Science.gov

Sample records for high-efficiency steam reformer

  1. Demonstration of a Highly Efficient Solid Oxide Fuel Cell Power System Using Adiabatic Steam Reforming and Anode Gas Recirculation

    SciTech Connect

    Powell, Michael R.; Meinhardt, Kerry D.; Sprenkle, Vincent L.; Chick, Lawrence A.; Mcvay, Gary L.

    2012-05-01

    Solid oxide fuel cells (SOFC) are currently being developed for a wide variety of applications because of their high efficiency at multiple power levels. Applications for SOFCs encompass a large range of power levels including 1-2 kW residential combined heat and power applications, 100-250 kW sized systems for distributed generation and grid extension, and MW-scale power plants utilizing coal. This paper reports on the development of a highly efficient, small-scale SOFC power system operating on methane. The system uses adiabatic steam reforming of methane and anode gas recirculation to achieve high net electrical efficiency. The anode exit gas is recirculated and all of the heat and water required for the endothermic reforming reaction are provided by the anode gas emerging from the SOFC stack. Although the single-pass fuel utilization is only about 55%, because of the anode gas recirculation the overall fuel utilization is up to 93%. The demonstrated system achieved gross power output of 1650 to 2150 watts with a maximum net LHV efficiency of 56.7% at 1720 watts. Overall system efficiency could be further improved to over 60% with use of properly sized blowers.

  2. Supported metal catalysts for alcohol/sugar alcohol steam reforming

    SciTech Connect

    Davidson, Stephen; Zhang, He; Sun, Junming; Wang, Yong

    2014-08-21

    Despite extensive studies on hydrogen production via steam reforming of alcohols and sugar alcohols, catalysts typically suffer a variety of issues from poor hydrogen selectivity to rapid deactivation. Here, we summarize recent advances in fundamental understanding of functionality and structure of catalysts for alcohol/sugar alcohol steam reforming, and provide perspectives on further development required to design highly efficient steam reforming catalysts.

  3. Steam reformer with catalytic combustor

    NASA Technical Reports Server (NTRS)

    Voecks, Gerald E. (Inventor)

    1990-01-01

    A steam reformer is disclosed having an annular steam reforming catalyst bed formed by concentric cylinders and having a catalytic combustor located at the center of the innermost cylinder. Fuel is fed into the interior of the catalytic combustor and air is directed at the top of the combustor, creating a catalytic reaction which provides sufficient heat so as to maintain the catalytic reaction in the steam reforming catalyst bed. Alternatively, air is fed into the interior of the catalytic combustor and a fuel mixture is directed at the top. The catalytic combustor provides enhanced radiant and convective heat transfer to the reformer catalyst bed.

  4. Steam reformer with catalytic combustor

    DOEpatents

    Voecks, Gerald E.

    1990-03-20

    A steam reformer is disclosed having an annular steam reforming catalyst bed formed by concentric cylinders and having a catalytic combustor located at the center of the innermost cylinder. Fuel is fed into the interior of the catalytic combustor and air is directed at the top of the combustor, creating a catalytic reaction which provides sufficient heat so as to maintain the catalytic reaction in the steam reforming catalyst bed. Alternatively, air is fed into the interior of the catalytic combustor and a fuel mixture is directed at the top. The catalytic combustor provides enhanced radiant and convective heat transfer to the reformer catalyst bed.

  5. Steam Reforming of Hydrocarbon Fuels

    SciTech Connect

    Ming, Qimin; Healey, T; Allen, Lloyd; Irving, Patricia M.

    2002-12-01

    has developed a proprietary catalyst formulation for the fuel processor that is being developed for use with polymer electrolyte membrane fuel cells. The catalyst has been tested for the steam reforming of various hydrocarbons such as natural gas, iso-octane, retail gasoline, and hexadecane. A 300h continuous test has shown that the catalyst has very stable performance for steam reforming of iso-octane at 800?C with a steam/C ratio of 3.6. The same catalyst was also tested for steam reforming hexadecane (a surrogate of diesel) for 73h as well as natural gas for over 150h continuously, without deactivation or carbon deposition. Sulfur tolerance of the catalyst was tested using iso-octane containing various concentrations of sulfur. There was no catalyst deactivation after a 220h continuous test using iso-octane with 100ppm sulfur. For comparison, a nickel catalyst (12wt.% Ni/Al2O3) was also tested using different levels of sulfur in iso-octane. The results indicated that the InnovaTek catalyst has a substantially improved sulfur resistance compared to the nickel catalysts currently used for steam reforming. In addition, a variation of the catalyst was also used to reduce CO concentration to < 1% by water gas shift reaction.

  6. Steam Hydrocarbon Cracking and Reforming

    ERIC Educational Resources Information Center

    Golombok, Michael

    2004-01-01

    The interactive methods of steam hydrocarbon reforming and cracking of the oil and chemical industries are scrutinized, with special focus on their resemblance and variations. The two methods are illustrations of equilibrium-controlled and kinetically-controlled processes, the analysis of which involves theories, which overlap and balance each…

  7. Method of steam reforming methanol to hydrogen

    DOEpatents

    Beshty, Bahjat S.

    1990-01-01

    The production of hydrogen by the catalyzed steam reforming of methanol is accomplished using a reformer of greatly reduced size and cost wherein a mixture of water and methanol is superheated to the gaseous state at temperatures of about 800.degree. to about 1,100.degree. F. and then fed to a reformer in direct contact with the catalyst bed contained therein, whereby the heat for the endothermic steam reforming reaction is derived directly from the superheated steam/methanol mixture.

