentation processes. In the hydraulically uninterrupted (pre-)settling phase, a sludge level depth was observed, which remained constant over the reactor surface and increased linearly according to the sludge volume. The settling and the thickening processes of this phase corresponded to a large extent to the well-known settling test in a one-litre measuring cylinder. During the discharge phase, the investigated settling rate was overlaid by the surface loading rate and the sludge level changed depending on the difference between those two parameters. The solid distribution of the A-phase indicated a formation of functional zones, which were influenced by the surface loading. The formation was comparable to the formation of layers in secondary settling tanks with vertical flow. The concentration equalisation between the biological reactor and the SU-reactor proved to be problematic during the circulation phase, because a type of internal sludge circulation occurred in the SU-reactor. A permanent sludge recirculation seems to be highly recommendable.

Catalytic Tar Reduction for Assistance in Thermal Conversion of Space Waste for Energy Production

NASA Technical Reports Server (NTRS)

Caraccio, Anne Joan; Devor, Robert William; Hintze, Paul E.; Muscatello, Anthony C.; Nur, Mononita

2014-01-01

The Trash to Gas (TtG) project investigates technologies for converting waste generated during spaceflight into various resources. One of these technologies was gasification, which employed a downdraft reactor designed and manufactured at NASA's Kennedy Space Center (KSC) for the conversion of simulated space trash to carbon dioxide. The carbon dioxide would then be converted to methane for propulsion and water for life support systems. A minor byproduct of gasification includes large hydrocarbons, also known as tars. Tars are unwanted byproducts that add contamination to the product stream, clog the reactor and cause complications in analysis instrumentation. The objective of this research was to perform reduction studies of a mock tar using select catalysts and choose the most effective for primary treatment within the KSC downdraft gasification reactor. Because the KSC reactor is operated at temperatures below typical gasification reactors, this study evaluates catalyst performance below recommended catalytic operating temperatures. The tar reduction experimentation was observed by passing a model tar vapor stream over the catalysts at similar conditions to that of the KSC reactor. Reduction in tar was determined using gas chromatography. Tar reduction efficiency and catalyst performances were evaluated at different temperatures.

Catalytic conversion of light alkanes. Final report, January 1, 1990--October 31, 1994

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

During the course of the first three years of the Cooperative Agreement (Phase I-III), we uncovered a family of metal perhaloporphyrin complexes which had unprecedented activity for the selective air-oxidation of fight alkanes to alcohols. The reactivity of fight hydrocarbon substrates with air or oxygen was in the order: isobutane>propane>ethane>methane, in accord with their homolytic bond dissociation energies. Isobutane was so reactive that the proof-of concept stage of a process for producing tert-butyl alcohol from isobutane was begun (Phase V). It was proposed that as more active catalytic systems were developed (Phases IV, VI), propane, then ethane and finally methanemore » oxidations will move into this stage (Phases VII through IX). As of this writing, however, the program has been terminated during the later stages of Phases V and VI so that further work is not anticipated. We made excellent progress during 1994 in generating a class of less costly new materials which have the potential for high catalytic activity. New routes were developed for replacing costly perfluorophenyl groups in the meso-position of metalloporphyrin catalysts with far less expensive and lower molecular weight perfluoromethyl groups.« less

Reactor for nano-focused x-ray diffraction and imaging under catalytic in situ conditions

NASA Astrophysics Data System (ADS)

Richard, M.-I.; Fernández, S.; Hofmann, J. P.; Gao, L.; Chahine, G. A.; Leake, S. J.; Djazouli, H.; De Bortoli, Y.; Petit, L.; Boesecke, P.; Labat, S.; Hensen, E. J. M.; Thomas, O.; Schülli, T.

2017-09-01

A reactor cell for in situ studies of individual catalyst nanoparticles or surfaces by nano-focused (coherent) x-ray diffraction has been developed. Catalytic reactions can be studied in flow mode in a pressure range of 10-2-103 mbar and temperatures up to 900 °C. This instrument bridges the pressure and materials gap at the same time within one experimental setup. It allows us to probe in situ the structure (e.g., shape, size, strain, faceting, composition, and defects) of individual nanoparticles using a nano-focused x-ray beam. Here, the setup was used to observe strain and facet evolution of individual model Pt catalysts during in situ experiments. It can be used for heating other (non-catalytically active) nanoparticles (e.g., nanowires) in inert or reactive gas atmospheres or vacuum as well.

Reactor for nano-focused x-ray diffraction and imaging under catalytic in situ conditions.

PubMed

Richard, M-I; Fernández, S; Hofmann, J P; Gao, L; Chahine, G A; Leake, S J; Djazouli, H; De Bortoli, Y; Petit, L; Boesecke, P; Labat, S; Hensen, E J M; Thomas, O; Schülli, T

2017-09-01

A reactor cell for in situ studies of individual catalyst nanoparticles or surfaces by nano-focused (coherent) x-ray diffraction has been developed. Catalytic reactions can be studied in flow mode in a pressure range of 10 -2 -10 3 mbar and temperatures up to 900 °C. This instrument bridges the pressure and materials gap at the same time within one experimental setup. It allows us to probe in situ the structure (e.g., shape, size, strain, faceting, composition, and defects) of individual nanoparticles using a nano-focused x-ray beam. Here, the setup was used to observe strain and facet evolution of individual model Pt catalysts during in situ experiments. It can be used for heating other (non-catalytically active) nanoparticles (e.g., nanowires) in inert or reactive gas atmospheres or vacuum as well.

Catalytic thermal cracking of postconsumer waste plastics to fuels. 2. Pilot-scale thermochemical conversion

USDA-ARS?s Scientific Manuscript database

Synthetic gasoline and diesel fuels were prepared via catalytic and noncatalytic pyrolysis of waste polyethylene and polypropylene plastics followed by distillation of plastic crude oils. Reaction conditions optimized using a 2 L batch reactor were applied to pilot-scale production of plastic crude ...

40 CFR 63.1567 - What are my requirements for inorganic HAP emissions from catalytic reforming units?

Code of Federal Regulations, 2013 CFR

2013-07-01

... different reactors in the catalytic reforming unit are regenerated in separate regeneration systems, then these emission limitations apply to each separate regeneration system. These emission limitations apply... catalyst rejuvenation operations during coke burn-off and catalyst regeneration. You can choose from the...

40 CFR 63.1567 - What are my requirements for inorganic HAP emissions from catalytic reforming units?

Code of Federal Regulations, 2012 CFR

2012-07-01

... different reactors in the catalytic reforming unit are regenerated in separate regeneration systems, then these emission limitations apply to each separate regeneration system. These emission limitations apply... catalyst rejuvenation operations during coke burn-off and catalyst regeneration. You can choose from the...

40 CFR 63.1567 - What are my requirements for inorganic HAP emissions from catalytic reforming units?

Code of Federal Regulations, 2014 CFR

2014-07-01

... different reactors in the catalytic reforming unit are regenerated in separate regeneration systems, then these emission limitations apply to each separate regeneration system. These emission limitations apply... catalyst rejuvenation operations during coke burn-off and catalyst regeneration. You can choose from the...

Influence of a three-phase separator configuration on the performance of an upflow anaerobic sludge bed reactor treating wastewater from a fruit-canning factory.

PubMed

Wongnoi, Rachbordin; Songkasiri, Warinthorn; Phalakornkule, Chantaraporn

2007-02-01

The objective of this study was to investigate the influence of a three-phase separator configuration on the performance of an upflow anaerobic sludge bed (USAB) treating wastewater from a fruit canning factory. The performances of two 30-L UASB reactors--one with a modified three-phase separator giving a spiral flow pattern and the other with a conventional configuration-were investigated in parallel. Wastewater, with a chemical oxygen demand (COD) concentration between 2000 and 7000 mg/L, was obtained from a fruit-canning factory. Based on the effluent data of the first 100 operation days, the UASB with the three-phase separator giving spiral flow patterns yielded up to 25% lower biomass washout. It also showed better efficiencies in treating wastewater--up to 60% lower effluent COD, up to 20% higher COD percent removal, and up to 29% higher biogas production. This work presents evidence of an improvement on the conventional physical design of a UASB.

Study on bubbly flow behavior in natural circulation reactor by thermal-hydraulic simulation tests with SF6-Gas and ethanol liquid

NASA Astrophysics Data System (ADS)

Kondo, Yoshiyuki; Suga, Keishi; Hibi, Koki; Okazaki, Toshihiko; Komeno, Toshihiro; Kunugi, Tomoaki; Serizawa, Akimi; Yoneda, Kimitoshi; Arai, Takahiro

2009-02-01

An advanced experimental technique has been developed to simulate two-phase flow behavior in a light water reactor (LWR). The technique applies three kinds of methods; (1) use of sulfur-hexafluoride (SF6) gas and ethanol (C2H5OH) liquid at atmospheric temperature and a pressure less than 1.0MPa, where the fluid properties are similar to steam-water ones in the LWR, (2) generation of bubble with a sintering tube, which simulates bubble generation on heated surface in the LWR, (3) measurement of detailed bubble distribution data with a bi-optical probe (BOP), (4) and measurement of liquid velocities with the tracer liquid. This experimental technique provides easy visualization of flows by using a large scale experimental apparatus, which gives three-dimensional flows, and measurement of detailed spatial distributions of two-phase flow. With this technique, we have carried out experiments simulating two-phase flow behavior in a single-channel geometry, a multi-rod-bundle one, and a horizontal-tube-bundle one on a typical natural circulation reactor system. Those experiments have clarified a) a flow regime map in a rod bundle on the transient region between bubbly and churn flow, b) three-dimensional flow behaviour in rod-bundles where inter-subassembly cross-flow occurs, c) bubble-separation behavior with consideration of reactor internal structures. The data have given analysis models for the natural circulation reactor design with good extrapolation.

Plasma generators, reactor systems and related methods

DOEpatents

Kong, Peter C [Idaho Falls, ID; Pink, Robert J [Pocatello, ID; Lee, James E [Idaho Falls, ID

2007-06-19

A plasma generator, reactor and associated systems and methods are provided in accordance with the present invention. A plasma reactor may include multiple sections or modules which are removably coupled together to form a chamber. Associated with each section is an electrode set including three electrodes with each electrode being coupled to a single phase of a three-phase alternating current (AC) power supply. The electrodes are disposed about a longitudinal centerline of the chamber and are arranged to provide and extended arc and generate an extended body of plasma. The electrodes are displaceable relative to the longitudinal centerline of the chamber. A control system may be utilized so as to automatically displace the electrodes and define an electrode gap responsive to measure voltage or current levels of the associated power supply.

Photocatalytic oxidation of tabun simulant-diethyl cyanophosphate: FTIR in situ investigation.

PubMed

Kolinko, P A; Kozlov, D V

2008-06-15

Gas phase photocatalytic oxidation of diethyl cyanophosphate vapor in a static reactor using TiO2 and modified TiO2 as the photocatalyst was studied with the FTIR in situ method. The transition metals Pt, Au, and Ag were used for TiO2 modification by the chemical and photochemical deposition methods as well as the mechanical mixture of TiO2 with manganese oxide to improve its adsorption and catalytic activity. Photocatalytic oxidation of diethyl cyanophosphate in a static reactor results in its complete mineralization with carbon dioxide, phosphoric and nitric acids, and water as the major final products. HCN was demonstrated to be the only toxic gaseous intermediate of diethyl cyanophosphate photocatalytic oxidation, formed as a result of diethyl cyanophosphate hydrolysis. Diethylphosphate and acetic and formic acids were registered as the surface intermediates. It was found that cyanhydric acid is oxidized slowly with the use of unmodified TiO2. The formation of surface cyanide complexes with Ag and Au ions could be responsible for the fast removal of HCN from the gas phase and its further photooxidation in the case of using TiO2 with deposited Au and Ag.

Gas phase heterogeneous catalytic oxidation of alkanes to aliphatic ketones and/or other oxygenates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Manhua; Wang, Xiang; Yeom, Younghoon

A catalyst, its method of preparation and its use for producing aliphatic ketones by subjecting alkanes C.sub.3 to C.sub.9 to a gas phase catalytic oxidation in the presence of air or oxygen, and, optionally, steam and/or one or more diluting gases. The catalyst comprises a catalytically active mixed metal oxide phase and a suitable support material onto and/or into which the active catalytic phase id dispersed.

Gas phase heterogeneous catalytic oxidation of alkanes to aliphatic ketones and/or other oxygenates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Manhua; Wang, Xiang; Yeom, Younghoon

A catalyst, its method of preparation and its use for producing aliphatic ketones by subjecting alkanes C.sub.3 to C.sub.9 to a gas phase catalytic oxidation in the presence of air or oxygen, and, optionally, steam and/or one or more diluting gases. The catalyst comprises a catalytically active mixed metal oxide phase and a suitable support material onto and/or into which the active catalytic phase is dispersed.

40 CFR 63.1567 - What are my requirements for inorganic HAP emissions from catalytic reforming units?

Code of Federal Regulations, 2011 CFR

2011-07-01

... reactors in the catalytic reforming unit are regenerated in separate regeneration systems, then these emission limitations apply to each separate regeneration system. These emission limitations apply to... rejuvenation operations during coke burn-off and catalyst regeneration. You can choose from the two options in...

Learning the Fundamentals of Kinetics and Reaction Engineering with the Catalytic Oxidation of Methane

ERIC Educational Resources Information Center

Cybulskis, Viktor J.; Smeltz, Andrew D.; Zvinevich, Yury; Gounder, Rajamani; Delgass, W. Nicholas; Ribeiro, Fabio H.

2016-01-01

Understanding catalytic chemistry, collecting and interpreting kinetic data, and operating chemical reactors are critical skills for chemical engineers. This laboratory experiment provides students with a hands-on supplement to a course in chemical kinetics and reaction engineering. The oxidation of methane with a palladium catalyst supported on…

APPARATUS FOR CATALYTICALLY COMBINING GASES

DOEpatents

Busey, H.M.

1958-08-12

A convection type recombiner is described for catalytically recombining hydrogen and oxygen which have been radiolytically decomposed in an aqueous homogeneous nuclear reactor. The device is so designed that the energy of recombination is used to circulate the gas mixture over the catalyst. The device consists of a vertical cylinder having baffles at its lower enda above these coarse screens having platinum and alumina pellets cemented thereon, and an annular passage for the return of recombined, condensed water to the reactor moderator system. This devicea having no moving parts, provides a simple and efficient means of removing the danger of accumulated hot radioactive, explosive gases, and restoring them to the moderator system for reuse.

Data and Summaries for Catalytic Destruction of a Surrogate Organic Hazardous Air Pollutant as a Potential Co-benefit for Coal-Fired Selective Catalytic Reduction Systems

EPA Pesticide Factsheets

Table 1 summarizes and explanis the Operating Conditions of the SCR Reactor used in the Benzene-Destruction.Table 2 summarizes and explains the Experimental Design and Test Results.Table 3 summarizes and explains the Estimates for Individual Effects and Cross Effects Obtained from the Linear Regression Models for Destruction of C6H6 and Reduction of NO.Fig. 1 shows the Down-flow SCR reactor system in detail.Fig. 2 shows the graphical summary of the Effect of the inlet C6H6 concentration to the SCR reactor on the destruction of C6H6.Fig.3 shows the summary of Carbon mass balance for C6H6 destruction promoted by the V2O5-WO3/TiO2 catalyst.This dataset is associated with the following publication:Lee , C., Y. Zhao, S. Lu, and W.R. Stevens. Catalytic Destruction of a Surrogate Organic Hazardous Air Polutant as a Potential Co-benefit for Coal-fired Selective Catalyst Reduction Systems. AMERICAN CHEMICAL SOCIETY. American Chemical Society, Washington, DC, USA, 30(3): 2240-2247, (2016).

[Studies on photo-electron-chemical catalytic degradation of the malachite green].

PubMed

Li, Ming-yu; Diao, Zeng-hui; Song, Lin; Wang, Xin-le; Zhang, Yuan-ming

2010-07-01

A novel two-compartment photo-electro-chemical catalytic reactor was designed. The TiO2/Ti thin film electrode thermally formed was used as photo-anode, and graphite as cathode and a saturated calomel electrode (SCE) as the reference electrode in the reactor. The anode compartment and cathode compartment were connected with the ionic exchange membrane in this reactor. Effects of initial pH, initial concentration of malachite green and connective modes between the anode compartment and cathode compartment on the decolorization efficiency of malachite green were investigated. The degradation dynamics of malachite green was studied. Based on the change of UV-visible light spectrum, the degradation process of malachite green was discussed. The experimental results showed that, during the time of 120 min, the decolouring ratio of the malachite green was 97.7% when initial concentration of malachite green is 30 mg x L(-1) and initial pH is 3.0. The catalytic degradation of malachite green was a pseudo-first order reaction. In the degradation process of malachite green the azo bond cleavage and the conjugated system of malachite green were attacked by hydroxyl radical. Simultaneity, the aromatic ring was oxidized. Finally, malachite green was degraded into other small molecular compounds.

Conceptual design and issues of the laser inertial fusion test (LIFT) reactor—targets and chamber systems

NASA Astrophysics Data System (ADS)

Norimatsu, T.; Kozaki, Y.; Shiraga, H.; Fujita, H.; Okano, K.; Members of LIFT Design Team

2017-11-01

We present the conceptual design of an experimental laser fusion plant known as the laser inertial fusion test (LIFT) reactor. The conceptual design aims at technically connecting a single-shot experiment and a commercial power plant. The LIFT reactor is designed on a three-phase scheme, where each phase has specific goals and the dedicated chambers of each phase are driven by the same laser. Technical issues related to the chamber technology including radiation safety to repeat burst mode operation are discussed in this paper.

Influence of Alumina Binder Content on Catalytic Performance of Ni/HZSM-5 for Hydrodeoxygenation of Cyclohexanone

PubMed Central

Kong, Xiangjin; Liu, Junhai

2014-01-01

The influence of the amount of alumina binders on the catalytic performance of Ni/HZSM-5 for hydrodeoxygenation of cyclohexanone was investigated in a fixed-bed reactor. N2 sorption, X-ray diffraction, H2-chemisorption and temperature-programmed desorption of ammonia were used to characterize the catalysts. It can be observed that the Ni/HZSM-5 catalyst bound with 30 wt.% alumina binder exhibited the best catalytic performance. The high catalytic performance may be due to relatively good Ni metal dispersion, moderate mesoporosity, and proper acidity of the catalyst. PMID:25009974

Influence of alumina binder content on catalytic performance of Ni/HZSM-5 for hydrodeoxygenation of cyclohexanone.

PubMed

Kong, Xiangjin; Liu, Junhai

2014-01-01

The influence of the amount of alumina binders on the catalytic performance of Ni/HZSM-5 for hydrodeoxygenation of cyclohexanone was investigated in a fixed-bed reactor. N2 sorption, X-ray diffraction, H2-chemisorption and temperature-programmed desorption of ammonia were used to characterize the catalysts. It can be observed that the Ni/HZSM-5 catalyst bound with 30 wt.% alumina binder exhibited the best catalytic performance. The high catalytic performance may be due to relatively good Ni metal dispersion, moderate mesoporosity, and proper acidity of the catalyst.

Comparison of the performance of MBBR and SBR systems for the treatment of anaerobic reactor biowaste effluent.

PubMed

Comett-Ambriz, I; Gonzalez-Martinez, S; Wilderer, P

2003-01-01

Anaerobic reactor biowaste effluent was treated with biofilm and activated sludge sequencing batch reactors to compare the performance of both systems. The treatment targets were organic carbon removal and nitrification. The pilot plant was operated in two phases. During the first phase, it was operated like a Moving Bed Biofilm Reactor (MBBR) with the Natrix media, with a specific surface area of 210 m2/m3. The MBBR was operated under Sequencing Batch Reactor (SBR) modality with three 8-hour cycles per day over 70 days. During the second phase of the experiment, the pilot plant was operated over 79 days as a SBR. In both phases the influent was fed to the reactor at a flow rate corresponding to a Hydraulic Retention Time (HRT) of 4 days. Both systems presented a good carbon removal for this specific wastewater. The Chemical Oxygen Demand (COD) total removal was 53% for MBBR and 55% for SBR. MBBR offered a higher dissolved COD removal (40%) than SBR (30%). The limited COD removal achieved is in agreement with the high COD to BOD5 ratio (1/3) of the influent wastewater. In both systems a complete nitrification was obtained. The different efficiencies in both systems are related to the different biomass concentrations.

CATALYTIC OXIDATION OF METHANE AT LOW SPACE VELOCITIES.

DTIC Science & Technology

methane in airstream through an inhouse designed and fabricated stainless steel reactor. The reactor contained either Hopcalite , 5% V2O5 - 5% MoO3 on...plotted for each catalyst flow rate combination and the effect of space velocity on conversion at constant temperature is shown for the Hopcalite and

TRICHLOROETHYLENE SORPTION AND OXIDATION USING A DUAL FUNCTION SORBENT/CATALYST IN A FALLING FURNACE REACTOR

EPA Science Inventory

A dual function medium (Cr-ZSM-5), capable of physisorbing trichloroethylene (TCE) at ambient temperature and catalytically oxidizing it at elevated temperature (-350 degrees C) was utilized in a novel continuous falling furnace reactor system to store and periodically destroy t...

Ex situ themo-catalytic upgrading of biomass pyrolysis vapors using a traveling wave microwave reactor

USDA-ARS?s Scientific Manuscript database

Microwave heating offers a number of advantages over conventional heating methods, such as, rapid and volumetric heating, precise temperature control, energy efficiency and lower temperature gradient. In this article we demonstrate the use of 2450 MHz microwave traveling wave reactor to heat the cat...

STUDY OF MERCURY OXIDATION BY SCR CATALYST IN AN ENTRAINED-FLOW REACTOR UNDER SIMULATED PRB CONDITIONS

EPA Science Inventory

A bench-scale entrained-flow reactor system was constructed for studying elemental mercury oxidation under selective catalytic reduction (SCR) reaction conditions. Simulated flue gas was doped with fly ash collected from a subbituminous Powder River Basin (PRB) coal-fired boiler ...

Development of toroid-type HTS DC reactor series for HVDC system

NASA Astrophysics Data System (ADS)

Kim, Kwangmin; Go, Byeong-Soo; Park, Hea-chul; Kim, Sung-kyu; Kim, Seokho; Lee, Sangjin; Oh, Yunsang; Park, Minwon; Yu, In-Keun

2015-11-01

This paper describes design specifications and performance of a toroid-type high-temperature superconducting (HTS) DC reactor. The first phase operation targets of the HTS DC reactor were 400 mH and 400 A. The authors have developed a real HTS DC reactor system during the last three years. The HTS DC reactor was designed using 2G GdBCO HTS wires. The HTS coils of the toroid-type DC reactor magnet were made in the form of a D-shape. The electromagnetic performance of the toroid-type HTS DC reactor magnet was analyzed using the finite element method program. A conduction cooling method was adopted for reactor magnet cooling. The total system has been successfully developed and tested in connection with LCC type HVDC system. Now, the authors are studying a 400 mH, kA class toroid-type HTS DC reactor for the next phase research. The 1500 A class DC reactor system was designed using layered 13 mm GdBCO 2G HTS wire. The expected operating temperature is under 30 K. These fundamental data obtained through both works will usefully be applied to design a real toroid-type HTS DC reactor for grid application.

Systems including catalysts in porous zeolite materials within a reactor for use in synthesizing hydrocarbons

DOEpatents

Rolllins, Harry W [Idaho Falls, ID; Petkovic, Lucia M [Idaho Falls, ID; Ginosar, Daniel M [Idaho Falls, ID

2012-07-24

Catalytic structures include a catalytic material disposed within a zeolite material. The catalytic material may be capable of catalyzing a formation of methanol from carbon monoxide and/or carbon dioxide, and the zeolite material may be capable of catalyzing a formation of hydrocarbon molecules from methanol. The catalytic material may include copper and zinc oxide. The zeolite material may include a first plurality of pores substantially defined by a crystal structure of the zeolite material and a second plurality of pores dispersed throughout the zeolite material. Systems for synthesizing hydrocarbon molecules also include catalytic structures. Methods for synthesizing hydrocarbon molecules include contacting hydrogen and at least one of carbon monoxide and carbon dioxide with such catalytic structures. Catalytic structures are fabricated by forming a zeolite material at least partially around a template structure, removing the template structure, and introducing a catalytic material into the zeolite material.

Hydrogen from catalytic reforming of biomass-derived hydrocarbons in liquid water

NASA Astrophysics Data System (ADS)

Cortright, R. D.; Davda, R. R.; Dumesic, J. A.

2002-08-01

Concerns about the depletion of fossil fuel reserves and the pollution caused by continuously increasing energy demands make hydrogen an attractive alternative energy source. Hydrogen is currently derived from nonrenewable natural gas and petroleum, but could in principle be generated from renewable resources such as biomass or water. However, efficient hydrogen production from water remains difficult and technologies for generating hydrogen from biomass, such as enzymatic decomposition of sugars, steam-reforming of bio-oils and gasification, suffer from low hydrogen production rates and/or complex processing requirements. Here we demonstrate that hydrogen can be produced from sugars and alcohols at temperatures near 500K in a single-reactor aqueous-phase reforming process using a platinum-based catalyst. We are able to convert glucose-which makes up the major energy reserves in plants and animals-to hydrogen and gaseous alkanes, with hydrogen constituting 50% of the products. We find that the selectivity for hydrogen production increases when we use molecules that are more reduced than sugars, with ethylene glycol and methanol being almost completely converted into hydrogen and carbon dioxide. These findings suggest that catalytic aqueous-phase reforming might prove useful for the generation of hydrogen-rich fuel gas from carbohydrates extracted from renewable biomass and biomass waste streams.

Hydrogen from catalytic reforming of biomass-derived hydrocarbons in liquid water.

PubMed

Cortright, R D; Davda, R R; Dumesic, J A

2002-08-29

Concerns about the depletion of fossil fuel reserves and the pollution caused by continuously increasing energy demands make hydrogen an attractive alternative energy source. Hydrogen is currently derived from nonrenewable natural gas and petroleum, but could in principle be generated from renewable resources such as biomass or water. However, efficient hydrogen production from water remains difficult and technologies for generating hydrogen from biomass, such as enzymatic decomposition of sugars, steam-reforming of bio-oils and gasification, suffer from low hydrogen production rates and/or complex processing requirements. Here we demonstrate that hydrogen can be produced from sugars and alcohols at temperatures near 500 K in a single-reactor aqueous-phase reforming process using a platinum-based catalyst. We are able to convert glucose -- which makes up the major energy reserves in plants and animals -- to hydrogen and gaseous alkanes, with hydrogen constituting 50% of the products. We find that the selectivity for hydrogen production increases when we use molecules that are more reduced than sugars, with ethylene glycol and methanol being almost completely converted into hydrogen and carbon dioxide. These findings suggest that catalytic aqueous-phase reforming might prove useful for the generation of hydrogen-rich fuel gas from carbohydrates extracted from renewable biomass and biomass waste streams.

Nanodispersed Suspensions of Zeolite Catalysts for Converting Dimethyl Ether into Olefins

NASA Astrophysics Data System (ADS)

Kolesnichenko, N. V.; Yashina, O. V.; Ezhova, N. N.; Bondarenko, G. N.; Khadzhiev, S. N.

2018-01-01

Nanodispersed suspensions that are effective in DME conversion and stable in the reaction zone in a three-phase system (slurry reactor) are obtained from MFI zeolite commercial samples (TsVM, IK-17-1, and CBV) in liquid media via ultrasonic treatment (UST). It is found that the dispersion medium, in which ultrasound affects zeolite commercial sample, has a large influence on particle size in the suspension. UST in the aqueous medium produces zeolite nanoparticles smaller than 50 nm, while larger particles of MFI zeolite samples form in silicone or hydrocarbon oils. Spectral and adsorption data show that when zeolites undergo UST in an aqueous medium, the acid sites are redistributed on the zeolite surface and the specific surface area of the mesopores increases. Preliminary UST in aqueous media of zeolite commercial samples (TsVM, IK-17-1, and CBV) affects the catalytic properties of MFI zeolite nanodispersed suspensions. The selectivity of samples when paraffins and olefins form is largely due to superacid sites consisting of OH groups of hydroxonium ion H3O+.

Fuel processing in integrated micro-structured heat-exchanger reactors

NASA Astrophysics Data System (ADS)

Kolb, G.; Schürer, J.; Tiemann, D.; Wichert, M.; Zapf, R.; Hessel, V.; Löwe, H.

Micro-structured fuel processors are under development at IMM for different fuels such as methanol, ethanol, propane/butane (LPG), gasoline and diesel. The target application are mobile, portable and small scale stationary auxiliary power units (APU) based upon fuel cell technology. The key feature of the systems is an integrated plate heat-exchanger technology which allows for the thermal integration of several functions in a single device. Steam reforming may be coupled with catalytic combustion in separate flow paths of a heat-exchanger. Reactors and complete fuel processors are tested up to the size range of 5 kW power output of a corresponding fuel cell. On top of reactor and system prototyping and testing, catalyst coatings are under development at IMM for numerous reactions such as steam reforming of LPG, ethanol and methanol, catalytic combustion of LPG and methanol, and for CO clean-up reactions, namely water-gas shift, methanation and the preferential oxidation of carbon monoxide. These catalysts are investigated in specially developed testing reactors. In selected cases 1000 h stability testing is performed on catalyst coatings at weight hourly space velocities, which are sufficiently high to meet the demands of future fuel processing reactors.

Immobilization of a Pleurotus ostreatus Laccase Mixture on Perlite and Its Application to Dye Decolourisation

PubMed Central

Salatino, Piero; Sannia, Giovanni

2014-01-01

In the present study, a crude laccase preparation from Pleurotus ostreatus was successfully immobilized on perlite, a cheap porous silica material, and tested for Remazol Brilliant Blue R (RBBR) decolourisation in a fluidized bed recycle reactor. Results showed that RBBR decolourisation is mainly due to enzyme action despite the occurrence of dye adsorption-related enzyme inhibition. Fine tuning of immobilization conditions allowed balancing the immobilization yield and the resulting rate of decolourisation, with the adsorption capacity of the solid biocatalyst. In the continuous lab scale reactor, a maximum conversion degree of 56.1% was achieved at reactor space-time of 4.2 h. Stability and catalytic parameters of the immobilized laccases were also assessed in comparison with the soluble counterparts, revealing an increase in stability, despite a reduction of the catalytic performances. Both effects are most likely ascribable to the occurrence of multipoint attachment phenomena. PMID:24895564

Microwave-Assisted Selective Hydrogenation of Furfural to Furfuryl Alcohol Employing a Green and Noble Metal-Free Copper Catalyst.

PubMed

Romano, Pedro N; de Almeida, João M A R; Carvalho, Yuri; Priecel, Peter; Falabella Sousa-Aguiar, Eduardo; Lopez-Sanchez, Jose A

2016-12-20

Green, inexpensive, and robust copper-based heterogeneous catalysts achieve 100 % conversion and 99 % selectivity in the conversion of furfural to furfuryl alcohol when using cyclopentyl-methyl ether as green solvent and microwave reactors at low H 2 pressures and mild temperatures. The utilization of pressurized microwave reactors produces a 3-4 fold increase in conversion and an unexpected enhancement in selectivity as compared to the reaction carried out at the same conditions using conventional autoclave reactors. The enhancement in catalytic rate produced by microwave irradiation is temperature dependent. This work highlights that using microwave irradiation in the catalytic hydrogenation of biomass-derived compounds is a very strong tool for biomass upgrade that offers immense potential in a large number of transformations where it could be a determining factor for commercial exploitation. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

New, efficient and viable system for ethanol fuel utilization on combined electric/internal combustion engine vehicles

NASA Astrophysics Data System (ADS)

Sato, André G.; Silva, Gabriel C. D.; Paganin, Valdecir A.; Biancolli, Ana L. G.; Ticianelli, Edson A.

2015-10-01

Although ethanol can be directly employed as fuel on polymer-electrolyte fuel cells (PEMFC), its low oxidation kinetics in the anode and the crossover to the cathode lead to a substantial reduction of energy conversion efficiency. However, when fuel cell driven vehicles are considered, the system may include an on board steam reformer for converting ethanol into hydrogen, but the hydrogen produced contains carbon monoxide, which limits applications in PEMFCs. Here, we present a system consisting of an ethanol dehydrogenation catalytic reactor for producing hydrogen, which is supplied to a PEMFC to generate electricity for electric motors. A liquid by-product effluent from the reactor can be used as fuel for an integrated internal combustion engine, or catalytically recycled to extract more hydrogen molecules. Power densities comparable to those of a PEMFC operating with pure hydrogen are attained by using the hydrogen rich stream produced by the ethanol dehydrogenation reactor.

Upgrading producer gas quality from rubber wood gasification in a radio frequency tar thermocatalytic treatment reactor.

PubMed

Anis, Samsudin; Zainal, Z A

2013-12-01

This study focused on improving the producer gas quality using radio frequency (RF) tar thermocatalytic treatment reactor. The producer gas containing tar, particles and water was directly passed at a particular flow rate into the RF reactor at various temperatures for catalytic and thermal treatments. Thermal treatment generates higher heating value of 5.76 MJ Nm(-3) at 1200°C. Catalytic treatments using both dolomite and Y-zeolite provide high tar and particles conversion efficiencies of about 97% on average. The result also showed that light poly-aromatic hydrocarbons especially naphthalene and aromatic compounds particularly benzene and toluene were still found even at higher reaction temperatures. Low energy intensive RF tar thermocatalytic treatment was found to be effective for upgrading the producer gas quality to meet the end user requirements and increasing its energy content. Copyright © 2013 Elsevier Ltd. All rights reserved.

Low temperature conversion of plastic waste into light hydrocarbons.

PubMed

Shah, Sajid Hussain; Khan, Zahid Mahmood; Raja, Iftikhar Ahmad; Mahmood, Qaisar; Bhatti, Zulfiqar Ahmad; Khan, Jamil; Farooq, Ather; Rashid, Naim; Wu, Donglei

2010-07-15

Advance recycling through pyrolytic technology has the potential of being applied to the management of plastic waste (PW). For this purpose 1 l volume, energy efficient batch reactor was manufactured locally and tested for pyrolysis of waste plastic. The feedstock for reactor was 50 g waste polyethylene. The average yield of the pyrolytic oil, wax, pyrogas and char from pyrolysis of PW were 48.6, 40.7, 10.1 and 0.6%, respectively, at 275 degrees C with non-catalytic process. Using catalyst the average yields of pyrolytic oil, pyrogas, wax and residue (char) of 50 g of PW was 47.98, 35.43, 16.09 and 0.50%, respectively, at operating temperature of 250 degrees C. The designed reactor could work at low temperature in the absence of a catalyst to obtain similar products as for a catalytic process. 2010 Elsevier B.V. All rights reserved.

Effect of torrefaction pretreatment and catalytic pyrolysis on the pyrolysis poly-generation of pine wood.

PubMed

Chen, Dengyu; Li, Yanjun; Deng, Minsi; Wang, Jiayang; Chen, Miao; Yan, Bei; Yuan, Qiqiang

2016-08-01

Torrefaction of pine wood was performed in a tube furnace at three temperatures (220, 250, and 280°C) for 30min. Then catalytic pyrolysis of raw and torrefied pine wood was performed using HZSM-5 catalyst in a fixed-bed pyrolysis reactor at 550°C for 15min. Torrefaction pretreatment and catalytic pyrolysis have an very important effect on the yield, property, and energy distribution of pyrolysis products. The results showed that the yield of biochar rapidly increased, while that of bio-oil decreased with increasing torrefaction temperature. The oxy-compound content of bio-oil, such as acids and aldehydes, sharply decreased. However, the aromatic hydrocarbon content not only increased but also further promoted by HZSM-5 catalyst. With highest mass yields and energy yields, biochar was also the very important product of pyrolysis. The oxygen content in biomass was mainly removed in the form of CO2 and H2O, leading to increasing CO2 content in non-condensable gas. Copyright © 2016 Elsevier Ltd. All rights reserved.

Improving gold catalysis of nitroarene reduction with surface Pd

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pretzer, Lori A.; Heck, Kimberly N.; Kim, Sean S.

2016-04-01

Nitroarene reduction reactions are commercialized catalytic processes that play a key role in the synthesisof many products including medicines, rubbers, dyes, and herbicides. Whereas bimetallic compositionshave been studied, a better understanding of the bimetallic structure effects may lead to improved indus-trial catalysts. In this work, the influence of surface palladium atoms supported on 3-nm Au nanoparticles(Pd-on-Au NPs) on catalytic activity for 4-nitrophenol reduction is explored. Batch reactor studies indi-cate Pd-on-Au NPs exhibit maximum catalytic activity at a Pd surface coverage of 150 sc%, with aninitial turnover frequency of ~3.7 mol-nitrophenol/mol-metalsurface/s, which was ~5.5× and ~13× moreactive than pure Au NPsmore » and Pd NPs, respectively. Pd NPs, Au NPs, and Pd-on-Au NPs below 175 sc%show compensation behavior. Three-dimensional Pd surface ensembles (with ~4–5 atoms) previouslyidentified through X-ray adsorption spectroscopy provide the active sites responsible for the catalyticmaximum. These results demonstrate the ability to adjust systematically a structural feature (i.e., Pdsurface coverage) to yield a more active material.« less

Single-reactor process for producing liquid-phase organic compounds from biomass

DOEpatents

Dumesic, James A.; Simonetti, Dante A.; Kunkes, Edward L.

2015-12-08

Disclosed is a method for preparing liquid fuel and chemical intermediates from biomass-derived oxygenated hydrocarbons. The method includes the steps of reacting in a single reactor an aqueous solution of a biomass-derived, water-soluble oxygenated hydrocarbon reactant, in the presence of a catalyst comprising a metal selected from the group consisting of Cr, Mn, Fe, Co, Ni, Cu, Mo, Tc, Ru, Rh, Pd, Ag, W, Re, Os, Ir, Pt, and Au, at a temperature, and a pressure, and for a time sufficient to yield a self-separating, three-phase product stream comprising a vapor phase, an organic phase containing linear and/or cyclic mono-oxygenated hydrocarbons, and an aqueous phase.

Single-reactor process for producing liquid-phase organic compounds from biomass

DOEpatents

Dumesic, James A [Verona, WI; Simonetti, Dante A [Middleton, WI; Kunkes, Edward L [Madison, WI

2011-12-13

Disclosed is a method for preparing liquid fuel and chemical intermediates from biomass-derived oxygenated hydrocarbons. The method includes the steps of reacting in a single reactor an aqueous solution of a biomass-derived, water-soluble oxygenated hydrocarbon reactant, in the presence of a catalyst comprising a metal selected from the group consisting of Cr, Mn, Fe, Co, Ni, Cu, Mo, Tc, Ru, Rh, Pd, Ag, W, Re, Os, Ir, Pt, and Au, at a temperature, and a pressure, and for a time sufficient to yield a self-separating, three-phase product stream comprising a vapor phase, an organic phase containing linear and/or cyclic mono-oxygenated hydrocarbons, and an aqueous phase.