  8. Steam reforming catalyst

    DOEpatents

    Kramarz, Kurt W.; Bloom, Ira D.; Kumar, Romesh; Ahmed, Shabbir; Wilkenhoener, Rolf; Krumpelt, Michael

    2001-01-01

    A method of forming a hydrogen rich gas from a source of hydrocarbon fuel. A vapor of the hydrocarbon fuel and steam is brought in contact with a two-part catalyst having a dehydrogenation powder portion and an oxide-ion conducting powder portion at a temperature not less than about 770.degree.C. for a time sufficient to generate the hydrogen rich. The H.sub.2 content of the hydrogen gas is greater than about 70 percent by volume. The dehydrogenation portion of the catalyst includes a group VIII metal, and the oxide-ion conducting portion is selected from a ceramic oxide from the group crystallizing in the fluorite or perovskite structure and mixtures thereof. The oxide-ion conducting portion of the catalyst is a ceramic powder of one or more of ZrO.sub.2, CeO.sub.2, Bi.sub.2 O.sub.3, (BiVO).sub.4, and LaGaO.sub.3.

  9. 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.

  10. Fuel cell integrated with steam reformer

    DOEpatents

    Beshty, Bahjat S.; Whelan, James A.

    1987-01-01

    A H.sub.2 -air fuel cell integrated with a steam reformer is disclosed wherein a superheated water/methanol mixture is fed to a catalytic reformer to provide a continuous supply of hydrogen to the fuel cell, the gases exhausted from the anode of the fuel cell providing the thermal energy, via combustion, for superheating the water/methanol mixture.

  11. Methanol Steam Reforming for Hydrogen Production

    SciTech Connect

    Palo, Daniel R.; Dagle, Robert A.; Holladay, Jamie D.

    2007-09-11

    Review article covering developments in methanol steam reforming in the context of PEM fuel cell power systems. Subjects covered include methanol background, use, and production, comparison to other fuels, power system considerations, militrary requirements, competing technologies, catalyst development, and reactor and system development and demonstration.

  12. Hydrogen Production via a High-Efficiency Low-Temperature Reformer

    SciTech Connect

    Paul KT Liu; Theo T. Tsotsis

    2006-05-31

    Fuel cells are promoted by the US government as a viable alternative for clean and efficient energy generation. It is anticipated that the fuel cell market will rise if the key technical barriers can be overcome. One of them is certainly fuel processing and purification. Existing fuel reforming processes are energy intensive, extremely complicated and capital intensive; these disadvantages handicap the scale-down of existing reforming process, targeting distributed or on-board/stationary hydrogen production applications. Our project involves the bench-scale demonstration of a high-efficiency low-temperature steam reforming process. Hydrogen production can be operated at 350 to 400ºC with our invention, as opposed to >800ºC of existing reforming. In addition, our proposed process improves the start-up deficiency of conventional reforming due to its low temperature operation. The objective of this project is to demonstrate the invented process concept via a bench scale unit and verify mathematical simulation for future process optimization study. Under this project, we have performed the experimental work to determine the adsorption isotherm, reaction kinetics, and membrane permeances required to perform the process simulation based upon the mathematical model developed by us. A ceramic membrane coated with palladium thin film fabricated by us was employed in this study. The adsorption isotherm for a selected hydrotalcite adsorbent was determined experimentally. Further, the capacity loss under cyclic adsorption/desorption was confirmed to be negligible. Finally a commercial steam reforming catalyst was used to produce the reaction kinetic parameters required for the proposed operating condition. With these input parameters, a mathematical simulation was performed to predict the performance of the invented process. According to our simulation, our invented hybrid process can deliver 35 to 55% methane conversion, in comparison with the 12 and 18-21% conversion of

  13. Hierarchically structured catalysts for cascade and selective steam reforming/hydrodeoxygenation reactions

    SciTech Connect

    Sun, Junming; Karim, Ayman M.; Li, Xiaohong S.; Rainbolt, James E.; Kovarik, Libor; Shin, Yongsoon; Wang, Yong

    2015-09-29

    We report a hierarchically structured catalyst with steam reforming and hydrodeoxygenation functionalities being deposited in the micropores and macropores, respectively. The catalyst is highly efficient to upgrade the pyrolysis vapors of pine forest product residual, resulting in a dramatically decreased acid content and increased hydrocarbon yield without external H2 supply.

  14. Hierarchically structured catalysts for cascade and selective steam reforming/hydrodeoxygenation reactions.

    PubMed

    Sun, Junming; Karim, Ayman M; Li, Xiaohong Shari; Rainbolt, James; Kovarik, Libor; Shin, Yongsoon; Wang, Yong

    2015-12-01

    We report a hierarchically structured catalyst with steam reforming and hydrodeoxygenation functionalities being deposited in the micropores and macropores, respectively. The catalyst is highly efficient to upgrade the pyrolysis vapors of pine forest product residual, resulting in a dramatically decreased acid content and increased hydrocarbon yield without external H2 supply. PMID:26462032

  15. Catalytic glycerol steam reforming for hydrogen production

    SciTech Connect

    Dan, Monica Mihet, Maria Lazar, Mihaela D.

    2015-12-23

    Hydrogen production from glycerol by steam reforming combine two major advantages: (i) using glycerol as raw material add value to this by product of bio-diesel production which is obtained in large quantities around the world and have a very limited utilization now, and (ii) by implication of water molecules in the reaction the efficiency of hydrogen generation is increased as each mol of glycerol produces 7 mol of H{sub 2}. In this work we present the results obtained in the process of steam reforming of glycerol on Ni/Al{sub 2}O{sub 3}. The catalyst was prepared by wet impregnation method and characterized through different methods: N{sub 2} adsorption-desorption, XRD, TPR. The catalytic study was performed in a stainless steel tubular reactor at atmospheric pressure by varying the reaction conditions: steam/carbon ratio (1-9), gas flow (35 ml/min -133 ml/min), temperature (450-650°C). The gaseous fraction of the reaction products contain: H{sub 2}, CH{sub 4}, CO, CO{sub 2}. The optimum reaction conditions as resulted from this study are: temperature 550°C, Gly:H{sub 2}O ratio 9:1 and Ar flow 133 ml/min. In these conditions the glycerol conversion to gaseous products was 43% and the hydrogen yield was 30%.

  16. Catalytic glycerol steam reforming for hydrogen production

    NASA Astrophysics Data System (ADS)

    Dan, Monica; Mihet, Maria; Lazar, Mihaela D.

    2015-12-01

    Hydrogen production from glycerol by steam reforming combine two major advantages: (i) using glycerol as raw material add value to this by product of bio-diesel production which is obtained in large quantities around the world and have a very limited utilization now, and (ii) by implication of water molecules in the reaction the efficiency of hydrogen generation is increased as each mol of glycerol produces 7 mol of H2. In this work we present the results obtained in the process of steam reforming of glycerol on Ni/Al2O3. The catalyst was prepared by wet impregnation method and characterized through different methods: N2 adsorption-desorption, XRD, TPR. The catalytic study was performed in a stainless steel tubular reactor at atmospheric pressure by varying the reaction conditions: steam/carbon ratio (1-9), gas flow (35 ml/min -133 ml/min), temperature (450-650°C). The gaseous fraction of the reaction products contain: H2, CH4, CO, CO2. The optimum reaction conditions as resulted from this study are: temperature 550°C, Gly:H2O ratio 9:1 and Ar flow 133 ml/min. In these conditions the glycerol conversion to gaseous products was 43% and the hydrogen yield was 30%.

  17. Hydrogen generation utilizing integrated CO2 removal with steam reforming

    DOEpatents

    Duraiswamy, Kandaswamy; Chellappa, Anand S

    2013-07-23

    A steam reformer may comprise fluid inlet and outlet connections and have a substantially cylindrical geometry divided into reforming segments and reforming compartments extending longitudinally within the reformer, each being in fluid communication. With the fluid inlets and outlets. Further, methods for generating hydrogen may comprise steam reformation and material adsorption in one operation followed by regeneration of adsorbers in another operation. Cathode off-gas from a fuel cell may be used to regenerate and sweep the adsorbers, and the operations may cycle among a plurality of adsorption enhanced reformers to provide a continuous flow of hydrogen.

  18. Compatibility of selected ceramics with steam-methane reformer environments

    SciTech Connect

    Keiser, J.R.; Howell, M.; Williams, J.J.; Rosenberg, R.A.

    1996-04-01

    Conventional steam reforming of methane to synthesis gas (CO and H{sub 2}) hasa conversion efficiency of about 85%. Replacement of metal tubes in the reformer with ceramic tubes offers the potential for operation at temperatures high enough to increase the efficiency to 98-99%. However, the two candidate ceramic materials being given strongest consideration, sintered alpha Si carbide and Si carbide particulate-strengthened alumina, have been shown to react with components of the reformer environment. Extent of degradation as a function of steam partial pressure and exposure time has been studied, and results suggest limits under which these structural ceramics can be used in advanced steam-methane reformers.

  19. Steam reforming of commercial ultra-low sulphur diesel

    NASA Astrophysics Data System (ADS)

    Boon, Jurriaan; van Dijk, Eric; de Munck, Sander; van den Brink, Ruud

    Two main routes for small-scale diesel steam reforming exist: low-temperature pre-reforming followed by well-established methane steam reforming on the one hand and direct steam reforming on the other hand. Tests with commercial catalysts and commercially obtained diesel fuels are presented for both processes. The fuels contained up to 6.5 ppmw sulphur and up to 4.5 vol.% of biomass-derived fatty acid methyl ester (FAME). Pre-reforming sulphur-free diesel at around 475 °C has been tested with a commercial nickel catalyst for 118 h without observing catalyst deactivation, at steam-to-carbon ratios as low as 2.6. Direct steam reforming at temperatures up to 800 °C has been tested with a commercial precious metal catalyst for a total of 1190 h with two catalyst batches at steam-to-carbon ratios as low as 2.5. Deactivation was neither observed with lower steam-to-carbon ratios nor for increasing sulphur concentration. The importance of good fuel evaporation and mixing for correct testing of catalysts is illustrated. Diesel containing biodiesel components resulted in poor spray quality, hence poor mixing and evaporation upstream, eventually causing decreasing catalyst performance. The feasibility of direct high temperature steam reforming of commercial low-sulphur diesel has been demonstrated.

  20. Performance tests for steam methane reformers

    SciTech Connect

    Wang, S.I.; DiMartino, S.P.; Patel, N.M.; Smith, D.D.