Catalytic cracking of the top phase fraction of bio-oil into upgraded liquid oil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sunarno; Chemical Engineering Department, Gadjah Mada University, Jalan Grafika No. 2 Bulaksumur,Yogyakarta 55281; Rochmadi,

The energy consumption is increasing, while oil reserves as a primary energy resource are decreasing, so that is the reason seeking alternative energy source is inevitable. Biomass especially oil palm empty fruit bunches (EFB) which is abundant in Indonesia can be processed into bio-oil by pyrolysis process. The potential for direct substitution of bio-oil for petroleum may be limited due to the high viscosity, high oxygen content, low heating value, and corrosiveness. Consequently, upgrading of the bio-oil before use is inevitable to give a wider variety of applications of its liquid product. Furthermore, upgrading process to improve the quality ofmore » bio-oil by reduction of oxygenates involves process such as catalytic cracking. The objective of this research is to study the effect of operation temperature on yield and composition of upgraded liquid oil and to determine physical properties. Bio-oil derived from EFB was upgraded through catalytic cracking using series tubular reactor under atmospheric pressure on a silica-alumina catalyst. Results show that increasing temperature from 450 to 600 °C, resulting in decreasing of upgraded liquid oil (ULO) yield, decreasing viscosity and density of ULO, but increasing in calorimetric value of ULO. The increasing temperature of cracking also will increase the concentration of gasoline and kerosene in ULO.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vardon, Derek R.; Settle, Amy E.; Vorotnikov, Vassili

Succinic acid is a biomass-derived platform chemical that can be catalytically converted in the aqueous phase to 1,4-butanediol (BDO), a prevalent building block used in the polymer and chemical industries. Despite significant interest, limited work has been reported regarding sustained catalyst performance and stability under continuous aqueous-phase process conditions. As such, this work examines Ru-Sn on activated carbon (AC) for the aqueous-phase conversion of succinic acid to BDO under batch and flow reactor conditions. Initially, powder Ru-Sn catalysts were screened to determine the most effective bimetallic ratio and provide a comparison to other monometallic (Pd, Pt, Ru) and bimetallic (Pt-Sn,more » Pd-Re) catalysts. Batch reactor tests determined that a ~1:1 metal weight ratio of Ru to Sn was effective for producing BDO in high yields, with complete conversion resulting in 82% molar yield. Characterization of the fresh Ru-Sn catalyst suggests that the sequential loading method results in Ru sites that are colocated and surface-enriched with Sn. Postbatch reaction characterization confirmed stable Ru-Sn material properties; however, upon a transition to continuous conditions, significant Ru-Sn/AC deactivation occurred due to stainless steel leaching of Ni that resulted in Ru-Sn metal crystallite restructuring to form discrete Ni-Sn sites. Computational modeling confirmed favorable energetics for Ru-Sn segregation and Ni-Sn formation at submonolayer Sn incorporation. To address stainless steel leaching, reactor walls were treated with an inert silica coating by chemical vapor deposition. With leaching reduced, stable Ru-Sn/AC performance was observed that resulted in a molar yield of 71% BDO and 15% tetrahydrofuran for 96 h of time on stream. Postreaction catalyst characterization confirmed low levels of Ni and Cr deposition, although early-stage islanding of Ni-Sn will likely be problematic for industrially relevant time scales (i.e., thousands of hours). Overall, these results (i) demonstrate the performance of Ru-Sn/AC for aqueous phase succinic acid reduction, (ii) provide insight into the Ru-Sn bimetallic structure and deactivation in the presence of leached Ni, and (iii) underscore the importance of compatible reactor metallurgy and durable catalysts.« less

Enzyme-Embedded, Microstructural Reactors for Industrial Biocatalysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baker, Sarah E.; Knipe, J. M.; Oakdale, J.

In this project we explored enzyme-catalyzed methane conversion to methanol. Industrial biological approaches to methane conversion using whole organisms are predicted to be more energy efficient than chemical approaches, but are limited by mass transfer of the gas phase reactants, methane and oxygen, to the organisms. We demonstrated that 3D printing the enzyme particulate Methane Mono Oxygenase (pMMO) embedded in a polymer can improve the kinetics of methane to methanol conversion. This improvement was likely due to the ability to increase the surface area of the catalytic material using 3D printing. We also demonstrated the first continuous use of pMMOmore » in a flow-through reactor. In order to understand the fundamental kinetic properties of pMMO, we conducted an in-depth study of pMMO kinetics using analytical tools developed in our lab. Finally, we developed a new copolymer system that allowed tuning of the gas permeability of the biocatalytic material.« less

Catalytic oxidation of gaseous reduced sulfur compounds using coal fly ash.

PubMed

Kastner, James R; Das, K C; Melear, Nathan D

2002-11-11

Activated carbon has been shown to oxidize reduced sulfur compounds, but in many cases it is too costly for large-scale environmental remediation applications. Alternatively, we theorized that coal fly ash, given its high metal content and the presence of carbon could act as an inexpensive catalytic oxidizer of reduced sulfur compounds for "odor" removal. Initial results indicate that coal fly ash can catalyze the oxidization of H(2)S and ethanethiol, but not dimethyl sulfide (DMS) and dimethyl disulfide (DMDS) at room temperature. In batch reactor systems, initial concentrations of 100-500 ppmv H(2)S or ethanethiol were reduced to 0-2 ppmv within 1-2 and 6-8 min, respectively. This was contrary to control systems without ash in which concentrations remained constant. Diethyl disulfide was formed from ethanethiol substantiating the claim that catalytic oxidation occurred. The presence of water increased the rate of adsorption/reaction of both H(2)S and ethanethiol for the room temperature reactions (23-25 degrees C). Additionally, in a continuous flow packed bed reactor, a gaseous stream containing an inlet H(2)S concentration of 400-500 ppmv was reduced to 200 ppmv at a 4.6s residence time. The removal efficiency remained at 50% for approximately 4.6h or 3500 reactor volumes. These results demonstrate the potential of using coal fly ash in reactors for removal of H(2)S and other reduced sulfur compounds.

Reactive Distillation and Air Stripping Processes for Water Recycling and Trace Contaminant Control

NASA Technical Reports Server (NTRS)

Boul, Peter J.; Lange, Kevin E.; Conger, Bruce; Anderson, Molly

2009-01-01

Reactive distillation designs are considered to reduce the presence of volatile organic compounds in the purified water. Reactive distillation integrates a reactor with a distillation column. A review of the literature in this field has revealed a variety of functional reactive columns in industry. Wastewater may be purified by a combination of a reactor and a distiller (e.g., the EWRS or VPCAR concepts) or, in principle, through a design which integrates the reactor with the distiller. A review of the literature in reactive distillation has identified some different designs in such combinations of reactor and distiller. An evaluation of reactive distillation and reactive air stripping is presented with regards to the reduction of volatile organic compounds in the contaminated water and air. Among the methods presented, an architecture is presented for the evaluation of the simultaneous oxidation of organics in air and water. These and other designs are presented in light of potential improvements in power consumptions and air and water purities for architectures which include catalytic activity integrated into the water processor. In particular, catalytic oxidation of organics may be useful as a tool to remove contaminants that more traditional distillation and/or air stripping columns may not remove. A review of the current leading edge at the commercial level and at the research frontier in catalytically active materials is presented. Themes and directions from the engineering developments in catalyst design are presented conceptually in light of developments in the nanoscale chemistry of a variety of catalyst materials.

TREATMENT OF METHYL TERT-BUTYL ETHER CONTAMINATED WATER USING PHOTOCATALYSIS

EPA Science Inventory

The feasibility of photo-oxidation treatment of methyl tert-butyl ether (MTBE) in water was investigated in three ways, 1) using a slurry falling film photo-reactor, 2) a batch solar reactor system, and 3) a combination of air-stripping and gas phase photooxidation system. MTBE-c...

Catalytic biofilms on structured packing for the production of glycolic acid.

PubMed

Li, Xuan Zhong; Hauer, Bernhard; Rosche, Bettina

2013-02-01

While structured packing modules are known to be efficient for surface wetting and gas-liquid exchange in abiotic surface catalysis, this model study explores structured packing as a growth surface for catalytic biofilms. Microbial biofilms have been proposed as self-immobilized and self-regenerating catalysts for the production of chemicals. A concern is that the complex and dynamic nature of biofilms may cause fluctuations in their catalytic performance over time or may affect process reproducibility. An aerated continuous trickle-bed biofilm reactor system was designed with a 3 L structured packing, liquid recycling and pH control. Pseudomonas diminuta established a biofilm on the stainless steel structured packing with a specific surface area of 500 m2 m-3 and catalyzed the oxidation of ethylene glycol to glycolic acid for over two months of continuous operation. A steady-state productivity of up to 1.6 gl-1h-1 was achieved at a dilution rate of 0.33 h-1. Process reproducibility between three independent runs was excellent, despite process interruptions and activity variations in cultures grown from biofilm effluent cells. The results demonstrate the robustness of a catalytic biofilm on structured packing, despite its dynamic nature. Implementation is recommended for whole-cell processes that require efficient gas-liquid exchange, catalyst retention for continuous operation, or improved catalyst stability.

Degradation of paracetamol by catalytic wet air oxidation and sequential adsorption - Catalytic wet air oxidation on activated carbons.

PubMed

Quesada-Peñate, I; Julcour-Lebigue, C; Jáuregui-Haza, U J; Wilhelm, A M; Delmas, H

2012-06-30

The concern about the fate of pharmaceutical products has raised owing to the increasing contamination of rivers, lakes and groundwater. The aim of this paper is to evaluate two different processes for paracetamol removal. The catalytic wet air oxidation (CWAO) of paracetamol on activated carbon was investigated both as a water treatment technique using an autoclave reactor and as a regenerative treatment of the carbon after adsorption in a sequential fixed bed process. Three activated carbons (ACs) from different source materials were used as catalysts: two microporous basic ACs (S23 and C1) and a meso- and micro-porous acidic one (L27). During the first CWAO experiment the adsorption capacity and catalytic performance of fresh S23 and C1 were higher than those of fresh L27 despite its higher surface area. This situation changed after AC reuse, as finally L27 gave the best results after five CWAO cycles. Respirometry tests with activated sludge revealed that in the studied conditions the use of CWAO enhanced the aerobic biodegradability of the effluent. In the ADOX process L27 also showed better oxidation performances and regeneration efficiency. This different ageing was examined through AC physico-chemical properties. Copyright © 2012 Elsevier B.V. All rights reserved.

Catalysts at work: From integral to spatially resolved X-ray absorption spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grunwaldt, Jan-Dierk; Kimmerle, Bertram; Baiker, Alfons

2009-09-25

Spectroscopic studies on heterogeneous catalysts have mostly been done in an integral mode. However, in many cases spatial variations in catalyst structure can occur, e.g. during impregnation of pre-shaped particles, during reaction in a catalytic reactor, or in microstructured reactors as the present overview shows. Therefore, spatially resolved molecular information on a microscale is required for a comprehensive understanding of theses systems, partly in ex situ studies, partly under stationary reaction conditions and in some cases even under dynamic reaction conditions. Among the different available techniques, X-ray absorption spectroscopy (XAS) is a well-suited tool for this purpose as the differentmore » selected examples highlight. Two different techniques, scanning and full-field X-ray microscopy/tomography, are described and compared. At first, the tomographic structure of impregnated alumina pellets is presented using full-field transmission microtomography and compared to the results obtained with a scanning X-ray microbeam technique to analyse the catalyst bed inside a catalytic quartz glass reactor. On the other hand, by using XAS in scanning microtomography, the structure and the distribution of Cu(0), Cu(I), Cu(II) species in a Cu/ZnO catalyst loaded in a quartz capillary microreactor could be reconstructed quantitatively on a virtual section through the reactor. An illustrating example for spatially resolved XAS under reaction conditions is the partial oxidation of methane over noble metal-based catalysts. In order to obtain spectroscopic information on the spatial variation of the oxidation state of the catalyst inside the reactor XAS spectra were recorded by scanning with a micro-focussed beam along the catalyst bed. Alternatively, full-field transmission imaging was used to efficiently determine the distribution of the oxidation state of a catalyst inside a reactor under reaction conditions. The new technical approaches together with quantitative data analysis and an appropriate in situ catalytic experiment allowed drawing important conclusions on the reaction mechanism, and the analytical strategy might be similarly applied in other case studies. The corresponding temperature profiles and the catalytic performance were measured by means of an IR-camera and mass spectrometric analysis. In a more advanced experiment the ignition process of the partial oxidation of methane was followed in a spatiotemporal manner which demonstrates that spatially resolved spectroscopic information can even be obtained in the subsecond scale.« less

40 CFR 63.1579 - What definitions apply to this subpart?

Code of Federal Regulations, 2014 CFR

2014-07-01

... regeneration of catalyst in situ in any one of several reactors (e.g., 4 or 5 separate reactors) that can be..., wet injection, or caustic injection control device that treats (in-situ) the catalytic reforming unit...) at specified intervals or at the owner's or operator's convenience for in situ catalyst regeneration...

40 CFR 63.1579 - What definitions apply to this subpart?

Code of Federal Regulations, 2013 CFR

2013-07-01

... regeneration of catalyst in situ in any one of several reactors (e.g., 4 or 5 separate reactors) that can be..., wet injection, or caustic injection control device that treats (in-situ) the catalytic reforming unit...) at specified intervals or at the owner's or operator's convenience for in situ catalyst regeneration...

40 CFR 63.1579 - What definitions apply to this subpart?

Code of Federal Regulations, 2012 CFR

2012-07-01

... regeneration of catalyst in situ in any one of several reactors (e.g., 4 or 5 separate reactors) that can be..., wet injection, or caustic injection control device that treats (in-situ) the catalytic reforming unit...) at specified intervals or at the owner's or operator's convenience for in situ catalyst regeneration...

Lithographically fabricated silicon microreactor for in situ characterization of heterogeneous catalysts—Enabling correlative characterization techniques

NASA Astrophysics Data System (ADS)

Baier, S.; Rochet, A.; Hofmann, G.; Kraut, M.; Grunwaldt, J.-D.

2015-06-01

We report on a new modular setup on a silicon-based microreactor designed for correlative spectroscopic, scattering, and analytic on-line gas investigations for in situ studies of heterogeneous catalysts. The silicon microreactor allows a combination of synchrotron radiation based techniques (e.g., X-ray diffraction and X-ray absorption spectroscopy) as well as infrared thermography and Raman spectroscopy. Catalytic performance can be determined simultaneously by on-line product analysis using mass spectrometry. We present the design of the reactor, the experimental setup, and as a first example for an in situ study, the catalytic partial oxidation of methane showing the applicability of this reactor for in situ studies.

Lithographically fabricated silicon microreactor for in situ characterization of heterogeneous catalysts—Enabling correlative characterization techniques.

PubMed

Baier, S; Rochet, A; Hofmann, G; Kraut, M; Grunwaldt, J-D

2015-06-01

We report on a new modular setup on a silicon-based microreactor designed for correlative spectroscopic, scattering, and analytic on-line gas investigations for in situ studies of heterogeneous catalysts. The silicon microreactor allows a combination of synchrotron radiation based techniques (e.g., X-ray diffraction and X-ray absorption spectroscopy) as well as infrared thermography and Raman spectroscopy. Catalytic performance can be determined simultaneously by on-line product analysis using mass spectrometry. We present the design of the reactor, the experimental setup, and as a first example for an in situ study, the catalytic partial oxidation of methane showing the applicability of this reactor for in situ studies.

Experimental heat transfer distribution on the SNAP 10A reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hopenfeld, J.; Toews, R.E.

1965-01-29

Heating distributions have been obtained for the SNAP 10A reactor by means of a thermal paint technique in the Rhodes and Bloxsom 60 in. hypersonic wind tunnel. Data and correlations are presented only for those reactor components where the ratio of the local heat transfer to that on the stagnation point of the calibration sphere was found to be independent of tunnel conditions. It is shown that these heating distributions can be applied directly to reentry conditions provided the thermally painted and the bare reactor surfaces are both catalytic to atom recombination.

Effect of Solids Retention Time on the Denitrification Potential of Anaerobically Digested Swine Waste

NASA Astrophysics Data System (ADS)

Kinyua, Maureen Njoki

Three continuously stirred tank reactors (CSTR) were operated in semi continuous mode treating swine waste using anaerobic digestion. The reactors were used to test the effect of solid retention time (SRT) on CH4 yield, total ammonia nitrogen (TAN) concentrations, % volatile solids (VS), chemical oxygen demand (COD) and volatile fatty acids (VFA) removal, readily biodegradable COD concentration and the denitrification potential for the effluent in a biological nutrient removal (BNR) system. During Phase I of the study, the three reactors were operated at the same 28 day SRT for 16 weeks. SRTs were then changed during the 12 week Phase II period. The SRTs studied were 14, 21 and 28 days, with the same organic loading rate (OLR) of 1.88 ± 0.2 kg VS/ m3-day. The reactor with the lowest SRT (14 days) had the highest VS and VFA removal at 73.6 and 67.6% and lowest TAN concentration at 0.78 g NH4+-N/L, followed by the 21 day and 28 day reactors. This was likely due to the fast microbial growth rates and substrate utilization rates in this reactor compared with the other two. The 14 day reactor had the highest CH4 yield at 0.33 m3CH 4/kg VS added and readily biodegradable COD concentration at 0.93 COD/L. The variations in CH4 yield and readily biodegradable COD concentrations between the three reactors were not statistically significant. Denitrification potential for the reactors was 1.20, 0.73 and 0.56 g COD/g N for 14, 21 and 28 day reactors, respectively, and the differences were statistically significant. None of the reactors achieved a denitrification potential of 5 g COD/g N, the amount required to use effluent of anaerobically digested swine waste as an internal carbon source in a BNR. This was attributed to operating conditions such as freezing and thawing of the raw swine waste that maximized CH4 yield and lowered the readily biodegradable COD concentration. In addition the 14 day reactor had low TAN concentrations thus increasing the denitrification potential of the centrate from that reactor.

NO—CO—O2 Reaction on a Metal Catalytic Surface using Eley—Rideal Mechanism

NASA Astrophysics Data System (ADS)

Waqar, Ahmad

2008-10-01

Interactions among the reacting species NO, CO and O2 on metal catalytic surfaces are studied by means of Monte Carlo simulation using the Eley-Rideal (ER) mechanism. The study of this three-component system is important for understanding of the reaction kinetics by varying the relative ratios of the reactants. It is found that contrary to the conventional Langmuir-Hinshelwood (LH) thermal mechanism in which two irreversible phase transitions are obtained between active states and poisoned states, a single phase transition is observed when the ER mechanism is combined with the LH mechanism. The phase diagrams of the surface coverage and the steady state production of CO2, N2 and N2 O are evaluated as a function of the partial pressures of the reactants in the gas phase. The continuous production of CO2 starts as soon as the CO pressure is switched on and the second order phase transition at the first critical point is eliminated, which is in agreement with the experimental findings.

Catalytic reaction in confined flow channel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Van Hassel, Bart A.

A chemical reactor comprises a flow channel, a source, and a destination. The flow channel is configured to house at least one catalytic reaction converting at least a portion of a first nanofluid entering the channel into a second nanofluid exiting the channel. The flow channel includes at least one turbulating flow channel element disposed axially along at least a portion of the flow channel. A plurality of catalytic nanoparticles is dispersed in the first nanofluid and configured to catalytically react the at least one first chemical reactant into the at least one second chemical reaction product in the flowmore » channel.« less

Transition-Metal Decorated Aluminum Nanocrystals.

PubMed

Swearer, Dayne F; Leary, Rowan K; Newell, Ryan; Yazdi, Sadegh; Robatjazi, Hossein; Zhang, Yue; Renard, David; Nordlander, Peter; Midgley, Paul A; Halas, Naomi J; Ringe, Emilie

2017-10-24

Recently, aluminum has been established as an earth-abundant alternative to gold and silver for plasmonic applications. Particularly, aluminum nanocrystals have shown to be promising plasmonic photocatalysts, especially when coupled with catalytic metals or oxides into "antenna-reactor" heterostructures. Here, a simple polyol synthesis is presented as a flexible route to produce aluminum nanocrystals decorated with eight varieties of size-tunable transition-metal nanoparticle islands, many of which have precedence as heterogeneous catalysts. High-resolution and three-dimensional structural analysis using scanning transmission electron microscopy and electron tomography shows that abundant nanoparticle island decoration in the catalytically relevant few-nanometer size range can be achieved, with many islands spaced closely to their neighbors. When coupled with the Al nanocrystal plasmonic antenna, these small decorating islands will experience increased light absorption and strong hot-spot generation. This combination makes transition-metal decorated aluminum nanocrystals a promising material platform to develop plasmonic photocatalysis, surface-enhanced spectroscopies, and quantum plasmonics.

Microwave-Based Oxidation State and Soot Loading Determination on Gasoline Particulate Filters with Three-Way Catalyst Coating for Homogenously Operated Gasoline Engines.

PubMed

Dietrich, Markus; Jahn, Christoph; Lanzerath, Peter; Moos, Ralf

2015-09-02

Recently, a novel method emerged to determine the oxygen storage degree of three way catalysts (TWC) by a microwave-based method. Up to now, this method has been investigated only in lab-scale reactors or under steady state conditions. This work expands those initial studies. A TWC-coated gasoline particulate filter was investigated in a dynamic engine test bench simulating a typical European driving cycle (NEDC). It could be shown that both the oxygen storage degree and the soot loading can be monitored directly, but not simultaneously due to their competitive effects. Under normal driving conditions, no soot accumulation was observed, related to the low raw emissions and the catalytic coating of the filter. For the first time, the quality factor of the cavity resonator in addition to the resonance frequency was used, with the benefit of less cross sensitivity to inconstant temperature and water. Therefore, a temperature dependent calibration of the microwave signal was created and applied to monitor the oxidation state in transient driving cycles. The microwave measurement mirrors the oxidation state determined by lambda probes and can be highly beneficial in start-stop phases (where lambda-probes do not work) and to determine the oxygen storage capacity (OSC) without unnecessary emissions.

Microwave-Based Oxidation State and Soot Loading Determination on Gasoline Particulate Filters with Three-Way Catalyst Coating for Homogenously Operated Gasoline Engines

PubMed Central

Dietrich, Markus; Jahn, Christoph; Lanzerath, Peter; Moos, Ralf

2015-01-01

Recently, a novel method emerged to determine the oxygen storage degree of three way catalysts (TWC) by a microwave-based method. Up to now, this method has been investigated only in lab-scale reactors or under steady state conditions. This work expands those initial studies. A TWC-coated gasoline particulate filter was investigated in a dynamic engine test bench simulating a typical European driving cycle (NEDC). It could be shown that both the oxygen storage degree and the soot loading can be monitored directly, but not simultaneously due to their competitive effects. Under normal driving conditions, no soot accumulation was observed, related to the low raw emissions and the catalytic coating of the filter. For the first time, the quality factor of the cavity resonator in addition to the resonance frequency was used, with the benefit of less cross sensitivity to inconstant temperature and water. Therefore, a temperature dependent calibration of the microwave signal was created and applied to monitor the oxidation state in transient driving cycles. The microwave measurement mirrors the oxidation state determined by lambda probes and can be highly beneficial in start-stop phases (where lambda-probes do not work) and to determine the oxygen storage capacity (OSC) without unnecessary emissions. PMID:26340629

Multifunctional nanocomposite hollow fiber membranes by solvent transfer induced phase separation.

PubMed

Haase, Martin F; Jeon, Harim; Hough, Noah; Kim, Jong Hak; Stebe, Kathleen J; Lee, Daeyeon

2017-11-01

The decoration of porous membranes with a dense layer of nanoparticles imparts useful functionality and can enhance membrane separation and anti-fouling properties. However, manufacturing of nanoparticle-coated membranes requires multiple steps and tedious processing. Here, we introduce a facile single-step method in which bicontinuous interfacially jammed emulsions are used to form nanoparticle-functionalized hollow fiber membranes. The resulting nanocomposite membranes prepared via solvent transfer-induced phase separation and photopolymerization have exceptionally high nanoparticle loadings (up to 50 wt% silica nanoparticles) and feature densely packed nanoparticles uniformly distributed over the entire membrane surfaces. These structurally well-defined, asymmetric membranes facilitate control over membrane flux and selectivity, enable the formation of stimuli responsive hydrogel nanocomposite membranes, and can be easily modified to introduce antifouling features. This approach forms a foundation for the formation of advanced nanocomposite membranes comprising diverse building blocks with potential applications in water treatment, industrial separations and as catalytic membrane reactors.

Advanced Coal Liquefaction Research and Development Facility, Wilsonville, Alabama. Run 260 with Black Thunder Mine subbituminous coal: Technical progress report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

This report presents the results of Run 260 performed at the Advanced Coal Liquefaction R&D Facility in Wilsonville. The run was started on July 17, 1990 and continued until November 14, 1990, operating in the Close-Coupled Integrated Two-Stage Liquefaction mode processing Black Thunder mine subbituminous coal (Wyodak-Anderson seam from Wyoming Powder River Basin). Both thermal/catalytic and catalytic/thermal tests were performed to determine the methods for reducing solids buildup in a subbituminous coal operation, and to improve product yields. A new, smaller interstage separator was tested to reduce solids buildup by increasing the slurry space velocity in the separator. In ordermore » to obtain improved coal and resid conversions (compared to Run 258) full-volume thermal reactor and 3/4-volume catalytic reactor were used. Shell 324 catalyst, 1/16 in. cylindrical extrudate, at a replacement rate of 3 lb/ton of MF coal was used in the catalytic stage. Iron oxide was used as slurry catalyst at a rate of 2 wt % MF coal throughout the run. (TNPS was the sulfiding agent.)« less

Stable carbonous catalyst particles and method for making and utilizing same

DOEpatents

Ganguli, Partha S.; Comolli, Alfred G.

2005-06-14

Stable carbonous catalyst particles composed of an inorganic catalytic metal/metal oxide powder and a carbonaceous binder material are formed having a basic inner substantially uniform-porous carbon coating of the catalytic powder, and may include an outer porous carbon coating layer. Suitable inorganic catalytic powders include zinc-chromite (ZnO/Cr.sub.2 03) and suitable carbonaceous liquid binders having molecular weight of 200-700 include partially polymerized furfuryl alcohol, which are mixed together, shaped and carbonized and partially oxidized at elevated temperature. Such stable carbonous catalyst particles such as 0.020-0.100 inch (0.51-2.54 mm) diameter extrudates, have total carbon content of 2-25 wt. % and improved crush strength of 1.0-5 1b/mn, 50-300 m.sup.2 /g surface area, and can be advantageously utilized in fixed bed or ebullated/fluidized bed reactor operations. This invention also includes method steps for making the stable carbonous catalyst particles having improved particle strength and catalytic activity, and processes for utilizing the active stable carbonous carbon-coated catalysts such as for syn-gas reactions in ebullated/fluidized bed reactors for producing alcohol products and Fischer-Tropsch synthesis liquid products.

A composite reactor with wetted-wall column for mineral carbonation study in three-phase systems.

PubMed

Zhu, Chen; Yao, Xizhi; Zhao, Liang; Teng, H Henry

2016-11-01

Despite the availability of various reactors designed to study gas-liquid reactions, no appropriate devices are available to accurately investigate triple-phased mineral carbonation reactions involving CO 2 gas, aqueous solutions (containing divalent cations), and carbonate minerals. This report presents a composite reactor that combines a modified conventional wetted-wall column, a pH control module, and an attachment to monitor precipitation reactions. Our test and calibration experiments show that the absorption column behaved largely in agreement with theoretical predictions and previous observations. Experimental confirmation of CO 2 absorption in NaOH and ethanolamine supported the effectiveness of the column for gas-liquid interaction. A test run in the CO 2 -NH 3 -MgCl 2 system carried out for real time investigation of the relevant carbonation reactions shows that the reactor's performance closely followed the expected reaction path reflected in pH change, the occurrence of precipitation, and the rate of NH 3 addition, indicating the appropriateness of the composite device in studying triple-phase carbonation process.

The effects of leachate recirculation with supplemental water addition on methane production and waste decomposition in a simulated tropical landfill.

PubMed

Sanphoti, N; Towprayoon, S; Chaiprasert, P; Nopharatana, A

2006-10-01

In order to increase methane production efficiency, leachate recirculation is applied in landfills to increase moisture content and circulate organic matter back into the landfill cell. In the case of tropical landfills, where high temperature and evaporation occurs, leachate recirculation may not be enough to maintain the moisture content, therefore supplemental water addition into the cell is an option that could help stabilize moisture levels as well as stimulate biological activity. The objectives of this study were to determine the effects of leachate recirculation and supplemental water addition on municipal solid waste decomposition and methane production in three anaerobic digestion reactors. Anaerobic digestion with leachate recirculation and supplemental water addition showed the highest performance in terms of cumulative methane production and the stabilization period time required. It produced an accumulated methane production of 54.87 l/kg dry weight of MSW at an average rate of 0.58 l/kg dry weight/d and reached the stabilization phase on day 180. The leachate recirculation reactor provided 17.04 l/kg dry weight at a rate of 0.14l/kg dry weight/d and reached the stabilization phase on day 290. The control reactor provided 9.02 l/kg dry weight at a rate of 0.10 l/kg dry weight/d, and reached the stabilization phase on day 270. Increasing the organic loading rate (OLR) after the waste had reached the stabilization phase made it possible to increase the methane content of the gas, the methane production rate, and the COD removal. Comparison of the reactors' efficiencies at maximum OLR (5 kgCOD/m(3)/d) in terms of the methane production rate showed that the reactor using leachate recirculation with supplemental water addition still gave the highest performance (1.56 l/kg dry weight/d), whereas the leachate recirculation reactor and the control reactor provided 0.69 l/kg dry weight/d and 0.43 l/kg dry weight/d, respectively. However, when considering methane composition (average 63.09%) and COD removal (average 90.60%), slight differences were found among these three reactors.

Ru-Sn/AC for the Aqueous-Phase Reduction of Succinic Acid to 1,4-Butanediol under Continuous Process Conditions

DOE PAGES

Vardon, Derek R.; Settle, Amy E.; Vorotnikov, Vassili; ...

2017-08-18

Succinic acid is a biomass-derived platform chemical that can be catalytically converted in the aqueous phase to 1,4-butanediol (BDO), a prevalent building block used in the polymer and chemical industries. Despite significant interest, limited work has been reported regarding sustained catalyst performance and stability under continuous aqueous-phase process conditions. As such, this work examines Ru-Sn on activated carbon (AC) for the aqueous-phase conversion of succinic acid to BDO under batch and flow reactor conditions. Initially, powder Ru-Sn catalysts were screened to determine the most effective bimetallic ratio and provide a comparison to other monometallic (Pd, Pt, Ru) and bimetallic (Pt-Sn,more » Pd-Re) catalysts. Batch reactor tests determined that a ~1:1 metal weight ratio of Ru to Sn was effective for producing BDO in high yields, with complete conversion resulting in 82% molar yield. Characterization of the fresh Ru-Sn catalyst suggests that the sequential loading method results in Ru sites that are colocated and surface-enriched with Sn. Postbatch reaction characterization confirmed stable Ru-Sn material properties; however, upon a transition to continuous conditions, significant Ru-Sn/AC deactivation occurred due to stainless steel leaching of Ni that resulted in Ru-Sn metal crystallite restructuring to form discrete Ni-Sn sites. Computational modeling confirmed favorable energetics for Ru-Sn segregation and Ni-Sn formation at submonolayer Sn incorporation. To address stainless steel leaching, reactor walls were treated with an inert silica coating by chemical vapor deposition. With leaching reduced, stable Ru-Sn/AC performance was observed that resulted in a molar yield of 71% BDO and 15% tetrahydrofuran for 96 h of time on stream. Postreaction catalyst characterization confirmed low levels of Ni and Cr deposition, although early-stage islanding of Ni-Sn will likely be problematic for industrially relevant time scales (i.e., thousands of hours). Overall, these results (i) demonstrate the performance of Ru-Sn/AC for aqueous phase succinic acid reduction, (ii) provide insight into the Ru-Sn bimetallic structure and deactivation in the presence of leached Ni, and (iii) underscore the importance of compatible reactor metallurgy and durable catalysts.« less

Non-catalytic transfer hydrogenation in supercritical CO2 for coal liquefaction

NASA Astrophysics Data System (ADS)

Elhussien, Hussien

This thesis presents the results of the investigation on developing and evaluating a low temperature (<150°C) non - catalytic process using a hydrogen transfer agent (instead of molecu-lar hydrogen) for coal dissolution in supercritical CO2. The main idea behind the thesis was that one hydrogen atom from water and one hydrogen atom from the hydrogen transfer agent (HTA) were used to hydrogenate the coal. The products of coal dissolution were non-polar and polar while the supercritical CO2, which enhanced the rates of hydrogenation and dissolution of the non-polar molecules and removal from the reaction site, was non-polar. The polar modifier (PM) for CO2 was added to the freed to aid in the dissolution and removal of the polar components. The addition of a phase transfer agent (PTA) allowed a seamless transport of the ions and by-product between the aqueous and organic phases. DDAB, used as the PTA, is an effective phase transfer catalyst and showed enhancement to the coal dissolution process. COAL + DH- +H 2O → COAL.H2 + DHO-- This process has a great feature due to the fact that the chemicals were obtained without requir-ing to first convert coal to CO and H2 units as in indirect coal liquefaction. The experiments were conducted in a unique reactor set up that can be connected through two lines. one line to feed the reactor with supercritical CO 2 and the other connected to gas chromatograph. The use of the supercritical CO2 enhanced the solvent option due to the chemical extraction, in addition to the low environmental impact and energy cost. In this thesis the experiment were conducted at five different temperatures from atmos-pheric to 140°C, 3000 - 6000 psi with five component of feed mixture, namely water, HTA, PTA, coal, and PM in semi batch vessels reactor system with a volume of 100 mL. The results show that the chemicals were obtained without requiring to first convert coal to CO and H2 units as in indirect coal liquefaction. The results show that the conversion was found to be 91.8% at opti-mum feed mixtures values of 3, 1.0 and 5.4 for water: PM, HTA: coal, water: coal respectively. With the oil price increase and growing in energy demand, the coal liquefaction remain affordable and available energy alternative.

Method of making a catalytic reactor for automobile

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vroman, W.R.

1976-09-07

A catalytic reactor is made by providing a generally cylindrical catalytic substrate of oval transverse section and clamping the same between paired housing shells to form a housing of oval section spaced from the substrate by means of a pair of wire mesh ropes seated within a corresponding pair of grooves extending around the periphery of the substrate at axially spaced locations. Each rope is compacted from a matrix of multiple layers of resilient stainless steel knitted wire and is interlocked with the housing by means of a pair of inwardly opening channels of the housing spaced axially by anmore » inwardly projecting rib of the housing. The grooves in the substrate are pressed radially into the latter while the same is in a plastic uncured condition, thereby to compact and reinforce the grooves to withstand the localized compressional force of the ropes seated therein after the substrate is cured and hardened and clamped between the housing shells.« less

Catalytic reactor for low-Btu fuels

DOEpatents

Smith, Lance; Etemad, Shahrokh; Karim, Hasan; Pfefferle, William C.

2009-04-21

An improved catalytic reactor includes a housing having a plate positioned therein defining a first zone and a second zone, and a plurality of conduits fabricated from a heat conducting material and adapted for conducting a fluid therethrough. The conduits are positioned within the housing such that the conduit exterior surfaces and the housing interior surface within the second zone define a first flow path while the conduit interior surfaces define a second flow path through the second zone and not in fluid communication with the first flow path. The conduit exits define a second flow path exit, the conduit exits and the first flow path exit being proximately located and interspersed. The conduits define at least one expanded section that contacts adjacent conduits thereby spacing the conduits within the second zone and forming first flow path exit flow orifices having an aggregate exit area greater than a defined percent of the housing exit plane area. Lastly, at least a portion of the first flow path defines a catalytically active surface.

Biocatalytic methanation of hydrogen and carbon dioxide in an anaerobic three-phase system.

PubMed

Burkhardt, M; Koschack, T; Busch, G

2015-02-01

A new type of anaerobic trickle-bed reactor was used for biocatalytic methanation of hydrogen and carbon dioxide under mesophilic temperatures and ambient pressure in a continuous process. The conversion of gaseous substrates through immobilized hydrogenotrophic methanogenic archaea in a biofilm is a unique feature of this type of reactor. Due to the formation of a three-phase system on the carrier surface and operation as a plug flow reactor without gas recirculation, a complete reaction could be observed. With a methane concentration higher than c(CH4) = 98%, the product gas exhibits a very high quality. A specific methane production of P(CH4) = 1.49 Nm(3)/(m(3)(SV) d) was achieved at a hydraulic loading rate of LR(H2) = 6.0 Nm(3)/(m(3)(SV) d). The relation between trickle flow through the reactor and productivity could be shown. An application for methane enrichment in combination with biogas facilities as a source of carbon dioxide has also been positively proven. Copyright © 2014 Elsevier Ltd. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Underwood, R.P.

As part of the DOE-sponsored contract Synthesis of Dimethyl Ether and Alternative Fuels in the Liquid Phase from Coal-Derived Syngas'' experimental evaluations of the one-step synthesis of alternative fuels were carried out. The objective of this work was to develop novel processes for converting coal-derived syngas to fuels or fuel additives. Building on a technology base acquired during the development of the Liquid Phase Methanol (LPMEOH) process, this work focused on the development of slurry reactor based processes. The experimental investigations, which involved bench-scale reactor studies, focused primarily on three areas: (1) One-step, slurry-phase syngas conversion to hydrocarbons or methanol/hydrocarbonmore » mixtures using a mixture of methanol synthesis catalyst and methanol conversion catalyst in the same slurry reactor. (2) Slurry-phase conversion of syngas to mixed alcohols using various catalysts. (3) One-step, slurry-phase syngas conversion to mixed ethers using a mixture of mixed alcohols synthesis catalyst and dehydration catalyst in the same slurry reactor. The experimental results indicate that, of the three types of processes investigated, slurry phase conversion of syngas to mixed alcohols shows the most promise for further process development. Evaluations of various mixed alcohols catalysts show that a cesium-promoted Cu/ZnO/Al[sub 2]O[sub 3] methanol synthesis catalyst, developed in Air Products' laboratories, has the highest performance in terms of rate and selectivity for C[sub 2+]-alcohols. In fact, once-through conversion at industrially practical reaction conditions yielded a mixed alcohols product potentially suitable for direct gasoline blending. Moreover, an additional attractive aspect of this catalyst is its high selectivity for branched alcohols, potential precursors to iso-olefins for use in etherification.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Underwood, R.P.

As part of the DOE-sponsored contract ``Synthesis of Dimethyl Ether and Alternative Fuels in the Liquid Phase from Coal-Derived Syngas`` experimental evaluations of the one-step synthesis of alternative fuels were carried out. The objective of this work was to develop novel processes for converting coal-derived syngas to fuels or fuel additives. Building on a technology base acquired during the development of the Liquid Phase Methanol (LPMEOH) process, this work focused on the development of slurry reactor based processes. The experimental investigations, which involved bench-scale reactor studies, focused primarily on three areas: (1) One-step, slurry-phase syngas conversion to hydrocarbons or methanol/hydrocarbonmore » mixtures using a mixture of methanol synthesis catalyst and methanol conversion catalyst in the same slurry reactor. (2) Slurry-phase conversion of syngas to mixed alcohols using various catalysts. (3) One-step, slurry-phase syngas conversion to mixed ethers using a mixture of mixed alcohols synthesis catalyst and dehydration catalyst in the same slurry reactor. The experimental results indicate that, of the three types of processes investigated, slurry phase conversion of syngas to mixed alcohols shows the most promise for further process development. Evaluations of various mixed alcohols catalysts show that a cesium-promoted Cu/ZnO/Al{sub 2}O{sub 3} methanol synthesis catalyst, developed in Air Products` laboratories, has the highest performance in terms of rate and selectivity for C{sub 2+}-alcohols. In fact, once-through conversion at industrially practical reaction conditions yielded a mixed alcohols product potentially suitable for direct gasoline blending. Moreover, an additional attractive aspect of this catalyst is its high selectivity for branched alcohols, potential precursors to iso-olefins for use in etherification.« less

Catalytic oxidation for treatment of ECLSS and PMMS waste streams

NASA Technical Reports Server (NTRS)

Akse, James R.; Jolly, Clifford D.

1991-01-01

It is shown that catalytic oxidation is an effective technique for the removal of trace organic contaminants in a multifiltration potable processor's effluent. Essential elements of this technology are devices that deliver oxygen to the influent, and remove gaseous reaction byproducts from the effluent, via hollow-tube, gas-permeable membranes. Iodine, which poisons existing catalysis, is removed by a small deiodination bed prior to catalytic reactor entrance. The catalyst used is a mixture of Pt and Ru deposited on carbon, operating at 125-160 C and 39-90 psi pressures.

Low and medium heating value coal gas catalytic combustor characterization

NASA Technical Reports Server (NTRS)

Schwab, J. A.

1982-01-01

Catalytic combustion with both low and medium heating value coal gases obtained from an operating gasifier was demonstrated. A practical operating range for efficient operation was determined, and also to identify potential problem areas were identified for consideration during stationary gas turbine engine design. The test rig consists of fuel injectors, a fuel-air premixing section, a catalytic reactor with thermocouple instrumentation and a single point, water cooled sample probe. The test rig included inlet and outlet transition pieces and was designed for installation into an existing test loop.

Low Absorption Vitreous Carbon Reactors for Operando XAS: A Case Study on Cu/Zeolites for Selective Catalytic Reduction of NOx by NH3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kispersky, Vincent F.; Kropf, A. Jeremy; Ribeiro, Fabio H.