    1982-08-01

    Most of the synthesis gas plants in operation in the United States for production of hydrogen, carbon monoxide, methanol, and ammonia use steam methane reforming (SMR). Economic projections indicate that the SMR plant may continue to be the most favorable process choice through the 1980s or until partial oxidation or coal gasification processes are technically proven. The complexity of an efficiently designed SMR plant for production of these chemicals requires a thorough understanding of many unit operations to correctly evaluate the performance of an operating plant. Air Products and Chemicals, Inc. (APCI) owns and operates various types of SMR plants for production of hydrogen and carbon monoxide gases for pipe line sales, liquid hydrogen for merchant sale, methanol and ammonia. Over the past few years, APCI has developed guidelines and procedures for plant performance tests done at its major SMR plants. This article documents the plant test procedure used in conducting onsite SMR plant performance tests.

  1. TWR Bench-Scale Steam Reforming Demonstration

    SciTech Connect

    Marshall, D.W.; Soelberg, N.R.

    2003-05-21

    The Idaho Nuclear Technology and Engineering Center (INTEC) was home to nuclear fuel reprocessing activities for decades at the Idaho National Engineering and Environmental Laboratory. As a result of the reprocessing activities, INTEC has accumulated approximately one million gallons of acidic, radioactive, sodium-bearing waste (SBW). The purpose of this demonstration was to investigate a reforming technology, offered by ThermoChem Waste Remediation, LLC, (TWR) for treatment of SBW into a ''road ready'' waste form that would meet the waste acceptance criteria for the Waste Isolation Pilot Plant (WIPP). TWR is the licensee of Manufacturing Technology Conservation International (MTCI) steam-reforming technology in the field of radioactive waste treatment. A non-radioactive simulated SBW was used based on the known composition of waste tank WM-180 at INTEC. Rhenium was included as a non-radioactive surrogate for technetium. Data was collected to determine the nature and characteristics of the product, the operability of the technology, the composition of the off-gases, and the fate of key radionuclides (cesium and technetium) and volatile mercury compounds. The product contained a low fraction of elemental carbon residues in the cyclone and filter vessel catches. Mercury was quantitatively stripped from the product but cesium, rhenium (Tc surrogate), and the heavy metals were retained. Nitrate residues were about 400 ppm in the product and NOx destruction exceeded 86%. The demonstration was successful.

  2. TWR Bench-Scale Steam Reforming Demonstration

    SciTech Connect

    D. W. Marshall; N. R. Soelberg

    2003-05-01

    The Idaho Nuclear Technology and Engineering Center (INTEC) was home to nuclear fuel reprocessing activities for decades at the Idaho National Engineering and Environmental Laboratory. As a result of the reprocessing activities, INTEC has accumulated approximately one million gallons of acidic, radioactive, sodium-bearing waste (SBW). The purpose of this demonstration was to investigate a reforming technology, offered by ThermoChem Waste Remediation, LLC, (TWR) for treatment of SBW into a "road ready" waste form that would meet the waste acceptance criteria for the Waste Isolation Pilot Plant (WIPP). TWR is the licensee of Manufacturing Technology Conservation International (MTCI) steam-reforming technology in the field of radioactive waste treatment. A non-radioactive simulated SBW was used based on the known composition of waste tank WM-180 at INTEC. Rhenium was included as a non-radioactive surrogate for technetium. Data was collected to determine the nature and characteristics of the product, the operability of the technology, the composition of the off-gases, and the fate of key radionuclides (cesium and technetium) and volatile mercury compounds. The product contained a low fraction of elemental carbon residues in the cyclone and filter vessel catches. Mercury was quantitatively stripped from the product but cesium, rhenium (Tc surrogate), and the heavy metals were retained. Nitrate residues were about 400 ppm in the product and NOx destruction exceeded 86%. The demonstration was successful.

  3. Fluidized Bed Steam Reformer (FBSR) monolith formation

    SciTech Connect

    Jantzen, C.M.

    2007-07-01

    Fluidized Bed Steam Reforming (FBSR) is being considered as an alternative technology for the immobilization of a wide variety of aqueous high sodium containing radioactive wastes at various DOE facilities in the United States. The addition of clay, charcoal, and a catalyst as co-reactants converts aqueous Low Activity Wastes (LAW) to a granular or 'mineralized' waste form while converting organic components to CO{sub 2} and steam, and nitrate/nitrite components, if any, to N{sub 2}. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage-like structures that atomically bond radionuclides like Tc-99 and anions such as SO{sub 4}, I, F, and Cl. The granular product has been shown to be as durable as LAW glass. Shallow land burial requires that the mineralized waste form be able to sustain the weight of soil overburden and potential intrusion by future generations. The strength requirement necessitates binding the granular product into a monolith. FBSR mineral products were formulated into a variety of monoliths including various cements, Ceramicrete, and hydro-ceramics. All but one of the nine monoliths tested met the <2 g/m{sup 2} durability specification for Na and Re (simulant for Tc-99) when tested using the Product Consistency Test (PCT; ASTM C1285). Of the nine monoliths tested the cements produced with 80-87 wt% FBSR product, the Ceramicrete, and the hydro-ceramic produced with 83.3 wt% FBSR product, met the compressive strength and durability requirements for an LAW waste form. (authors)