2012-01-01

We describe the use of vitreous carbon as an improved reactor material for an operando X-ray absorption spectroscopy (XAS) plug-flow reactor. These tubes significantly broaden the operating range for operando experiments. Using selective catalytic reduction (SCR) of NO x by NH₃ on Cu/Zeolites (SSZ-13, SAPO-34 and ZSM-5) as an example reaction, we illustrate the high-quality XAS data achievable with these reactors. The operando experiments showed that in Standard SCR conditions of 300 ppm NO, 300 ppm NH₃, 5% O₂, 5% H₂O, 5% CO₂ and balance He at 200 °C, the Cu was a mixture of Cu(I) and Cu(II) oxidation states.more » XANES and EXAFS fitting found the percent of Cu(I) to be 15%, 45% and 65% for SSZ-13, SAPO-34 and ZSM-5, respectively. For Standard SCR, the catalytic rates per mole of Cu for Cu/SSZ-13 and Cu/SAPO-34 were about one third of the rate per mole of Cu on Cu/ZSM-5. Based on the apparent lack of correlation of rate with the presence of Cu(I), we propose that the reaction occurs via a redox cycle of Cu(I) and Cu(II). Cu(I) was not found in in situSCR experiments on Cu/Zeolites under the same conditions, demonstrating a possible pitfall of in situ measurements. A Cu/SiO₂ catalyst, reduced in H₂ at 300 °C, was also used to demonstrate the reactor's operando capabilities using a bending magnet beamline. Analysis of the EXAFS data showed the Cu/SiO₂ catalyst to be in a partially reduced Cu metal–Cu(I) state. In addition to improvements in data quality, the reactors are superior in temperature, stability, strength and ease of use compared to previously proposed borosilicate glass, polyimide tubing, beryllium and capillary reactors. The solid carbon tubes are non-porous, machinable, can be operated at high pressure (tested at 25 bar), are inert, have high material purity and high X-ray transmittance.« less

Catalyst and method for aqueous phase reactions

DOEpatents

Elliott, Douglas C.; Hart, Todd R.

1999-01-01

The present invention is a catalyst in the form of a plurality of porous particles wherein each particle is a support having nickel metal catalytic phase or reduced nickel deposited thereon in a first dispersed phase and an additional metal deposited onto the support in a second dispersed phase. The additional metal is effective in retarding or reducing agglomeration or sintering of the nickel metal catalytic phase without substantially affecting the catalytic activity, thereby increasing the life time of the catalyst.

Lithographically fabricated silicon microreactor for in situ characterization of heterogeneous catalysts—Enabling correlative characterization techniques

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baier, S.; Rochet, A.; Hofmann, G.

2015-06-15

We report on a new modular setup on a silicon-based microreactor designed for correlative spectroscopic, scattering, and analytic on-line gas investigations for in situ studies of heterogeneous catalysts. The silicon microreactor allows a combination of synchrotron radiation based techniques (e.g., X-ray diffraction and X-ray absorption spectroscopy) as well as infrared thermography and Raman spectroscopy. Catalytic performance can be determined simultaneously by on-line product analysis using mass spectrometry. We present the design of the reactor, the experimental setup, and as a first example for an in situ study, the catalytic partial oxidation of methane showing the applicability of this reactor formore » in situ studies.« less

[Feasibility of treatment of landfill leachates by external loop three phase fluidized bed-constructed wetland system].

PubMed

Zhang, Jin-Sheng; Yuan, Xing-Zhong; Zeng, Guang-Ming; Dong, Bei-Bei; Liang, Yun-Shan

2009-11-01

In this study, the system composed with the external loop fluidized bed reactor and constructed wetland was used to treat the landfill leachate. The change of water quality for the landfill leachate treated by this system was investigated. The experimental results indicated that the COD and NH4(+) -N of the influent reduced from 4000 mg x L(-1) and 300 mg x L(-1) to 1 500 mg x L(-1) and 150 mg x L(-1) after the external loop three phase fluidized bed reactor and steady at 200 mg x L(-1) and 10 mg x L(-1) behind treated by the constructed wetland. The heavy metals of Cd, Zn, Pb were also reduced for treatment by external loop three phase fluidized bed reactor. They were steady at 0.01 mg x L(-1), 0.5 mg x L(-1), 0.1 mg x L(-1) from 0.12 mg x L(-1), 3.0 mg x L(-1), 1.4 mg x L(-1) because of the constructed wetland. We also compared the different plants for the efficiency, the results showed that whatever plants, there was little effects on the efficiency of the COD and NH4(+) -N, but the effect of heavy metal was markedness.

Study on the decomposition of trace benzene over V2O5–WO3/TiO2-based catalysts in simulated flue gas

EPA Science Inventory

Trace levels (1 and 10 ppm) of gaseous benzene were catalytically decomposed in a fixed-bed catalytic reactor with monolithic oxides of vanadium and tungsten supported on titanium oxide (V2O5–WO3/TiO2) catalysts under conditions simulating the cooling of waste incineration flue g...

Novel Attrition-Resistant Fischer Tropsch Catalyst

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weast, Logan, E.; Staats, William, R.

2009-05-01

There is a strong national interest in the Fischer-Tropsch synthesis process because it offers the possibility of making liquid hydrocarbon fuels from reformed natural gas or coal and biomass gasification products. This project explored a new approach that had been developed to produce active, attrition-resistant Fischer-Tropsch catalysts that are based on glass-ceramic materials and technology. This novel approach represented a promising solution to the problem of reducing or eliminating catalyst attrition and maximizing catalytic activity, thus reducing costs. The technical objective of the Phase I work was to demonstrate that glass-ceramic based catalytic materials for Fischer-Tropsch synthesis have resistance tomore » catalytic deactivation and reduction of particle size superior to traditional supported Fischer-Tropsch catalyst materials. Additionally, these novel glass-ceramic-based materials were expected to exhibit catalytic activity similar to the traditional materials. If successfully developed, the attrition-resistant Fischer-Tropsch catalyst materials would be expected to result in significant technical, economic, and social benefits for both producers and public consumers of Fischer-Tropsch products such as liquid fuels from coal or biomass gasification. This program demonstrated the anticipated high attrition resistance of the glass-ceramic materials. However, the observed catalytic activity of the materials was not sufficient to justify further development at this time. Additional testing documented that a lack of pore volume in the glass-ceramic materials limited the amount of surface area available for catalysis and consequently limited catalytic activity. However, previous work on glass-ceramic catalysts to promote other reactions demonstrated that commercial levels of activity can be achieved, at least for those reactions. Therefore, we recommend that glass-ceramic materials be considered again as potential Fischer-Tropsch catalysts if it can be demonstrated that materials with adequate pore volume can be produced. During the attrition resistance tests, it was learned that the glass-ceramic materials are very abrasive. Attention should be paid in any further developmental efforts to the potential for these hard, abrasive materials to damage reactors.« less

Catalytic conversion of light alkanes: Quarterly report, January 1-March 31, 1992

DOE Office of Scientific and Technical Information (OSTI.GOV)

Biscardi, J.; Bowden, P.T.; Durante, V.A.

The first Quarterly Report of 1992 on the Catalytic Conversion of Light Alkanes reviews the work done between January 1. 1992 and March 31, 1992 on the Cooperative Agreement. The mission of this work is to devise a new catalyst which can be used in a simple economic process to convert the light alkanes in natural gas to oxygenate products which can either be used as clean-burning, high octane liquid fuels, as fuel components or as precursors to liquid hydrocarbon transportation fuel. During the past quarter we have continued to design, prepare, characterize and test novel catalysts for the mildmore » selective reaction of light hydrocarbons with air or oxygen to produce alcohols directly. These catalysts are designed to form active metal oxo (MO) species and to be uniquely active for the homolytic cleavage of the carbon-hydrogen bonds in light alkanes producing intermediates which can form alcohols. We continue to investigate three molecular environments for the active catalytic species that we are trying to generate: electron-deficient porphryinic macrocycles (PHASE I), polyoxometallates (PHASE II), and regular oxidic lattices including zeolites and related structures as well as other molecular surface structures having metal oxo groups (PHASE III).« less

3D printing in chemical engineering and catalytic technology: structured catalysts, mixers and reactors.

PubMed

Parra-Cabrera, Cesar; Achille, Clement; Kuhn, Simon; Ameloot, Rob

2018-01-02

Computer-aided fabrication technologies combined with simulation and data processing approaches are changing our way of manufacturing and designing functional objects. Also in the field of catalytic technology and chemical engineering the impact of additive manufacturing, also referred to as 3D printing, is steadily increasing thanks to a rapidly decreasing equipment threshold. Although still in an early stage, the rapid and seamless transition between digital data and physical objects enabled by these fabrication tools will benefit both research and manufacture of reactors and structured catalysts. Additive manufacturing closes the gap between theory and experiment, by enabling accurate fabrication of geometries optimized through computational fluid dynamics and the experimental evaluation of their properties. This review highlights the research using 3D printing and computational modeling as digital tools for the design and fabrication of reactors and structured catalysts. The goal of this contribution is to stimulate interactions at the crossroads of chemistry and materials science on the one hand and digital fabrication and computational modeling on the other.

CFD simulation of fatty acid methyl ester production in bubble column reactor

NASA Astrophysics Data System (ADS)

Salleh, N. S. Mohd; Nasir, N. F.

2017-09-01

Non-catalytic transesterification is one of the method that was used to produce the fatty acid methyl ester (FAME) by blowing superheated methanol bubbles continuously into the vegetable oil without using any catalyst. This research aimed to simulate the production of FAME from palm oil in a bubble column reactor. Computational Fluid Dynamic (CFD) simulation was used to predict the distribution of fatty acid methyl ester and other product in the reactor. The fluid flow and component of concentration along the reaction time was investigated and the effects of reaction temperature (523 K and 563 K) on the non-catalytic transesterification process has been examined. The study was carried out using ANSYS CFX 17.1. The finding from the study shows that increasing the temperature leads to higher amount of fatty acid methyl ester can be produced in shorter time. On the other hand, concentration of the component such as triglyceride (TG), glycerol (GL) and fatty acid methyl ester (FAME) can be known when reaching the optimum condition.

Engineering Porous Polymer Hollow Fiber Microfluidic Reactors for Sustainable C-H Functionalization.

PubMed

He, Yingxin; Rezaei, Fateme; Kapila, Shubhender; Rownaghi, Ali A

2017-05-17

Highly hydrophilic and solvent-stable porous polyamide-imide (PAI) hollow fibers were created by cross-linking of bare PAI hollow fibers with 3-aminopropyl trimethoxysilane (APS). The APS-grafted PAI hollow fibers were then functionalized with salicylic aldehyde for binding catalytically active Pd(II) ions through a covalent postmodification method. The catalytic activity of the composite hollow fiber microfluidic reactors (Pd(II) immobilized APS-grafted PAI hollow fibers) was tested via heterogeneous Heck coupling reaction of aryl halides under both batch and continuous-flow reactions in polar aprotic solvents at high temperature (120 °C) and low operating pressure. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma (ICP) analyses of the starting and recycled composite hollow fibers indicated that the fibers contain very similar loadings of Pd(II), implying no degree of catalyst leaching from the hollow fibers during reaction. The composite hollow fiber microfluidic reactors showed long-term stability and strong control over the leaching of Pd species.

Removal of toxic Cr(VI) ions from tannery industrial wastewater using a newly designed three-phase three-dimensional electrode reactor

NASA Astrophysics Data System (ADS)

Grace Pavithra, K.; Senthil Kumar, P.; Carolin Christopher, Femina; Saravanan, A.

2017-11-01

In this research, the wastewater samples were collected from leather tanning industry at different time intervals. The parameters like pH, electrical conductivity, temperature, turbidity, chromium and chemical oxygen demand (COD) of the samples were analyzed. A three-phase three-dimensional fluidized type electrode reactor (FTER) was newly designed for the effective removal of toxic pollutants from wastewater. The influencing parameters were optimized for the maximum removal of toxic pollutants from wastewater. The optimum condition for the present system was calculated as: contact time of 30 min, applied voltage of 3 V and the particle electrodes of 15 g. The particle electrode was characterized by using FT-IR analysis. Langmuir-Hinshelwood and pseudo-second order kinetic models were fits well with the experimental data. The results showed that the FTER can be successfully employed for the treatment of industrial wastewater.

Carbonaceous material for production of hydrogen from low heating value fuel gases

DOEpatents

Koutsoukos, Elias P.

1989-01-01

A process for the catalytic production of hydrogen, from a wide variety of low heating value fuel gases containing carbon monoxide, comprises circulating a carbonaceous material between two reactors--a carbon deposition reactor and a steaming reactor. In the carbon deposition reactor, carbon monoxide is removed from a fuel gas and is deposited on the carbonaceous material as an active carbon. In the steaming reactor, the reactive carbon reacts with steam to give hydrogen and carbon dioxide. The carbonaceous material contains a metal component comprising from about 75% to about 95% cobalt, from about 5% to about 15% iron, and up to about 10% chromium, and is effective in suppressing the production of methane in the steaming reactor.

Characterization of ozone decomposition in a soil slurry: kinetics and mechanism.

PubMed

Lim, Hyung-Nam; Choi, Hechul; Hwang, Tae-Moon; Kang, Joon-Wun

2002-01-01

A series of soil slurry experiments were performed in a carefully conceived reactor set-up to investigate the characteristics of the catalytic decomposition of ozone on a sand and iron surface. Real time on-line monitoring of ozone in the reaction module was possible using flow injection analysis coupled with a computer-controlled UV detector and data acquisition system. The effects of the soil media and size, ozone dosage, pH and p-CBA as a probe compound were examined at the given experimental conditions. Two apparent phases existed, and ozone instantaneously decomposed within one second in the first phase. These were defined as the instantaneous ozone demand (ID) phase, and the relatively slow decay stage. The interactions of ozone with the soil organic matter (SOM) and metal oxides were attributed mostly to the instantaneous decomposition of ozone. From the probe (p-CBA) experiments, 60-68% of total p-CBA removal occurred during the ID phase. The generation of hydroxyl radicals (OH.) was demonstrated and was closely related with metal oxides as well as SOM. Metal oxides in soil surface were considered to have relatively faster reaction rate with ozone and provide more favorable reactive sites to generate higher amount of OH. than SOM. Even at one-tenth concentration of the sands, a goethite-induced catalytic reaction outfitted the removal rate ofp-CBA among all the soils tested. More than 40% of total p-CBA removal occurred on the soil surface. It was inferred that the radical reaction with the probe compound seemed to take place not only on the soil surface but also in the solid-liquid interface. Ozone decomposition and the reaction between OH. and p-CBA appeared to be independent of any change in pH.

Influence of biomass pretreatment on upgrading of bio-oil: Comparison of dry and hydrothermal torrefaction.

PubMed

Xu, Xiwei; Tu, Ren; Sun, Yan; Li, Zhiyu; Jiang, Enchen

2018-08-01

The dry and hydrothermal torrefacation of on Camellia Shell (CS) was carried on three different devices- batch autoclave, quartz tube, and auger reactor. The torrefied bio-char products were investigated via TGA, elemental analysis and industrial analysis. Moreover, the pyrolysis and catalytic pyrolysis properties of torrefied bio-char were investigated. The results showed torrefaction significantly influenced the content of hemicellulose in CS. And hydrothermal torrefaction via batch autoclave and dry torrefaction via auger reactors promoted the hemicellulose to strip from the CS. Quartz tube and auger reactor were beneficial for devolatilization and improving heat value of torrefied bio-char. The result showed that the main products were phenols and acids. And hydrothermal torrefaction pretreatment effectively reduced the acids content from 34.5% to 13.2% and enriched the content of phenols (from 27.23% to 60.05%) in bio-oil due to the decreasing of hemicellulos in torrefied bio-char. And the catalyst had slight influence on the bio-oil distribution. Copyright © 2018 Elsevier Ltd. All rights reserved.

Transmutation of All German Transuranium under Nuclear Phase Out Conditions – Is This Feasible from Neutronic Point of View?

PubMed Central

Merk, Bruno; Litskevich, Dzianis

2015-01-01

The German government has decided for the nuclear phase out, but a decision on a strategy for the management of the highly radioactive waste is not defined yet. Partitioning and Transmutation (P&T) could be considered as a technological option for the management of highly radioactive waste, therefore a wide study has been conducted. In the study group objectives for P&T and the boundary conditions of the phase out have been discussed. The fulfillment of the given objectives is analyzed from neutronics point of view using simulations of a molten salt reactor with fast neutron spectrum. It is shown that the efficient transmutation of all existing transuranium isotopes would be possible from neutronic point of view in a time frame of about 60 years. For this task three reactors of a mostly new technology would have to be developed and a twofold life cycle consisting of a transmuter operation and a deep burn phase would be required. A basic insight for the optimization of the time duration of the deep burn phase is given. Further on, a detailed balance of different isotopic inventories is given to allow a deeper understanding of the processes during transmutation in the molten salt fast reactor. The effect of modeling and simulation is investigated based on three different modeling strategies and two different code versions. PMID:26717509

Transmutation of All German Transuranium under Nuclear Phase Out Conditions - Is This Feasible from Neutronic Point of View?

PubMed

Merk, Bruno; Litskevich, Dzianis

2015-01-01

The German government has decided for the nuclear phase out, but a decision on a strategy for the management of the highly radioactive waste is not defined yet. Partitioning and Transmutation (P&T) could be considered as a technological option for the management of highly radioactive waste, therefore a wide study has been conducted. In the study group objectives for P&T and the boundary conditions of the phase out have been discussed. The fulfillment of the given objectives is analyzed from neutronics point of view using simulations of a molten salt reactor with fast neutron spectrum. It is shown that the efficient transmutation of all existing transuranium isotopes would be possible from neutronic point of view in a time frame of about 60 years. For this task three reactors of a mostly new technology would have to be developed and a twofold life cycle consisting of a transmuter operation and a deep burn phase would be required. A basic insight for the optimization of the time duration of the deep burn phase is given. Further on, a detailed balance of different isotopic inventories is given to allow a deeper understanding of the processes during transmutation in the molten salt fast reactor. The effect of modeling and simulation is investigated based on three different modeling strategies and two different code versions.

Removal of ammonia solutions used in catalytic wet oxidation processes.

PubMed

Hung, Chang Mao; Lou, Jie Chung; Lin, Chia Hua

2003-08-01

Ammonia (NH(3)) is an important product used in the chemical industry, and is common place in industrial wastewater. Industrial wastewater containing ammonia is generally either toxic or has concentrations or temperatures such that direct biological treatment is unfeasible. This investigation used aqueous solutions containing more of ammonia for catalytic liquid-phase oxidation in a trickle-bed reactor (TBR) based on Cu/La/Ce composite catalysts, prepared by co-precipitation of Cu(NO(3))(2), La(NO(3))(2), and Ce(NO(3))(3) at 7:2:1 molar concentrations. The experimental results indicated that the ammonia conversion of the wet oxidation in the presence of the Cu/La/Ce composite catalysts was determined by the Cu/La/Ce catalyst. Minimal ammonia was removed from the solution by the wet oxidation in the absence of any catalyst, while approximately 91% ammonia removal was achieved by wet oxidation over the Cu/La/Ce catalyst at 230 degrees C with oxygen partial pressure of 2.0 MPa. Furthermore, the effluent streams were conducted at a liquid hourly space velocity of under 9 h(-1) in the wet catalytic processes, and a reaction pathway was found linking the oxidizing ammonia to nitric oxide, nitrogen and water. The solution contained by-products, including nitrates and nitrites. Nitrite selectivity was minimized and ammonia removal maximized when the feed ammonia solution had a pH of around 12.0.

Zircon Supported Copper Catalysts for the Steam Reforming of Methanol

NASA Astrophysics Data System (ADS)

Widiastri, M.; Fendy, Marsih, I. N.

2008-03-01

Steam reforming of methanol (SRM) is known as one of the most favorable catalytic processes for producing hydrogen. Current research on zirconia, ZrO2 supported copper catalyst revealed that CuO/ZrO2 as an active catalyst for the SRM. Zircon, ZrSiO4 is available from the by-product of tin mining. In the work presented here, the catalytic properties of CuO/ZrSiO4 with various copper oxide compositions ranging from 2.70% (catalyst I), 4.12% (catalyst II), and 7.12%-mass (catalyst III), synthesized by an incipient wetness impregnation technique, were investigated to methanol conversion, selectivity towards CO formation, and effect of ZnO addition (7.83%CuO/8.01%ZnO/ZrSiO4 = catalyst V). The catalytic activity was obtained using a fixed bed reactor and the zircon supported catalyst activity was compared to those of CuO/ZnO/Al2O3 catalyst (catalyst IV) and commercial Kujang LTSC catalyst. An X-ray powder diffraction (XRD) analysis was done to identify the abundant phases of the catalysts. The catalysts topography and particle diameter were measured with scanning electron microscopy (SEM) and composition of the catalysts was measured by SEM-EDX, scanning electron microscope-energy dispersive using X-ray analysis. The results of this research provide information on the possibility of using zircon (ZrSiO4) as solid support for SRM catalysts.

Catalytic Upgrading of Biomass Pyrolysis Oxygenates with Vacuum Gas Oil Using a Davison Circulating Riser Reactor

DOE PAGES

Jarvis, Mark W.; Olstad, Jessica; Parent, Yves; ...

2018-01-02

We investigate and quantitate the changes in hydrocarbon product composition while evaluating the performance and operability of the National Renewable Energy Laboratory's Davison Circulating Riser (DCR) reactor system when biomass model compounds are cofed with traditional fluid catalyst cracking (FCC) feeds and catalyst: vacuum gas oil (VGO) and equilibrium zeolite catalyst (E-Cat). Three compounds (acetic acid, guaiacol, and sorbitan monooleate) were selected to represent the major classes of oxygenates present in biomass pyrolysis vapors. These vapors can contain 30-50% oxygen as oxygenates, which create conversion complications (increased reactivity and coking) when integrating biomass vapors and liquids into fuel and chemicalmore » processes long dominated by petroleum feedstocks. We used these model compounds to determine the appropriate conditions for coprocessing with petroleum and ultimately pure pyrolysis vapors only as compared with standard baseline conditions obtained with VGO and E-Cat only in the DCR. Model compound addition decreased the DCR catalyst circulation rate, which controls reactor temperature and measures reaction heat demand, while increasing catalyst coking rates. Liquid product analyses included 2-dimensional gas chromatography time-of-flight mass spectroscopy (2D GCxGC TOFS), simulated distillation (SIM DIST), 13C NMR, and carbonyl content. Aggregated results indicated that the model compounds were converted during reaction, and despite functional group differences, product distributions for each model compound were very similar. In addition, we determined that adding model compounds to the VGO feed did not significantly affect the DCR's operability or performance. Future work will assess catalytic upgrading of biomass pyrolysis vapor to fungible hydrocarbon products using upgrading catalysts currently being developed at NREL and at Johnson Matthey.« less

Catalytic Upgrading of Biomass Pyrolysis Oxygenates with Vacuum Gas Oil Using a Davison Circulating Riser Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jarvis, Mark W.; Olstad, Jessica; Parent, Yves

We investigate and quantitate the changes in hydrocarbon product composition while evaluating the performance and operability of the National Renewable Energy Laboratory's Davison Circulating Riser (DCR) reactor system when biomass model compounds are cofed with traditional fluid catalyst cracking (FCC) feeds and catalyst: vacuum gas oil (VGO) and equilibrium zeolite catalyst (E-Cat). Three compounds (acetic acid, guaiacol, and sorbitan monooleate) were selected to represent the major classes of oxygenates present in biomass pyrolysis vapors. These vapors can contain 30-50% oxygen as oxygenates, which create conversion complications (increased reactivity and coking) when integrating biomass vapors and liquids into fuel and chemicalmore » processes long dominated by petroleum feedstocks. We used these model compounds to determine the appropriate conditions for coprocessing with petroleum and ultimately pure pyrolysis vapors only as compared with standard baseline conditions obtained with VGO and E-Cat only in the DCR. Model compound addition decreased the DCR catalyst circulation rate, which controls reactor temperature and measures reaction heat demand, while increasing catalyst coking rates. Liquid product analyses included 2-dimensional gas chromatography time-of-flight mass spectroscopy (2D GCxGC TOFS), simulated distillation (SIM DIST), 13C NMR, and carbonyl content. Aggregated results indicated that the model compounds were converted during reaction, and despite functional group differences, product distributions for each model compound were very similar. In addition, we determined that adding model compounds to the VGO feed did not significantly affect the DCR's operability or performance. Future work will assess catalytic upgrading of biomass pyrolysis vapor to fungible hydrocarbon products using upgrading catalysts currently being developed at NREL and at Johnson Matthey.« less

Radiocarbon tracer measurements of atmospheric hydroxyl radical concentrations

NASA Technical Reports Server (NTRS)

Campbell, M. J.; Farmer, J. C.; Fitzner, C. A.; Henry, M. N.; Sheppard, J. C.

1986-01-01

The usefulness of the C-14 tracer in measurements of atmospheric hydroxyl radical concentration is discussed. The apparatus and the experimental conditions of three variations of a radiochemical method of atmosphere analysis are described and analyzed: the Teflon bag static reactor, the flow reactor (used in the Wallops Island tests), and the aircraft OH titration reactor. The procedure for reduction of the aircraft reactor instrument data is outlined. The problems connected with the measurement of hydroxyl radicals are discussed. It is suggested that the gas-phase radioisotope methods have considerable potential in measuring tropospheric impurities present in very low concentrations.

61. VIEW LOOKING NORTHWEST AT A SIGNAL REACTOR OR CHOKE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

61. VIEW LOOKING NORTHWEST AT A SIGNAL REACTOR OR CHOKE COIL. WITHIN THE PROTECTIVE ENCLOSURE IS AN AIR AND PORCELAIN INSULATED COIL OF 5/8' DIAMETER STRANDED COPPER WIRE. REACTOR COILS WERE PLACED IN SERIES WITH EACH LEG OF THREE PHASE GENERATORS. THEIR FUNCTION WAS TO MODERATE SURGES OF CURRENT CAUSED BY LIGHTNING STRIKES, OPEN OR SHORT CIRCUIT PROBLEMS ON THE LINE. - New York, New Haven & Hartford Railroad, Cos Cob Power Plant, Sound Shore Drive, Greenwich, Fairfield County, CT

Low Cost Olefin Production from Shale Gas by Laser Enhanced Pyrolysis through Spatial Beam Decoherence. Phase 1 Final Report.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hutton, Phillip N.

This report describes research into an innovative laser-enhanced catalytic pyrolysis technology that has the potential to significantly decrease the cost of cracking ethane and other alkanes found in shale gas ethylene. Similar to how water is resonantly heated by microwaves, a CO 2 laser can resonantly heat ethylene, producing radicals that convert ethane to ethylene at lower reactor temperatures. Proof of concept experiments were performed to determine if commercial grade CO 2 lasers at one-twenty fifth the cost of scientific grade lasers could crack ethane at lower temperatures than conventional technology. Cr doped MgO catalyst was then inserted in themore » reaction chamber to further increase conersion rates.« less

Dual-channel microreactor for gas-liquid syntheses.

PubMed

Park, Chan Pil; Kim, Dong-Pyo

2010-07-28

A microreactor consisting of two microfluidic channels that are separated by a thin membrane is devised for intimate contact between gas and liquid phases. Gas flowing in one microchannel can diffuse into the liquid flowing in the other microchannel through the thin membrane. An oxidative Heck reaction carried out in the dual-channel (DC) microreactor, in which gaseous oxygen plays a key role in the catalytic reaction, shows the significant improvement that can be made over the traditional batch reactor and the conventional segmental microreactor in terms of yield, selectivity, and reaction time. It also allows independent control of the flow of the gaseous reagent. The proposed DC microreactor should prove to be a powerful tool for fully exploring gas-liquid microchemistry.

Performance Characterization of a Prototype Ultra-Short Channel Monolith Catalytic Reactor for Air Quality Control Applications

NASA Technical Reports Server (NTRS)

Perry, J. L.; Tomes, K. M.; Roychoudhury, S.; Tatara, J. D.

2005-01-01

Contaminated air and process gases, whether in a crewed spacecraft cabin atmosphere, the working volume of a microgravity science or ground-based laboratory experiment facility, or the exhaust from an automobile, are pervasive problems that ultimately effect human health, performance, and well-being. The need for highly-effective, economical decontamination processes spans a wide range of terrestrial and space flight applications. Adsorption processes are used widely for process gas decontamination. Most industrial packed bed adsorption processes use activated carbon because it is cheap and highly effective. Once saturated, however, the adsorbent is a concentrated source of contaminants. Industrial applications either dump or regenerate the activated carbon. Regeneration may be accomplished in-situ or at an off-site location. In either case, concentrated contaminated waste streams must be handled appropriately to minimize environmental impact. As economic and regulatory forces drive toward minimizing waste and environmental impact, thermal catalytic oxidation is becoming more attractive. Through novel reactor and catalyst design, more complete contaminant destruction and greater resistance to poisoning can achieved leading to less waste handling, process down-time, and maintenance. Performance of a prototype thermal catalytic reactor, based on ultra-short channel monolith (USCM) catalyst substrate design, under a variety of process flow and contaminant loading conditions is discussed. The experimental results are evaluated against present and future air quality control and process gas purification processes used on board crewed spacecraft.

Catalysis in high-temperature fuel cells.

PubMed

Föger, K; Ahmed, K

2005-02-17

Catalysis plays a critical role in solid oxide fuel cell systems. The electrochemical reactions within the cell--oxygen dissociation on the cathode and electrochemical fuel combustion on the anode--are catalytic reactions. The fuels used in high-temperature fuel cells, for example, natural gas, propane, or liquid hydrocarbons, need to be preprocessed to a form suitable for conversion on the anode-sulfur removal and pre-reforming. The unconverted fuel (economic fuel utilization around 85%) is commonly combusted using a catalytic burner. Ceramic Fuel Cells Ltd. has developed anodes that in addition to having electrochemical activity also are reactive for internal steam reforming of methane. This can simplify fuel preprocessing, but its main advantage is thermal management of the fuel cell stack by endothermic heat removal. Using this approach, the objective of fuel preprocessing is to produce a methane-rich fuel stream but with all higher hydrocarbons removed. Sulfur removal can be achieved by absorption or hydro-desulfurization (HDS). Depending on the system configuration, hydrogen is also required for start-up and shutdown. Reactor operating parameters are strongly tied to fuel cell operational regimes, thus often limiting optimization of the catalytic reactors. In this paper we discuss operation of an authothermal reforming reactor for hydrogen generation for HDS and start-up/shutdown, and development of a pre-reformer for converting propane to a methane-rich fuel stream.

The sugar model: catalytic flow reactor dynamics of pyruvaldehyde synthesis from triose catalyzed by poly-l-lysine contained in a dialyzer

NASA Technical Reports Server (NTRS)

Weber, A. L.

2001-01-01

The formation of pyruvaldehyde from triose sugars was catalyzed by poly-l-lysine contained in a small dialyzer with a 100 molecular weight cut off (100 MWCO) suspended in a much larger triose substrate reservoir at pH 5.5 and 40 degrees C. The polylysine confined in the dialyzer functioned as a catalytic flow reactor that constantly brought in triose from the substrate reservoir by diffusion to offset the drop in triose concentration within the reactor caused by its conversion to pyruvaldehyde. The catalytic polylysine solution (400 mM, 0.35 mL) within the dialyzer generated pyruvaldehyde with a synthetic intensity (rate/volume) that was 3400 times greater than that of the triose substrate solution (12 mM, 120 mL) outside the dialyzer. Under the given conditions the final yield of pyruvaldehyde was greater than twice the weight of the polylysine catalyst. During the reaction the polylysine catalyst was poisoned presumably by reaction of its amino groups with aldehyde reactants and products. Similar results were obtained using a dialyzer with a 500 MWCO. The dialyzer method of catalyst containment was selected because it provides a simple and easily manipulated experimental system for studying the dynamics and evolutionary development of confined autocatalytic processes related to the origin of life under anaerobic conditions.

Chemical compatibility issues associated with use of SiC/SiC in advanced reactor concepts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilson, Dane F.

2015-09-01

Silicon carbide/silicon carbide (SiC/SiC) composites are of interest for components that will experience high radiation fields in the High Temperature Gas Cooled Reactor (HTGR), the Very High Temperature Reactor (VHTR), the Sodium Fast Reactor (SFR), or the Fluoride-cooled High-temperature Reactor (FHR). In all of the reactor systems considered, reactions of SiC/SiC composites with the constituents of the coolant determine suitability of materials of construction. The material of interest is nuclear grade SiC/SiC composites, which consist of a SiC matrix [high-purity, chemical vapor deposition (CVD) SiC or liquid phase-sintered SiC that is crystalline beta-phase SiC containing small amounts of alumina-yttria impurity],more » a pyrolytic carbon interphase, and somewhat impure yet crystalline beta-phase SiC fibers. The interphase and fiber components may or may not be exposed, at least initially, to the reactor coolant. The chemical compatibility of SiC/SiC composites in the three reactor environments is highly dependent on thermodynamic stability with the pure coolant, and on reactions with impurities present in the environment including any ingress of oxygen and moisture. In general, there is a dearth of information on the performance of SiC in these environments. While there is little to no excess Si present in the new SiC/SiC composites, the reaction of Si with O 2 cannot be ignored, especially for the FHR, in which environment the product, SiO 2, can be readily removed by the fluoride salt. In all systems, reaction of the carbon interphase layer with oxygen is possible especially under abnormal conditions such as loss of coolant (resulting in increased temperature), and air and/ or steam ingress. A global outline of an approach to resolving SiC/SiC chemical compatibility concerns with the environments of the three reactors is presented along with ideas to quickly determine the baseline compatibility performance of SiC/SiC.« less

Numerical investigation of flow and heat transfer in a novel configuration multi-tubular fixed bed reactor for propylene to acrolein process

NASA Astrophysics Data System (ADS)

Jiang, Bin; Hao, Li; Zhang, Luhong; Sun, Yongli; Xiao, Xiaoming

2015-01-01

In the present contribution, a numerical study of fluid flow and heat transfer performance in a pilot-scale multi-tubular fixed bed reactor for propylene to acrolein oxidation reaction is presented using computational fluid dynamics (CFD) method. Firstly, a two-dimensional CFD model is developed to simulate flow behaviors, catalytic oxidation reaction, heat and mass transfer adopting porous medium model on tube side to achieve the temperature distribution and investigate the effect of operation parameters on hot spot temperature. Secondly, based on the conclusions of tube-side, a novel configuration multi-tubular fixed-bed reactor comprising 790 tubes design with disk-and-doughnut baffles is proposed by comparing with segmental baffles reactor and their performance of fluid flow and heat transfer is analyzed to ensure the uniformity condition using molten salt as heat carrier medium on shell-side by three-dimensional CFD method. The results reveal that comprehensive performance of the reactor with disk-and-doughnut baffles is better than that of with segmental baffles. Finally, the effects of operating conditions to control the hot spots are investigated. The results show that the flow velocity range about 0.65 m/s is applicable and the co-current cooling system flow direction is better than counter-current flow to control the hottest temperature.

Process to convert biomass and refuse derived fuel to ethers and/or alcohols

DOEpatents

Diebold, James P.; Scahill, John W.; Chum, Helena L.; Evans, Robert J.; Rejai, Bahman; Bain, Richard L.; Overend, Ralph P.

1996-01-01

A process for conversion of a feedstock selected from the group consisting of biomass and refuse derived fuel (RDF) to provide reformulated gasoline components comprising a substantial amount of materials selected from the group consisting of ethers, alcohols, or mixtures thereof, comprising: drying said feedstock; subjecting said dried feedstock to fast pyrolysis using a vortex reactor or other means; catalytically cracking vapors resulting from said pyrolysis using a zeolite catalyst; condensing any aromatic byproduct fraction; catalytically alkylating any benzene present in said vapors after condensation; catalytically oligomerizing any remaining ethylene and propylene to higher olefins; isomerizing said olefins to reactive iso-olefins; and catalytically reacting said iso-olefins with an alcohol to form ethers or with water to form alcohols.

Parametric Investigation of the Kinetics of Growth of Carbon-Nanotube Arrays on Iron Nanoparticles in the Process of Chemical Vapor Deposition of Hydrocarbons

NASA Astrophysics Data System (ADS)

Futko, S. I.; Shulitski, B. G.; Labunov, V. A.; Ermolaevaa, E. M.

2015-03-01

On the basis of the kinetic model of synthesis of carbon nanotubes on iron nanoparticles in the process of chemical vapor deposition of hydrocarbons, the parametric dependences of characteristics of arrays of vertically oriented nanotubes on the temperature of their synthesis, the concentration of acetylene in a reactor, and the diameter of the catalyst nanoparticles were investigated. It is shown that the maximum on the temperature dependence of the rate of growth of carbon nanotubes, detected in experiments at a temperature of ~700oC is due to the competing processes of increasing the catalytic activity of iron nanoparticles and decreasing the acetylene concentration because of the signifi cant gas-phase decomposition of acetylene in the reactor before it enters the substrate with the catalyst. Our calculations have shown that the indicated maximum arises near the transition point separating the low-temperature region where multiwall nanotubes are predominantly synthesized from the higher-temperature region of generation of single-wall nanotubes in the process of chemical vapor deposition of hydrocarbons.

Critical size of crystalline ZrO(2) nanoparticles synthesized in near- and supercritical water and supercritical isopropyl alcohol.

PubMed

Becker, Jacob; Hald, Peter; Bremholm, Martin; Pedersen, Jan S; Chevallier, Jacques; Iversen, Steen B; Iversen, Bo B

2008-05-01

Nanocrystalline ZrO(2) samples with narrow size distributions and mean particle sizes below 10 nm have been synthesized in a continuous flow reactor in near and supercritical water as well as supercritical isopropyl alcohol using a wide range of temperatures, pressures, concentrations and precursors. The samples were comprehensively characterized by powder X-ray diffraction (PXRD), transmission electron microscopy (TEM), and small-angle X-ray scattering (SAXS), and the influence of the synthesis parameters on the particle size, particle size distribution, shape, aggregation and crystallinity was studied. On the basis of the choice of synthesis parameters either monoclinic or tetragonal zirconia phases can be obtained. The results suggest a critical particle size of 5-6 nm for nanocrystalline monoclinic ZrO(2) under the present conditions, which is smaller than estimates reported in the literature. Thus, very small monoclinic ZrO(2) particles can be obtained using a continuous flow reactor. This is an important result with respect to improvement of the catalytic properties of nanocrystalline ZrO(2).

A submerged ceramic membrane reactor for the p-nitrophenol hydrogenation over nano-sized nickel catalysts.

PubMed

Chen, R Z; Sun, H L; Xing, W H; Jin, W Q; Xu, N P

2009-02-01

The catalytic hydrogenation of p-nitrophenol to p-aminophenol over nano-sized nickel catalysts was carried out in a submerged ceramic membrane reactor. It has been demonstrated that the submerged ceramic membrane reactor is more suitable for the p-nitrophenol hydrogenation over nano-sized nickel catalysts compared with the side-stream ceramic membrane reactor, and the membrane module configuration has a great influence on the reaction rate of p-nitrophenol hydrogenation and the membrane treating capacity. The deactivation of nano-sized nickel is mainly caused by the adsorption of impurity on the surface of nickel and the increase of oxidation degree of nickel.

Thermal Catalytic Oxidation of Airborne Contaminants by a Reactor Using Ultra-Short Channel Length, Monolithic Catalyst Substrates

NASA Technical Reports Server (NTRS)

Perry, J. L.; Tomes, K. M.; Tatara, J. D.

2005-01-01

Contaminated air, whether in a crewed spacecraft cabin or terrestrial work and living spaces, is a pervasive problem affecting human health, performance, and well being. The need for highly effective, economical air quality processes spans a wide range of terrestrial and space flight applications. Typically, air quality control processes rely on absorption-based processes. Most industrial packed-bed adsorption processes use activated carbon. Once saturated, the carbon is either dumped or regenerated. In either case, the dumped carbon and concentrated waste streams constitute a hazardous waste that must be handled safely while minimizing environmental impact. Thermal catalytic oxidation processes designed to address waste handling issues are moving to the forefront of cleaner air quality control and process gas decontamination processes. Careful consideration in designing the catalyst substrate and reactor can lead to more complete contaminant destruction and poisoning resistance. Maintenance improvements leading to reduced waste handling and process downtime can also be realized. Performance of a prototype thermal catalytic reaction based on ultra-short waste channel, monolith catalyst substrate design, under a variety of process flow and contaminant loading conditions, is discussed.

Hydrothermal gasification of Cladophora glomerata macroalgae over its hydrochar as a catalyst for hydrogen-rich gas production.

PubMed

Safari, Farid; Norouzi, Omid; Tavasoli, Ahmad

2016-12-01

A tubular batch micro-reactor system was used for hydrothermal gasification (HTG) of Cladophora glomerata (C. glomerata) as green macroalgae found in the southern coast of the Caspian Sea, Iran. Non-catalytic tests were performed to determine the optimum condition for hydrogen production. Hydrochar, as a solid residue of non-catalytic HTG was characterized by BET, FESEM, and ICP-OES methods to determine its physiochemical properties. Surface area and pore volume of C. glomerata increased drastically after HTG. Also, the aqueous products were identified and quantified by GC-MS and GC-FID methods. Hydrochar was loaded to the reactor to determine its catalytic effect on HTG. HTG was promoted by inorganic compounds in the hydrochar and its porosity. The maximum hydrogen yield of 9.63mmol/g was observed in the presence of algal hydrochar with the weight ratio of 0.4 to feedstock. Also, acids production was inhibited while phenol production was promoted in the presence of hydrochar. Copyright © 2016 Elsevier Ltd. All rights reserved.

Optimization of Boiling Water Reactor Loading Pattern Using Two-Stage Genetic Algorithm

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kobayashi, Yoko; Aiyoshi, Eitaro

2002-10-15

A new two-stage optimization method based on genetic algorithms (GAs) using an if-then heuristic rule was developed to generate optimized boiling water reactor (BWR) loading patterns (LPs). In the first stage, the LP is optimized using an improved GA operator. In the second stage, an exposure-dependent control rod pattern (CRP) is sought using GA with an if-then heuristic rule. The procedure of the improved GA is based on deterministic operators that consist of crossover, mutation, and selection. The handling of the encoding technique and constraint conditions by that GA reflects the peculiar characteristics of the BWR. In addition, strategies suchmore » as elitism and self-reproduction are effectively used in order to improve the search speed. The LP evaluations were performed with a three-dimensional diffusion code that coupled neutronic and thermal-hydraulic models. Strong axial heterogeneities and constraints dependent on three dimensions have always necessitated the use of three-dimensional core simulators for BWRs, so that optimization of computational efficiency is required. The proposed algorithm is demonstrated by successfully generating LPs for an actual BWR plant in two phases. One phase is only LP optimization applying the Haling technique. The other phase is an LP optimization that considers the CRP during reactor operation. In test calculations, candidates that shuffled fresh and burned fuel assemblies within a reasonable computation time were obtained.« less

Investigation of a catalytic gas generator for the Space Shuttle APU. [hydrazine Auxiliary Propulsion Unit

NASA Technical Reports Server (NTRS)

Emmons, D. L.; Huxtable, D. D.; Blevins, D. R.

1974-01-01

An investigation was conducted to establish the capability of a monopropellant hydrazine catalytic gas generator to meet the requirements specified for the Space Shuttle APU. Detailed analytical and experimental studies were conducted on potential problem areas including long-term nitriding effects on materials, design variables affecting catalyst life, vehicle vibration effects, and catalyst oxidation/contamination. A full-scale gas generator, designed to operate at a chamber pressure of 750 psia and a flow rate of 0.36 lbm/sec, was fabricated and subjected to three separate life test series. The objective of the first test series was to demonstrate the capability of the gas generator to successfully complete 20 simulated Space Shuttle missions in steady-state operation. The gas generator was then refurbished and subjected to a second series of tests to demonstrate the pulse-mode capability of the gas generator during 20 simulated missions. The third series of tests was conducted with a refurbished reactor to further demonstrate pulse-mode capability with a modified catalyst bed.

Advanced treatment of biologically pretreated coal gasification wastewater by a novel integration of heterogeneous catalytic ozonation and biological process.

PubMed

Zhuang, Haifeng; Han, Hongjun; Jia, Shengyong; Hou, Baolin; Zhao, Qian

2014-08-01

Advanced treatment of biologically pretreated coal gasification wastewater (CGW) was investigated employing heterogeneous catalytic ozonation integrated with anoxic moving bed biofilm reactor (ANMBBR) and biological aerated filter (BAF) process. The results indicated that catalytic ozonation with the prepared catalyst (i.e. MnOx/SBAC, sewage sludge was converted into sludge based activated carbon (SBAC) which loaded manganese oxides) significantly enhanced performance of pollutants removal by generated hydroxyl radicals. The effluent of catalytic ozonation process was more biodegradable and less toxic than that in ozonation alone. Meanwhile, ANMBBR-BAF showed efficient capacity of pollutants removal in treatment of the effluent of catalytic ozonation at a shorter reaction time, allowing the discharge limits to be met. Therefore, the integrated process with efficient, economical and sustainable advantages was suitable for advanced treatment of real biologically pretreated CGW. Copyright © 2014 Elsevier Ltd. All rights reserved.

VUV photo-oxidation of gaseous benzene combined with ozone-assisted catalytic oxidation: Effect on transition metal catalyst

NASA Astrophysics Data System (ADS)

Huang, Haibao; Lu, Haoxian; Zhan, Yujie; Liu, Gaoyuan; Feng, Qiuyu; Huang, Huiling; Wu, Muyan; Ye, Xinguo

2017-01-01

Volatile organic compounds (VOCs) cause the major air pollution concern. In this study, a series of ZSM-5 supported transition metals were prepared by impregnation method. They were combined with vacuum UV (VUV) photo-oxidation in a continuous-flow packed-bed reactor and used for the degradation of benzene, a typical toxic VOCs. Compared with VUV photo-oxidation alone, the introduction of catalysts can greatly enhance benzene oxidation under the help of O3, the by-products from VUV irradiation, via ozone-assisted catalytic oxidation (OZCO). The catalytic activity of transition metals towards benzene oxidation followed the order: Mn > Co > Cu > Ni > Fe. Mn achieved the best catalytic activity due to the strongest capability for O3 catalytic decomposition and utilization. Benzene and O3 removal efficiency reached as high as 97% and 100% after 360 min, respectively. O3 was catalytically decomposed, generating highly reactive oxidants such as rad OH and rad O for benzene oxidation.

Computational Flow Modeling of Hydrodynamics in Multiphase Trickle-Bed Reactors

NASA Astrophysics Data System (ADS)

Lopes, Rodrigo J. G.; Quinta-Ferreira, Rosa M.

2008-05-01

This study aims to incorporate most recent multiphase models in order to investigate the hydrodynamic behavior of a TBR in terms of pressure drop and liquid holdup. Taking into account transport phenomena such as mass and heat transfer, an Eulerian k-fluid model was developed resulting from the volume averaging of the continuity and momentum equations and solved for a 3D representation of the catalytic bed. Computational fluid dynamics (CFD) model predicts hydrodynamic parameters quite well if good closures for fluid/fluid and fluid/particle interactions are incorporated in the multiphase model. Moreover, catalytic performance is investigated with the catalytic wet oxidation of a phenolic pollutant.

CONTROL OF INDUSTRIAL VOC (VOLATILE ORGANIC COMPOUND) EMISSIONS BY CATALYTIC INCINERATION. VOLUME 8. CATALYTIC INCINERATOR PERFORMANCE AT INDUSTRIAL SITE C-6

EPA Science Inventory

The report is part of a two-phase EPA effort to assess the performance, suitability, and costs of various technologies to control emissions of volatile organic compounds (VOCs). In Phase 1, information was assembled from the literature on the use and cost of using catalytic incin...

CONTROL OF INDUSTRIAL VOC (VOLATILE ORGANIC COMPOUND) EMISSIONS BY CATALYTIC INCINERATION. VOLUME 1. ASSESSMENT OF CATALYTIC INCINERATION AND COMPETING CONTROLS

EPA Science Inventory

The report is part of a two-phase EPA effort to assess the performance, suitability, and costs of various technologies to control emissions of volatile organic compounds (VOCs). In Phase 1, information was assembled from the literature on the use and cost of using catalytic incin...

CONTROL OF INDUSTRIAL VOC (VOLATILE ORGANIC COMPOUND) EMISSIONS BY CATALYTIC INCINERATION. VOLUME 7. CATALYTIC INCINERATOR PERFORMANCE AT INDUSTRIAL SITE C-5

EPA Science Inventory

The report is part of a two-phase EPA effort to assess the performance, suitability, and costs of various technologies to control emissions of volatile organic compounds (VOCs). In Phase 1, information was assembled from the literature on the use and cost of using catalytic incin...

CONTROL OF INDUSTRIAL VOC (VOLATILE ORGANIC COMPOUND) EMISSIONS BY CATALYTIC INCINERATION. VOLUME 5. CATALYTIC INCINERATOR PERFORMANCE AT INDUSTRIAL SITE C-3

EPA Science Inventory

The report is part of a two-phase EPA effort to assess the performance, suitability, and costs of various technologies to control emissions of volatile organic compounds (VOCs). In Phase 1, information was assembled from the literature on the use and cost of using catalytic incin...

Evaluation of the Parameters and Conditions of Process in the Ethylbenzene Dehydrogenation with Application of Permselective Membranes to Enhance Styrene Yield.

PubMed

Araújo, Paulo Jardel P; Leite, Manuela Souza; Ravagnani, Teresa M Kakuta

2016-01-01

Styrene is an important monomer in the manufacture of thermoplastic. Most of it is produced by the catalytic dehydrogenation of ethylbenzene. In this process that depends on reversible reactions, the yield is usually limited by the establishment of thermodynamic equilibrium in the reactor. The styrene yield can be increased by using a hybrid process, with reaction and separation simultaneously. It is proposed using permselective composite membrane to remove hydrogen and thus suppress the reverse and secondary reactions. This paper describes the simulation of a dehydrogenation process carried out in a tubular fixed-bed reactor wrapped in a permselective composite membrane. A mathematical model was developed, incorporating the various mass transport mechanisms found in each of the membrane layers and in the catalytic fixed bed. The effects of the reactor feed conditions (temperature, steam-to-oil ratio, and the weight hourly space velocity), the fixed-bed geometry (length, diameter, and volume), and the membrane geometry (thickness of the layers) on the styrene yield were analyzed. These variables were used to determine experimental conditions that favour the production of styrene. The simulation showed that an increase of 40.98% in the styrene yield, compared to a conventional fixed-bed process, could be obtained by wrapping the reactor in a permselective composite membrane.

A Discrepancy-Based Methodology for Nuclear Training Program Evaluation.

ERIC Educational Resources Information Center

Cantor, Jeffrey A.

1991-01-01

A three-phase comprehensive process for commercial nuclear power training program evaluation is presented. The discrepancy-based methodology was developed after the Three Mile Island nuclear reactor accident. It facilitates analysis of program components to identify discrepancies among program specifications, actual outcomes, and industry…

Liquid-phase oxidation of cyclohexanone over cerium oxide catalyst

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shen, H.C.; Weng, H.S.

Catalytic oxidation of cyclohexanone in the liquid phase with glacial acetic acid as the solvent over cerium oxide was studied between 5 and 15 atm and 98 and 118 {degrees} C in a batch reactor. The products were adipic acid, glutaric acid, succinic acid, caprolactone, carbon oxides, etc. The reaction undergoes a short induction period prior to a rapid reaction regime. In both regimes, the reaction is independent of oxygen pressure when the system pressure is above 10 atm. The induction period is inversely proportional to both of the catalyst weight and cyclohexanone concentration.During the rapid reaction regime, the reactionmore » rate was found to be proportional to the 0.5 power of the catalyst weight and to the 1.5 power of the cyclohexanone concentration. Reaction mechanisms and rate expressions are proposed. The carbon oxides produced in this study were much lower than those previously reported. The cerium oxide catalyst is stable during the reaction.« less

Effect of hydrothermal liquefaction aqueous phase recycling on bio-crude yields and composition.

PubMed

Biller, Patrick; Madsen, René B; Klemmer, Maika; Becker, Jacob; Iversen, Bo B; Glasius, Marianne

2016-11-01

Hydrothermal liquefaction (HTL) is a promising thermo-chemical processing technology for the production of biofuels but produces large amounts of process water. Therefore recirculation of process water from HTL of dried distillers grains with solubles (DDGS) is investigated. Two sets of recirculation on a continuous reactor system using K2CO3 as catalyst were carried out. Following this, the process water was recirculated in batch experiments for a total of 10 rounds. To assess the effect of alkali catalyst, non-catalytic HTL process water recycling was performed with 9 recycle rounds. Both sets of experiments showed a large increase in bio-crude yields from approximately 35 to 55wt%. The water phase and bio-crude samples from all experiments were analysed via quantitative gas chromatography-mass spectrometry (GC-MS) to investigate their composition and build-up of organic compounds. Overall the results show an increase in HTL conversion efficiency and a lower volume, more concentrated aqueous by-product following recycling. Copyright © 2016 Elsevier Ltd. All rights reserved.

Process to convert biomass and refuse derived fuel to ethers and/or alcohols

DOEpatents

Diebold, J.P.; Scahill, J.W.; Chum, H.L.; Evans, R.J.; Rejai, B.; Bain, R.L.; Overend, R.P.

1996-04-02

A process is described for conversion of a feedstock selected from the group consisting of biomass and refuse derived fuel (RDF) to provide reformulated gasoline components comprising a substantial amount of materials selected from the group consisting of ethers, alcohols, or mixtures thereof, comprising: drying said feedstock; subjecting said dried feedstock to fast pyrolysis using a vortex reactor or other means; catalytically cracking vapors resulting from said pyrolysis using a zeolite catalyst; condensing any aromatic byproduct fraction; catalytically alkylating any benzene present in said vapors after condensation; catalytically oligomerizing any remaining ethylene and propylene to higher olefins; isomerizing said olefins to reactive iso-olefins; and catalytically reacting said iso-olefins with an alcohol to form ethers or with water to form alcohols. 35 figs.

U.S. EPA SBIR Award Recipient Receives 2015 Tibbetts Award

EPA Pesticide Factsheets

Precision Combustion Inc. (PCI), an EPA SBIR award recipient , received the 2015 Tibbetts Award for developing and manufacturing advanced performance catalytic reactors and systems for energy, defense and environmental applications.

Performance of a catalytic reactor at simulated gas turbine combustor operating conditions

NASA Technical Reports Server (NTRS)

Anderson, D. N.; Tacina, R. R.; Mroz, T. S.

1975-01-01

The performance of a catalytic reactor 12 cm in diameter and 17 cm long was evaluated at simulated gas turbine combustor operating conditions using premixed propane and air. Inlet temperatures of 600 and 800 K, pressures of 3 and 6 atm, and reference velocities of 9 to 30 m/s were tested. Data were taken for equivalence ratios as high as 0.43. The operating range was limited on the low-temperature side by very poor efficiency; the minimum exit temperature for good performance ranged from 1400 to 1600 K depending on inlet conditions. As exit temperatures were raised above this minimum, emissions of unburned hydrocarbons decreased, carbon monoxide emissions became generally less than 1 g CO/kg fuel, and nitrogen oxides were less than about 0.1 g NO2/kg fuel.

Ceramic membranes for catalytic membrane reactors with high ionic conductivities and low expansion properties

DOEpatents

Mackay, Richard; Sammells, Anthony F.

2000-01-01

Ceramics of the composition: Ln.sub.x Sr.sub.2-x-y Ca.sub.y B.sub.z M.sub.2-z O.sub.5+.delta. where Ln is an element selected from the fblock lanthanide elements and yttrium or mixtures thereof; B is an element selected from Al, Ga, In or mixtures thereof; M is a d-block transition element of mixtures thereof; 0.01.ltoreq.x.ltoreq.1.0; 0.01.ltoreq.y.ltoreq.0.7; 0.01.ltoreq.z.ltoreq.1.0 and .delta. is a number that varies to maintain charge neutrality are provided. These ceramics are useful in ceramic membranes and exhibit high ionic conductivity, high chemical stability under catalytic membrane reactor conditions and low coefficients of expansion. The materials of the invention are particularly useful in producing synthesis gas.

Operando characterization of catalysts through use of a portable microreactor

DOE PAGES

Zhao, Shen; Li, Yuanyuan; Stavitski, Eli; ...

2015-10-09

To provide new understandings of the mechanisms of catalytic reactions, improved methods are needed than can monitor changes in the electronic, structural and chemical properties of catalysts, doing so in the operando conditions in which catalysts work. We describe here a microreactor-based approach that integrates the capabilities of advanced x-ray, electron, optical and gas-phase compositional analysis techniques in operando conditions. For several exemplary catalytic systems, we demonstrate how this approach enables characterization of three major factors contributing to structure-property correlations evidenced in heterogeneously catalyzed reactions, namely: the atomic structure and elemental compositions of nanocatalysts; the physiochemical properties of the supportmore » and catalyst-support interfaces; and the gas and surface-phase chemistry occurring under operando conditions. We highlight the generality of the approach as well as outline opportunities for future developments.« less

Materials and methods for the separation of oxygen from air

DOEpatents

MacKay, Richard; Schwartz, Michael; Sammells, Anthony F.

2003-07-15

Metal oxides particularly useful for the manufacture of catalytic membranes for gas-phase oxygen separation processes having the formula: O.sub.5+z where: x and x' are greater than 0; y and y' are greater than 0; x+x' is equal to 2; y+y' is less than or equal to 2; z is a number that makes the metal oxide charge neutral; A is an element selected from the lanthanide elements; A' is an element selected from Be, Mg, Ca, Sr, Ba and Ra; A" is an element selected from the f block lanthanides, Be, Mg, Ca, Sr, Ba and Ra; B is an element selected from the group consisting of Al, Ga, In or mixtures thereof and B" is Co or Mg, with the exception that when B" is Mg, A' and A" are not Mg. The metal oxides are useful for preparation of dense membranes which may be formed from dense thin films of the mixed metal oxide on a porous metal oxide element. The invention also provides methods and catalytic reactors for oxygen separation and oxygen enrichment of oxygen deficient gases which employ mixed conducting metal oxides of the above formula.

Low pressure catalytic co-conversion of biogenic waste (rapeseed cake) and vegetable oil.

PubMed

Giannakopoulou, Kanellina; Lukas, Michael; Vasiliev, Aleksey; Brunner, Christoph; Schnitzer, Hans

2010-05-01

Zeolite catalysts of three types (H-ZSM-5, Fe-ZSM-5 and H-Beta) were tested in the catalytic co-conversion of rapeseed cake and safflower oil into bio-fuel. This low pressure process was carried out at the temperatures of 350 and 400 degrees Celsius. The yields and compositions of the product mixtures depended on the catalyst nature and the process temperatures. The produced organic phases consisted mainly of hydrocarbons, fatty acids and nitriles. This mixture possessed improved characteristics (e.g. heating value, water content, density, viscosity, pH) compared with the bio-oils, making possible its application as a bio-fuel. The most effective catalyst, providing the highest yield of organic liquid phase, was the highly acidic/wide-pore H-Beta zeolite. The products obtained on this catalyst demonstrated the highest degree of deoxygenation and the higher HHV (Higher Heating Value). The aqueous liquid phase contained water-soluble carboxylic acids, phenols and heterocyclic compounds. Copyright 2009 Elsevier Ltd. All rights reserved.

Development of a Novel Catalytic Membrane Reactor for Heterogeneous Catalysis in Supercritical CO2

PubMed Central

Islam, Nazrul M.; Chatterjee, Maya; Ikushima, Yutaka; Yokoyama, Toshiro; Kawanami, Hajime

2010-01-01

A novel type of high-pressure membrane reactor has been developed for hydrogenation in supercritical carbon dioxide (scCO2). The main objectives of the design of the reactor are the separate feeding of hydrogen and substrate in scCO2 for safe reactions in a continuous flow process, and to reduce the reaction time. By using this new reactor, hydrogenation of cinnamaldehyde into hydrocinnamaldehyde has been successfully carried out with 100% selectivity at 50 °C in 10 MPa (H2: 1 MPa, CO2: 9 MPa) with a flow rate of substrate ranging from 0.05 to 1.0 mL/min. PMID:20162008

High-rate anaerobic treatment system for solid/lipid-rich wastewater using anaerobic baffled reactor with scum recovery.

PubMed

Fujihira, Takuya; Seo, Shogo; Yamaguchi, Takashi; Hatamoto, Masashi; Tanikawa, Daisuke

2018-04-27

A laboratory scale experiment was conducted to investigate the treatment of solid/lipid-rich wastewater with an anaerobic baffled reactor (ABR) and a down-flow hanging sponge (DHS) reactor. In this study, experimental periods were divided into three phases to explore efficient treatment of solids and lipids in wastewater. In ABR, >90% of the influent chemical oxygen demand (COD) was removed and >70% of the removed COD was converted to methane under steady-state conditions during each phase. During this period, >4.5 kg COD m -3  d -1 was achieved on an average in Phases 1 and 3. Biogas contributed to scum formation, and the scum was categorized into lipid-rich and sludge-containing types, which have energy potentials of 53.4 and 212 kcal/kg-wet weight, respectively. Therefore, by recovering solids and lipids, which formed persistent scum, ABR can be applied as a high-rate treatment for solid/lipid-rich wastewater. Copyright © 2018 Elsevier Ltd. All rights reserved.

Manned space flight nuclear system safety. Volume 3: Reactor system preliminary nuclear safety analysis. Part 2: Accident Model Document (AMD)

NASA Technical Reports Server (NTRS)

1972-01-01

The Accident Model Document is one of three documents of the Preliminary Safety Analysis Report (PSAR) - Reactor System as applied to a Space Base Program. Potential terrestrial nuclear hazards involving the zirconium hydride reactor-Brayton power module are identified for all phases of the Space Base program. The accidents/events that give rise to the hazards are defined and abort sequence trees are developed to determine the sequence of events leading to the hazard and the associated probabilities of occurence. Source terms are calculated to determine the magnitude of the hazards. The above data is used in the mission accident analysis to determine the most probable and significant accidents/events in each mission phase. The only significant hazards during the prelaunch and launch ascent phases of the mission are those which arise form criticality accidents. Fission product inventories during this time period were found to be very low due to very limited low power acceptance testing.

An evaluation of the vapor phase catalytic ammonia removal process for use in a Mars transit vehicle.

PubMed

Flynn, M; Borchers, B

1998-01-01

This article describes the design specification of the Vapor Phase Catalytic Ammonia Removal (VPCAR) process and the relative benefits of its utilization in a Mars Transit Vehicle application. The VPCAR process is a wastewater treatment technology that combines distillation with high-temperature catalytic oxidation of volatile impurities such as ammonia and organic compounds.

Sequencing Language and Activities in Teaching High School Chemistry. A Report to the National Science Foundation.

ERIC Educational Resources Information Center

Abraham, Michael R.; Renner, John W.

A learning cycle consists of three phases: exploration; conceptual invention; and expansion of an idea. These phases parallel Piaget's functioning model of assimilation, disequilibrium and accomodation, and organization respectively. The learning cycle perceives students as actors rather than reactors to the environment. Inherent in that…

Process for separating dissolved solids from a liquid using an anti-solvent and multiple effect evaporators

DOEpatents

Daniels, Edward J.; Jody, Bassam J.; Bonsignore, Patrick V.

1994-01-01

A process and system for treating aluminum salt cake containing water soluble halide salts by contacting the salt cake with water to dissolve water soluble halide salts forming a saturated brine solution. Transporting a portion of about 25% of the saturated brine solution to a reactor and introducing into the saturated brine solution at least an equal volume of a water-miscible low-boiling organic material such as acetone to precipitate a portion of the dissolved halide salts forming a three-phase mixture of an aqueous-organic-salt solution phase and a precipitated salt phase and an organic rich phase. The precipitated salt phase is separated from the other phases and the organic rich phase is recycled to the reactor. The remainder of the saturated brine solution is sent to a multiple effect evaporator having a plurality of stages with the last stage thereof producing low grade steam which is used to boil off the organic portion of the solution which is recycled.

Process for separating dissolved solids from a liquid using an anti-solvent and multiple effect evaporators

DOEpatents

Daniels, E.J.; Jody, B.J.; Bonsignore, P.V.

1994-07-19

A process and system are disclosed for treating aluminum salt cake containing water soluble halide salts by contacting the salt cake with water to dissolve water soluble halide salts forming a saturated brine solution. Transporting a portion of about 25% of the saturated brine solution to a reactor and introducing into the saturated brine solution at least an equal volume of a water-miscible low-boiling organic material such as acetone to precipitate a portion of the dissolved halide salts forming a three-phase mixture of an aqueous-organic-salt solution phase and a precipitated salt phase and an organic rich phase. The precipitated salt phase is separated from the other phases and the organic rich phase is recycled to the reactor. The remainder of the saturated brine solution is sent to a multiple effect evaporator having a plurality of stages with the last stage thereof producing low grade steam which is used to boil off the organic portion of the solution which is recycled. 3 figs.

COMPARISON OF MERCURY CAPTURE EFFICIENCIES OF THREE DIFFERENT IN SITU GENERATED SORBENTS

EPA Science Inventory

Three different sorbent materials (Ti, Si and Ca based) were compared for their mercury capture efficiencies in an entrained flow reactor. Agglomerated particles with a high specific surface area were generated in situ by injecting gas phase sorbent precursors into a high tempera...

Leachate flush strategies for managing volatile fatty acids accumulation in leach-bed reactors.

PubMed

Riggio, S; Torrijos, M; Vives, G; Esposito, G; van Hullebusch, E D; Steyer, J P; Escudié, R

2017-05-01

In anaerobic leach-bed reactors (LBRs) co-digesting an easily- and a slowly-degradable substrate, the importance of the leachate flush both on extracting volatile fatty acids (VFAs) at the beginning of newly-started batches and on their consumption in mature reactors was tested. Regarding VFA extraction three leachate flush-rate conditions were studied: 0.5, 1 and 2Lkg -1 TSd -1 . Results showed that increasing the leachate flush-rate during the acidification phase is essential to increase degradation kinetics. After this initial phase, leachate injection is less important and the flush-rate could be reduced. The injection in mature reactors of leachate with an acetic acid concentration of 5 or 10gL -1 showed that for an optimized VFA consumption in LBRs, VFAs should be provided straight after the methane production peak in order to profit from a higher methanogenic activity, and every 6-7h to maintain a high biogas production rate. Copyright © 2017 Elsevier Ltd. All rights reserved.

Simultaneous organic nitrogen and sulfate removal in an anaerobic GAC fluidised bed reactor.

PubMed

Fdz-Polanco, F; Fdz-Polanco, M; Fernandez, N; Urueña, M A; García, P A; Villaverde, S

2001-01-01

A granular activated carbon (GAC) anaerobic fluidised bed reactor treating vinasse from an ethanol distillery of sugar beet molasses was operated for 250 days under three different organic loading rates. The reactor showed good performance in terms of organic matter removal and methane production but an anomalous behaviour in terms of unusual high concentrations of molecular nitrogen and low concentration of hydrogen sulphide in the biogas. The analysis of the different nitrogenous and sulphur compounds and the mass balances of these species in the liquid and gas phases clearly indicated an uncommon evolution of nitrogen and sulphur in the reactor. Up to 55% of the TKN and up to 80% of the sulphur disappear in the liquid phase. This is the opposite to any previously reported results in the bibliography. The new postulated anaerobic process of ammonia and sulphate removal seems to follow the mechanism: SO4 = +2 NH4+-->S + N2 + 4H2O (delta G degree = -47.8 kJ/mol).

Comparative study of activated carbon, natural zeolite, and green sand supports for CuOX and ZnO sites as ozone decomposition catalyst

NASA Astrophysics Data System (ADS)

Azhariyah, A. S.; Pradyasti, A.; Dianty, A. G.; Bismo, S.

2018-03-01

This research was based on ozone decomposition in industrial environment. Ozone is harmful to human. Therefore, catalysts were made as a mask filter to decompose ozone. Comparison studies of catalyst supports were done using Granular Activated Carbon (GAC), Natural Zeolite (NZ), and Green Sand (GS). GAC showed the highest catalytic activity compared to other supports with conversion of 98%. Meanwhile, the conversion using NZ was only 77% and GS had been just 27%. GAC had the highest catalytic activity because it had the largest pore volume, which is 0.478 cm3/g. So GAC was used as catalyst supports. To have a higher conversion in ozone decomposition, GAC was impregnated with metal oxide as the active site of the catalyst. Active site comparison was made using CuOX and ZnO as the active site. Morphology, composition, and crystal phase were analyzed using SEM-EDX, XRF, and XRD methods. Mask filter, which contained catalysts for ozone decomposition, was tested using a fixed bed reactor at room temperature and atmospheric pressure. The result of conversion was analyzed using iodometric method. CuOX/GAC and ZnO/GAC 2%-w showed the highest catalytic activity and conversion reached 100%. From the durability test, CuOX/GAC 2%-w was better than ZnO/GAC 2%-w because the conversion of ozone to oxygen reached 100% with the lowest conversion was 70% for over eight hours.

Silver metal nano-matrixes as high efficiency and versatile catalytic reactors for environmental remediation

NASA Astrophysics Data System (ADS)

Dumée, Ludovic F.; Yi, Zhifeng; Tardy, Blaise; Merenda, Andrea; Des Ligneris, Elise; Dagastine, Ray R.; Kong, Lingxue

2017-03-01

Nano-porous metallic matrixes (NMMs) offer superior surface to volume ratios as well as enhanced optical, photonic, and electronic properties to bulk metallic materials. Such behaviours are correlated to the nano-scale inter-grain metal domains that favour the presence of electronic vacancies. In this work, continuous 3D NMMs were synthesized for the first time through a simple diffusion-reduction process whereby the aerogel matrix was functionalized with (3-Mercaptopropyl)trimethoxysilane. The surface energy of the silica monolith templates was tuned to improve the homogeneity of the reduction process while thiol functionalization facilitated the formation of a high density of seeding points for metal ions to reduce. The diameter of NMMs was between 2 and 1000 nm, corresponding to a silver loading between 1.23 and 41.16 at.%. A rates of catalytic degradation kinetics of these NMMS which is three orders of magnitude higher than those of the non-functionalized silver-silica structures. Furthermore, the enhancement in mechanical stability at nanoscale which was evaluated by Atomic Force Microscopy force measurements, electronic density and chemical inertness was assessed and critically correlated to their catalytic potential. This strategy opens up new avenues for design of complex architectures of either single or multi-metal alloy NMMs with enhanced surface properties for various applications.

Silver metal nano-matrixes as high efficiency and versatile catalytic reactors for environmental remediation

PubMed Central

Dumée, Ludovic F.; Yi, Zhifeng; Tardy, Blaise; Merenda, Andrea; des Ligneris, Elise; Dagastine, Ray R.; Kong, Lingxue

2017-01-01

Nano-porous metallic matrixes (NMMs) offer superior surface to volume ratios as well as enhanced optical, photonic, and electronic properties to bulk metallic materials. Such behaviours are correlated to the nano-scale inter-grain metal domains that favour the presence of electronic vacancies. In this work, continuous 3D NMMs were synthesized for the first time through a simple diffusion-reduction process whereby the aerogel matrix was functionalized with (3-Mercaptopropyl)trimethoxysilane. The surface energy of the silica monolith templates was tuned to improve the homogeneity of the reduction process while thiol functionalization facilitated the formation of a high density of seeding points for metal ions to reduce. The diameter of NMMs was between 2 and 1000 nm, corresponding to a silver loading between 1.23 and 41.16 at.%. A rates of catalytic degradation kinetics of these NMMS which is three orders of magnitude higher than those of the non-functionalized silver-silica structures. Furthermore, the enhancement in mechanical stability at nanoscale which was evaluated by Atomic Force Microscopy force measurements, electronic density and chemical inertness was assessed and critically correlated to their catalytic potential. This strategy opens up new avenues for design of complex architectures of either single or multi-metal alloy NMMs with enhanced surface properties for various applications. PMID:28332602

Development of Vapor-Phase Catalytic Ammonia Removal System

NASA Technical Reports Server (NTRS)

Flynn, Michael; Fisher, John; Kiss, Mark; Borchers, Bruce; Tleimat, Badawi; Tleimat, Maher; Quinn, Gregory; Fort, James; Nalette, Tim; Baker, Gale;

Surface hydrophobicity and acidity effect on alumina catalyst in catalytic methanol dehydration reaction

PubMed Central

Osman, Ahmed I; Thompson, Jillian; Halawy, Samih A; Mohamed, Mohamed A

2017-01-01

Abstract BACKGROUND Methanol to dimethyl ether (MTD) is considered one of the main routes for the production of clean bio‐fuel. The effect of copper loading on the catalytic performance of different phases of alumina that formed by calcination at two different temperatures was examined for the dehydration of methanol to dimethyl ether (DME). RESULTS A range of Cu loadings of (1, 2, 4, 6, 10 and 15% Cu wt/wt) on Al2O3 calcined at 350 and 550 °C were prepared and characterized by TGA, XRD, BET, NH3‐TPD, TEM, H2‐TPR, SEM, EDX, XPS and DRIFT‐Pyridine techniques. The prepared catalysts were used in a fixed bed reactor under reaction conditions in which the temperature ranged from 180–300 °C with weight hourly space velocity (WHSV) = 12.1 h‐1. It was observed that all catalysts calcined at 550 °C (γ‐Al2O3 support phase) exhibited higher activity than those calcined at 350 °C (γ‐AlOOH), and this is due to the phase support change. Furthermore, the optimum Cu loading was found to be 6% Cu/γ‐Al2O3 with this catalyst also showing a high degree of stability under steady state conditions and this is attributed to the enhancement in surface acidity and hydrophobicity. CONCLUSION The addition of copper to the support improved the catalyst properties and activity. For all the copper modified catalysts, the optimum catalyst with high degree of activity and stability was 6% copper loaded on gamma alumina. © 2017 The Authors. Journal of Chemical Technology & Biotechnology published by John Wiley & Sons Ltd on behalf of Society of Chemical Industry. PMID:29200585

IAEA international studies on irradiation embrittlement of reactor pressure vessel steels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brumovsky, M.; Steele, L.E.

1997-02-01

In last 25 years, three phases a Co-operative Research Programme on Irradiation Embrittlement of Reactor Pressure Vessel Steels has been organized by the International Atomic Energy Agency. This programme started with eight countries in 1971 and finally 16 countries took part in phase III of the Programme in 1983. Several main efforts were put into preparation of the programme, but the principal task was concentrated on an international comparison of radiation damage characterization by different laboratories for steels of {open_quotes}old{close_quotes} (with high impurity contents) and {open_quotes}advanced{close_quotes} (with low impurity contents) types as well as on development of small scale fracturemore » mechanics procedures applicable to reactor pressure vessel surveillance programmes. This year, a new programme has been opened, concentrated mostly on small scale fracture mechanics testing.« less

Catalytic evaluation on liquid phase oxidation of vanillyl alcohol using air and H2O2 over mesoporous Cu-Ti composite oxide

NASA Astrophysics Data System (ADS)

Saha, Subrata; Hamid, Sharifah Bee Abd; Ali, Tammar Hussein

2017-02-01

A mesoporous, highly crystalline Cu-Ti composite oxide catalyst was prepared via facile, simple and modified solution method varying Cu and Ti ratio for selective liquid phase oxidation of vanillyl alcohol. Various spectroscopic procedures were employed to systematically characterize the catalyst structural and physicochemical properties. The defect chemistry of the catalyst was confirmed from the presence of surface defects revealed through HRTEM imagery between the TiO2 (101) and Cu3TiO4 (012) planes, complemented by the XRD profiling. Further, presence of oxygen vacancy evidenced by O 1s XPS spectra were observed on the catalyst surface. Moreover, the stoichiometry of Cu and Ti in the catalyst synthesis protocol was notably found to be the vital determinant to alter the redox properties of Cu-Ti composite oxide catalyst supported by H2-TPR. O2-TPD analysis. Moreover, a rational investigation was done using different oxidants such as air and H2O2 with variables reaction conditions. The catalyst was active for liquid phase oxidation of vanillyl alcohol to vanillin with performance of 66% conversion and 71% selectivity using H2O2 in base free condition. And also, catalytic activity was significantly improved by 94% conversion with 86% selectivity to vanillin in liquid phase aerobic oxidation at the optimum reaction conditions. To expand the superiority of the catalyst, three times reusability study was also examined with appreciable catalytic activity.

Biomass-derived Syngas Utilization for Fuels and Chemicals - Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dayton, David C

2010-03-24

Executive Summary The growing gap between petroleum production and demand, mounting environmental concerns, and increasing fuel prices have stimulated intense interest in research and development (R&D) of alternative fuels, both synthetic and bio-derived. Currently, the most technically defined thermochemical route for producing alternative fuels from lignocellulosic biomass involves gasification/reforming of biomass to produce syngas (carbon monoxide [CO] + hydrogen [H2]), followed by syngas cleaning, Fischer-Tropsch synthesis (FTS) or mixed alcohol synthesis, and some product upgrading via hydroprocessing or separation. A detailed techno-economic analysis of this type of process has recently been published [1] and it highlights the need for technicalmore » breakthroughs and technology demonstration for gas cleanup and fuel synthesis. The latter two technical barrier areas contribute 40% of the total thermochemical ethanol cost and 70% of the production cost, if feedstock costs are factored out. Developing and validating technologies that reduce the capital and operating costs of these unit operations will greatly reduce the risk for commercializing integrated biomass gasification/fuel synthesis processes for biofuel production. The objective of this project is to develop and demonstrate new catalysts and catalytic processes that can efficiently convert biomass-derived syngas into diesel fuel and C2-C4 alcohols. The goal is to improve the economics of the processes by improving the catalytic activity and product selectivity, which could lead to commercialization. The project was divided into 4 tasks: Task 1: Reactor Systems: Construction of three reactor systems was a project milestone. Construction of a fixed-bed microreactor (FBR), a continuous stirred tank reactor (CSTR), and a slurry bubble column reactor (SBCR) were completed to meet this milestone. Task 2: Iron Fischer-Tropsch (FT) Catalyst: An attrition resistant iron FT catalyst will be developed and tested. Task 3: Chemical Synthesis: Promising process routes will be identified for synthesis of selected chemicals from biomass-derived syngas. A project milestone was to select promising mixed alcohol catalysts and screen productivity and performance in a fixed bed micro-reactor using bottled syngas. This milestone was successfully completed in collaboration withour catalyst development partner. Task 4: Modeling, Engineering Evaluation, and Commercial Assessment: Mass and energy balances of conceptual commercial embodiment for FT and chemical synthesis were completed.« less

Nonthermal plasma technology for organic destruction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heath, W.O.; Birmingham, J.G.

1995-06-01

Pacific Northwest Laboratory (PNL) is investigating the use of nonthermal, electrically driven plasmas for destroying organic contaminants near ambient temperatures and pressures. Three different plasma systems have been developed to treat organics in air, water, and soil. These systems are the Gas-Phase Corona Reactor (GPCR)III for treating air, the Liquid-Phase Corona Reactor for treating water, and In Situ Corona for treating soils. This presentation focuses on recent technical developments, commercial status, and project costs of OPCR as a cost-effective alternative to other air-purification technologies that are now in use to treat off-gases from site-remediation efforts as well as industrial emissions.

Novel Fast Pyrolysis/Catalytic Technology for the Production of Stable Upgraded Liquids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oyama, Ted; Agblevor, Foster; Battaglia, Francine

The objective of the proposed research is the demonstration and development of a novel biomass pyrolysis technology for the production of a stable bio-oil. The approach is to carry out catalytic hydrodeoxygenation (HDO) and upgrading together with pyrolysis in a single fluidized bed reactor with a unique two-level design that permits the physical separation of the two processes. The hydrogen required for the HDO will be generated in the catalytic section by the water-gas shift reaction employing recycled CO produced from the pyrolysis reaction itself. Thus, the use of a reactive recycle stream is another innovation in this technology. Themore » catalysts will be designed in collaboration with BASF Catalysts LLC (formerly Engelhard Corporation), a leader in the manufacture of attrition-resistant cracking catalysts. The proposed work will include reactor modeling with state-of-the-art computational fluid dynamics in a supercomputer, and advanced kinetic analysis for optimization of bio-oil production. The stability of the bio-oil will be determined by viscosity, oxygen content, and acidity determinations in real and accelerated measurements. A multi-faceted team has been assembled to handle laboratory demonstration studies and computational analysis for optimization and scaleup.« less

Effective conversion of biomass tar into fuel gases in a microwave reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anis, Samsudin, E-mail: samsudin-anis@yahoo.com; Zainal, Z. A., E-mail: mezainal@usm.my

2016-06-03

This work deals with conversion of naphthalene (C{sub 10}H{sub 8}) as a biomass tar model compound by means of thermal and catalytic treatments. A modified microwave oven with a maximum output power of 700 W was used as the experimental reactor. Experiments were performed in a wide temperature range of 450-1200°C at a predetermined residence time of 0.24-0.5 s. Dolomite and Y-zeolite were applied to convert naphthalene catalytically into useful gases. Experimental results on naphthalene conversion showed that conversion efficiency and yield of gases increased significantly with the increase of temperature. More than 90% naphthalene conversion efficiency was achieved bymore » thermal treatment at 1200°C and 0.5 s. Nevertheless, this treatment was unfavorable for fuel gases production. The main product of this treatment was soot. Catalytic treatment provided different results with that of thermal treatment in which fuel gases formation was found to be the important product of naphthalene conversion. At a high temperature of 900°C, dolomite had better conversion activity where almost 40 wt.% of naphthalene could be converted into hydrogen, methane and other hydrocarbon gases.« less

New Developments in the Field of Reaction Technology: The Multiparallel Reactor HPMR 50-96

PubMed Central

Allwardt, Arne; Wendler, Christian; Thurow, Kerstin

2005-01-01

Catalytic high-pressure reactions play an important role in classic bulk chemistry. The optimization of common reactions, the search for new and more effective catalysts, and the increasing use of catalytic pressure reactions in the field of drug development call for high-parallel reaction systems. A crucial task of current developments, apart from the parameters of pressure, temperature, and number of reaction chambers, is, in this respect, the systems' integration into complex laboratory automation environments. PMID:18924722

Reactor vessel using metal oxide ceramic membranes

DOEpatents

Anderson, Marc A.; Zeltner, Walter A.