  4. FLUIDIZED BED STEAM REFORMER MONOLITH FORMATION

    SciTech Connect

    Jantzen, C

    2006-12-22

    Fluidized Bed Steam Reforming (FBSR) is being considered as an alternative technology for the immobilization of a wide variety of aqueous high sodium containing radioactive wastes at various DOE facilities in the United States. The addition of clay, charcoal, and a catalyst as co-reactants converts aqueous Low Activity Wastes (LAW) to a granular or ''mineralized'' waste form while converting organic components to CO{sub 2} and steam, and nitrate/nitrite components, if any, to N{sub 2}. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage-like structures that atomically bond radionuclides like Tc-99 and anions such as SO{sub 4}, I, F, and Cl. The granular product has been shown to be as durable as LAW glass. Shallow land burial requires that the mineralized waste form be able to sustain the weight of soil overburden and potential intrusion by future generations. The strength requirement necessitates binding the granular product into a monolith. FBSR mineral products were formulated into a variety of monoliths including various cements, Ceramicrete, and hydroceramics. All but one of the nine monoliths tested met the <2g/m{sup 2} durability specification for Na and Re (simulant for Tc-99) when tested using the Product Consistency Test (PCT; ASTM C1285). Of the nine monoliths tested the cements produced with 80-87 wt% FBSR product, the Ceramicrete, and the hydroceramic produced with 83.3 wt% FBSR product, met the compressive strength and durability requirements for an LAW waste form.

  5. Steam reforming of DOE complex waste simulants

    SciTech Connect

    Miller, J.E.; Kuehne, P.B.

    1995-03-01

    Sandia National Laboratories has worked with Synthetica Technologies and Manufacturing and Technology Conversion International (MTCl) to demonstrate the applicability of their commercial steam reforming technologies for treating DOE low-level mixed wastes. Previously, Synthetica successfully demonstrated destruction of a Sandia formulated lab trash simulant. During November 1994 Synthetica did not adequately process the aqueous halogenated organic liquid mixed waste simulant (MWTP-2110) formulated by the DOE Mixed Waste Integrated Program (MWIP). Testing at MTCl is ongoing and initial results appear to be favorable. Approximately 200 lbs each of the MWIP aqueous halogenated organic liquids (MWTP-2110), and absorbed aqueous and organic liquids (MWTP-3113/3114) simulants have been processed. At 1650{degree}F, destruction efficiencies of greater than 99% were obtained for tetrachloroethylene, toluene, and 1,2 dichlorobenzene. Product cases consisted primarily of H{sub 2}, C0{sub 2}, CO, and CH{sub 4} and had higher heating values of up to 355 BTU/SCF. Conclusions concerning the suitability of the MTCI process for treating DOE mixed wastes will be drawn upon the completion of testing.

  6. Hydrogen-based power generation from bioethanol steam reforming

    NASA Astrophysics Data System (ADS)

    Tasnadi-Asztalos, Zs.; Cormos, C. C.; Agachi, P. S.

    2015-12-01

    This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production from renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO2 emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint.

  7. Hydrogen-based power generation from bioethanol steam reforming

    SciTech Connect

    Tasnadi-Asztalos, Zs. Cormos, C. C. Agachi, P. S.

    2015-12-23

    This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production from renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO{sub 2} emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint.

  8. Biomass to hydrogen via fast pyrolysis and catalytic steam reforming

    SciTech Connect

    Chornet, E.; Wang, D.; Montane, D.

    1995-09-01

    Fast pyrolysis of biomass results in a pyrolytic oil which is a mixture of (a) carbohydrate-derived acids, aldehydes and polyols, (b) lignin-derived substituted phenolics, and (c) extractives-derived terpenoids and fatty acids. The conversion of this pyrolysis oil into H{sub 2} and CO{sub 2} is thermodynamically favored under appropriate steam reforming conditions. Our efforts have focused in understanding the catalysis of steam reforming which will lead to a successful process at reasonable steam/carbon ratios arid process severities. The experimental work, carried out at the laboratory and bench scale levels, has centered on the performance of Ni-based catalysts using model compounds as prototypes of the oxygenates present in the pyrolysis oil. Steam reforming of acetic acid, hydroxyacetaldehyde, furfural and syringol has been proven to proceed rapidly within a reasonable range of severities. Time-on-stream studies are now underway using a fixed bed barometric pressure reactor to ascertain the durability of the catalysts and thus substantiate the scientific and technical feasibility of the catalytic reforming option. Economic analyses are being carried out in parallel to determine the opportunity zones for the combined fast pyrolysis/steam reforming approach. A discussion on the current state of the project is presented.

  9. Methanol Steam Reformer on a Silicon Wafer

    SciTech Connect

    Park, H; Malen, J; Piggott, T; Morse, J; Sopchak, D; Greif, R; Grigoropoulos, C; Havstad, M; Upadhye, R

    2004-04-15

    A study of the reforming rates, heat transfer and flow through a methanol reforming catalytic microreactor fabricated on a silicon wafer are presented. Comparison of computed and measured conversion efficiencies are shown to be favorable. Concepts for insulating the reactor while maintaining small overall size and starting operation from ambient temperature are analyzed.