1992-08-11

A reaction vessel for use in photoelectrochemical reactions includes as its reactive surface a metal oxide porous ceramic membrane of a catalytic metal such as titanium. The reaction vessel includes a light source and a counter electrode. A provision for applying an electrical bias between the membrane and the counter electrode permits the Fermi levels of potential reaction to be favored so that certain reactions may be favored in the vessel. The electrical biasing is also useful for the cleaning of the catalytic membrane.

Two-phase anaerobic digestion of vegetable market waste fraction of municipal solid waste and development of improved technology for phase separation in two-phase reactor.

PubMed

Majhi, Bijoy Kumar; Jash, Tushar

2016-12-01

Biogas production from vegetable market waste (VMW) fraction of municipal solid waste (MSW) by two-phase anaerobic digestion system should be preferred over the single-stage reactors. This is because VMW undergoes rapid acidification leading to accumulation of volatile fatty acids and consequent low pH resulting in frequent failure of digesters. The weakest part in the two-phase anaerobic reactors was the techniques applied for solid-liquid phase separation of digestate in the first reactor where solubilization, hydrolysis and acidogenesis of solid organic waste occur. In this study, a two-phase reactor which consisted of a solid-phase reactor and a methane reactor was designed, built and operated with VMW fraction of Indian MSW. A robust type filter, which is unique in its implementation method, was developed and incorporated in the solid-phase reactor to separate the process liquid produced in the first reactor. Experiments were carried out to assess the long term performance of the two-phase reactor with respect to biogas production, volatile solids reduction, pH and number of occurrence of clogging in the filtering system or choking in the process liquid transfer line. The system performed well and was operated successfully without the occurrence of clogging or any other disruptions throughout. Biogas production of 0.86-0.889m 3 kg -1 VS, at OLR of 1.11-1.585kgm -3 d -1 , were obtained from vegetable market waste, which were higher than the results reported for similar substrates digested in two-phase reactors. The VS reduction was 82-86%. The two-phase anaerobic digestion system was demonstrated to be stable and suitable for the treatment of VMW fraction of MSW for energy generation. Copyright © 2016 Elsevier Ltd. All rights reserved.

Heat transfer in three-phase fluidization and bubble-columns with high gas holdups

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumar, S.; Kusakabe, K.; Fan, L.S.

1993-08-01

Bubble column and three-phase fluidized bed reactors have wide applications in biotechnological and petroleum processes (Deckwer, 1985; Fan, 1989). In such biotechnological processes as fermentation and waste water treatment, small bubbles of oxygen and/or nitrogen are introduced in the column to enhance oxygen transfer and to ensure the stability of immobilized cell particles. In addition, tiny bubbles are produced during the biological process due to the production of surface active compounds. The presence of these small bubbles causes an increase in the gas holdup of the system. High gas holdups are also characteristics of industrial processes such as coal liquefactionmore » and hydrotreating of residual oils. Good understanding of the transport properties of three-phase fluidized beds with high gas holdups is essential to the design, control and optimum operations of the commercial reactors employed in the above-mentioned processes. Heat-transfer studies in three-phase fluidized beds have been reviewed recently by Kim and Laurent (1991). Past studies focused primarily on the measurements of time-averaged heat transfer from the column wall to bed (Chiu and Ziegler 1983; Muroyama et al., 1986) or on immersed heating objects to bed (Baker et al., 1978; Kato et al., 1984) in aqueous systems. Recently, Kumar et al. (1992) provided a mechanistic understanding of the heat transfer in bubbly-liquid and liquid-solid systems. The purpose of this work is to investigate the heat transfer in a three-phase fluidized bed under high gas holdup conditions. The associated hydrodynamic behavior of the system is also studied.« less

Reactor process using metal oxide ceramic membranes

DOEpatents

Anderson, Marc A.

1994-01-01

A reaction vessel for use in photoelectrochemical reactions includes as its reactive surface a metal oxide porous ceramic membrane of a catalytic metal such as titanium. The reaction vessel includes a light source and a counter electrode. A provision for applying an electrical bias between the membrane and the counter electrode permits the Fermi levels of potential reaction to be favored so that certain reactions may be favored in the vessel. The electrical biasing is also useful for the cleaning of the catalytic membrane. Also disclosed is a method regenerating a porous metal oxide ceramic membrane used in a photoelectrochemical catalytic process by periodically removing the reactants and regenerating the membrane using a variety of chemical, thermal, and electrical techniques.

On-site generation of hydrogen from ethanol

DOT National Transportation Integrated Search

2008-01-01

Supercritical water is a synergistic, non-catalytic media for the reformation of crude ethanol feedstocks into hydrogen. The kinetics of the supercritical water reformation of ethanol was experimentally studied in a tubular reactor made of Inconel 62...

Nitrogen removal from wastewater by a catalytic oxidation method.

PubMed

Huang, T L; Macinnes, J M; Cliffe, K R

2001-06-01

The ammonia-containing waste produced in industries is usually characterized by high concentration and high temperature, and is not treatable by biological methods directly. In this study, a hydrophobic Pt/SDB catalyst was first used in a trickle-bed reactor to remove ammonia from wastewater. In the reactor, both stripping and catalytic oxidation occur simultaneously. It was found that higher temperature and higher oxygen partial pressure enhanced the ammonia removal. A reaction pathway, which involves oxidizing ammonia to nitric oxide, which then further reacts with ammonia to produce nitrogen and water, was confirmed. Small amounts of by-products, nitrites and nitrates were also detected in the resultant reaction solution. These compounds came from the absorption of nitrogen oxides. Both the minimum NO2- selectivity and maximum ammonia removal were achieved when the resultant pH of treated water was near 7.5 for a feed of unbuffered ammonia solution.

Two-Photon Laser-Induced Fluorescence O and N Atoms for the Study of Heterogeneous Catalysis in a Diffusion Reactor

NASA Technical Reports Server (NTRS)

Pallix, Joan B.; Copeland, Richard A.; Arnold, James O. (Technical Monitor)

1995-01-01

Advanced laser-based diagnostics have been developed to examine catalytic effects and atom/surface interactions on thermal protection materials. This study establishes the feasibility of using laser-induced fluorescence for detection of O and N atom loss in a diffusion tube to measure surface catalytic activity. The experimental apparatus is versatile in that it allows fluorescence detection to be used for measuring species selective recombination coefficients as well as diffusion tube and microwave discharge diagnostics. Many of the potential sources of error in measuring atom recombination coefficients by this method have been identified and taken into account. These include scattered light, detector saturation, sample surface cleanliness, reactor design, gas pressure and composition, and selectivity of the laser probe. Recombination coefficients and their associated errors are reported for N and O atoms on a quartz surface at room temperature.

Artemisinin production by plant hairy root cultures in gas- and liquid-phase bioreactors.

PubMed

Patra, Nivedita; Srivastava, Ashok K

2016-01-01

Alternative biotechnological protocol for large-scale artemisinin production was established. It featured enhanced growth and artemisinin production by cultivation of hairy roots in nutrient mist bioreactor (NMB) coupled with novel cultivation strategies. Artemisinin is used for the treatment of cerebral malaria. Presently, its main source is from seasonal plant Artemisia annua. This study featured investigation of growth and artemisinin production by A. annua hairy roots (induced by Agrobacterium rhizogenes-mediated genetic transformation of explants) in three bioreactor configurations-bubble column reactor, NMB and modified NMB particularly to establish their suitability for commercial production. It was observed that cultivation of hairy roots in a non-stirred bubble column reactor exhibited a biomass accumulation of 5.68 g/l only while batch cultivation in a custom-made NMB exhibited a higher biomass concentration of 8.52 g/l but relatively lower artemisinin accumulation of 0.22 mg/g was observed in this reactor. A mixture of submerged liquid-phase growth (for 5 days) followed by gas-phase cultivation in nutrient mist reactor operation strategy (for next 15 days) was adopted for hairy root cultivation in this investigation. Reasonably, high (23.02 g/l) final dry weight along with the artemisinin accumulation (1.12 mg/g, equivalent to 25.78 mg/l artemisinin) was obtained in this bioreactor, which is the highest reported artemisinin yield in the gas-phase NMB cultivation.

Transient Catalytic Combustor Model With Detailed Gas and Surface Chemistry

NASA Technical Reports Server (NTRS)

Struk, Peter M.; Dietrich, Daniel L.; Mellish, Benjamin P.; Miller, Fletcher J.; Tien, James S.

2005-01-01

In this work, we numerically investigate the transient combustion of a premixed gas mixture in a narrow, perfectly-insulated, catalytic channel which can represent an interior channel of a catalytic monolith. The model assumes a quasi-steady gas-phase and a transient, thermally thin solid phase. The gas phase is one-dimensional, but it does account for heat and mass transfer in a direction perpendicular to the flow via appropriate heat and mass transfer coefficients. The model neglects axial conduction in both the gas and in the solid. The model includes both detailed gas-phase reactions and catalytic surface reactions. The reactants modeled so far include lean mixtures of dry CO and CO/H2 mixtures, with pure oxygen as the oxidizer. The results include transient computations of light-off and system response to inlet condition variations. In some cases, the model predicts two different steady-state solutions depending on whether the channel is initially hot or cold. Additionally, the model suggests that the catalytic ignition of CO/O2 mixtures is extremely sensitive to small variations of inlet equivalence ratios and parts per million levels of H2.

Formaldehyde and methanol formation from reaction of carbon monoxide and hydrogen on neutral Fe2S2 clusters in the gas phase.

PubMed

Yin, Shi; Wang, Zhechen; Bernstein, Elliot R

2013-04-07

Reaction of CO with H2 on neutral FemSn clusters in a fast flow reactor is investigated both experimentally and theoretically. Single photon ionization at 118 nm is used to detect neutral cluster distributions through time of flight mass spectrometry. FemSn clusters are generated through laser ablation of a mixed iron-sulfur target in the presence of a pure helium carrier gas. A strong size dependent reactivity of (FeS)m clusters toward CO is characterized. The reaction FeS + CO → Fe + OCS is found for the FeS cluster, and the association product Fe2S2CO is observed for the Fe2S2 cluster. Products Fe2S2(13)COH2 and Fe2S2(13)COH4 are identified for reactions of (13)CO and H2 on Fe2S2 clusters: this suggests that the Fe2S2 cluster has a high catalytic activity for hydrogenation reactions of CO to form formaldehyde and methanol. Density functional theory (DFT) calculations are performed to explore the potential energy surfaces for the two reactions: Fe2S2 + CO + 2H2 → Fe2S2 + CH3OH; and Fe2S2 + CO + H2 → Fe2S2 + CH2O. A barrierless, thermodynamically favorable pathway is obtained for both catalytic processes. Catalytic cycles for formaldehyde and methanol formation from CO and H2 on a Fe2S2 cluster are proposed based on our experimental and theoretical investigations. The various reaction mechanisms explored by DFT are in good agreement with the experimental results. Condensed phase iron sulfide, which contains exposed Fe2S2 units on its surface, is suggested to be a good catalyst for low temperature formaldehyde/methanol synthesis.

Purification of Active Myrosinase from Plants by Aqueous Two-Phase Counter-Current Chromatography

PubMed Central

Wade, Kristina L.; Ito, Yoichiro; Ramarathnam, Aarthi; Holtzclaw, W. David; Fahey, Jed W.

2014-01-01

Introduction Myrosinase (thioglucoside glucohydrolase; E.C. 3.2.1.147), is a plant enzyme of increasing interest and importance to the biomedical community. Myrosinase catalyses the formation of isothiocyanates such as sulforaphane (frombroccoli) and 4-(α-l-rhamnopyranosyloxy)benzyl isothiocyanate (from moringa), which are potent inducers of the cytoprotective phase-2 response in humans, by hydrolysis of their abundant glucosinolate (β-thioglucoside N-hydroxysulphate) precursors. Objective To develop an aqueous two-phase counter-current chromatography (CCC) system for the rapid, three-step purification of catalytically active myrosinase. Methods A high-concentration potassium phosphate and polyethylene glycol biphasic aqueous two-phase system (ATPS) is used with a newly developed CCC configuration that utilises spiral-wound, flat-twisted tubing (with an ovoid cross-section). Results Making the initial crude plant extract directly in the ATPS and injecting only the lower phase permitted highly selective partitioning of the myrosinase complex before a short chromatography on a spiral disk CCC. Optimum phase retention and separation of myrosinase from other plant proteins afforded a 60-fold purification. Conclusion Catalytically active myrosinase is purified from 3-day broccoli sprouts, 7-day daikon sprouts, mustard seeds and the leaves of field-grown moringa trees, in a CCC system that is predictably scalable. PMID:25130502

Purification of active myrosinase from plants by aqueous two-phase counter-current chromatography.

PubMed

Wade, Kristina L; Ito, Yoichiro; Ramarathnam, Aarthi; Holtzclaw, W David; Fahey, Jed W

2015-01-01

Myrosinase (thioglucoside glucohydrolase; E.C. 3.2.1.147), is a plant enzyme of increasing interest and importance to the biomedical community. Myrosinase catalyses the formation of isothiocyanates such as sulforaphane (from broccoli) and 4-(α-l-rhamnopyranosyloxy)benzyl isothiocyanate (from moringa), which are potent inducers of the cytoprotective phase-2 response in humans, by hydrolysis of their abundant glucosinolate (β-thioglucoside N-hydroxysulphate) precursors. To develop an aqueous two-phase counter-current chromatography (CCC) system for the rapid, three-step purification of catalytically active myrosinase. A high-concentration potassium phosphate and polyethylene glycol biphasic aqueous two-phase system (ATPS) is used with a newly developed CCC configuration that utilises spiral-wound, flat-twisted tubing (with an ovoid cross-section). Making the initial crude plant extract directly in the ATPS and injecting only the lower phase permitted highly selective partitioning of the myrosinase complex before a short chromatography on a spiral disk CCC. Optimum phase retention and separation of myrosinase from other plant proteins afforded a 60-fold purification. Catalytically active myrosinase is purified from 3-day broccoli sprouts, 7-day daikon sprouts, mustard seeds and the leaves of field-grown moringa trees, in a CCC system that is predictably scalable. Copyright © 2014 John Wiley & Sons, Ltd.

Contributions of phase, sulfur vacancies, and edges to the hydrogen evolution reaction catalytic activity of porous molybdenum disulfide nanosheets

DOE PAGES

Yin, Ying; Han, Jiecai; Zhang, Yumin; ...

2016-06-07

Molybdenum disulfide (MoS 2) is a promising nonprecious catalyst for the hydrogen evolution reaction (HER) that has been extensively studied due to its excellent performance, but the lack of understanding of the factors that impact its catalytic activity hinders further design and enhancement of MoS 2-based electrocatalysts. Here, by using novel porous (holey) metallic 1T phase MoS 2 nanosheets synthesized by a liquid-ammonia-assisted lithiation route, we systematically investigated the contributions of crystal structure (phase), edges, and sulfur vacancies (S-vacancies) to the catalytic activity toward HER from five representative MoS 2 nanosheet samples, including 2H and 1T phase, porous 2H andmore » 1T phase, and sulfur-compensated porous 2H phase. Superior HER catalytic activity was achieved in the porous 1T phase MoS 2 nanosheets that have even more edges and S-vacancies than conventional 1T phase MoS 2. A comparative study revealed that the phase serves as the key role in determining the HER performance, as 1T phase MoS 2 always outperforms the corresponding 2H phase MoS 2 samples, and that both edges and S-vacancies also contribute significantly to the catalytic activity in porous MoS 2 samples. Then, using combined defect characterization techniques of electron spin resonance spectroscopy and positron annihilation lifetime spectroscopy to quantify the S-vacancies, the contributions of each factor were individually elucidated. Furthermore, this study presents new insights and opens up new avenues for designing electrocatalysts based on MoS 2 or other layered materials with enhanced HER performance.« less

Contributions of phase, sulfur vacancies, and edges to the hydrogen evolution reaction catalytic activity of porous molybdenum disulfide nanosheets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yin, Ying; Han, Jiecai; Zhang, Yumin

Molybdenum disulfide (MoS 2) is a promising nonprecious catalyst for the hydrogen evolution reaction (HER) that has been extensively studied due to its excellent performance, but the lack of understanding of the factors that impact its catalytic activity hinders further design and enhancement of MoS 2-based electrocatalysts. Here, by using novel porous (holey) metallic 1T phase MoS 2 nanosheets synthesized by a liquid-ammonia-assisted lithiation route, we systematically investigated the contributions of crystal structure (phase), edges, and sulfur vacancies (S-vacancies) to the catalytic activity toward HER from five representative MoS 2 nanosheet samples, including 2H and 1T phase, porous 2H andmore » 1T phase, and sulfur-compensated porous 2H phase. Superior HER catalytic activity was achieved in the porous 1T phase MoS 2 nanosheets that have even more edges and S-vacancies than conventional 1T phase MoS 2. A comparative study revealed that the phase serves as the key role in determining the HER performance, as 1T phase MoS 2 always outperforms the corresponding 2H phase MoS 2 samples, and that both edges and S-vacancies also contribute significantly to the catalytic activity in porous MoS 2 samples. Then, using combined defect characterization techniques of electron spin resonance spectroscopy and positron annihilation lifetime spectroscopy to quantify the S-vacancies, the contributions of each factor were individually elucidated. Furthermore, this study presents new insights and opens up new avenues for designing electrocatalysts based on MoS 2 or other layered materials with enhanced HER performance.« less

Synchronization algorithm for three-phase voltages of an inverter and a grid

NASA Astrophysics Data System (ADS)

Nos, O. V.

2017-07-01

This paper presents the results of designing a joint phase-locked loop for adjusting the phase shifts (speed) and Euclidean norm of three-phase voltages of an inverter to the same grid parameters. The design can be used, in particular, to match the potentials of two parallel-connected power sources for the fundamental harmonic at the moments of switching the stator windings of an induction AC motor from a converter to a centralized power-supply system and back. Technical implementation of the developed synchronization algorithm will significantly reduce the inductance of the current-balancing reactor and exclude emergency operation modes in the electric motor power circuit.

Testing of Performance of a Scroll Pump in Support of Improved Vapor Phase Catalytic Ammonia Removal (VPCAR) Mass Reduction

NASA Technical Reports Server (NTRS)

Nahra, Henry K.; Kraft, Thomas G.; Yee, Glenda F.; Jankovsky, Amy L.; Flynn, Michael

2006-01-01

This paper describes the results of ground testing of a scroll pump with a potential of being a substitute for the current vacuum pump of the Vapor Phase Catalytic Ammonia Reduction (VPCAR). Assessments of the pressure-time, pump-down time, pump power and the pump noise were made for three configurations of the pump the first of which was without the gas ballast, the second with the gas ballast installed but not operating and the third with the gas ballast operating. The tested scroll pump exhibited optimum characteristics given its mass and power requirements. The pump down time required to reach a pressure of 50 Torr ranged from 60 minutes without the ballast to about 120 minutes with the gas ballast operational. The noise emission and the pump power were assessed in this paper as well.

Advanced thermally stable jet fuels: Technical progress report, October 1994--December 1994

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schobert, H.H.; Eser, S.; Song, C.

There are five tasks within this project on thermally stable coal-based jet fuels. Progress on each of the tasks is described. Task 1, Investigation of the quantitative degradation chemistry of fuels, has 5 subtasks which are described: Literature review on thermal stability of jet fuels; Pyrolytic and catalytic reactions of potential endothermic fuels: cis- and trans-decalin; Use of site specific {sup 13}C-labeling to examine the thermal stressing of 1-phenylhexane: A case study for the determination of reaction kinetics in complex fuel mixtures versus model compound studies; Estimation of critical temperatures of jet fuels; and Surface effects on deposit formation inmore » a flow reactor system. Under Task 2, Investigation of incipient deposition, the subtask reported is Uncertainty analysis on growth and deposition of particles during heating of coal-derived aviation gas turbine fuels; under Task 3, Characterization of solid gums, sediments, and carbonaceous deposits, is subtask, Studies of surface chemistry of PX-21 activated carbon during thermal degradation of jet A-1 fuel and n-dodecane; under Task 4, Coal-based fuel stabilization studies, is subtask, Exploratory screening and development potential of jet fuel thermal stabilizers over 400 C; and under Task 5, Exploratory studies on the direct conversion of coal to high quality jet fuels, are 4 subtasks: Novel approaches to low-severity coal liquefaction and coal/resid co-processing using water and dispersed catalysts; Shape-selective naphthalene hydrogenation for production of thermally stable jet fuels; Design of a batch mode and a continuous mode three-phase reactor system for the liquefaction of coal and upgrading of coal liquids; and Exploratory studies on coal liquids upgrading using mesopores molecular sieve catalysts. 136 refs., 69 figs., 24 tabs.« less

Glycerol Production and Transformation: A Critical Review with Particular Emphasis on Glycerol Reforming Reaction for Producing Hydrogen in Conventional and Membrane Reactors.

PubMed

Bagnato, Giuseppe; Iulianelli, Adolfo; Sanna, Aimaro; Basile, Angelo

2017-03-23

Glycerol represents an emerging renewable bio-derived feedstock, which could be used as a source for producing hydrogen through steam reforming reaction. In this review, the state-of-the-art about glycerol production processes is reviewed, with particular focus on glycerol reforming reactions and on the main catalysts under development. Furthermore, the use of membrane catalytic reactors instead of conventional reactors for steam reforming is discussed. Finally, the review describes the utilization of the Pd-based membrane reactor technology, pointing out the ability of these alternative fuel processors to simultaneously extract high purity hydrogen and enhance the whole performances of the reaction system in terms of glycerol conversion and hydrogen yield.

Glycerol Production and Transformation: A Critical Review with Particular Emphasis on Glycerol Reforming Reaction for Producing Hydrogen in Conventional and Membrane Reactors

PubMed Central

Bagnato, Giuseppe; Iulianelli, Adolfo; Sanna, Aimaro; Basile, Angelo

2017-01-01

Glycerol represents an emerging renewable bio-derived feedstock, which could be used as a source for producing hydrogen through steam reforming reaction. In this review, the state-of-the-art about glycerol production processes is reviewed, with particular focus on glycerol reforming reactions and on the main catalysts under development. Furthermore, the use of membrane catalytic reactors instead of conventional reactors for steam reforming is discussed. Finally, the review describes the utilization of the Pd-based membrane reactor technology, pointing out the ability of these alternative fuel processors to simultaneously extract high purity hydrogen and enhance the whole performances of the reaction system in terms of glycerol conversion and hydrogen yield. PMID:28333121

Catalytic Destruction of Chlorinated Volatile Organic Compounds

DTIC Science & Technology

1993-08-01

Figure 1. The glass reactor passed through two furnaces. Both the furnaces were Lindberg 55035 hinged tube type. The top furnace served the purpose...10. HC1 Scrubber 10 11 12 11 13 11. Thermocouples 12. Manometer Tap 13. Glass Wool Figure 1. Schematic of the Reactor were used to check the...In the case of catalyst pellets, a thin layer of glass wool was used to hold the bed in place. The chlorinated hydrocarbon feed was introduced into

Evaluation of the Parameters and Conditions of Process in the Ethylbenzene Dehydrogenation with Application of Permselective Membranes to Enhance Styrene Yield

PubMed Central

Araújo, Paulo Jardel P.; Leite, Manuela Souza; Kakuta Ravagnani, Teresa M.

2016-01-01

Styrene is an important monomer in the manufacture of thermoplastic. Most of it is produced by the catalytic dehydrogenation of ethylbenzene. In this process that depends on reversible reactions, the yield is usually limited by the establishment of thermodynamic equilibrium in the reactor. The styrene yield can be increased by using a hybrid process, with reaction and separation simultaneously. It is proposed using permselective composite membrane to remove hydrogen and thus suppress the reverse and secondary reactions. This paper describes the simulation of a dehydrogenation process carried out in a tubular fixed-bed reactor wrapped in a permselective composite membrane. A mathematical model was developed, incorporating the various mass transport mechanisms found in each of the membrane layers and in the catalytic fixed bed. The effects of the reactor feed conditions (temperature, steam-to-oil ratio, and the weight hourly space velocity), the fixed-bed geometry (length, diameter, and volume), and the membrane geometry (thickness of the layers) on the styrene yield were analyzed. These variables were used to determine experimental conditions that favour the production of styrene. The simulation showed that an increase of 40.98% in the styrene yield, compared to a conventional fixed-bed process, could be obtained by wrapping the reactor in a permselective composite membrane. PMID:27069982

Investigation of the degradation mechanism of catalytic wires during oxidation of ammonia process

NASA Astrophysics Data System (ADS)

Pura, Jarosław; Wieciński, Piotr; Kwaśniak, Piotr; Zwolińska, Marta; Garbacz, Halina; Zdunek, Joanna; Laskowski, Zbigniew; Gierej, Maciej

2016-12-01

The most common catalysts for the ammonia oxidation process are 80 μm diameter platinum-rhodium wires knitted or woven into the form of a gauze. In an aggressive environment and under extreme conditions (temperature 800-900 °C, intensive gas flow, high pressure) precious elements are drained from the surface of the wires. Part of this separated material quickly decomposes on the surface in the form of characteristic "cauliflower-shape protrusions". The rest of the platinum is captured by palladium-nickel catalytic-capture gauzes located beneath. In our investigation we focused on the effects of the degradation of gauzes from one industrial catalytic system. The aim of the study was to compare the degree and the mechanism of degradation of gauzes from a different part of the reactor. The study covered PtRh7 catalytic and PdNi5 catalytic-capture gauzes. X-ray computer microtomography investigation revealed that despite strong differences in morphology, each Pt-Rh wire has a similar specific surface area. This indicates that the oxidation process and morphological changes of the wires occur in a self-regulating balance, resulting in the value of the specific surface area of the catalyst. Microtomography analysis of Pd-Ni wires revealed strong redevelopment of the wires' surface, which is related to the platinum capture phenomenon. Scanning electron microscope observations also revealed the nanostructure in the cauliflower-shape protrusions and large grains in the wires' preserved cores. The high temperature in the reactor and the long-term nature of the process do not favor the occurrence of the nanostructure in this type of material. Further and detailed analysis of this phenomena will provide a better understanding of the precious metals etching and deposition processes during oxidation.

Pre-Conceptual Design for Northstar ⁹⁹Mo Process Tritium Removal System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nobile, Arthur; Reichert, Heidi; Hollis, William Kirk

2016-01-12

In this report we describe a preliminary concept for a Tritium Removal System (TRS) to remove tritium that is generated in the ⁹⁹Mo production process. Preliminary calculations have been performed to evaluate an approximate size for the system. The concept described utilizes well-established detritiation technology based on catalytic oxidation of tritium and tritiated hydrocarbons to water in a high temperature (400 °C) reactor and capture of water in a molecular sieve bed. The TRS concept involves use of a single system that would cycle through each of the seven online target systems and remove tritium that has been accumulated aftermore » one week’s run time. The TRS would perform cleanup operations on each target system for a period of approximately 24 hours. This would occur while the system is still online and just prior to target replacement, so tritium levels would at their minimum values for target replacement. In the concept, during normal operation a small fraction (1%) of the helium recirculating in the system would be diverted through the TRS and returned to the flow loop. With this approach sufficient levels of detritiation can be accomplished in a 24 hour period. In the study it was found that because of the need to maintain low oxygen levels in the system (<100 ppm) this increases the size of the catalytic reactor. As a result of this finding, consideration should be given to other methods for removing tritium from the system. Other methods such as catalytic exchange of tritium with an unsaturated organic compound and subsequent trapping on activated carbon or molecular sieve could offer advantages of reducing reactor size and operation at lower reactor temperature. However the most significant advantage of such an approach would be the ability to operate in very low oxygen environments, which would eliminate any concerns for oxidation of the target.« less

Separation of metallic residues from the dissolution of a high-burnup BWR fuel using nitrogen trifluoride

DOE Office of Scientific and Technical Information (OSTI.GOV)

McNamara, Bruce K.; Buck, Edgar C.; Soderquist, Chuck Z.

2014-03-23

Nitrogen trifluoride (NF 3) was used to fluorinate the metallic residue from the dissolution of a high burnup, boiling water reactor fuel (~70 MWd/kgU). The metallic residue included the noble metal phase (containing ruthenium, rhodium, palladium, technetium, and molybdenum), and smaller amounts of zirconium, selenium, tellurium, and silver. Exposing the noble metal phase to 10% NF 3 in argon between 400 and 550°C, removed molybdenum and technetium near 400°C as their volatile fluorides, and ruthenium near 500C as its volatile fluoride. The events were thermally and temporally distinct and the conditions specified are a recipe to separate these transition metalsmore » from each other and from the noble metal phase nonvolatile residue. Depletion of the volatile fluorides resulted in substantial exothermicity. Thermal excursion behavior was recorded under non-adiabatic, isothermal conditions that typically minimize heat release. Physical characterization of the metallic noble phase and its thermal behavior are consistent with high kinetic velocity reactions encouraged by the nanoparticulate phase or perhaps catalytic influences of the mixed platinum metals with nearly pure phase structure. Post-fluorination, only two phases were present in the residual nonvolatile fraction. These were identified as a nano-crystalline, metallic palladium cubic phase and a hexagonal rhodium trifluoride (RhF 3) phase. The two phases were distinct as the sub-µm crystallites of metallic palladium were in contrast to the RhF 3 phase, which grew from the parent nano-crystalline noble-metal phase during fluorination, to acicular crystals exceeding 20-µm in length.« less

Hydrogen production through aqueous-phase reforming of ethylene glycol in a washcoated microchannel.

PubMed

D'Angelo, M Fernanda Neira; Ordomsky, Vitaly; Paunovic, Violeta; van der Schaaf, John; Schouten, Jaap C; Nijhuis, T Alexander

2013-09-01

Aqueous-phase reforming (APR) of biocarbohydrates is conducted in a catalytically stable washcoated microreactor where multiphase hydrogen removal enhances hydrogen efficiency. Single microchannel experiments are conducted following a simplified model based on the microreactor concept. A coating method to deposit a Pt-based catalyst on the microchannel walls is selected and optimized. APR reactivity tests are performed by using ethylene glycol as the model compound. Optimum results are achieved with a static washcoating technique; a highly uniform and well adhered 5 μm layer is deposited on the walls of a 320 μm internal diameter (ID) microchannel in one single step. During APR of ethylene glycol, the catalyst layer exhibits high stability over 10 days after limited initial deactivation. The microchannel presents higher conversion and selectivity to hydrogen than a fixed-bed reactor. The benefits of using a microreactor for APR can be further enhanced by utilizing increased Pt loadings, higher reaction temperatures, and larger carbohydrates (e.g., glucose). The use of microtechnology for aqueous-phase reforming will allow for a great reduction in the reformer size, thus rendering it promising for distributed hydrogen production. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Steam conversion of liquefied petroleum gas and methane in microchannel reactor

NASA Astrophysics Data System (ADS)

Dimov, S. V.; Gasenko, O. A.; Fokin, M. I.; Kuznetsov, V. V.

2018-03-01

This study presents experimental results of steam conversion of liquefied petroleum gas and methane in annular catalytic reactor - heat exchanger. The steam reforming was done on the Rh/Al2O3 nanocatalyst with the heat applied through the microchannel gap from the outer wall. Concentrations of the products of chemical reactions in the outlet gas mixture are measured at different temperatures of reactor. The range of channel wall temperatures at which the ratio of hydrogen and carbon oxide in the outlet mixture grows substantially is determined. Data on the composition of liquefied petroleum gas conversion products for the ratio S/C = 5 was received for different GHVS.

Reacting Flow in the Entrance to a Channel with Surface and Gas-Phase Kinetics

NASA Astrophysics Data System (ADS)

Mikolaitis, David; Griffen, Patrick

2006-11-01

In many catalytic reactors the conversion process is most intense at the very beginning of the channel where the flow is not yet fully developed; hence there will be important interactions between the developing flow field and reaction. To study this problem we have written an object-oriented code for the analysis of reacting flow in the entrance of a channel where both surface reaction and gas-phase reaction are modeled with detailed kinetics. Fluid mechanical momentum and energy equations are modeled by parabolic ``boundary layer''-type equations where streamwise gradient terms are small and the pressure is constant in the transverse direction. Transport properties are modeled with mixture-averaging and the chemical kinetic sources terms are evaluated using Cantera. Numerical integration is done with Matlab using the function pdepe. Calculations were completed using mixtures of methane and air flowing through a channel with platinum walls held at a fixed temperature. GRI-Mech 3.0 was used to describe the gas-phase chemistry and Deutchmann's methane-air-platinum model was used for the surface chemistry. Ignition in the gas phase is predicted for high enough wall temperatures. A hot spot forms away from the walls just before ignition that is fed by radicals produced at the surface.

High density gold nanoparticles immobilized on surface via plasma deposited APTES film for decomposing organic compounds in microchannels

NASA Astrophysics Data System (ADS)

Rao, Xi; Guyon, Cédric; Ognier, Stephanie; Da Silva, Bradley; Chu, Chenglin; Tatoulian, Michaël; Hassan, Ali Abou

2018-05-01

Immobilization of colloidal particles (e.g. gold nanoparticles (AuNps)) on the inner surface of micro-/nano- channels has received a great interest for catalysis. A novel catalytic ozonation setup using a gold-immobilized microchannel reactor was developed in this work. To anchor AuNps, (3-aminopropyl) triethoxysilane (APTES) with functional amine groups was deposited using plasma enhanced chemical vapor deposition (PECVD) process. The results clearly evidenced that PECVD processing exhibited relatively high efficiency for grafting amine groups and further immobilizing AuNPs. The catalytic activity of gold immobilized microchannel was evaluated by pyruvic acid ozonation. The decomposition rate calculated from High Performance Liquid Chromatography (HPLC) indicated a much better catalytic performance of gold in microchannel than that in batch. The results confirmed immobilizing gold nanoparticles on plasma deposited APTES for preparing catalytic microreactors is promising for the wastewater treatment in the future.

Strand transfer inhibitors of HIV-1 integrase: bringing IN a new era of antiretroviral therapy.

PubMed

McColl, Damian J; Chen, Xiaowu

2010-01-01

HIV-1 integrase (IN) is one of three essential enzymes (along with reverse transcriptase and protease) encoded by the viral pol gene. IN mediates two critical reactions during viral replication; firstly 3'-end processing (3'EP) of the double-stranded viral DNA ends and then strand transfer (STF) which joins the viral DNA to the host chromosomal DNA forming a functional integrated proviral DNA. IN is a 288 amino acid protein containing three functional domains, the N-terminal domain (NTD), catalytic core domain (CCD) and the C-terminal domain (CTD). The CCD contains three conserved catalytic residues, Asp64, Asp116 and Glu152, which coordinate divalent metal ions essential for the STF reaction. Intensive research over the last two decades has led to the discovery and development of small molecule inhibitors of the IN STF reaction (INSTIs). INSTIs are catalytic inhibitors of IN, and act to chelate the divalent metal ions in the CCD. One INSTI, raltegravir (RAL, Merck Inc.) was approved in late 2007 for the treatment of HIV-1 infection in patients with prior antiretroviral (ARV) treatment experience and was recently approved also for first line therapy. A second INSTI, elvitegravir (EVG, Gilead Sciences, Inc.) is currently undergoing phase 3 studies in ARV treatment-experienced patients and phase 2 studies in ARV naïve patients as part of a novel fixed dose combination. Several additional INSTIs are in early stage clinical development. This review will discuss the discovery and development of this novel class of antiretrovirals. This article forms part of a special issue of Antiviral Research marking the 25th anniversary of antiretroviral drug discovery and development, Vol 85, issue 1, 2010. Copyright 2009. Published by Elsevier B.V.

Progress in catalytic ignition fabrication and modeling : fabrication part 2.

DOT National Transportation Integrated Search

2012-06-01

The ignition temperature and heat generation from oxidation of methane on a platinum catalyst were : determined experimentally. A 127 micron diameter platinum coiled wire was placed crosswise in a : quartz tube of a plug flow reactor. A source meter ...

An atmospheric pressure flow reactor: Gas phase kinetics and mechanism in tropospheric conditions without wall effects

NASA Technical Reports Server (NTRS)

Koontz, Steven L.; Davis, Dennis D.; Hansen, Merrill

1988-01-01

A new type of gas phase flow reactor, designed to permit the study of gas phase reactions near 1 atm of pressure, is described. A general solution to the flow/diffusion/reaction equations describing reactor performance under pseudo-first-order kinetic conditions is presented along with a discussion of critical reactor parameters and reactor limitations. The results of numerical simulations of the reactions of ozone with monomethylhydrazine and hydrazine are discussed, and performance data from a prototype flow reactor are presented.

Catalytic igniters and their use to ignite lean hydrogen-air mixtures

DOEpatents

McLean, William J.; Thorne, Lawrence R.; Volponi, Joanne V.

1988-01-01

A catalytic igniter which can ignite a hydrogen-air mixture as lean as 5.5% hydrogen with induction times ranging from 20 s to 400 s, under conditions which may be present during a loss-of-liquid-coolant accident at a light water nuclear reactor comprises (a) a perforate catalytically active substrate, such as a platinum coated ceramic honeycomb or wire mesh screen, through which heated gases produced by oxidation of the mixture can freely flow and (b) a plurality of thin platinum wires mounted in a thermally conductive manner on the substrate and positioned thereon so as to be able to receive heat from the substrate and the heated gases while also in contact with unoxidized gases.

Reactor process using metal oxide ceramic membranes

DOEpatents

Anderson, M.A.

1994-05-03

A reaction vessel for use in photoelectrochemical reactions includes as its reactive surface a metal oxide porous ceramic membrane of a catalytic metal such as titanium. The reaction vessel includes a light source and a counter electrode. A provision for applying an electrical bias between the membrane and the counter electrode permits the Fermi levels of potential reaction to be favored so that certain reactions may be favored in the vessel. The electrical biasing is also useful for the cleaning of the catalytic membrane. Also disclosed is a method regenerating a porous metal oxide ceramic membrane used in a photoelectrochemical catalytic process by periodically removing the reactants and regenerating the membrane using a variety of chemical, thermal, and electrical techniques. 2 figures.

Nickel/ruthenium catalyst and method for aqueous phase reactions

DOEpatents

Elliott, D.C.; Sealock, J.L.

1998-09-29

A method of hydrogenation is described using a catalyst in the form of a plurality of porous particles wherein each particle is a support having nickel metal catalytic phase or reduced nickel deposited thereon in a first dispersed phase and an additional ruthenium metal deposited onto the support in a second dispersed phase. The additional ruthenium metal is effective in retarding or reducing agglomeration or sintering of the nickel metal catalytic phase thereby increasing the life time of the catalyst during hydrogenation reactions. 2 figs.

Nickel/ruthenium catalyst and method for aqueous phase reactions

DOEpatents

Elliott, Douglas C.; Sealock, John L.

1998-01-01

A method of hydrogenation using a catalyst in the form of a plurality of porous particles wherein each particle is a support having nickel metal catalytic phase or reduced nickel deposited thereon in a first dispersed phase and an additional ruthenium metal deposited onto the support in a second dispersed phase. The additional ruthenium metal is effective in retarding or reducing agglomeration or sintering of the nickel metal catalytic phase thereby increasing the life time of the catalyst during hydrogenation reactions.