  10. Multifunctional Porous Graphene for High-Efficiency Steam Generation by Heat Localization.

    PubMed

    Ito, Yoshikazu; Tanabe, Yoichi; Han, Jiuhui; Fujita, Takeshi; Tanigaki, Katsumi; Chen, Mingwei

    2015-08-01

    Multifunctional nanoporous graphene is realized as a heat generator to convert solar illumination into high-energy steam. The novel 3D nanoporous graphene demonstrates a highly energy-effective steam generation with an energy conversation of 80%. PMID:26079440

  11. CHARM COST-EFFECTIVE HIGH-EFFICIENCY ADVANCED REFORMING MODULE FINAL TECHNICAL REPORT

    SciTech Connect

    Pollica, Darryl; Cross, James C; Sharma, Atul; Shi, Yanlong; Clawson, Lawrence; O'Brien, Chris; Gilhooly, Kara; Kim, Changsik; Quet, Pierre-Francois

    2009-09-02

    Background Creation of a hydrogen infrastructure is an important prerequisite of widespread fuel cell commercialization, especially for the automotive market. Hydrogen is an attractive fuel since it offers an opportunity to replace petroleum-based fuels, but hydrogen occurs naturally only in chemical compounds like water or hydrocarbons that must be chemically converted to produce it. While an ultimate goal is to produce hydrogen through renewable energy sources, steam methane reforming (SMR) of natural gas is currently the most economical solution to initiate the transition to a hydrogen economy. Centralized hydrogen generation using large industrial SMR plants is already in place to serve customers. Yet, because of the weight and size of cylinders needed to contain hydrogen gas or liquid, transportation of hydrogen may only be economical for short distances. Consequently, distributed natural gas reforming, which trades off the economies of scale of large plants for simplified delivery logistics, is an attractive alternative that could address immediate problems with the lack of hydrogen infrastructure.

  12. CATALYTIC STEAM REFORMING OF CHLOROCARBONS: METHLYCHLORIDE. (R822721C633)

    EPA Science Inventory

    The effective destruction of trichloroethane, trichloroethylene and perchloroethylene by steam reforming with a commercial nickel catalyst has been demonstrated. Conversion levels of up to 0.99999 were attained in both laboratory and semi-pilot experiments, with the products c...

  13. Steam Reforming of Low-Level Mixed Waste

    SciTech Connect

    1998-01-01

    Under DOE Contract No. DE-AR21-95MC32091, Steam Reforming of Low-Level Mixed Waste, ThermoChem has successfully designed, fabricated and operated a nominal 90 pound per hour Process Development Unit (PDU) on various low-level mixed waste surrogates. The design construction, and testing of the PDU as well as performance and economic projections for a 500- lb/hr demonstration and commercial system are described. The overall system offers an environmentally safe, non-incinerating, cost-effective, and publicly acceptable method of processing LLMW. The steam-reforming technology was ranked the No. 1 non-incineration technology for destruction of hazardous organic wastes in a study commissioned by the Mixed Waste Focus Area published April 1997.1 The ThermoChem steam-reforming system has been developed over the last 13 years culminating in this successful test campaign on LLMW surrogates. Six surrogates were successfidly tested including a 750-hour test on material simulating a PCB- and Uranium- contaminated solid waste found at the Portsmouth Gaseous Diffusion Plant. The test results indicated essentially total (>99.9999oA) destruction of RCRA and TSCA hazardous halogenated organics, significant levels of volume reduction (> 400 to 1), and retention of radlonuclides in the volume-reduced solids. Cost studies have shown the steam-reforming system to be very cost competitive with more conventional and other emerging technologies.

  14. Thermodynamic analysis of acetic acid steam reforming for hydrogen production

    NASA Astrophysics Data System (ADS)

    Goicoechea, Saioa; Ehrich, Heike; Arias, Pedro L.; Kockmann, Norbert

    2015-04-01

    A thermodynamic analysis of hydrogen generation by acetic acid steam reforming has been carried out with respect to applications in solid oxide fuel cells. The effect of operating parameters on equilibrium composition has been examined focusing especially on hydrogen and carbon monoxide production, which are the fuels in this type of fuel cell. The temperature, steam to acetic acid ratio, and to a lesser extent pressure affect significantly the equilibrium product distribution due to their influence on steam reforming, thermal decomposition and water-gas shift reaction. The study shows that steam reforming of acetic acid with a steam to acetic acid ratio of 2 to 1 is thermodynamically feasible with hydrogen, carbon monoxide and water as the main products at the equilibrium at temperatures higher than 700 °C, and achieving CO/CO2 ratios higher than 1. Thus, it can be concluded that within the operation temperature range of solid oxide fuel cells - between 700 °C and 1000 °C - the production of a gas rich in hydrogen and carbon monoxide is promoted.

  15. Steam methane reforming in molten carbonate salt. Final report

    SciTech Connect

    Erickson, D.C.

    1996-05-01

    This report documents the work accomplished on the project {open_quotes}Steam Methane Reforming in Molten Carbonate Salt.{close_quotes}. This effort has established the conceptual basis for molten carbonate-based steam reforming of methane. It has not proceeded to prototype verification, because corrosion concerns have led to reluctance on the part of large hydrogen producers to adopt the technology. Therefore the focus was shifted to a less corrosive embodiment of the same technology. After considerable development effort it was discovered that a European company (Catalysts and Chemicals Europe) was developing a similar process ({open_quotes}Regate{close_quotes}). Accordingly the focus was shifted a second time, to develop an improvement which is generic to both types of reforming. That work is still in progress, and shows substantial promise.