Hydrocarbon Liquid Production from Biomass via Hot-Vapor-Filtered Fast Pyrolysis and Catalytic Hydroprocessing of the Bio-oil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Elliott, Douglas C.; Wang, Huamin; French, Richard

2014-08-14

Hot-vapor filtered bio-oils were produced from two different biomass feedstocks, oak and switchgrass, and the oils were evaluated in hydroprocessing tests for production of liquid hydrocarbon products. Hot-vapor filtering reduced bio-oil yields and increased gas yields. The yields of fuel carbon as bio-oil were reduced by ten percentage points by hot-vapor filtering for both feedstocks. The unfiltered bio-oils were evaluated alongside the filtered bio-oils using a fixed bed catalytic hydrotreating test. These tests showed good processing results using a two-stage catalytic hydroprocessing strategy. Equal-sized catalyst beds, a sulfided Ru on carbon catalyst bed operated at 220°C and a sulfided CoMomore » on alumina catalyst bed operated at 400°C were used with the entire reactor at 100 atm operating pressure. The products from the four tests were similar. The light oil phase product was fully hydrotreated so that nitrogen and sulfur were below the level of detection, while the residual oxygen ranged from 0.3 to 2.0%. The density of the products varied from 0.80 g/ml up to 0.86 g/ml over the period of the test with a correlated change of the hydrogen to carbon atomic ratio from 1.79 down to 1.57, suggesting some loss of catalyst activity through the test. These tests provided the data needed to assess the suite of liquid fuel products from the process and the activity of the catalyst in relationship to the existing catalyst lifetime barrier for the technology.« less

Development/Modernization of an Advanced Non-Light Water Reactor Probabilistic Risk Assessment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Henneke, Dennis W.; Robinson, James

In 2015, GE Hitachi Nuclear Energy (GEH) teamed with Argonne National Laboratory (Argonne) to perform Research and Development (R&D) of next-generation Probabilistic Risk Assessment (PRA) methodologies for the modernization of an advanced non-Light Water Reactor (non-LWR) PRA. This effort built upon a PRA developed in the early 1990s for GEH’s Power Reactor Inherently Safe Module (PRISM) Sodium Fast Reactor (SFR). The work had four main tasks: internal events development modeling the risk from the reactor for hazards occurring at-power internal to the plant; an all hazards scoping review to analyze the risk at a high level from external hazards suchmore » as earthquakes and high winds; an all modes scoping review to understand the risk at a high level from operating modes other than at-power; and risk insights to integrate the results from each of the three phases above. To achieve these objectives, GEH and Argonne used and adapted proven PRA methodologies and techniques to build a modern non-LWR all hazards/all modes PRA. The teams also advanced non-LWR PRA methodologies, which is an important outcome from this work. This report summarizes the project outcomes in two major phases. The first phase presents the methodologies developed for non-LWR PRAs. The methodologies are grouped by scope, from Internal Events At-Power (IEAP) to hazards analysis to modes analysis. The second phase presents details of the PRISM PRA model which was developed as a validation of the non-LWR methodologies. The PRISM PRA was performed in detail for IEAP, and at a broader level for hazards and modes. In addition to contributing methodologies, this project developed risk insights applicable to non-LWR PRA, including focus-areas for future R&D, and conclusions about the PRISM design.« less

Catalytic wet air oxidation of coke-plant wastewater on ruthenium-based eggshell catalysts in a bubbling bed reactor.

PubMed

Yang, M; Sun, Y; Xu, A H; Lu, X Y; Du, H Z; Sun, C L; Li, C

2007-07-01

Catalytic wet air of coke-plant wastewater was studied in a bubbling bed reactor. Two types of supported Ru-based catalysts, eggshell and uniform catalysts, were employed. Compared with the results in the wet air oxidation of coke-plant wastewater, supported Ru uniform catalysts showed high activity for chemical oxygen demand (COD) and ammonia/ammonium compounds (NH3-N) removal at temperature of 250 degrees C and pressure of 4.8 MPa, and it has been demonstrated that the catalytic activity of uniform catalyst depended strongly on the distribution of active sites of Ru on catalyst. Compared to the corresponding uniform catalysts with the same Ru loading (0.25 wt.% and 0.1 wt.%, respectively), the eggshell catalysts showed higher activities for CODcr removal and much higher activities for NH3-N degradation. The high activity of eggshell catalyst for treatment of coke-plant wastewater can be attributed to the higher density of active Ru sites in the shell layer than that of the corresponding uniform catalyst with the same Ru loading. It has been also evidenced that the active Ru sites in the internal core of uniform catalyst have very little or no contribution to CODcr and NH3-N removal in the total oxidation of coke-plant wastewater.

A hybrid process combining homogeneous catalytic ozonation and membrane distillation for wastewater treatment.

PubMed

Zhang, Yong; Zhao, Peng; Li, Jie; Hou, Deyin; Wang, Jun; Liu, Huijuan

2016-10-01

A novel catalytic ozonation membrane reactor (COMR) coupling homogeneous catalytic ozonation and direct contact membrane distillation (DCMD) was developed for refractory saline organic pollutant treatment from wastewater. An ozonation process took place in the reactor to degrade organic pollutants, whilst the DCMD process was used to recover ionic catalysts and produce clean water. It was found that 98.6% total organic carbon (TOC) and almost 100% salt were removed and almost 100% metal ion catalyst was recovered. TOC in the permeate water was less than 16 mg/L after 5 h operation, which was considered satisfactory as the TOC in the potassium hydrogen phthalate (KHP) feed water was as high as 1000 mg/L. Meanwhile, the membrane distillation flux in the COMR process was 49.8% higher than that in DCMD process alone after 60 h operation. Further, scanning electron microscope images showed less amount and smaller size of contaminants on the membrane surface, which indicated the mitigation of membrane fouling. The tensile strength and FT-IR spectra tests did not reveal obvious changes for the polyvinylidene fluoride membrane after 60 h operation, which indicated the good durability. This novel COMR hybrid process exhibited promising application prospects for saline organic wastewater treatment. Copyright © 2016 Elsevier Ltd. All rights reserved.

Low Concentration Fe-Doped Alumina Catalysts Using Sol-Gel and Impregnation Methods: The Synthesis, Characterization and Catalytic Performance during the Combustion of Trichloroethylene.

PubMed

Maldonado, Carolina Solis; De la Rosa, Javier Rivera; Lucio-Ortiz, Carlos J; Hernández-Ramírez, Aracely; Barraza, Felipe F Castillón; Valente, Jaime S

2014-03-12

The role of iron in two modes of integration into alumina catalysts was studied at 0.39 wt% Fe and tested in trichloroethylene combustion. One modified alumina was synthesized using the sol-gel method with Fe added in situ during hydrolysis; another modification was performed using calcined alumina, prepared using the sol-gel method and impregnated with Fe. Several characterization techniques were used to study the level of Fe modification in the γ-Al₂O₃ phase formed and to correlate the catalytic properties during trichloroethylene (TCE) combustion. The introduction of Fe in situ during the sol-gel process influenced the crystallite size, and three iron species were generated, namely, magnetite, maghemite and hematite. The impregnated Fe-alumina formed hematite and maghemite, which were highly dispersed on the γ-Al₂O 3 surface. The X-ray photoelectron spectra (XPS), FT-IR and Mössbauer spectroscopy analyses revealed how Fe interacted with the γ-Al₂O₃ lattice in both catalysts. The impregnated Fe-catalyst showed the best catalytic performance compared to the catalyst that was Fe-doped in situ by the sol-gel method; both had better catalytic activity than pure alumina. This difference in activity was correlated with the accessibility of the reactants to the hematite iron species on the surface. The chlorine poisoning for all three catalysts was less than 1.8%.

Fast Pyrolysis Oil Stabilization: An Integrated Catalytic and Membrane Approach for Improved Bio-oils. Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

George W. Huber; Upadhye, Aniruddha A.; Ford, David M.

This University of Massachusetts, Amherst project, "Fast Pyrolysis Oil Stabilization: An Integrated Catalytic and Membrane Approach for Improved Bio-oils" started on 1st February 2009 and finished on August 31st 2011. The project consisted following tasks: Task 1.0: Char Removal by Membrane Separation Technology The presence of char particles in the bio-oil causes problems in storage and end-use. Currently there is no well-established technology to remove char particles less than 10 micron in size. This study focused on the application of a liquid-phase microfiltration process to remove char particles from bio-oil down to slightly sub-micron levels. Tubular ceramic membranes of nominalmore » pore sizes 0.5 and 0.8m were employed to carry out the microfiltration, which was conducted in the cross-flow mode at temperatures ranging from 38 to 45 C and at three different trans-membrane pressures varying from 1 to 3 bars. The results demonstrated the removal of the major quantity of char particles with a significant reduction in overall ash content of the bio-oil. The results clearly showed that the cake formation mechanism of fouling is predominant in this process. Task 2.0 Acid Removal by Membrane Separation Technology The feasibility of removing small organic acids from the aqueous fraction of fast pyrolysis bio-oils using nanofiltration (NF) and reverse osmosis (RO) membranes was studied. Experiments were carried out with a single solute solutions of acetic acid and glucose, binary solute solutions containing both acetic acid and glucose, and a model aqueous fraction of bio-oil (AFBO). Retention factors above 90% for glucose and below 0% for acetic acid were observed at feed pressures near 40 bar for single and binary solutions, so that their separation in the model AFBO was expected to be feasible. However, all of the membranes were irreversibly damaged when experiments were conducted with the model AFBO due to the presence of guaiacol in the feed solution. Experiments with model AFBO excluding guaiacol were also conducted. NF membranes showed retention factors of glucose greater than 80% and of acetic acid less than 15% when operated at transmembrane pressures near 60 bar. Task 3.0 Acid Removal by Catalytic Processing It was found that the TAN reduction in bio-oil was very difficult using low temperature hydrogenation in flow and batch reactors. Acetic acid is very resilient to hydrogenation and we could only achieve about 16% conversion for acetic acid. Although it was observed that acetic acid was not responsible for instability of aqueous fraction of bio-oil during ageing studies (described in task 5). The bimetallic catalyst PtRe/ceria-zirconia was found to be best catalyst because its ability to convert the acid functionality with low conversion to gas phase carbon. Hydrogenation of the whole bio-oil was carried out at 125°C, 1450 psi over Ru/C catalyst in a flow reactor. Again, negligible acetic acid conversion was obtained in low temperature hydrogenation. Hydrogenation experiments with whole bio-oil were difficult to perform because of difficulty to pumping the high viscosity oil and reactor clogging. Task 4.0 Acid Removal using Ion Exchange Resins DOWEX M43 resin was used to carry out the neutralization of bio-oil using a packed bed column. The pH of the bio-oil increased from 2.43 to 3.7. The GC analysis of the samples showed that acetic acid was removed from the bio-oil during the neutralization and recovered in the methanol washing. But it was concluded that process would not be economical at large scale as it is extremely difficult to regenerate the resin once the bio-oil is passed over it. Task 5.0 Characterization of Upgraded Bio-oils We investigated the viscosity, microstructure, and chemical composition of bio-oils prepared by a fast pyrolysis approach, upon aging these fuels at 90ºC for periods of several days. Our results suggest that the viscosity increase is not correlated with the acids or char present in the bio-oils. The viscosity increase is due to formation of high molecular weight polymeric species over time. Our work also suggests that hydrogenation of the samples is beneficial in eliminating the viscosity increase. Task 6.0 Commercialization Assessment Renewable Oil International LLC (ROI) was responsible for Task 6.0, Commercialization Assessment. As part of this effort ROI focused on methods to reduce char carryover in the vapor stream from the fast pyrolysis reactor and residence time of the vapor in the reactor. Changes were made in the bio-oil recovery methodology and a reactor sweep gas used to reduce vapor residence time. Cyclones were placed in the vapor stream to reduce char particulate carryover. Microfiltration of the bio-oil was also researched to remove char particulate from the bio-oil. The capital cost for these improvements would be less than 2% of the total plant capital cost.« less

Kinetic analysis of butyrylcholinesterase-catalyzed hydrolysis of acetanilides.

PubMed

Masson, Patrick; Froment, Marie-Thérèse; Gillon, Emilie; Nachon, Florian; Darvesh, Sultan; Schopfer, Lawrence M

2007-09-01

The aryl-acylamidase (AAA) activity of butyrylcholinesterase (BuChE) has been known for a long time. However, the kinetic mechanism of aryl-acylamide hydrolysis by BuChE has not been investigated. Therefore, the catalytic properties of human BuChE and its peripheral site mutant (D70G) toward neutral and charged aryl-acylamides were determined. Three neutral (o-nitroacetanilide, m-nitroacetanilide, o-nitrophenyltrifluoroacetamide) and one positively charged (3-(acetamido) N,N,N-trimethylanilinium, ATMA) acetanilides were studied. Hydrolysis of ATMA by wild-type and D70G enzymes showed a long transient phase preceding the steady state. The induction phase was characterized by a hysteretic "burst". This reflects the existence of two enzyme states in slow equilibrium with different catalytic properties. Steady-state parameters for hydrolysis of the three acetanilides were compared to catalytic parameters for hydrolysis of esters giving the same acetyl intermediate. Wild-type BuChE showed substrate activation while D70G displayed a Michaelian behavior with ATMA as with positively charged esters. Owing to the low affinity of BuChE for amide substrates, the hydrolysis kinetics of neutral amides was first order. Acylation was the rate-determining step for hydrolysis of aryl-acetylamide substrates. Slow acylation of the enzyme, relative to that by esters may, in part, be due suboptimal fit of the aryl-acylamides in the active center of BuChE. The hypothesis that AAA and esterase active sites of BuChE are non-identical was tested with mutant BuChE. It was found that mutations on the catalytic serine, S198C and S198D, led to complete loss of both activities. The silent variant (FS117) had neither esterase nor AAA activity. Mutation in the peripheral site (D70G) had the same effect on esterase and AAA activities. Echothiophate inhibited both activities identically. It was concluded that the active sites for esterase and AAA activities are identical, i.e. S198. This excludes any other residue present in the gorge for being the catalytic nucleophile pole.

Using ceramic membranes for the separation of hydrogen produced by dehydrogenation of perhydro- m-terphenyl

NASA Astrophysics Data System (ADS)

Kalenchuk, A. N.; Bogdan, V. I.; Kustov, L. M.

2015-01-01

The efficiency of a variety of ceramic membranes for the purification of hydrogen obtained by dehydrogenation of perhydro- m-terphenyl in a catalytic flow reactor from vapors of initial hydrocarbons and dehydrogenation products is investigated.

Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Resende, Karen A.; Hori, Carla E.; Noronha, Fabio B.

The impact of particle size of ZrO 2-supported Pd and of alloying with Ag was explored for hydrogenation of phenol in aqueous phase. Kinetic assessments were performed in a batch reactor, on monometallic Pd/ZrO 2 samples with different Pd loadings (0.5%, 1% and 2%), as well as on a 1% PdAg/ZrO 2 sample. The catalytic activity normalized to accessible Pd (turnover frequency, TOF) increased with the particle size of Pd. Reaction orders in phenol and H 2 and lower activation energies suggest that smaller particles bind the reacting substrates more strongly, leading to higher surface coverages by phenol. But, surprisingly,more » smaller Pd particles exhibited lower TOFs. The lower activity of the small Pd particles is attributed to lower activation entropies for the strongly bound species. Furthermore, the presence of Ag increased the catalyst activity by decreasing the apparent energy of activation and increasing the coverages of phenol and H 2, without negatively affecting the activation entropy.« less

Aqueous phase hydrogenation of phenol catalyzed by Pd and PdAg on ZrO 2

DOE PAGES

Resende, Karen A.; Hori, Carla E.; Noronha, Fabio B.; ...

2017-08-05

The impact of particle size of ZrO 2-supported Pd and of alloying with Ag was explored for hydrogenation of phenol in aqueous phase. Kinetic assessments were performed in a batch reactor, on monometallic Pd/ZrO 2 samples with different Pd loadings (0.5%, 1% and 2%), as well as on a 1% PdAg/ZrO 2 sample. The catalytic activity normalized to accessible Pd (turnover frequency, TOF) increased with the particle size of Pd. Reaction orders in phenol and H 2 and lower activation energies suggest that smaller particles bind the reacting substrates more strongly, leading to higher surface coverages by phenol. But, surprisingly,more » smaller Pd particles exhibited lower TOFs. The lower activity of the small Pd particles is attributed to lower activation entropies for the strongly bound species. Furthermore, the presence of Ag increased the catalyst activity by decreasing the apparent energy of activation and increasing the coverages of phenol and H 2, without negatively affecting the activation entropy.« less

Catalytic membrane reactor for water and wastewater treatment

NASA Astrophysics Data System (ADS)

Heng, Samuel

A double membrane reactor was fabricated and assessed for continuous treatment of water containing organic contaminants by ozonation. This innovative reactor consisted of a zeolite membrane prepared on the inner surface of a porous a-alumina support, which served as water selective extractor and active contactor, and a porous stainless membrane which was the ozone gas diffuser. The coupling of membrane separation and chemical oxidation was found to be highly beneficial to both processes. The total organic carbon (TOC) removal rate at the retentate was enhanced by up to 2.2 times, as compared to membrane ozonation. Simultaneously, clean water (< 2 mg C.L-1 ) was consistently produced on the permeate side, using a feed solution containing up to 1000 mg C.L-1, while the retentate was concentrated and treated. Most significantly, the addition of an adsorbing material, as a bed or a coated layer, onto the pores of the membrane support, was shown to further enhance TOC degradation, permeated TOC concentration, permeate flux, and moreover, ozone yield. The achievements of this project included: (1) The development of a novel low-temperature zeolite membrane activation method that generates consistently high quality membranes (i.e. high reproducibility and fewer defects). (2) The demonstration that gamma-alumina and gamma-alumina supported catalysts do not have significant activity and that the TOC removal enhancement usually observed during catalytic ozonation was due primarily to the contribution of adsorption and metal leaching. Thermogravimetric analysis (TGA) and elemental analysis (EA) of the spent catalyst showed that, during catalytic ozonation, oxygenated by-products of increased adsorbability were concentrated onto the gamma-alumina contactor, and were subsequently degraded. (3) The development of a method for coating high surface area gamma-alumina layers onto the grains of zeolite membrane support used as the active membrane contactor.

Kinetic phase transitions and reactive windows in reactions of monomers on two-dimensional lattices

NASA Astrophysics Data System (ADS)

Cortés, Joaquín; Puschmann, Heinrich; Valencia, Eliana

1997-01-01

Some conceptual considerations are made and Monte Carlo simulation studies are carried out to analyze a series of catalytic reactions of two and three monomers on a square lattice of sites. Two aspects are considered: The increase in the system's degrees of freedom, leading to the formation of reactive sites that allow a change in the character of one of the kinetic phase transitions from the first order to a second order transition, and the classification and reactivity of the new system class.

Evaluation of Catalytic and Thermal Cracking in a JP-8 Fueled Pulsed Detonation Engine (Postprint)

DTIC Science & Technology

2007-09-01

this research. Each 0.91-m-long heat exchanger was fabricated with a 50.8-mm-dia, inconel - 625 , Schedule-10 inner tube and a 63.5-mm-dia, inconel -600...detonation tube had an inconel heat exchanger (described later). The PDE cycle consisted of three equally timed phases--fill, fire, and purge, as shown in...prevent phase change. The fuel was pressure fed to the inlet of the fuel heating system (FHS). The FHS consisted of two inconel heat exchangers, a

Multi-Purpose Thermal Hydraulic Loop: Advanced Reactor Technology Integral System Test (ARTIST) Facility for Support of Advanced Reactor Technologies

DOE Office of Scientific and Technical Information (OSTI.GOV)

James E. O'Brien; Piyush Sabharwall; SuJong Yoon

2001-11-01

Effective and robust high temperature heat transfer systems are fundamental to the successful deployment of advanced reactors for both power generation and non-electric applications. Plant designs often include an intermediate heat transfer loop (IHTL) with heat exchangers at either end to deliver thermal energy to the application while providing isolation of the primary reactor system. In order to address technical feasibility concerns and challenges a new high-temperature multi-fluid, multi-loop test facility “Advanced Reactor Technology Integral System Test facility” (ARTIST) is under development at the Idaho National Laboratory. The facility will include three flow loops: high-temperature helium, molten salt, and steam/water.more » Details of some of the design aspects and challenges of this facility, which is currently in the conceptual design phase, are discussed« less

Development of a three-dimensional core dynamics analysis program for commercial boiling water reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bessho, Yasunori; Yokomizo, Osamu; Yoshimoto, Yuichiro

1997-03-01

Development and qualification results are described for a three-dimensional, time-domain core dynamics analysis program for commercial boiling water reactors (BWRs). The program allows analysis of the reactor core with a detailed mesh division, which eliminates calculational ambiguity in the nuclear-thermal-hydraulic stability analysis caused by reactor core regional division. During development, emphasis was placed on high calculational speed and large memory size as attained by the latest supercomputer technology. The program consists of six major modules, namely a core neutronics module, a fuel heat conduction/transfer module, a fuel channel thermal-hydraulic module, an upper plenum/separator module, a feedwater/recirculation flow module, and amore » control system module. Its core neutronics module is based on the modified one-group neutron kinetics equation with the prompt jump approximation and with six delayed neutron precursor groups. The module is used to analyze one fuel bundle of the reactor core with one mesh (region). The fuel heat conduction/transfer module solves the one-dimensional heat conduction equation in the radial direction with ten nodes in the fuel pin. The fuel channel thermal-hydraulic module is based on separated three-equation, two-phase flow equations with the drift flux correlation, and it analyzes one fuel bundle of the reactor core with one channel to evaluate flow redistribution between channels precisely. Thermal margin is evaluated by using the GEXL correlation, for example, in the module.« less

Effect of the addition of fatty by-products from the refining of vegetable oil on methane production in co-digestion.

PubMed

Torrijos, M; Sousbie, P; Badey, L; Bosque, F; Steyer, J P

2012-01-01

The purpose of this work was to investigate the effects of the addition of by-products from the refining of vegetable oil on the behavior of co-digestion reactors treating a mixture of grass, cow dung and fruit and vegetable waste. Three by-products were used: one soapstock, one used winterization earth and one skimming of aeroflotation of the effluents. Three 15 l reactors were run in parallel and fed five times a week. In a first phase of 4 weeks, the three reactors were fed with the co-digestion substrates alone (grass, cow dung and fruit and vegetable waste) at an organic loading rate (OLR) of 1.5 g VS/kg d (VS: volatile solids). Then, a different by-product from the refining of oil was added to the feed of each reactor at an OLR of 0.5 g VS/kg d, generating a 33% increase in the OLR. The results show that the addition of by-products from the refining of oil is an efficient way of increasing the methane production of co-digestion reactors thanks to high methane yield of such by-products (0.69-0.77 l CH(4)/g VS loaded). In fact, in this work, it was possible to raise the methane production of the reactors by about 60% through a 33% increase in the OLR thanks to the addition of the by-products from the refining of vegetable oil.

Optimization of a horizontal-flow biofilm reactor for the removal of methane at low temperatures.

PubMed

Clifford, E; Kennelly, C; Walsh, R; Gerrity, S; Reilly, E O; Collins, G

2012-10-01

Three pilot-scale, horizontal-flow biofilm reactors (HFBRs 1-3) were used to treat methane (CH4)-contaminated air to assess the potential of this technology to manage emissions from agricultural activities, waste and wastewater treatment facilities, and landfills. The study was conducted over two phases (Phase 1, lasting 90 days and Phase 2, lasting 45 days). The reactors were operated at 10 degrees C (typical of ambient air and wastewater temperatures in northern Europe), and were simultaneously dosed with CH4-contaminated air and a synthetic wastewater (SWW). The influent loading rates to the reactors were 8.6 g CH4/m3/hr (4.3 g CH4/m2 TPSA/hr; where TPSA is top plan surface area). Despite the low operating temperatures, an overall average removal of 4.63 g CH4/m3/day was observed during Phase 2. The maximum removal efficiency (RE) for the trial was 88%. Potential (maximum) rates of methane oxidation were measured and indicated that biofilm samples taken from various regions in the HFBRs had mostly equal CH4 removal potential. In situ activity rates were dependent on which part of the reactor samples were obtained. The results indicate the potential of the HFBR, a simple and robust technology, to biologically treat CH4 emissions. The results of this study indicate that the HFBR technology could be effectively applied to the reduction of greenhouse gas emissions from wastewater treatment plants and agricultural facilities at lower temperatures common to northern Europe. This could reduce the carbon footprint of waste treatment and agricultural livestock facilities. Activity tests indicate that methanotrophic communities can be supported at these temperatures. Furthermore, these data can lead to improved reactor design and optimization by allowing conditions to be engineered to allow for improved removal rates, particularly at lower temperatures. The technology is simple to construct and operate, and with some optimization of the liquid phase to improve mass transfer, the HFBR represents a viable, cost-effective solution for these emissions.

In situ Mössbauer investigation of iron oxide catalyst in water gas shift reaction - Impact of oxyreduction potential and temperature

NASA Astrophysics Data System (ADS)

Cherkezova-Zheleva, Z.; Mitov, I.

2010-03-01

The aim of the study is to obtain the exact state of iron oxide catalyst active phase in reaction conditions, as well as the correlation between the active phase and catalytic properties of iron-containing catalysts. In situ Mössbauer spectroscopy is the major investigation technique. It is established that the change of reaction conditions (temperature and gas reaction mixture) lead to redistribution of the relative weight of spectra components and influence mainly tetrahedrally and octahedrally coordinated cations in Fe3O4 phase. It was concluded, that the active sites of the catalyst in studied reaction are probably pairs of Fe3++Fe2+-(Fe2.5+) ions, i.e. the mixed valance iron ions. The obtained catalytic activity can be explained with combination of the natural thermo-activated and catalytically induced electron exchange and better synchronizing of oxidation and reduction steps of the catalytic reaction.

Using heat pipe to make isotherm condition in catalytic converters of sulfuric acid plants

NASA Astrophysics Data System (ADS)

Yousefi, M.; Pahlavanzadeh, H.; Sadrameli, S. M.

2017-08-01

In this study, for the first time, it is tried to construct a pilot reactor, for surveying the possibility of creating isothermal condition in the catalytic convertors where SO2 is converted to SO3 in the sulfuric acid plants by heat pipe. The thermodynamic and thermo-kinetic conditions were considered the same as the sulfuric acid plants converters. Also, influence of SO2 gas flow rate on isothermal condition, has been studied. A thermo-siphon type heat pipe contains the sulfur + 5% iodine as working fluid, was used for disposing the heat of reaction from catalytic bed. Our results show that due to very high energy-efficiency, isothermal and passive heat transfer mechanism of heat pipe, it is possible to reach more than 95% conversion in one isothermal catalytic bed. As the results, heat pipe can be used as a certain piece of equipment to create isothermal condition in catalytic convertors of sulphuric acid plants. With this work a major evaluation in design of sulphuric acid plants can be taken place.

Catalytic processes for space station waste conversion

NASA Technical Reports Server (NTRS)

Schoonover, M. W.; Madsen, R. A.

1986-01-01

Catalytic techniques for processing waste products onboard space vehicles were evaluated. The goal of the study was the conversion of waste to carbon, wash water, oxygen and nitrogen. However, the ultimate goal is conversion to plant nutrients and other materials useful in closure of an ecological life support system for extended planetary missions. The resulting process studied involves hydrolysis at 250 C and 600 psia to break down and compact cellulose material, distillation at 100 C to remove water, coking at 450 C and atmospheric pressure, and catalytic oxidation at 450 to 600 C and atmospheric pressure. Tests were conducted with a model waste to characterize the hydrolysis and coking processes. An oxidizer reactor was sized based on automotive catalytic conversion experience. Products obtained from the hydrolysis and coking steps included a solid residue, gases, water condensate streams, and a volatile coker oil. Based on the data obtained, sufficient component sizing was performed to make a preliminary comparison of the catalytic technique with oxidation for processing waste for a six-man spacecraft. Wet oxidation seems to be the preferred technique from the standpoint of both component simplicity and power consumption.

Catalytic fast pyrolysis of durian rind using silica-alumina catalyst: Effects of pyrolysis parameters.

PubMed

Tan, Y L; Abdullah, A Z; Hameed, B H

2018-05-18

Silica-alumina catalyst was prepared and used in the catalytic fast pyrolysis of durian rind in a drop-type two-stage reactor. The effects of catalytic temperature (400 °C-600 °C) and catalyst-to-durian rind ratio (1:30-3:30) were evaluated. Bio-oil yield was increased with increased catalytic temperature due to considerable dehydration process, but it was reduced with high catalyst loading due to the overcracking of organics into light gases. Silica-alumina catalyst possessed good selectivity and the products changed according to the temperature. The major components in bio-oil were hydrocarbons, furan derivatives, and aromatic compounds at 400 °C, 500 °C, and 600 °C, respectively. The hydrogen and carbon contents of bio-oil were reduced with high catalyst loading due to the overcracking of organics, and the deoxygenation process became unfavorable. The silica-alumina catalyst worked well in catalytic fast pyrolysis of durian rind, and the condition may be adjusted based on the desired products. Copyright © 2018 Elsevier Ltd. All rights reserved.

CONTINUOUS FLOW MICROWAVE REACTORS FOR ORGANIC SYNTHESIS: HYDRODECHLORINATION, HETROCYCLIZATION, ISOMERIZATION

EPA Science Inventory

Microwave heating has been sought as a convenient way of enhancing chemical processes. The advantages of microwave heating, such as selective direct heating of materials of a catalytic site, minimized fouling on hot surfaces, process simplicity, rapid startup, as well as the pos...

CONTINUOUS MICROWAVE REACTORS FOR ORGANIC SYNTHESIS: HYDRODECHLORINATION AND HYDROLYSIS

EPA Science Inventory

Microwave heating has been sought as a convenient way of enhancing chemical processes. The advantages of microwave heating, such as selective direct heating of materials of a catalytic site, minimized fouling on hot surfaces, process simplicity, rapid startup, as well as the poss...

PHOTOOXIDATION OF HYDROCARBONS TO PARTIAL OXYGENATES IN AN AQUEOUS ENVIRONMENT [EXHIBIT, POSTER

EPA Science Inventory

The USEPA is researching the use of alternative oxidation technologies (AOT's) as a catalytic process for the selective oxidation of hydrocarbon substrates. One AOT currently under investigation is the use of photocatalysis employed with a laminar thin-film falling reactor. Thi...

Baseline Fracture Toughness and CGR testing of alloys X-750 and XM-19 (EPRI Phase I)

DOE Office of Scientific and Technical Information (OSTI.GOV)

J. H. Jackson; S. P. Teysseyre

2012-10-01

The Advanced Test Reactor National Scientific User Facility (ATR NSUF) and Electric Power Research Institute (EPRI) formed an agreement to test representative alloys used as reactor structural materials as a pilot program toward establishing guidelines for future ATR NSUF research programs. This report contains results from the portion of this program established as Phase I (of three phases) that entails baseline fracture toughness, stress corrosion cracking (SCC), and tensile testing of selected materials for comparison to similar tests conducted at GE Global Research. The intent of this Phase I research program is to determine baseline properties for the materials ofmore » interest prior to irradiation, and to ensure comparability between laboratories using similar testing techniques, prior to applying these techniques to the same materials after having been irradiated at the Advanced Test Reactor (ATR). The materials chosen for this research are the nickel based super alloy X-750, and nitrogen strengthened austenitic stainless steel XM-19. A spare core shroud upper support bracket of alloy X-750 was purchased by EPRI from Southern Co. and a section of XM-19 plate was purchased by EPRI from GE-Hitachi. These materials were sectioned at GE Global Research and provided to INL.« less

Baseline Fracture Toughness and CGR testing of alloys X-750 and XM-19 (EPRI Phase I)

DOE Office of Scientific and Technical Information (OSTI.GOV)

J. H. Jackson; S. P. Teysseyre

2012-02-01

The Advanced Test Reactor National Scientific User Facility (ATR NSUF) and Electric Power Research Institute (EPRI) formed an agreement to test representative alloys used as reactor structural materials as a pilot program toward establishing guidelines for future ATR NSUF research programs. This report contains results from the portion of this program established as Phase I (of three phases) that entails baseline fracture toughness, stress corrosion cracking (SCC), and tensile testing of selected materials for comparison to similar tests conducted at GE Global Research. The intent of this Phase I research program is to determine baseline properties for the materials ofmore » interest prior to irradiation, and to ensure comparability between laboratories using similar testing techniques, prior to applying these techniques to the same materials after having been irradiated at the Advanced Test Reactor (ATR). The materials chosen for this research are the nickel based super alloy X-750, and nitrogen strengthened austenitic stainless steel XM-19. A spare core shroud upper support bracket of alloy X-750 was purchased by EPRI from Southern Co. and a section of XM-19 plate was purchased by EPRI from GE-Hitachi. These materials were sectioned at GE Global Research and provided to INL.« less

Two stages catalytic pyrolysis of refuse derived fuel: production of biofuel via syncrude.

PubMed

Miskolczi, N; Buyong, F; Angyal, A; Williams, P T; Bartha, L

2010-11-01

Thermo-catalytic pyrolysis of refuse derived fuels with different catalysts had been conducted in a two stages process due to its important potential value as fuel. The first stage was a pure thermal pyrolysis in a horizontal tubular reactor with feed rate of 0.5kg hourly. The second stage was a semi-batch process in the presence of catalysts. Results showed that the tested catalysts significantly have affected the quantity of products. E.g. gas yield could be increased with 350% related to the catalyst free case using ZSM-5, while that of pyrolytic oil was 115% over Y-zeolite. Gases consisted of mainly CO and CO(2) obtained from the tubular reactor, while dominantly hydrocarbons from the second stage. Ni-Mo-catalyst and Co-Mo-catalyst had shown activity in pyrolytic oil upgrading via in-situ hydrogenation-dehydrogenation reactions. Sulphur, nitrogen and chlorine level in pyrolytic oils could be significantly declined by using of catalysts.

Metallization of DNA hydrogel: application of soft matter host for preparation and nesting of catalytic nanoparticles

NASA Astrophysics Data System (ADS)

Zinchenko, Anatoly; Che, Yuxin; Taniguchi, Shota; Lopatina, Larisa I.; G. Sergeyev, Vladimir; Murata, Shizuaki

2016-07-01

Nanoparticles (NPs) of Au, Ag, Pt, Pd, Cu and Ni of 2-3 nm average-size and narrow-size distributions were synthesized in DNA cross-linked hydrogels by reducing corresponding metal precursors by sodium borohydride. DNA hydrogel plays a role of a universal reactor in which the reduction of metal precursor results in the formation of 2-3 nm ultrafine metal NPs regardless of metal used. Hydrogels metallized with various metals showed catalytic activity in the reduction of nitroaromatic compounds, and the catalytic activity of metallized hydrogels changed as follows: Pd > Ag ≈ Au ≈ Cu > Ni > Pt. DNA hydrogel-based "soft catalysts" elaborated in this study are promising for green organic synthesis in aqueous media as well as for biomedical in vivo applications.

Liquid-phase chemical hydrogen storage: catalytic hydrogen generation under ambient conditions.

PubMed

Jiang, Hai-Long; Singh, Sanjay Kumar; Yan, Jun-Min; Zhang, Xin-Bo; Xu, Qiang

2010-05-25

There is a demand for a sufficient and sustainable energy supply. Hence, the search for applicable hydrogen storage materials is extremely important owing to the diversified merits of hydrogen energy. Lithium and sodium borohydride, ammonia borane, hydrazine, and formic acid have been extensively investigated as promising hydrogen storage materials based on their relatively high hydrogen content. Significant advances, such as hydrogen generation temperatures and reaction kinetics, have been made in the catalytic hydrolysis of aqueous lithium and sodium borohydride and ammonia borane as well as in the catalytic decomposition of hydrous hydrazine and formic acid. In this Minireview we briefly survey the research progresses in catalytic hydrogen generation from these liquid-phase chemical hydrogen storage materials.

Catalytic oxidation of toluene: comparative study over powder and monolithic manganese-nickel mixed oxide catalysts.

PubMed

Duplančić, Marina; Tomašić, Vesna; Gomzi, Zoran

2017-07-05

This paper is focused on development of the metal monolithic structure for total oxidation of toluene at low temperature. The well-adhered catalyst, based on the mixed oxides of manganese and nickel, is washcoated on the Al/Al 2 O 3 plates as metallic support. For the comparison purposes, results observed for the manganese-nickel mixed oxide supported on the metallic monolith are compared with those obtained using powder type of the same catalyst. Prepared manganese-nickel mixed oxides in both configurations show remarkable low-temperature activity for the toluene oxidation. The reaction temperature T 50 corresponding to 50% of the toluene conversion is observed at temperatures of ca. 400-430 K for the powder catalyst and at ca. 450-490 K for the monolith configuration. The appropriate mathematical models, such as one-dimensional (1D) pseudo-homogeneous model of the fixed bed reactor and the 1D heterogeneous model of the metal monolith reactor, are applied to describe and compare catalytic performances of both reactors. Validation of the applied models is performed by comparing experimental data with theoretical predictions. The obtained results confirmed that the reaction over the monolithic structure is kinetically controlled, while in the case of the powder catalyst the reaction rate is influenced by the intraphase diffusion.

Integrated detoxification methodology of hazardous phenolic wastewaters in environmentally based trickle-bed reactors: Experimental investigation and CFD simulation.

PubMed

Lopes, Rodrigo J G; Almeida, Teresa S A; Quinta-Ferreira, Rosa M

2011-05-15

Centralized environmental regulations require the use of efficient detoxification technologies for the secure disposal of hazardous wastewaters. Guided by federal directives, existing plants need reengineering activities and careful analysis to improve their overall effectiveness and to become environmentally friendly. Here, we illustrate the application of an integrated methodology which encompasses the experimental investigation of catalytic wet air oxidation and CFD simulation of trickle-bed reactors. As long as trickle-bed reactors are determined by the flow environment coupled with chemical kinetics, first, on the optimization of prominent numerical solution parameters, the CFD model was validated with experimental data taken from a trickle bed pilot plant specifically designed for the catalytic wet oxidation of phenolic wastewaters. Second, several experimental and computational runs were carried out under unsteady-state operation to evaluate the dynamic performance addressing the TOC concentration and temperature profiles. CFD computations of total organic carbon conversion were found to agree better with experimental data at lower temperatures. Finally, the comparison of test data with simulation results demonstrated that this integrated framework was able to describe the mineralization of organic matter in trickle beds and the validated consequence model can be exploited to promote cleaner remediation technologies of contaminated waters. Copyright © 2011 Elsevier B.V. All rights reserved.

Effect of oxygen vacancies and phases on catalytic properties of hydrogen-treated nanoceria particles

NASA Astrophysics Data System (ADS)

Lan, Yuan-Pei; Sohn, Hong Yong

2018-03-01

Nanoceria powder was treated by hydrogen or air at different temperatures and atmospheres, and the phases, oxygen vacancies, catalytic properties of the treated samples were investigated. After treating, the crystallites on the ceria surface were fused, and the SEM and TEM images indicated that the particle size increased with treatment temperature. Both Raman and XPS spectra showed the oxygen vacancies in nanoceria increased with treatment temperature in hydrogen, and at the same temperature CeO2 treated in hydrogen had a higher Ce3+ fraction than that treated in air. The nanoceria after being treated in hydrogen at 900 °C contained the Ce2O3 phase together with CeO2 which was revealed by XRD and TEM results. Oxygen vacancies were found to enhance CO conversion, but the high temperature needed to generate the oxygen vacancies caused the fusion of the crystallites on the ceria surface and thus its area decreased, which resulted in lower catalytic activity. The catalytic activity of nanoceria treated in hydrogen at 900 °C measured higher than that of the ceria powders treated at 700 °C in hydrogen or 900 °C in air, which indicated that the Ce2O3 phase present in the treated nanoceria particles enhanced the catalytic activity.

Quantitative Phase Composition of TiO 2-Coated Nanoporous-Au Monoliths by X-ray Absorption Spectroscopy and Correlations to Catalytic

DOE PAGES

Bagge-Hansen, Michael; Wichmann, Andre; Wittstock, Arne; ...

2014-02-03

Porous titania/metal composite materials have many potential applications in the fields of green catalysis, energy harvesting, and storage in which both the overall morphology of the nanoporous host material and the crystallographic phase of the titania (TiO 2) guest determine the material’s performance. New insights into the structure–function relationships of these materials were obtained by near-edge X-ray absorption fine structure (NEXAFS) spectroscopy that, for example, provides quantitative crystallographic phase composition from ultrathin, nanostructured titania films, including sensitivity to amorphous components. We demonstrate that crystallographic phase, morphology, and catalytic activity of TiO 2-functionalized nanoporous gold (np-Au) can be controlled by amore » simple annealing procedure (T < 1300 K). The material was prepared by atomic layer deposition of ~2 nm thick TiO 2 on millimeter-sized samples of np-Au (40–50 nm mean ligament size) and catalytically investigated with respect to aerobic CO oxidation. Moreover, the annealing-induced changes in catalytic activity are correlated with concurrent morphology and phase changes as provided by cross-sectional scanning electron microscopy, transmission electron microscopy, and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy.« less

Characterizing fluid dynamics in a bubble column aimed for the determination of reactive mass transfer

NASA Astrophysics Data System (ADS)

Kováts, Péter; Thévenin, Dominique; Zähringer, Katharina

2018-02-01

Bubble column reactors are multiphase reactors that are used in many process engineering applications. In these reactors a gas phase comes into contact with a fluid phase to initiate or support reactions. The transport process from the gas to the liquid phase is often the limiting factor. Characterizing this process is therefore essential for the optimization of multiphase reactors. For a better understanding of the transfer mechanisms and subsequent chemical reactions, a laboratory-scale bubble column reactor was investigated. First, to characterize the flow field in the reactor, two different methods have been applied. The shadowgraphy technique is used for the characterisation of the bubbles (bubble diameter, velocity, shape or position) for various process conditions. This technique is based on particle recognition with backlight illumination, combined with particle tracking velocimetry (PTV). The bubble trajectories in the column can also be obtained in this manner. Secondly, the liquid phase flow has been analysed by particle image velocimetry (PIV). The combination of both methods, delivering relevant information concerning disperse (bubbles) and continuous (liquid) phases, leads to a complete fluid dynamical characterization of the reactor, which is the pre-condition for the analysis of mass transfer between both phases.