  16. Application of Flexible Micro Temperature Sensor in Oxidative Steam Reforming by a Methanol Micro Reformer

    PubMed Central

    Lee, Chi-Yuan; Lee, Shuo-Jen; Shen, Chia-Chieh; Yeh, Chuin-Tih; Chang, Chi-Chung; Lo, Yi-Man

    2011-01-01

    Advances in fuel cell applications reflect the ability of reformers to produce hydrogen. This work presents a flexible micro temperature sensor that is fabricated based on micro-electro-mechanical systems (MEMS) technology and integrated into a flat micro methanol reformer to observe the conditions inside that reformer. The micro temperature sensor has higher accuracy and sensitivity than a conventionally adopted thermocouple. Despite various micro temperature sensor applications, integrated micro reformers are still relatively new. This work proposes a novel method for integrating micro methanol reformers and micro temperature sensors, subsequently increasing the methanol conversion rate and the hydrogen production rate by varying the fuel supply rate and the water/methanol ratio. Importantly, the proposed micro temperature sensor adequately controls the interior temperature during oxidative steam reforming of methanol (OSRM), with the relevant parameters optimized as well. PMID:22319407

  17. Effect of Cobalt Particle Size on Acetone Steam Reforming

    SciTech Connect

    Sun, Junming; Zhang, He; Yu, Ning; Davidson, Stephen D.; Wang, Yong

    2015-06-11

    Carbon-supported cobalt nanoparticles with different particle sizes were synthesized and characterized by complementary characterization techniques such as X-ray diffraction, N-2 sorption, acetone temperature-programmed desorption, transmission electron microscopy, and CO chemisorption. Using acetone steam reforming reaction as a probe reaction, we revealed a volcano-shape curve of the intrinsic activity (turnover frequency of acetone) and the CO2 selectivity as a function of the cobalt particle size with the highest activity and selectivity observed at a particle size of approximately 12.8nm. Our results indicate that the overall performance of acetone steam reforming is related to a combination of particle-size-dependent acetone decomposition, water dissociation, and the oxidation state of the cobalt nanoparticles.

  18. STEAM REFORMING OF CHLOROCARBONS: CHLORINATED AROMATICS. (R826694C633)

    EPA Science Inventory

    Effective dechlorination of chloroaromatics, such as C6H5Cl, 1,2-C6H4Cl2, 1,3-C6H4Cl2 and 1,2,4-C6H3Cl3, using catalytic steam reforming has been confirmed ...

  19. Hydrogen production by sorption-enhanced steam reforming of glycerol.

    PubMed

    Dou, Binlin; Dupont, Valerie; Rickett, Gavin; Blakeman, Neil; Williams, Paul T; Chen, Haisheng; Ding, Yulong; Ghadiri, Mojtaba

    2009-07-01

    Catalytic steam reforming of glycerol for H(2) production has been evaluated experimentally in a continuous flow fixed-bed reactor. The experiments were carried out under atmospheric pressure within a temperature range of 400-700 degrees C. A commercial Ni-based catalyst and a dolomite sorbent were used for the steam reforming reactions and in situ CO(2) removal. The product gases were measured by on-line gas analysers. The results show that H(2) productivity is greatly increased with increasing temperature and the formation of methane by-product becomes negligible above 500 degrees C. The results suggest an optimal temperature of approximately 500 degrees C for the glycerol steam reforming with in situ CO(2) removal using calcined dolomite as the sorbent, at which the CO(2) breakthrough time is longest and the H(2) purity is highest. The shrinking core model and the 1D-diffusion model describe well the CO(2) removal under the conditions of this work. PMID:19318245

  20. Steam reforming of low-level mixed waste. Final report

    SciTech Connect

    1998-06-01

    ThermoChem has successfully designed, fabricated and operated a nominal 90 pound per hour Process Development Unit (PDU) on various low-level mixed waste surrogates. The design, construction, and testing of the PDU as well as performance and economic projections for a 300-lb/hr demonstration and commercial system are described. The overall system offers an environmentally safe, non-incinerating, cost-effective, and publicly acceptable method of processing LLMW. The steam-reforming technology was ranked the No. 1 non-incineration technology for destruction of hazardous organic wastes in a study commissioned by the Mixed Waste Focus Area and published in April 1997. The ThermoChem steam-reforming system has been developed over the last 13 years culminating in this successful test campaign on LLMW surrogates. Six surrogates were successfully tested including a 750-hour test on material simulating a PCB- and Uranium-contaminated solid waste found at the Portsmouth Gaseous Diffusion Plant. The test results indicated essentially total (> 99.9999%) destruction of RCRA and TSCA hazardous halogenated organics, significant levels of volume reduction (> 400 to 1), and retention of radionuclides in the volume-reduced solids. Economic evaluations have shown the steam-reforming system to be very cost competitive with more conventional and other emerging technologies.

  1. Steam Methane Reformation Testing for Air-Independent Solid Oxide Fuel Cell Systems

    NASA Technical Reports Server (NTRS)

    Mwara, Kamwana N.

    2015-01-01

    Recently, NASA has been looking into utilizing landers that can be propelled by LOX-CH (sub 4), to be used for long duration missions. Using landers that utilize such propellants, also provides the opportunity to use solid oxide fuel cells as a power option, especially since they are able to process methane into a reactant through fuel reformation. One type of reformation, called steam methane reformation, is a process to reform methane into a hydrogen-rich product by reacting methane and steam (fuel cell exhaust) over a catalyst. A steam methane reformation system could potentially use the fuel cell's own exhaust to create a reactant stream that is hydrogen-rich, and requires less internal reforming of the incoming methane. Also, steam reformation may hold some advantages over other types of reforming, such as partial oxidation (PROX) reformation. Steam reformation does not require oxygen, while up to 25 percent can be lost in PROX reformation due to unusable CO (sub 2) reformation. NASA's Johnson Space Center has conducted various phases of steam methane reformation testing, as a viable solution for in-space reformation. This has included using two different types of catalysts, developing a custom reformer, and optimizing the test system to find the optimal performance parameters and operating conditions.