Improvement of yields and rates during enzymatic hydrolysis of cellulose to glucose. Progress report, March 1, 1979-May 31, 1979

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sundstrom, D W; Klei, H E; Coughlin, R W

1979-05-01

The objective of this program is to show that the conversion of cellulose to glucose can be significantly increased by enzymatically removing the inhibitory cellobiose from the reaction system using immobilized ..beta..-glucosidase (..beta..-G). An enzymatic catalyst was prepared and used in a fluidized bed with cellobiose as the substrate, only a 10% loss of activity was observed during a 500 hour period. Cellulose was hydrolyzed in two batch reactors operated side-by-side, with one reactor containing immobilized ..beta..-G and cellulose and the other reactor containing an equal amount of cellulose only. After 30 hours the reactor containing the immobilized ..beta..-G hadmore » 100% more glucose, indicating that the catalytic removal of the cellobiose had a significant effect upon the production of glucose.« less

RuO2 supported NaY zeolite catalysts: Effect of preparation methods on catalytic performance during aerobic oxidation of benzyl alcohol

NASA Astrophysics Data System (ADS)

Jung, Dasom; Lee, Sunwoo; Na, Kyungsu

2017-10-01

The effects of preparation method for RuO2 supported zeolite catalysts on the catalytic consequences during the aerobic oxidation of benzyl alcohol to benzaldehyde were investigated. Three preparation methods, i.e., (i) simultaneous crystallization of the zeolite framework in the presence of RuCl3 (Ru(SC)/NaY), (ii) post ion-exchange with RuCl3 on the zeolite framework (Ru(IE)/NaY), and (iii) post support of preformed Ru metal nanoparticles on the zeolite surface (Ru(PS)/NaY), were used to construct three different RuO2 supported NaY zeolite catalysts. The catalyst performance was investigated as functions of the reaction time and temperature, in correlation with the structural changes of the catalysts, as analyzed by X-ray diffraction (XRD). The results revealed that the catalytic consequences were dramatically affected by the preparation methods. Although similar conversion was achieved with all three catalysts, the turnover frequency (TOF) differed. The Ru(PS)/NaY catalyst exhibited the highest TOF (33-48 h-1), whereas the other catalysts produced much lower TOFs (9-12 h-1). The Ru(PS)/NaY catalyst also had the highest activation energy (Ea) of 48.39 kJ mol-1, whereas the Ru(SC)/NaY and Ru(IE)/NaY catalysts had Ea values of 18.58 and 24.11 kJ mol-1, respectively. Notably, the Ru(PS)/NaY catalyst yielded a significantly higher pre-exponential factor of 5.22 × 105 h-1, which is about 5 orders of magnitude larger than that of the Ru(SC)/NaY catalyst (7.15 × 100 h-1). This suggests that collision between benzyl alcohol and molecular oxygen was very intensive on the Ru(PS)/NaY catalyst, which explains the higher TOF of the Ru(PS)/NaY catalyst relative to the others in spite of the higher Ea value of the former. In terms of recyclability, the pristine crystallinity of the zeolite framework was maintained in the Ru(SC)/NaY catalyst and the RuO2 phase exhibited an insignificant loss of the initial activity up to three catalytic cycles, whereas Ru(PS)/NaY showed slight loss of activity and Ru(IE)/NaY showed a significant loss of activity due to the disappearance of the RuO2 phase.

Fast formation of aerobic granules by combining strong hydraulic selection pressure with overstressed organic loading rate.

PubMed

Liu, Yong-Qiang; Tay, Joo-Hwa

2015-09-01

The combined strong hydraulic selection pressure (HSP) with overstressed organic loading rate (OLR) as a fast granulation strategy was used to enhance aerobic granulation. To investigate the wide applicability of this strategy to different scenarios and its relevant mechanism, different settling times, different inoculums, different exchange ratios, different reactor configurations, and different shear force were used in this study. It was found that clear granules were formed within 24 h and steady state reached within three days when the fast granulation strategy was used in a lab-scale reactor seeded with well settled activated sludge (Reactor 2). However, granules appeared after 2-week operation and reached steady state after one month at the traditional step-wise decreased settling time from 20 to 2 min with OLR of 6 g COD/L·d (Reactor 1). With the fast granulation strategy, granules appeared within 24 h even with bulking sludge as seed to start up Reactor 3, but 6-day lag phase was observed compared with Reactor 2. Both Reactor 2 and Reactor 3 experienced sigmoidal growth curve in terms of biomass accumulation and granule size increase after granulation. In addition, the reproducible results in pilot-scale reactors (Reactor 5 and Reactor 6) with diameter of 20 cm and height/diameter ratio (H/D) of 4 further proved that reactor configuration and fluid flow pattern had no effect on the aerobic granulation when the fast granulation strategy was employed, but biomass accumulation experienced a short lag phase too in Reactor 5 and Reactor 6. Although overstressed OLR was favorable for fast granulation, it also led to the fluffy granules after around two-week operation. However, the stable 6-month operation of Reactor 3 demonstrated that the rapidly formed granules were able to maintain long-term stability by reducing OLR from 12 g COD/L·d to 6 g COD/L·d. A mechanism of fast granulation with the strategy of combined strong HSP and OLR was proposed to explain results and guide the operation with this fast strategy. Copyright © 2015 Elsevier Ltd. All rights reserved.

Hydrogen and sulfur recovery from hydrogen sulfide wastes

DOEpatents

Harkness, J.B.L.; Gorski, A.J.; Daniels, E.J.

1993-05-18

A process is described for generating hydrogen and elemental sulfur from hydrogen sulfide waste in which the hydrogen sulfide is [dis]associated under plasma conditions and a portion of the hydrogen output is used in a catalytic reduction unit to convert sulfur-containing impurities to hydrogen sulfide for recycle, the process also including the addition of an ionizing gas such as argon to initiate the plasma reaction at lower energy, a preheater for the input to the reactor and an internal adjustable choke in the reactor for enhanced coupling with the microwave energy input.

Hydrogen and sulfur recovery from hydrogen sulfide wastes

DOEpatents

Harkness, John B. L.; Gorski, Anthony J.; Daniels, Edward J.

1993-01-01

A process for generating hydrogen and elemental sulfur from hydrogen sulfide waste in which the hydrogen sulfide is associated under plasma conditions and a portion of the hydrogen output is used in a catalytic reduction unit to convert sulfur-containing impurities to hydrogen sulfide for recycle, the process also including the addition of an ionizing gas such as argon to initiate the plasma reaction at lower energy, a preheater for the input to the reactor and an internal adjustable choke in the reactor for enhanced coupling with the microwave energy input.

Removal of hydrogen sulfide as ammonium sulfate from hydropyrolysis product vapors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marker, Terry L.; Felix, Larry G.; Linck, Martin B.

A system and method for processing biomass into hydrocarbon fuels that includes processing a biomass in a hydropyrolysis reactor resulting in hydrocarbon fuels and a process vapor stream and cooling the process vapor stream to a condensation temperature resulting in an aqueous stream. The aqueous stream is sent to a catalytic reactor where it is oxidized to obtain a product stream containing ammonia and ammonium sulfate. A resulting cooled product vapor stream includes non-condensable process vapors comprising H.sub.2, CH.sub.4, CO, CO.sub.2, ammonia and hydrogen sulfide.

Removal of hydrogen sulfide as ammonium sulfate from hydropyrolysis product vapors

DOEpatents

Marker, Terry L; Felix, Larry G; Linck, Martin B; Roberts, Michael J

2014-10-14

A system and method for processing biomass into hydrocarbon fuels that includes processing a biomass in a hydropyrolysis reactor resulting in hydrocarbon fuels and a process vapor stream and cooling the process vapor stream to a condensation temperature resulting in an aqueous stream. The aqueous stream is sent to a catalytic reactor where it is oxidized to obtain a product stream containing ammonia and ammonium sulfate. A resulting cooled product vapor stream includes non-condensable process vapors comprising H.sub.2, CH.sub.4, CO, CO.sub.2, ammonia and hydrogen sulfide.

Fundamentals of Chemical Processes.

ERIC Educational Resources Information Center

Moser, William R.

1985-01-01

Describes a course that provides students with a fundamental understanding of the chemical, catalytic, and engineering sciences related to the chemical reactions taking place in a variety of reactors of different configurations. Also describes the eight major lecture topics, course examinations, and term papers. The course schedule is included.…

Daniel Carpenter | NREL

Science.gov Websites

Daniel.Carpenter@nrel.gov | 303-384-6709 Orcid ID http://orcid.org/0000-0001-7625-9308 Research Interests Impact of ), especially related to blending low-cost, sustainable feedstocks into the biofuels supply chain Design thermochemical and catalytic experimental reactor systems Affiliated Research Programs Feedstocks (PI) Biomass

The effect of clay catalyst on the chemical composition of bio-oil obtained by co-pyrolysis of cellulose and polyethylene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Solak, Agnieszka; Rutkowski, Piotr, E-mail: piotr.rutkowski@pwr.wroc.pl

2014-02-15

Highlights: • Non-catalytic and catalytic fast pyrolysis of cellulose/polyethylene blend was carried out in a laboratory scale reactor. • Optimization of process temperature was done. • Optimization of clay catalyst type and amount for co-pyrolysis of cellulose and polyethylene was done. • The product yields and the chemical composition of bio-oil was investigated. - Abstract: Cellulose/polyethylene (CPE) mixture 3:1, w/w with and without three clay catalysts (K10 – montmorillonite K10, KSF – montmorillonite KSF, B – Bentonite) addition were subjected to pyrolysis at temperatures 400, 450 and 500 °C with heating rate of 100 °C/s to produce bio-oil with highmore » yield. The pyrolytic oil yield was in the range of 41.3–79.5 wt% depending on the temperature, the type and the amount of catalyst. The non-catalytic fast pyrolysis at 500 °C gives the highest yield of bio-oil (79.5 wt%). The higher temperature of catalytic pyrolysis of cellulose/polyethylene mixture the higher yield of bio-oil is. Contrarily, increasing amount of montmorillonite results in significant, almost linear decrease in bio-oil yield followed by a significant increase of gas yield. The addition of clay catalysts to CPE mixture has a various influence on the distribution of bio-oil components. The addition of montmorillonite K10 to cellulose/polyethylene mixture promotes the deepest conversion of polyethylene and cellulose. Additionally, more saturated than unsaturated hydrocarbons are present in resultant bio-oils. The proportion of liquid hydrocarbons is the highest when a montmorillonite K10 is acting as a catalyst.« less

Tar Production from Biomass Pyrolysis in a Fluidized Bed Reactor: A Novel Turbulent Multiphase Flow Formulation

NASA Technical Reports Server (NTRS)

Bellan, J.; Lathouwers, D.

2000-01-01

A novel multiphase flow model is presented for describing the pyrolysis of biomass in a 'bubbling' fluidized bed reactor. The mixture of biomass and sand in a gaseous flow is conceptualized as a particulate phase composed of two classes interacting with the carrier gaseous flow. The solid biomass is composed of three initial species: cellulose, hemicellulose and lignin. From each of these initial species, two new solid species originate during pyrolysis: an 'active' species and a char, thus totaling seven solid-biomass species. The gas phase is composed of the original carrier gas (steam), tar and gas; the last two species originate from the volumetric pyrolysis reaction. The conservation equations are derived from the Boltzmann equations through ensemble averaging. Stresses in the gaseous phase are the sum of the Newtonian and Reynolds (turbulent) contributions. The particulate phase stresses are the sum of collisional and Reynolds contributions. Heat transfer between phases, and heat transfer between classes in the particulate phase is modeled, the last resulting from collisions between sand and biomass. Closure of the equations must be performed by modeling the Reynolds stresses for both phases. The results of a simplified version (first step) of the model are presented.

Fischer-Tropsch Slurry Reactor modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Soong, Y.; Gamwo, I.K.; Harke, F.W.

1995-12-31

This paper reports experimental and theoretical results on hydrodynamic studies. The experiments were conducted in a hot-pressurized Slurry-Bubble Column Reactor (SBCR). It includes experimental results of Drakeol-10 oil/nitrogen/glass beads hydrodynamic study and the development of an ultrasonic technique for measuring solids concentration. A model to describe the flow behavior in reactors was developed. The hydrodynamic properties in a 10.16 cm diameter bubble column with a perforated-plate gas distributor were studied at pressures ranging from 0.1 to 1.36 MPa, and at temperatures from 20 to 200{degrees}C, using a dual hot-wire probe with nitrogen, glass beads, and Drakeol-10 oil as the gas,more » solid, and liquid phase, respectively. It was found that the addition of 20 oil wt% glass beads in the system has a slight effect on the average gas holdup and bubble size. A well-posed three-dimensional model for bed dynamics was developed from an ill-posed model. The new model has computed solid holdup distributions consistent with experimental observations with no artificial {open_quotes}fountain{close_quotes} as predicted by the earlier model. The model can be applied to a variety of multiphase flows of practical interest. An ultrasonic technique is being developed to measure solids concentration in a three-phase slurry reactor. Preliminary measurements have been made on slurries consisting of molten paraffin wax, glass beads, and nitrogen bubbles at 180 {degrees}C and 0.1 MPa. The data show that both the sound speed and attenuation are well-defined functions of both the solid and gas concentrations in the slurries. The results suggest possibilities to directly measure solids concentration during the operation of an autoclave reactor containing molten wax.« less

Research progress on catalytic denitrification technology in chemical industry

NASA Astrophysics Data System (ADS)

Jin, Yezhi

2017-12-01

In recent years, due to the rising emission of NOx annually, attention has been aroused widely by people on more and more severe environmental problems. This paper first discusses applying NOx removal and control technologies and relating chemical principles. Of many technologies, selective reduction reaction (SCR) is the most widely used. Catalysts, the concentration of NOx at the entrance of SCR catalytic reactor, reaction temperature, NH3/NOx mole ratio and NH3 slip rate analyzed later contributes to the removal efficiency of NOx. Finally, the processing and configuration of SCR de-NOx system are briefly introduced.

Phonological studies of the new gas-induced agitated reactor using computational fluid dynamics.

PubMed

Yang, T C; Hsu, Y C; Wang, S F

2001-06-01

An ozone-induced agitated reactor has been found to be very effective in degrading industrial wastewater. However, the cost of the ozone generation as well as its short residence time in reactors has restricted its application in a commercial scale. An innovated gas-induced draft tube installed inside a conventional agitated reactor was proved to effectively retain the ozone in a reactor. The setup was demonstrated to significantly promote the ozone utilization rate up to 96% from the conventional rate of 60% above the onset speed. This work investigates the mixing mechanism of an innovated gas-induced reactor for the future scale-up design by using the technique of computational fluid dynamics. A three-dimensional flow model was proposed to compute the liquid-gas free surface as well as the flow patterns inside the reactor. The turbulent effects generated by two 45 degrees pitch-blade turbines were considered and the two phases mixing phenomena were also manipulated by the Eulerian-Eulerian techniques. The consistency of the free surface profiles and the fluid flow patterns proved a good agreement between computational results and the experimental observation.

Bench-Scale Monolith Autothermal Reformer Catalyst Screening Evaluations in a Micro-Reactor With Jet-A Fuel

NASA Technical Reports Server (NTRS)

Tomsik, Thomas M.; Yen, Judy C.H.; Budge, John R.

2006-01-01

Solid oxide fuel cell systems used in the aerospace or commercial aviation environment require a compact, light-weight and highly durable catalytic fuel processor. The fuel processing method considered here is an autothermal reforming (ATR) step. The ATR converts Jet-A fuel by a reaction with steam and air forming hydrogen (H2) and carbon monoxide (CO) to be used for production of electrical power in the fuel cell. This paper addresses the first phase of an experimental catalyst screening study, looking at the relative effectiveness of several monolith catalyst types when operating with untreated Jet-A fuel. Six monolith catalyst materials were selected for preliminary evaluation and experimental bench-scale screening in a small 0.05 kWe micro-reactor test apparatus. These tests were conducted to assess relative catalyst performance under atmospheric pressure ATR conditions and processing Jet-A fuel at a steam-to-carbon ratio of 3.5, a value higher than anticipated to be run in an optimized system. The average reformer efficiencies for the six catalysts tested ranged from 75 to 83 percent at a constant gas-hourly space velocity of 12,000 hr 1. The corresponding hydrocarbon conversion efficiency varied from 86 to 95 percent during experiments run at reaction temperatures between 750 to 830 C. Based on the results of the short-duration 100 hr tests reported herein, two of the highest performing catalysts were selected for further evaluation in a follow-on 1000 hr life durability study in Phase II.

Size, shape, and compositional effects on the order-disorder phase transitions in Au-Cu and Pt-M (M = Fe, Co, and Ni) nanocluster alloys.

PubMed

Kaatz, Forrest H; Bultheel, Adhemar

2018-08-24

Au-Cu and Pt-M (M = Fe, Co, and Ni) nanocluster alloys are currently being investigated world-wide by many researchers for their interesting catalytic and nanophase properties. The low temperature behavior of the phase diagrams is not well understood for alloys with nanometer sizes and shapes. We consider two models for low temperature ordering in the phase diagrams of Au-Cu and Pt-M nanocluster alloys. These models are valid for sizes ∼5 nm and approach bulk values for sizes ∼20 nm. We study the phase transitions in nanoclusters with cubic, octahedral, and cuboctahedral shapes, covering the compositions of interest. These models are based on studying the melting temperatures in nanoclusters using the regular solution, mixing model for alloys. From our data, experiments on nanocubes about 5 nm in size, of stoichiometric AuCu and PtM composition, could help differentiate between the models. Dispersion data shows that for the three shapes considered, octahedra have the highest percentage of surface atoms for the same relative diameter. We summarize the effects of structural ordering on the catalytic activity and suggest a method to avoid sintering during annealing of Pt-M alloys.

Kinetics of methane production and biodegradation of linear alkylbenzene sulfonate from laundry wastewater.

PubMed

Motteran, Fabrício; Braga, Juliana K; Silva, Edson L; Varesche, Maria Bernadete A

2016-12-05

This study evaluates the kinetics of methane production and degradation of standard linear alkylbenzene sulfonate (LAS) (50 ± 3.5 mg/L) and LAS from laundry wastewater (85 ± 2.1 mg/L) in anaerobic batch reactors at 30°C with different sources of inoculum. The inocula were obtained by auto-fermentation (AFM) and UASB reactors from wastewater treatment of poultry slaughterhouse (SGH), swine production (SWT) and wastewater treatment thermophilic of sugarcane industry (THR). The study was divided into three phases: synthetic substrate (Phase I), standard LAS (Phase II) and LAS from laundry wastewater (Phase III). For SGH, the highest values for cumulative methane productions (1,844.8 ± 149 µmol-Phase II), methane production rate (70.8 ± 88 µmol/h-Phase II and 4.01 ± 07 µmol/h-Phase III) were observed. The use of thermophilic biomass (THR) incubated at 30°C was not favorable for methane production and LAS biodegradation, but the highest kinetic coefficient degradation (k 1 app ) was obtained for LAS (0.33 ± 0.3 h) compared with mesophilic biomass (SGH and SWT) (0.13 ± 0.02 h). Therefore, both LAS sources influenced the kinetics of methane production and organic matter degradation. For SGH, inoculum obtained the highest LAS degradation. In the SGH inoculum sequenced by MiSeq-Illumina was identified genera (VadinCA02, Candidatus Cloacamonas, VadinHB04, PD-UASB-13) related to degrade toxic compounds. Therefore, it recommended the reactor mesophilic inoculum UASB (SGH) for the LAS degradation.

Detailed surface reaction mechanism in a three-way catalyst.

PubMed

Chatterjee, D; Deutschmann, O; Warnatz, J

2001-01-01

Monolithic three-way catalysts are applied to reduce the emission of combustion engines. The design of such a catalytic converter is a complex process involving the optimization of different physical and chemical parameters (in the simplest case, e.g., length, cell densities or metal coverage of the catalyst). Numerical simulation can be used as an effective tool for the investigation of the catalytic properties of a catalytic converter and for the prediction of the performance of the catalyst. To attain this goal, a two-dimensional flow-field description is coupled with a detailed surface reaction model (gas-phase reactions can be neglected in three-way catalysts). This surface reaction mechanism (with C3H6 taken as representative of unburnt hydrocarbons) was developed using sub-mechanisms recently developed for hydrogen, carbon monoxide and methane oxidation, literature values for C3H6 oxidation, and estimates for the remaining unknown reactions. Results of the simulation of a monolithic single channel are used to validate the surface reaction mechanism. The performance of the catalyst was simulated under lean, nearly stoichiometric and rich conditions. For these characteristic conditions, the oxidation of propene and carbon monoxide and the reduction of NO on a typical Pt/Rh coated three-way catalyst were simulated as a function of temperature. The numerically predicted conversion data are compared with experimentally measured data. The simulation further reveals the coupling between chemical reactions and transport processes within the monolithic channel.

A CFD model for biomass fast pyrolysis in fluidized-bed reactors

NASA Astrophysics Data System (ADS)

Xue, Qingluan; Heindel, T. J.; Fox, R. O.

2010-11-01

A numerical study is conducted to evaluate the performance and optimal operating conditions of fluidized-bed reactors for fast pyrolysis of biomass to bio-oil. A comprehensive CFD model, coupling a pyrolysis kinetic model with a detailed hydrodynamics model, is developed. A lumped kinetic model is applied to describe the pyrolysis of biomass particles. Variable particle porosity is used to account for the evolution of particle physical properties. The kinetic scheme includes primary decomposition and secondary cracking of tar. Biomass is composed of reference components: cellulose, hemicellulose, and lignin. Products are categorized into groups: gaseous, tar vapor, and solid char. The particle kinetic processes and their interaction with the reactive gas phase are modeled with a multi-fluid model derived from the kinetic theory of granular flow. The gas, sand and biomass constitute three continuum phases coupled by the interphase source terms. The model is applied to investigate the effect of operating conditions on the tar yield in a fluidized-bed reactor. The influence of various parameters on tar yield, including operating temperature and others are investigated. Predicted optimal conditions for tar yield and scale-up of the reactor are discussed.

Catalytic pyrolysis of waste furniture sawdust for bio-oil production.

PubMed

Uzun, Başak B; Kanmaz, Gülin

2014-07-01

In this study, the catalytic pyrolysis of waste furniture sawdust in the presence of ZSM-5, H-Y and MCM-41 (10 wt % of the biomass sample) was carried out in order to increase the quality of the liquid product at the various pyrolysis temperatures of 400, 450, 500 and 550(o)C. In the non-catalytic work, the maximum oil yield was obtained as 42% at 500(o)C in a fixed-bed reactor system. In the catalytic work, the maximum oil yield was decreased to 37.48, 30.04 and 29.23% in the presence of ZSM-5, H-Y and MCM-41, respectively. The obtained pyrolysis oils were analyzed by various spectroscopic and chromatographic techniques. It was determined that the use of a catalyst decreased acids and increased valuable organics found in the bio-oil. The removal of oxygen from bio-oil was confirmed with the results of the elemental analysis and gas chromatography-mass spectrometry. © The Author(s) 2014.

Ti(IV)-doped γ-Fe2O3 nanoparticles possessing unique textural and chemical properties: Enhanced suppression of phase transformation and promising catalytic activity

NASA Astrophysics Data System (ADS)

Khaleel, Abbas; Parvin, Maliha; AlTabaji, Moahmmed; Al-zamly, Ahmed

2018-03-01

Nanostructured Ti(IV)-doped γ-Fe2O3 was prepared via a sol-gel method, and the effect of doping on the phase stability, textural properties, and catalytic activity was investigated. Well-dispersed 10% Ti in γ-Fe2O3 structure was found to significantly suppress its conversion to α-Fe2O3. While undoped product contained both phases, γ- and α-Fe2O3, at 400 °C, its doped counterpart contained γ-Fe2O3 as the sole phase at temperatures as high as 500 °C and partial conversion started only at 550 °C. Doping also resulted in modified textural properties, including smaller particles, larger surface areas, and higher mesoporosity, as well as enhanced reducibility and catalytic activity.

Immobilization of NTPDase-1 from Trypanosoma cruzi and Development of an Online Label-Free Assay.

PubMed

Calil, Felipe Antunes; Lima, Juliana Maria; de Oliveira, Arthur Henrique Cavalcante; Mariotini-Moura, Christiane; Fietto, Juliana Lopes Rangel; Cardoso, Carmen Lucia

2016-01-01

The use of IMERs (Immobilized Enzyme Reactors) as a stationary phase coupled to high performance chromatographic systems is an interesting approach in the screening of new ligands. In addition, IMERs offer many advantages over techniques that employ enzymes in solution. The enzyme nucleoside triphosphate diphosphohydrolase (NTPDase-1) from Trypanosoma cruzi acts as a pathogen infection facilitator, so it is a good target in the search for inhibitors. In this paper, immobilization of NTPDase-1 afforded ICERs (Immobilized Capillary Enzyme Reactors). A liquid chromatography method was developed and validated to monitor the ICER activity. The conditions for the application of these bioreactors were investigated, and excellent results were obtained. The enzyme was successfully immobilized, as attested by the catalytic activity detected in the Tc NTPDase-1-ICER chromatographic system. Kinetic studies on the substrate ATP gave K M of 0.317 ± 0.044 mmol·L -1 , which still presented high affinity compared to in solution. Besides that, the ICER was stable for 32 days, enough time to investigate samples of possible inhibitors, including especially the compound Suramin, that inhibited 51% the enzyme activity at 100  µ mol·L -1 , which is in accordance with the data for the enzyme in solution.

Immobilization of NTPDase-1 from Trypanosoma cruzi and Development of an Online Label-Free Assay

PubMed Central

Lima, Juliana Maria; de Oliveira, Arthur Henrique Cavalcante

2016-01-01

The use of IMERs (Immobilized Enzyme Reactors) as a stationary phase coupled to high performance chromatographic systems is an interesting approach in the screening of new ligands. In addition, IMERs offer many advantages over techniques that employ enzymes in solution. The enzyme nucleoside triphosphate diphosphohydrolase (NTPDase-1) from Trypanosoma cruzi acts as a pathogen infection facilitator, so it is a good target in the search for inhibitors. In this paper, immobilization of NTPDase-1 afforded ICERs (Immobilized Capillary Enzyme Reactors). A liquid chromatography method was developed and validated to monitor the ICER activity. The conditions for the application of these bioreactors were investigated, and excellent results were obtained. The enzyme was successfully immobilized, as attested by the catalytic activity detected in the TcNTPDase-1-ICER chromatographic system. Kinetic studies on the substrate ATP gave K M of 0.317 ± 0.044 mmol·L−1, which still presented high affinity compared to in solution. Besides that, the ICER was stable for 32 days, enough time to investigate samples of possible inhibitors, including especially the compound Suramin, that inhibited 51% the enzyme activity at 100 µmol·L−1, which is in accordance with the data for the enzyme in solution. PMID:28070446

Electronic transport in mixed-phase hydrogenated amorphous/nanocrystalline silicon thin films

NASA Astrophysics Data System (ADS)

Wienkes, Lee Raymond

Interest in mixed-phase silicon thin film materials, composed of an amorphous semiconductor matrix in which nanocrystalline inclusions are embedded, stems in part from potential technological applications, including photovoltaic and thin film transistor technologies. Conventional mixed-phase silicon films are produced in a single plasma reactor, where the conditions of the plasma must be precisely tuned, limiting the ability to adjust the film and nanoparticle parameters independently. The films presented in this thesis are deposited using a novel dual-plasma co-deposition approach in which the nanoparticles are produced separately in an upstream reactor and then injected into a secondary reactor where an amorphous silicon film is being grown. The degree of crystallinity and grain sizes of the films are evaluated using Raman spectroscopy and X-ray diffraction respectively. I describe detailed electronic measurements which reveal three distinct conduction mechanisms in n-type doped mixed-phase amorphous/nanocrystalline silicon thin films over a range of nanocrystallite concentrations and temperatures, covering the transition from fully amorphous to ~30% nanocrystalline. As the temperature is varied from 470 to 10 K, we observe activated conduction, multiphonon hopping (MPH) and Mott variable range hopping (VRH) as the nanocrystal content is increased. The transition from MPH to Mott-VRH hopping around 100K is ascribed to the freeze out of the phonon modes. A conduction model involving the parallel contributions of these three distinct conduction mechanisms is shown to describe both the conductivity and the reduced activation energy data to a high accuracy. Additional support is provided by measurements of thermal equilibration effects and noise spectroscopy, both done above room temperature (>300 K). This thesis provides a clear link between measurement and theory in these complex materials.

Sustainable resource recovery and energy conversion processes using microbial electrochemical technologies

NASA Astrophysics Data System (ADS)

Yates, Matthew D.

Microbial Electrochemical Technologies (METs) are emerging technological platforms for the conversion of waste into usable products. METs utilize naturally occurring bacteria, called exoelectrogens, capable of transferring electrons to insoluble terminal electron acceptors. Electron transfer processes in the exoelectrogen Geobacter sulfurreducens were exploited here to develop sustainable processes for synthesis of industrially and socially relevant end products. The first process examined was the removal of soluble metals from solution to form catalytic nanoparticles and nanoporous structures. The second process examined was the biocatalytic conversion of electrons into hydrogen gas using electrons supplied directly to an electrode. Nanoparticle formation is desirable because materials on the nanoscale possess different physical, optical, electronic, and mechanical properties compared to bulk materials. In the first process, soluble palladium was used to form catalytic palladium nanoparticles using extracellular electron transfer (EET) processes of G. sulfurreducens, typically the dominant member of mixedculture METs. Geobacter cells reduced the palladium extracellularly using naturally produced pili, which provided extracellular adsorption and reduction sites to help delay the diffusion of soluble metals into the cell. The extracellular reduction prevented cell inactivation due to formation of intracellular particles, and therefore the cells could be reused in multiple palladium reduction cycles. A G. sulfurreducens biofilm was next investigated as a biotemplate for the formation of a nanoporous catalytic palladium structure. G. sulfurreducens biofilms have a dense network of pili and extracellular cytochromes capable of high rates of electron transfer directly to an electrode surface. These pili and cytochromes provide a dense number of reduction sites for nanoparticle formation without the need for any synthetic components. The cells within the biofilm also can act as natural agents for preventing agglomeration of nanoparticles, and subsequent decrease of active surface area, on the electrode surface. The cell template was carbonized and removed via thermal treatments, leaving a catalytically active mesoporous palladium structure. The biotemplated mesoporous structure had a high surface area composed of nanoparticles, and a high pore volume and surface area. The biotemplated porous structure also exhibited an increased catalytic activity compared to an electroplated palladium electrode and an electrode coated with synthetically produced palladium nanoparticles attached to the surface with a Nafion binder. The biotemplated mesoporous structure was found to be an alternative process to form a porous structure directly on an electrode using only materials and processes that naturally occur in G. sulfurreducens biofilms. Biotemplated catalytic structures are an alternative method to form a porous structure with high catalytic activity without using any synthetic compounds. However, their uses in large scale processes require that the catalyst layer be durable. The electrochemical and mechanical stability of biotemplated mesoporous structures was tested on different support materials (polished graphite, carbon paper, carbon cloth, and stainless steel) subjected to electrochemical and/or mechanical stress. Carbon paper was found to withstand the most electrochemical and mechanical stress of the four different support materials tested. Polished graphite was able to withstand electrochemical stress, but deteriorated under a combination of electrochemical and mechanical stress. Different readily available and inexpensive polymers (polyaniline and polydimethylsiloxane) were also tested against a widely used polymer (NafionRTM) to stabilize the palladium catalyst on the polished graphite surface. The polyaniline was the most effective binder because it enhanced the catalytic activity and could be electropolymerized around the catalyst, giving the greatest amount of control over the thickness of the polymer layer. The second process studied used exoelectrogenic bacteria in METs for the conversion of electrons to hydrogen via water electrolysis in a biocathodic system. Naturally occurring biocatalytic cell material on the cathode surface was used to lower the cathode overpotential. Different cell cultures ( G. sulfurreducens, Methanosarcina barkeri, and Escherichia coli) were tested for their effect on hydrogen formation using electrons supplied to an insoluble electrode. The mode of hydrogen production was investigated by monitoring hydrogen production over three to five months using G. sulfurreducens biofilms (pregrown under anodic conditions with acetate) that were: (1) not supplied with an organic carbon source for cell growth and maintenance, (2) killed with ethanol, or (3) supplied with lactate, an organic carbon source and electron donor for G. sulfurreducens. Hydrogen was produced at a rate 10--20 times higher over five months in reactors that were either not given organic carbon or killed with ethanol, compared to reactors with lactate added. The methanogen, M. barkeri, was also tested as a biocatalyst because it is able to grow autotrophically. However, M. barkeri cells did not grow in the reactor with the electrode potential poised, based on the lack of evidence for methane production. Despite the lack of cell activity, the rate of hydrogen production with M. barkeri was similar to the rate observed in killed G. sulfurreducens reactors. The addition of E. coli, a non-exoelectrogenic bacteria, resulted in an initial elevated hydrogen gas production, but hydrogen production rates similar to background levels after three months. No cells were detected on the electrode surfaces after five months using scanning electron microscopy and unique metals, such as iron, nickel, cobalt, and zinc, were detected on the electrode surfaces exposed to cells. The identifiable peptides extracted from the electrodes were found to be derived primarily from metalloproteins produced by G. sulfurreducens and M. barkeri cells. These findings show that hydrogen can be produced in a biocathodic system by abiotic cell material attached to a graphite electrode surface and that it does not require electron uptake by living cells.

Catalytic bioreactors and methods of using same

DOEpatents

Worden, Robert Mark; Liu, Yangmu Chloe

2017-07-25

Various embodiments provide a bioreactor for producing a bioproduct comprising one or more catalytically active zones located in a housing and adapted to keep two incompatible gaseous reactants separated when in a gas phase, wherein each of the one or more catalytically active zones may comprise a catalytic component retainer and a catalytic component retained within and/or thereon. Each of the catalytically active zones may additionally or alternatively comprise a liquid medium located on either side of the catalytic component retainer. Catalytic component may include a microbial cell culture located within and/or on the catalytic component retainer, a suspended catalytic component suspended in the liquid medium, or a combination thereof. Methods of using various embodiments of the bioreactor to produce a bioproduct, such as isobutanol, are also provided.

Electroconductivity technique for the measurement of axial variation of holdups in three-phase fluidized beds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Begovich, J.M.; Watson, J.S.

1978-03-01

An electroconductivity technique is described which can be used not only for determining the overall phase holdups in a three-phase fluidized bed, but, more importantly, it can also be used for determining the local holdups as a function of height in the column. One disadvantage of the technique is that it can only be applied to systems with electroconductive liquids. However, since most real or prototype systems use either water or can be simulated with a fluid that can readily be made electroconductive, this handicap does not seem to be too severe. The technique has been applied successfully to amore » number of systems, including porous alumina beads, if a correction is made for their internal porosity. It has shown the existence of the transition region as the bed goes from a three-phase to a two-phase system. Further work should result in correlations for the distribution of the three phases throughout the entire column. These predictive equations will help in the rational design of reactors in which local conditions throughout the bed must be considered.« less

Thermo-Catalytic Reforming of municipal solid waste.

PubMed

Ouadi, Miloud; Jaeger, Nils; Greenhalf, Charles; Santos, Joao; Conti, Roberto; Hornung, Andreas

2017-10-01

Municipal Solid Waste (MSW) refers to a heterogeneous mixture composed of plastics, paper, metal, food and other miscellaneous items. Local authorities commonly dispose of this waste by either landfill or incineration which are both unsustainable practices. Disposing of organic wastes via these routes is also becoming increasingly expensive due to rising landfill taxes and transport costs. The Thermo-Catalytic Reforming (TCR®) process, is a proposed valorisation route to transform organic wastes and residues, such as MSW, into sustainable energy vectors including (H 2 rich synthesis gas, liquid bio-oil and solid char). The aim herein, was to investigate the conversion of the organic fraction of MSW into fuels and chemicals utilising the TCR technology in a 2kg/h continuous pilot scale reactor. Findings show that MSW was successfully processed with the TCR after carrying out a feedstock pre-treatment step. Approximately, 25wt.% of the feedstock was converted into phase separated liquids, composed of 19wt.% aqueous phase and 6wt.% organic phase bio-oil. The analysis of the bio-oil fraction revealed physical and chemical fuel properties, higher heating value (HHV) of 38MJ/kg, oxygen content <7wt.% and water content <4wt.%. Due to the bio-oil's chemical and physical properties, the bio-oil was found to be directly miscible with fossil diesel when blended at a volume ratio of 50:50. The mass balance closure was 44wt.% synthesis gas, with a H 2 content of 36vol% and HHV of 17.23MJ/Nm 3 , and 31 wt.% char with a HHV of 17MJ/kg. The production of high quantities of H 2 gas and highly de-oxygenated organic liquids makes downstream hydrogen separation and subsequent hydro-deoxygenation of the produced bio-oil a promising upgrading step to achieve drop-in transportation fuels from MSW. Copyright © 2017 Elsevier Ltd. All rights reserved.

Immobilization of lambda exonuclease onto polymer micropillar arrays for the solid-phase digestion of dsDNAs.

PubMed

Oliver-Calixte, Nyoté J; Uba, Franklin I; Battle, Katrina N; Weerakoon-Ratnayake, Kumuditha M; Soper, Steven A

2014-05-06

The process of immobilizing enzymes onto solid supports for bioreactions has some compelling advantages compared to their solution-based counterpart including the facile separation of enzyme from products, elimination of enzyme autodigestion, and increased enzyme stability and activity. We report the immobilization of λ-exonuclease onto poly(methylmethacrylate) (PMMA) micropillars populated within a microfluidic device for the on-chip digestion of double-stranded DNA. Enzyme immobilization was successfully accomplished using 3-(3-dimethylaminopropyl) carbodiimide/N-hydroxysuccinimide (EDC/NHS) coupling to carboxylic acid functionalized PMMA micropillars. Our results suggest that the efficiency for the catalysis of dsDNA digestion using λ-exonuclease, including its processivity and reaction rate, were higher when the enzyme was attached to a solid support compared to the free solution digestion. We obtained a clipping rate of 1.0 × 10(3) nucleotides s(-1) for the digestion of λ-DNA (48.5 kbp) by λ-exonuclease. The kinetic behavior of the solid-phase reactor could be described by a fractal Michaelis-Menten model with a catalytic efficiency nearly 17% better than the homogeneous solution-phase reaction. The results from this work will have important ramifications in new single-molecule DNA sequencing strategies that employ free mononucleotide identification.

Synthesis of three-dimensional reduced graphene oxide layer supported cobalt nanocrystals and their high catalytic activity in F-T CO2 hydrogenation.

PubMed

He, Fei; Niu, Na; Qu, Fengyu; Wei, Shuquan; Chen, Yujin; Gai, Shili; Gao, Peng; Wang, Yan; Yang, Piaoping

2013-09-21

The reduced graphene oxide (rGO) supported cobalt nanocrystals have been synthesized through an in situ crystal growth method using Co(acac)2 under solvothermal conditions by using DMF as the solvent. By carefully controlling the reaction temperature, the phase transition of the cobalt nanocrystals from the cubic phase to the hexagonal phase has been achieved. Moreover, the microscopic structure and morphology as well as the reduction process of the composite have been investigated in detail. It is found that oxygen-containing functional groups on the graphene oxide (GO) can greatly influence the formation process of the Co nanocrystals by binding the Co(2+) cations dissociated from the Co(acac)2 in the initial reaction solution at 220 °C, leading to the 3D reticular structure of the composite. Furthermore, this is the first attempt to use a Co/rGO composite as the catalyst in the F-T CO2 hydrogenation process. The catalysis testing results reveal that the as-synthesized 3D structured composite exhibits ideal catalytic activity and good stability, which may greatly extend the scope of applications for this kind of graphene-based metal hybrid material.

Low Concentration Fe-Doped Alumina Catalysts Using Sol-Gel and Impregnation Methods: The Synthesis, Characterization and Catalytic Performance during the Combustion of Trichloroethylene

PubMed Central

Maldonado, Carolina Solis; De la Rosa, Javier Rivera; Lucio-Ortiz, Carlos J.; Hernández-Ramírez, Aracely; Castillón Barraza, Felipe F.; Valente, Jaime S.

2014-01-01

The role of iron in two modes of integration into alumina catalysts was studied at 0.39 wt% Fe and tested in trichloroethylene combustion. One modified alumina was synthesized using the sol-gel method with Fe added in situ during hydrolysis; another modification was performed using calcined alumina, prepared using the sol-gel method and impregnated with Fe. Several characterization techniques were used to study the level of Fe modification in the γ-Al2O3 phase formed and to correlate the catalytic properties during trichloroethylene (TCE) combustion. The introduction of Fe in situ during the sol-gel process influenced the crystallite size, and three iron species were generated, namely, magnetite, maghemite and hematite. The impregnated Fe-alumina formed hematite and maghemite, which were highly dispersed on the γ-Al2O3 surface. The X-ray photoelectron spectra (XPS), FT-IR and Mössbauer spectroscopy analyses revealed how Fe interacted with the γ-Al2O3 lattice in both catalysts. The impregnated Fe-catalyst showed the best catalytic performance compared to the catalyst that was Fe-doped in situ by the sol-gel method; both had better catalytic activity than pure alumina. This difference in activity was correlated with the accessibility of the reactants to the hematite iron species on the surface. The chlorine poisoning for all three catalysts was less than 1.8%. PMID:28788556

EVALUATION OF SCR CATALYSTS FOR COMBINED CONTROL OF NOX AND MERCURY

EPA Science Inventory

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

CATALYTIC HYDRODECHLORINATION OF 1,3-DICHLOROPROPENE. (R826694C626)

EPA Science Inventory

The hydrodechlorination reactions of 1,3-dichloropropene, a component of the waste stream from epichlorohydrin manufacturing, were examined over a variety of catalysts in a packed-bed microreactor. The reactor operated between 7.5–9 Mpa and 325°C and rates of ...

40 CFR 63.1579 - What definitions apply to this subpart?

Code of Federal Regulations, 2011 CFR

2011-07-01

... process characterized by continual batch regeneration of catalyst in situ in any one of several reactors... device that treats (in-situ) the catalytic reforming unit recirculating coke burn exhaust gases for acid... or operator's convenience for in situ catalyst regeneration. Sulfur recovery unit means a process...

40 CFR 63.1579 - What definitions apply to this subpart?

Code of Federal Regulations, 2010 CFR

2010-07-01

... process characterized by continual batch regeneration of catalyst in situ in any one of several reactors... device that treats (in-situ) the catalytic reforming unit recirculating coke burn exhaust gases for acid... or operator's convenience for in situ catalyst regeneration. Sulfur recovery unit means a process...

A natural-gas fuel processor for a residential fuel cell system

NASA Astrophysics Data System (ADS)

Adachi, H.; Ahmed, S.; Lee, S. H. D.; Papadias, D.; Ahluwalia, R. K.; Bendert, J. C.; Kanner, S. A.; Yamazaki, Y.

A system model was used to develop an autothermal reforming fuel processor to meet the targets of 80% efficiency (higher heating value) and start-up energy consumption of less than 500 kJ when operated as part of a 1-kWe natural-gas fueled fuel cell system for cogeneration of heat and power. The key catalytic reactors of the fuel processor - namely the autothermal reformer, a two-stage water gas shift reactor and a preferential oxidation reactor - were configured and tested in a breadboard apparatus. Experimental results demonstrated a reformate containing ∼48% hydrogen (on a dry basis and with pure methane as fuel) and less than 5 ppm CO. The effects of steam-to-carbon and part load operations were explored.

An Evaluation of the Vapor Phase Catalytic Ammonia Removal Process for Use in a Mars Transit Vehicle

NASA Technical Reports Server (NTRS)

Flynn, Michael; Borchers, Bruce

1998-01-01

An experimental program has been developed to evaluate the potential of the Vapor Phase Catalytic Ammonia Reduction (VPCAR) technology for use as a Mars Transit Vehicle water purification system. Design modifications which will be required to ensure proper operation of the VPCAR system in reduced gravity are also evaluated. The VPCAR system is an integrated wastewater treatment technology that combines a distillation process with high temperature catalytic oxidation. The distillation portion of the system utilizes a vapor compression distillation process to provide an energy efficient phase change separation. This portion of the system removes any inorganic salts and large molecular weight, organic contaminates, i.e., non-volatile, from the product water stream and concentrates these contaminates into a byproduct stream. To oxidize the volatile organic compounds and ammonia, a vapor phase, high temperature catalytic oxidizer is used. This catalytic system converts these compounds along with the aqueous product into CO2, H2O, and N2O. A secondary catalytic bed can then be used to reduce the N2O to nitrogen and oxygen (although not evaluated in this study). This paper describes the design specification of the VPCAR process, the relative benefits of its utilization in a Mars Transit Vehicle, and the design modification which will be required to ensure its proper operation in reduced gravity. In addition, the results of an experimental evaluation of the processors is presented. This evaluation presents the processors performance based upon product water purity, water recovery rates, and power.

Method of preparing and utilizing a catalyst system for an oxidation process on a gaseous hydrocarbon stream

DOEpatents

Berry, David A; Shekhawat, Dushyant; Smith, Mark; Haynes, Daniel

2013-07-16

The disclosure relates to a method of utilizing a catalyst system for an oxidation process on a gaseous hydrocarbon stream with a mitigation of carbon accumulation. The system is comprised of a catalytically active phase deposited onto an oxygen conducting phase, with or without supplemental support. The catalytically active phase has a specified crystal structure where at least one catalytically active metal is a cation within the crystal structure and coordinated with oxygen atoms within the crystal structure. The catalyst system employs an optimum coverage ratio for a given set of oxidation conditions, based on a specified hydrocarbon conversion and a carbon deposition limit. Specific embodiments of the catalyst system are disclosed.

Perspectives on multifield models

DOE Office of Scientific and Technical Information (OSTI.GOV)

Banerjee, S.

1997-07-01

Multifield models for prediction of nuclear reactor thermalhydraulics are reviewed from the viewpoint of their structure and requirements for closure relationships. Their strengths and weaknesses are illustrated with examples, indicating that they are effective in predicting separated and distributed flow regimes, but have problems for flows with large oscillations. Needs for multifield models are also discussed in the context of reactor operations and accident simulations. The highest priorities for future developments appear to relate to closure relationships for three-dimensional multifield models with emphasis on those needed for calculations of phase separation and entrainment/de-entrainment in complex geometries.

Investigation of a para-ortho hydrogen reactor for application to spacecraft sensor cooling

NASA Technical Reports Server (NTRS)

Nast, T. C.

1983-01-01

The utilization of solid hydrogen in space for sensor and instrument cooling is a very efficient technique for long term cooling or for cooling at high heat rates. The solid hydrogen can provide temperatures as low as 7 to 8 K to instruments. Vapor cooling is utilized to reduce parasitic heat inputs to the 7 to 8 K stage and is effective in providing intermediate cooling for instrument components operating at higher temperatures. The use of solid hydrogen in place of helium may lead to weight reductions as large as a factor of ten and an attendent reduction in system volume. The results of an investigation of a catalytic reactor for use with a solid hydrogen cooling system is presented. Trade studies were performed on several configurations of reactor to meet the requirements of high reactor efficiency with low pressure drop. Results for the selected reactor design are presented for both liquid hydrogen systems operating at near atmospheric pressure and the solid hydrogen cooler operating as low as 1 torr.

Production of ammonia from plasma-catalytic decomposition of urea: Effects of carrier gas composition.

PubMed

Fan, Xing; Li, Jian; Qiu, Danqi; Zhu, Tianle

2018-04-01

Effects of carrier gas composition (N 2 /air) on NH 3 production, energy efficiency regarding NH 3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an Al 2 O 3 -packed dielectric barrier discharge (DBD) reactor at room temperature. Results show that the presence of O 2 in the carrier gas accelerates the conversion of urea but leads to less generation of NH 3 . The final yield of NH 3 in the gas phase decreased from 70.5%, 78.7%, 66.6% and 67.2% to 54.1%, 51.7%, 49.6% and 53.4% for applied voltages of 17, 19, 21 and 23kV, respectively when air was used as the carrier gas instead of N 2 . From the viewpoint of energy savings, however, air carrier gas is better than N 2 due to reduced energy consumption and increased energy efficiency for decomposition of a fixed amount of urea. Carrier gas composition has little influence on the major decomposition pathways of urea under the synergetic effects of plasma and Al 2 O 3 catalyst to give NH 3 and CO 2 as the main products. Compared to a small amount of N 2 O formed with N 2 as the carrier gas, however, more byproducts including N 2 O and NO 2 in the gas phase and NH 4 NO 3 in solid deposits were produced with air as the carrier gas, probably due to the unproductive consumption of NH 3 , the possible intermediate HNCO and even urea by the abundant active oxygen species and nitrogen oxides generated in air-DBD plasma. Copyright © 2017. Published by Elsevier B.V.

Modification of UASB reactor by using CFD simulations for enhanced treatment of municipal sewage.

PubMed

Das, Suprotim; Sarkar, Supriya; Chaudhari, Sanjeev

2018-02-01

Up-flow anaerobic sludge blanket (UASB) has been in use since last few decades for the treatment of organic wastewaters. However, the performance of UASB reactor is quite low for treatment of low strength wastewaters (LSWs) due to less biogas production leading to poor mixing. In the present research work, a modification was done in the design of UASB to improve mixing of reactor liquid which is important to enhance the reactor performance. The modified UASB (MUASB) reactor was designed by providing a slanted baffle along the height of the reactor having an angle of 5.7° with the vertical wall. A two-dimensional computational fluid dynamics (CFD) simulation of three phase gas-liquid-solid flow in MUASB reactor was performed and compared with conventional UASB reactor. The CFD study indicated better mixing in terms of vorticity magnitude in MUASB reactor as compared to conventional UASB, which was reflected in the reactor performance. The performance of MUASB was compared with conventional UASB reactor for the onsite treatment of domestic sewage as LSW. Around 16% higher total chemical oxygen demand removal efficiency was observed in MUASB reactor as compared to conventional UASB during this study. Therefore, this MUASB model demonstrates a qualitative relationship between mixing and performance during the treatment of LSW. From the study, it seems that MUASB holds promise for field applications.

Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

DOE PAGES

Li, Y.; Zakharov, D.; Zhao, S.; ...

2015-06-29

Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction—ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. Lastly,more » this method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.« less

Catalytic pyrolysis of black-liquor lignin by co-feeding with different plastics in a fluidized bed reactor.

PubMed

Zhang, Huiyan; Xiao, Rui; Nie, Jianlong; Jin, Baosheng; Shao, Shanshan; Xiao, Guomin

2015-09-01

Catalytic co-pyrolysis of black-liquor lignin and waste plastics (polyethylene, PE; polypropylene PP; polystyrene, PS) was conducted in a fluidized bed. The effects of temperature, plastic to lignin ratio, catalyst and plastic types on product distributions were studied. Both aromatic and olefin yields increased with increasing PE proportion. Petrochemical yield of co-pyrolysis of PE and lignin was LOSA-1 > spent FCC > Gamma-Al2O3 > sand. The petrochemical yield with LOSA-1 is 43.9% which is more than two times of that without catalyst. The feedstock for co-pyrolysis with lignin is polystyrene > polyethylene > polypropylene. Catalytic co-pyrolysis of black-liquor lignin with PS produced the maximum aromatic yield (55.3%), while co-pyrolysis with PE produced the maximum olefin yield (13%). Copyright © 2015 Elsevier Ltd. All rights reserved.

Multifunctional two-stage riser fluid catalytic cracking process.

PubMed

Zhang, Jinhong; Shan, Honghong; Chen, Xiaobo; Li, Chunyi; Yang, Chaohe

This paper described the discovering process of some shortcomings of the conventional fluid catalytic cracking (FCC) process and the proposed two-stage riser (TSR) FCC process for decreasing dry gas and coke yields and increasing light oil yield, which has been successfully applied in 12 industrial units. Furthermore, the multifunctional two-stage riser (MFT) FCC process proposed on the basis of the TSR FCC process was described, which were carried out by the optimization of reaction conditions for fresh feedstock and cycle oil catalytic cracking, respectively, by the coupling of cycle oil cracking and light FCC naphtha upgrading processes in the second-stage riser, and the specially designed reactor for further reducing the olefin content of gasoline. The pilot test showed that it can further improve the product quality, increase the diesel yield, and enhance the conversion of heavy oil.

One-dimensional biomass fast pyrolysis model with reaction kinetics integrated in an Aspen Plus Biorefinery Process Model

DOE PAGES

Humbird, David; Trendewicz, Anna; Braun, Robert; ...

2017-01-12

A biomass fast pyrolysis reactor model with detailed reaction kinetics and one-dimensional fluid dynamics was implemented in an equation-oriented modeling environment (Aspen Custom Modeler). Portions of this work were detailed in previous publications; further modifications have been made here to improve stability and reduce execution time of the model to make it compatible for use in large process flowsheets. The detailed reactor model was integrated into a larger process simulation in Aspen Plus and was stable for different feedstocks over a range of reactor temperatures. Sample results are presented that indicate general agreement with experimental results, but with higher gasmore » losses caused by stripping of the bio-oil by the fluidizing gas in the simulated absorber/condenser. Lastly, this integrated modeling approach can be extended to other well-defined, predictive reactor models for fast pyrolysis, catalytic fast pyrolysis, as well as other processes.« less

One-dimensional biomass fast pyrolysis model with reaction kinetics integrated in an Aspen Plus Biorefinery Process Model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Humbird, David; Trendewicz, Anna; Braun, Robert

A biomass fast pyrolysis reactor model with detailed reaction kinetics and one-dimensional fluid dynamics was implemented in an equation-oriented modeling environment (Aspen Custom Modeler). Portions of this work were detailed in previous publications; further modifications have been made here to improve stability and reduce execution time of the model to make it compatible for use in large process flowsheets. The detailed reactor model was integrated into a larger process simulation in Aspen Plus and was stable for different feedstocks over a range of reactor temperatures. Sample results are presented that indicate general agreement with experimental results, but with higher gasmore » losses caused by stripping of the bio-oil by the fluidizing gas in the simulated absorber/condenser. Lastly, this integrated modeling approach can be extended to other well-defined, predictive reactor models for fast pyrolysis, catalytic fast pyrolysis, as well as other processes.« less

Catalytic cracking of non-edible sunflower oil over ZSM-5 for hydrocarbon bio-jet fuel.

PubMed

Zhao, Xianhui; Wei, Lin; Julson, James; Qiao, Qiquan; Dubey, Ashish; Anderson, Gary

2015-03-25

Non-edible sunflower oils that were extracted from sunflower residual wastes were catalytically cracked over a ZSM-5 catalyst in a fixed-bed reactor at three different reaction temperatures: 450°C, 500°C and 550°C. The catalyst was characterized using XRD, FT-IR, BET and SEM. Characterizations of the upgraded sunflower oils, hydrocarbon fuels, distillation residues and non-condensable gases were carried out. The effect of the reaction temperature on the yield and quality of liquid products was discussed. The results showed that the reaction temperature affected the hydrocarbon fuel yield but had a minor influence on its properties. The highest conversion efficiency from sunflower oils to hydrocarbon fuels was 30.1%, which was obtained at 550°C. The reaction temperature affected the component content of the non-condensable gases. The non-condensable gases generated at 550°C contained the highest content of light hydrocarbons (C1-C5), CO, CO2 and H2. Compared to raw sunflower oils, the properties of hydrocarbon fuels including the dynamic viscosity, pH, moisture content, density, oxygen content and heating value were improved. Copyright © 2015 Elsevier B.V. All rights reserved.

Single-phase and two-phase anaerobic digestion of fruit and vegetable waste: Comparison of start-up, reactor stability and process performance

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ganesh, Rangaraj; Torrijos, Michel, E-mail: michel.torrijos@supagro.inra.fr; Sousbie, Philippe

Highlights: • Single-phase and two-phase systems were compared for fruit and vegetable waste digestion. • Single-phase digestion produced a methane yield of 0.45 m{sup 3} CH{sub 4}/kg VS and 83% VS removal. • Substrate solubilization was high in acidification conditions at 7.0 kg VS/m{sup 3} d and pH 5.5–6.2. • Energy yield was lower by 33% for two-phase system compared to the single-phase system. • Simple and straight-forward operation favored single phase process over two-phase process. - Abstract: Single-phase and two-phase digestion of fruit and vegetable waste were studied to compare reactor start-up, reactor stability and performance (methane yield, volatilemore » solids reduction and energy yield). The single-phase reactor (SPR) was a conventional reactor operated at a low loading rate (maximum of 3.5 kg VS/m{sup 3} d), while the two-phase system consisted of an acidification reactor (TPAR) and a methanogenic reactor (TPMR). The TPAR was inoculated with methanogenic sludge similar to the SPR, but was operated with step-wise increase in the loading rate and with total recirculation of reactor solids to convert it into acidification sludge. Before each feeding, part of the sludge from TPAR was centrifuged, the centrifuge liquid (solubilized products) was fed to the TPMR and centrifuged solids were recycled back to the reactor. Single-phase digestion produced a methane yield of 0.45 m{sup 3} CH{sub 4}/kg VS fed and VS removal of 83%. The TPAR shifted to acidification mode at an OLR of 10.0 kg VS/m{sup 3} d and then achieved stable performance at 7.0 kg VS/m{sup 3} d and pH 5.5–6.2, with very high substrate solubilization rate and a methane yield of 0.30 m{sup 3} CH{sub 4}/kg COD fed. The two-phase process was capable of high VS reduction, but material and energy balance showed that the single-phase process was superior in terms of volumetric methane production and energy yield by 33%. The lower energy yield of the two-phase system was due to the loss of energy during hydrolysis in the TPAR and the deficit in methane production in the TPMR attributed to COD loss due to biomass synthesis and adsorption of hard COD onto the flocs. These results including the complicated operational procedure of the two-phase process and the economic factors suggested that the single-phase process could be the preferred system for FVW.« less

Processing and synthesis of multi-metallic nano oxide ceramics via liquid-feed flame spray pyrolysis

NASA Astrophysics Data System (ADS)

Azurdia, Jose Antonio

The liquid-feed flame spray pyrolysis (LF-FSP) process aerosolizes metal-carboxylate precursors dissolved in alcohol with oxygen and combusts them at >1500°C. The products are quenched rapidly (˜10s msec) to < 400°C. By selecting the appropriate precursor mixtures, the compositions of the resulting oxide nanopowders can be tailored easily, which lends itself to combinatorial studies of systems facilitating material property optimization. The resulting nanopowders typically consist of single crystal particles with average particle sizes (APS) < 35 nm, specific surface areas (SSA) of 20-60 m2/g and spherical morphology. LF-FSP provides access to novel single phase nanopowders, known phases at compositions outside their published phase diagrams, intimate mixing at nanometer length scales in multi metallic oxide nanopowders, and control of stoichiometry to ppm levels. The materials produced may exhibit unusual properties including structural, catalytic, and photonic ones and lower sintering temperatures. Prior studies used LF-FSP to produce MgAl2O4 spinel for applications in transparent armor and IR radomes. In these studies, a stable spinel structure with a (MgO)0.1(Al2O3)0.9 composition well outside the known phase field was observed. The work reported here extends this observation to two other spinel systems: Al2O3-NiO, Al2O3-CoOx; followed by three series of transition metal binary oxides, NiO-CoO, NiO-MoO3, NiO-CuO. The impetus to study spinels derives both from the fact that a number of them are known transparent ceramics, but also others offer high SSAs coupled with unusual phases that suggest potentially novel catalytic materials. Because LF-FSP provides access to any composition, comprehensive studies of the entire tie-lines were conducted rather than just compositions of value for catalytic applications. Initial efforts established baseline properties for the nano aluminate spinels, then three binary transition metal oxide sets (Ni-Co, Ni-Mo and Ni-Cu) known for their catalytic properties. These materials then serve as baseline studies for ternary systems, such as Al:(Ni-Co)O, or Al(Ni-Cu)O likely to offer superior catalytic properties because of the relatively high SSA Al2O3. The final chapter returns to photonic materials, in the MgO-Y2O 3 system targeting transparent ceramics through select compositions along the tie-line. The work presented here builds on the MgAl2O 4 spinel material and continues to develop the processing techniques required to achieve transparent nano-grained ceramic materials. Thus the overall goal of this dissertation was to systematically produce novel nano-oxide materials and characterized their material properties. The first chapters focus on solid solutions at low Ni or Co amounts that form phase pure spinels outside the expected composition range, at 21-22 mol % NiO and CoO. Additionally, (NiO)0.22(Al2O3) 0.78 was found to be very stable, as it did not convert to alpha-Al 2O3 plus cubic-NiO on heating to 1200°C for 10 h. The last chapter is a preliminary step toward identifying optimal Y 2O3-MgO powders that can be transparent ceramics. Ball milling led to much higher adsorption of surface species. Preliminary sintering studies of the this system showed that vacuum has the largest effect on lowering the temperature of maximum shrinkage rate by ≤ 80°C.

DOE Office of Scientific and Technical Information (OSTI.GOV)

NONE

The objective of Task 1 is to prepare and evaluate catalysts and to develop efficient reactor systems for the selective conversion of hydrogen-lean synthesis gas to alcohol fuel extender and octane enhancers. Task 1 is subdivided into three separate subtasks: laboratory and equipment setup; catalysis research; and reaction engineering and modeling. Research at West Virginia University (WVU) is focused on molybdenum-based catalysts for higher alcohol synthesis. Parallel research carried out at Union Carbide Corporation (UCC) is focused on transition-metal-oxide catalysts. During this time period, at WVU, we tried several methods to eliminate problems related to condensation of heavier products whenmore » reduced Mo-Ni-K/C materials were used as catalysts. We then resumed our kinetic study on the reduced Mo-Ni-K/C materials were used as catalysts. We then resumed our kinetic study on the reduced Mo-Ni-K/C catalysts. We have also obtained same preliminary results in our attempts to analyze quantitatively the temperature-programmed reduction spectra for C- supported Mo-based catalysts. We have completed the kinetic study for the sulfided Co-K-MoS{sub 2}/C catalyst. We have compared the results of methanol synthesis using the membrane reactor with those using a simple plug-flow reactor. At UCC, the complete characterization of selected catalysts has been completed. The results suggest that catalyst pretreatment under different reducing conditions yield different surface compositions and thus different catalytic reactivities.« less

Gallium-rich Pd-Ga phases as supported liquid metal catalysts

NASA Astrophysics Data System (ADS)

Taccardi, N.; Grabau, M.; Debuschewitz, J.; Distaso, M.; Brandl, M.; Hock, R.; Maier, F.; Papp, C.; Erhard, J.; Neiss, C.; Peukert, W.; Görling, A.; Steinrück, H.-P.; Wasserscheid, P.

2017-09-01

A strategy to develop improved catalysts is to create systems that merge the advantages of heterogeneous and molecular catalysis. One such system involves supported liquid-phase catalysts, which feature a molecularly defined, catalytically active liquid film/droplet layer adsorbed on a porous solid support. In the past decade, this concept has also been extended to supported ionic liquid-phase catalysts. Here we develop this idea further and describe supported catalytically active liquid metal solutions (SCALMS). We report a liquid mixture of gallium and palladium deposited on porous glass that forms an active catalyst for alkane dehydrogenation that is resistant to coke formation and is thus highly stable. X-ray diffraction and X-ray photoelectron spectroscopy, supported by theoretical calculations, confirm the liquid state of the catalytic phase under the reaction conditions. Unlike traditional heterogeneous catalysts, the supported liquid metal reported here is highly dynamic and catalysis does not proceed at the surface of the metal nanoparticles, but presumably at homogeneously distributed metal atoms at the surface of a liquid metallic phase.

Catalytic Ethanol Dehydration to Ethylene over Nanocrystalline χ- and γ-Al2O3 Catalysts.

PubMed

Janlamool, Jakrapan; Jongsomjit, Bunjerd

2017-01-01

The study is aimed to investigate the combination of nanocrystalline γ- and χ- alumina that displays the attractive chemical and physical properties for the catalytic dehydration of ethanol. The correlation between the acid density and ethanol conversion was observed. The high acid density apparently results in high catalytic activity, especially for the equally mixed γ- and χ- phase alumina (G50C50). In order to obtain a better understanding on how different catalysts would affect the ethylene yield, one of the most powerful techniques such as X-ray photoelectron spectroscopy (XPS) was performed. Hence, the different O 1s surface atoms can be identified and divided into three types including lattice oxygen (O, 530.7 eV), surface hydroxyl (OH, 532.1 eV) and lattice water (H 2 O, 532.9 eV). It was remarkably found that the large amount of O 1s surface atoms in lattice water can result in increased ethylene yield. In summary, the appearance of metastable χ-alumina structure exhibited better catalytic activity and ethylene yield than γ- alumina. Thus, the introduction of metastable χ- alumina structure into γ- alumina enhanced catalytic activity and ethylene yield. As the result, it was found that the G50C50 catalyst exhibits the ethylene yield (80%) at the lowest reaction temperature ca. 250°C among other catalysts.

Bimetallic catalysts for continuous catalytic wet air oxidation of phenol.

PubMed

Fortuny, A; Bengoa, C; Font, J; Fabregat, A

1999-01-29

Catalytic wet oxidation has proved to be effective at eliminating hazardous organic compounds, such as phenol, from waste waters. However, the lack of active long-life oxidation catalysts which can perform in aqueous phase is its main drawback. This study explores the ability of bimetallic supported catalysts to oxidize aqueous phenol solutions using air as oxidant. Combinations of 2% of CoO, Fe2O3, MnO or ZnO with 10% CuO were supported on gamma-alumina by pore filling, calcined and later tested. The oxidation was carried out in a packed bed reactor operating in trickle flow regime at 140 degrees C and 900 kPa of oxygen partial pressure. Lifetime tests were conducted for 8 days. The pH of the feed solution was also varied. The results show that all the catalysts tested undergo severe deactivation during the first 2 days of operation. Later, the catalysts present steady activity until the end of the test. The highest residual phenol conversion was obtained for the ZnO-CuO, which was significantly higher than that obtained with the 10% CuO catalyst used as reference. The catalyst deactivation is related to the dissolution of the metal oxides from the catalyst surface due to the acidic reaction conditions. Generally, the performance of the catalysts was better when the pH of the feed solution was increased.

Hydrocarbon liquid production via the bioCRACK process and catalytic hydroprocessing of the product oil

DOE PAGES

Schwaiger, Nickolaus; Elliott, Douglas C.; Ritzberger, Jurgen; ...

2015-01-01

Continuous hydroprocessing of liquid phase pyrolysis bio-oil, provided by BDI-BioEnergy International bioCRACK pilot plant at OMV Refinery in Schwechat/Vienna Austria was investigated. These hydroprocessing tests showed promising results using catalytic hydroprocessing strategies developed for unfractionated bio-oil. A sulfided base metal catalyst (CoMo on Al2O3) was evaluated. The bed of catalyst was operated at 400 °C in a continuous-flow reactor at a pressure of 12.1 MPa with flowing hydrogen. The condensed liquid products were analyzed and found that the hydrocarbon liquid was significantly hydrotreated so that nitrogen and sulfur were below the level of detection (<0.05), while the residual oxygen rangedmore » from 0.7 to 1.2%. The density of the products varied from 0.71 g/mL up to 0.79 g/mL with a correlated change of the hydrogen to carbon atomic ratio from 2.1 down to 1.9. The product quality remained high throughout the extended tests suggesting minimal loss of catalyst activity through the test. These tests provided the data needed to assess the quality of liquid fuel products obtained from the bioCRACK process as well as the activity of the catalyst for comparison with products obtained from hydrotreated fast pyrolysis bio-oils from fluidized-bed operation.« less

Aromatic chemicals by iron-catalyzed hydrotreatment of lignin pyrolysis vapor.

PubMed

Olcese, Roberto Nicolas; Lardier, George; Bettahar, Mohammed; Ghanbaja, Jaafar; Fontana, Sébastien; Carré, Vincent; Aubriet, Frédéric; Petitjean, Dominique; Dufour, Anthony

2013-08-01

Lignin is a potential renewable material for the production of bio-sourced aromatic chemicals. We present the first hydrotreatment of lignin pyrolysis vapors, before any condensation, using inexpensive and sustainable iron-silica (Fe/SiO2 ) and iron-activated carbon (Fe/AC) catalysts. Lignin pyrolysis was conducted in a tubular reactor and vapors were injected in a fixed bed of catalysts (673 K, 1 bar) with stacks to investigate the profile of coke deposit. More than 170 GC-analyzable compounds were identified by GCxGC (heart cutting)/flame ionization detector mass spectrometry. Lignin oligomers were analyzed by very high resolution mass spectrometry, called the "petroleomic" method. They are trapped by the catalytic fixed bed and, in particular, by the AC. The catalysts showed a good selectivity for the hydrodeoxygenation of real lignin vapors to benzene, toluene, xylenes, phenol, cresols, and alkyl phenols. The spent catalysts were characterized by temperature-programmed oxidation, transmission electron microscopy (TEM), and N2 sorption. Micropores in the Fe/AC catalyst are completely plugged by coke deposits, whereas the mesoporous structure of Fe/SiO2 is unaffected. TEM images reveal two different types of coke deposit: 1) catalytic coke deposited in the vicinity of iron particles and 2) thermal coke (carbonaceous particles ≈1 μm in diameter) formed from the gas-phase growth of lignin oligomers. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mihaela Grigore; Richard Sakurovs; David French

Gasification of coke contributes to its degradation in the blast furnace. In this study, the effect of gasification on the inherent catalytic minerals in cokes and their reciprocal influence on gasification are investigated. The catalytic mineral phases identified in the cokes used in this study were metallic iron, iron sulfides, and iron oxides. Metallic iron and pyrrhotite were rapidly oxidized during gasification to iron oxide. The catalysts had a strong influence on the apparent rates at the initial stages of reaction. As gasification proceeds, their effect on the reaction rate diminishes as a result of reducing the surface contact betweenmore » catalyst and carbon matrix because of carbon consumption around the catalyst particles; with extended burnout the reactivity of the coke becomes increasingly dependent on surface area. The reaction rate in the initial stages was also influenced by the particle size of the catalytic minerals; for a given catalytic iron level, the cokes whose catalytic minerals were more finely dispersed had a higher apparent reaction rate than cokes containing larger catalytic particles. Iron, sodium, and potassium in the amorphous phase did not appear to affect the reaction rate. 40 refs., 16 figs., 6 tabs.« less

The start-up of denitrifying phosphorus removal system by using nitrite as electron acceptor

NASA Astrophysics Data System (ADS)

Li, W.; Liu, J.; Sun, H. Z.; Fu, J. X.; Gao, Y.; Sun, J.

2017-08-01

The inoculation of short-cut denitrifying polyphosphate-accumulating organisms (DPAOs) mainly included two-phase inoculation and three-phase inoculation. The short-cut denitrifying phosphorus removal bacteria were quickly inoculated by sequencing batch reactor (SBR) to treatment domestic wastewater. The results showed that the average effluent concentration of TP was 0.85 mg/L after 132 cycles by 44 days in two-phase inoculation. The removal rates of NO2 --N, TP and COD were 94.73%, 95.47% and 89.96% after 126 cycles by 42 days in three-phase inoculation, and the effluent concentrations were separately 1.31 mg/L, 0.45 mg/L and 17.07 mg/L, which reached the first A class requirement of Urban sewage treatment plant pollutant discharge standard. It was indicated that the efficiency of three-phase inoculation was higher. Anoxic phosphorus uptake was influenced seriously by anaerobic residual carbon, and it was the difference of the two inoculations.

A novel kinetic modeling method for the stabilization phase of the composting process for biodegradation of solid wastes.

PubMed

Ebrahimzadeh, Reza; Ghazanfari Moghaddam, Ahmad; Sarcheshmehpour, Mehdi; Mortezapour, Hamid

2017-12-01

Biomass degradation kinetics of the composting process for kitchen waste, pruned elm tree branches and sheep manure were studied to model changes in volatile solids (VS) over time. Three experimental reactors containing raw mixtures with a carbon to nitrogen (C/N) ratio of 27:1 and a moisture content of 65% were prepared. During the composting process two of the reactors used forced air and the third used natural aeration. The composting stabilization phases in all reactors were completed in 30 days. During this period, composting indexes such as temperature, moisture content and VS changes were recorded. Elementary reactions were used for kinetics modeling of the degradation process. Results showed that the numerical values of rate constant ( k) for zero-order ranged from 0.86 to 1.03 VS×day -1 , for first-order models it ranged from 0.01 to 0.02 day -1 , for second-order the range was from 1.36×10 -5 to 1.78×10 -5 VS -1 ×day -1 and for n-order the rate constant ranged from 0.031 to 0.095 VS (1-n) ×day -1 . The resulting models were validated by comparing statistical parameters. Evaluation of the models showed that, in the aerated reactors, the n-order models (less than 1) successfully estimated the VS changes. In the non-aeration reactor, for the second-order model good agreement was achieved between the simulated and actual quantities of VS. Also, half-life time provided a useful criterion for the estimation of expected time for completion of different phases of composting.

Role of oil derived carbonaceous phase in the performance of sewage sludge-based materials as media for desulfurizaton of digester gas

NASA Astrophysics Data System (ADS)

Kante, Karifala; Qiu, Jieshan; Zhao, Zongbin; Chang, Yu; Bandosz, Teresa J.

2008-02-01

Desulfurization adsorbents for purification of digester gas were prepared by pyrolysis of sewage sludge impregnated with spent mineral oil. To evaluate the changes in the structural and chemical properties the pyrolysis time and temperature varied. The materials were characterized using adsorption of nitrogen, FTIR, XRD, ICP, SEM and thermal analysis. Their catalytic activity was tested in the removal of hydrogen sulfide from simulated mixture of digester gas. The results indicated the importance of new carbon phase from the oil precursor. It provided mesoporosity, which increased the dispersion of catalytic phase and space for storage of surface reaction products. The results indicated that the adsorbents obtained at 950 °C are much more active in the process of hydrogen sulfide oxidation than those obtained at 650 °C. Moreover, longer heat treatment is also beneficial for the development of surface catalytic properties. Extensive pyrolysis stabilizes carbon phase via increasing its degree of aromatization and provides activation agents for this phase coming from decomposition and rearrangement of inorganic phase.

Four-Component Catalytic Machinery: Reversible Three-State Control of Organocatalysis by Walking Back and Forth on a Track.

PubMed

Mittal, Nikita; Özer, Merve S; Schmittel, Michael

2018-04-02

A three-component supramolecular walker system is presented where a two-footed ligand (biped) walks back and forth on a tetrahedral 3D track upon the addition and removal of copper(I) ions, respectively. The addition of N-methylpyrrolidine as a catalyst to the walker system generates a four-component catalytic machinery, which acts as a three-state switchable catalytic ensemble in the presence of substrates for a conjugate addition. The copper(I)-ion-initiated walking process of the biped ligand on the track regulates the catalytic activity in three steps: ON versus int ON (intermediate ON) versus OFF. To establish the operation of the four-component catalytic machinery in a mixture of all constituents, forward and backward cycles were performed in situ illustrating that both the walking process and catalytic action are fully reversible and reproducible.

Seed and blanket fuel arrangement for dual-phase nuclear reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Congdon, S.P.; Fawcett, R.M.

1992-09-22

This patent describes a fuel management method for a dual-phase nuclear reactor, it comprises: installing a fuel bundle at a first core location accessed by coolant through a relatively small aperture, each of the bundles having a predetermined group of fuel elements; operating the reactor a first time; shutting down the reactor; reinstalling the fuel bundle at a second core location accessed by coolant through a relatively large aperture; and operating the reactor a second time.

Catalytic diversity in self-propagating peptide assemblies

NASA Astrophysics Data System (ADS)

Omosun, Tolulope O.; Hsieh, Ming-Chien; Childers, W. Seth; Das, Dibyendu; Mehta, Anil K.; Anthony, Neil R.; Pan, Ting; Grover, Martha A.; Berland, Keith M.; Lynn, David G.

2017-08-01

The protein-only infectious agents known as prions exist within cellular matrices as populations of assembled polypeptide phases ranging from particles to amyloid fibres. These phases appear to undergo Darwinian-like selection and propagation, yet remarkably little is known about their accessible chemical and biological functions. Here we construct simple peptides that assemble into well-defined amyloid phases and define paracrystalline surfaces able to catalyse specific enantioselective chemical reactions. Structural adjustments of individual amino acid residues predictably control both the assembled crystalline order and their accessible catalytic repertoire. Notably, the density and proximity of the extended arrays of enantioselective catalytic sites achieve template-directed polymerization of new polymers. These diverse amyloid templates can now be extended as dynamic self-propagating templates for the construction of even more complex functional materials.

Solid state proton and electron mediating membrane and use in catalytic membrane reactors

DOEpatents

White, James H.; Schwartz, Michael; Sammells, Anthony F.

2001-01-01

Mixed electron- and proton-conducting metal oxide materials are provided. These materials are useful in fabrication of membranes for use in catalytic membrane reactions, particularly for promoting dehydrogenation of hydrocarbons, oligomerization of hydrocarbons and for the decomposition of hydrogen-containing gases. Membrane materials are perovskite compounds of the formula: AB.sub.1-x B'.sub.x O.sub.3-y where A=Ca, Sr, or Ba; B=Ce, Tb, Pr or Th; B'=Ti, V, Cr, Mn, Fe, Co, Ni or Cu; 0.2.ltoreq.x.ltoreq.0.5, and y is a number sufficient to neutralize the charge in the mixed metal oxide material.

Solid state proton and electron mediating membrane and use in catalytic membrane reactors

DOEpatents

White, James H.; Schwartz, Michael; Sammells, Anthony F.

2000-01-01

Mixed electron- and proton-conducting metal oxide materials are provided. These materials are useful in fabrication of membranes for use in catalytic membrane reactions, particularly for promoting dehydrogenation of hydrocarbons, oligomerization of hydrocarbons and for the decomposition of hydrogen-containing gases. Membrane materials are perovskite compounds of the formula: AB.sub.1-x B'.sub.x O.sub.3-y where A=Ca, Sr, or Ba; B=Ce, Tb, Pr or Th; B'=Ti, V, Cr, Mn, Fe, Co, Ni or Cu; 0.2

Catalytic combustion with incompletely vaporized residual fuel

NASA Technical Reports Server (NTRS)

Rosfjord, T. J.

1981-01-01

Catalytic combustion of fuel lean mixtures of incompletely vaporized residual fuel and air was investigated. The 7.6 cm diameter, graded cell reactor was constructed from zirconia spinel substrate and catalyzed with a noble metal catalyst. Streams of luminous particles exited the rector as a result of fuel deposition and carbonization on the substrate. Similar results were obtained with blends of No. 6 and No. 2 oil. Blends of shale residual oil and No. 2 oil resulted in stable operation. In shale oil blends the combustor performance degraded with a reduced degree of fuel vaporization. In tests performed with No. 2 oil a similar effect was observed.

Demonstrating the Effect of Interphase Mass Transfer in a Transparent Fluidized Bed Reactor

ERIC Educational Resources Information Center

Saayman, Jean; Nicol, Willie

2011-01-01

A demonstration experiment is described that employs the ozone decomposition reaction at ambient conditions on Fe2O3 impregnated Fluidized Catalytic Cracking (FCC) catalyst. Using a two-dimensional see-through column the importance of interphase mass transfer is clearly illustrated by the significant difference in ozone conversion between the…

Current problems in applied mathematics and mathematical modeling

NASA Astrophysics Data System (ADS)

Alekseev, A. S.

Papers are presented on mathematical modeling noting applications to such fields as geophysics, chemistry, atmospheric optics, and immunology. Attention is also given to models of ocean current fluxes, atmospheric and marine interactions, and atmospheric pollution. The articles include studies of catalytic reactors, models of global climate phenomena, and computer-assisted atmospheric models.

Compression Ratio and Catalyst Aging Effects on Aqueous Ethanol Ignition (Year 2) : Part 2 Catalyst Aging and Effects of Water on Ignition

DOT National Transportation Integrated Search

2009-09-01

A tubular plug-flow reactor under low Reynolds Numbers Re flow regimes, along with a 127 um diameter coiled platinum (Pt) wire, were used to study catalytic surface reactions of nonflammable, fuel-lean mixtures of propane, oxygen, and water vapor dil...

STUDY OF THE EFFECT OF CHLORINE ADDITION ON MERCURY OXIDATION BY SCR CATALYST UNDER SIMULATED SUBBITUMINOUS COAL FLUE GAS

EPA Science Inventory

An entrained flow reactor is used to study the effect of addition of chlorine-containing species on the oxidation of elemental mercury (Hgo)by a selective catalytic reduction (SCR) catalyst in simulated subbituminous coal combustion flue gas. The combustion flue gas was doped wit...

Catalytic Oxidative Dehydration of Butanol Isomers: 1-Butanol, 2-Butanol, and Isobutanol

DTIC Science & Technology

2011-09-01

butanol, 2-butanol, and isobutanol using a millisecond contact time reactor. Both alumina foam and rhodium -alumina foam catalysts convert these four...such as n-octane, into mixtures of olefins (10). A rhodium /cerium catalyst has been proposed in the past to convert biodiesel into olefins (11). The