  2. Methanol steam reforming in a fuel cell drive system

    NASA Astrophysics Data System (ADS)

    Wiese, W.; Emonts, B.; Peters, R.

    Within the framework of the Joule III project a compact methanol reformer (CMR) with a specific weight of 2 kg/kW (lower heating value of H 2) was developed. This CMR contains a methanol and water vaporizer, a steam reformer, a heat carrier circuit and a catalytic burner unit. A laboratory fixed-bed reactor consisting of four tubes which could be filled with different amounts of catalyst was used to investigate the catalyst performance and the ageing behaviour. A hydrogen yield of 10 m N3/(h l Cat) can be achieved at 280°C. In this case, the methanol conversion rate is 95% and the dry product gas contains 0.9% CO. A linear decrease of the catalyst activity was observed which can be described by a loss of active catalyst mass of 5.5 mg/h. The catalyst was operated for more than 1000 h without having exhibited activity losses that made a catalyst change necessary. Besides, the stationary behaviour of the reforming reactor, the dynamic behaviour was studied. The time needed for start-up procedures has to be improved for reformers of a next generation. Moreover, the hydrogen production during reformer load changes will be discussed. Simulations of the power train in driving cycles show the different states of a reformer during dynamic operation.

  3. THOR Bench-Scale Steam Reforming Demonstration

    SciTech Connect

    D. W. Marshall; N. R. Soelberg; K. M. Shaber

    2003-05-01

    The Idaho Nuclear Technology and Engineering Center (INTEC) was home to nuclear fuel reprocessing activities for decades at the Idaho National Engineering and Environmental Laboratory. As a result of the reprocessing activities, INTEC has accumulated approximately one million gallons of acidic, radioactive, sodium-bearing waste (SBW). The purpose of this demonstration was to investigate a reforming technology, offered by THORsm Treatment Technologies, LLC, for treatment of SBW into a "road ready" waste form that would meet the waste acceptance criteria for the Waste Isolation Pilot Plant (WIPP). A non-radioactive simulated SBW was used based on the known composition of waste tank WM-180 at INTEC. Rhenium was included as a non-radioactive surrogate for technetium. Data was collected to determine the nature and characteristics of the product, the operability of the technology, the composition of the off-gases, and the fate of key radionuclides (cesium and technetium) and volatile mercury compounds. The product contained a low fraction of elemental carbon residues in the cyclone and filter vessel catches. Mercury was quantitatively stripped from the product but cesium, rhenium (Tc surrogate), and the heavy metals were retained. Nitrates were not detected in the product and NOx destruction exceeded 98%. The demonstration was successful.

  4. THOR Bench-Scale Steam Reforming Demonstration

    SciTech Connect

    Marshall, D.W.; Soelberg, N.R.; Shaber, K.M.

    2003-05-21

    The Idaho Nuclear Technology and Engineering Center (INTEC) was home to nuclear fuel reprocessing activities for decades at the Idaho National Engineering and Environmental Laboratory. As a result of the reprocessing activities, INTEC has accumulated approximately one million gallons of acidic, radioactive, sodium-bearing waste (SBW). The purpose of this demonstration was to investigate a reforming technology, offered by THORsm Treatment Technologies, LLC, for treatment of SBW into a ''road ready'' waste form that would meet the waste acceptance criteria for the Waste Isolation Pilot Plant (WIPP). A non-radioactive simulated SBW was used based on the known composition of waste tank WM-180 at INTEC. Rhenium was included as a non-radioactive surrogate for technetium. Data was collected to determine the nature and characteristics of the product, the operability of the technology, the composition of the off-gases, and the fate of key radionuclides (cesium and technetium) and volatile mercury compounds. The product contained a low fraction of elemental carbon residues in the cyclone and filter vessel catches. Mercury was quantitatively stripped from the product but cesium, rhenium (Tc surrogate), and the heavy metals were retained. Nitrates were not detected in the product and NOx destruction exceeded 98%. The demonstration was successful.

  5. Thermodynamic analysis of carbon formation boundary and reforming performance for steam reforming of dimethyl ether

    NASA Astrophysics Data System (ADS)

    Faungnawakij, Kajornsak; Kikuchi, Ryuji; Eguchi, Koichi

    Thermodynamic analysis of dimethyl ether steam reforming (DME SR) was investigated for carbon formation boundary, DME conversion, and hydrogen yield for fuel cell application. The equilibrium calculation employing Gibbs free minimization was performed to figure out the required steam-to-carbon ratio (S/C = 0-5) and reforming temperature (25-1000 °C) where coke formation was thermodynamically unfavorable. S/C, reforming temperature and product species strongly contributed to the coke formation and product composition. When chemical species DME, methanol, CO 2, CO, H 2, H 2O and coke were considered, complete conversion of DME and hydrogen yield above 78% without coke formation were achieved at the normal operating temperatures of molten carbonate fuel cell (600 °C) and solid oxide fuel cell (900 °C), when S/C was at or above 2.5. When CH 4 was favorable, production of coke and that of hydrogen were significantly suppressed.

  6. Syngas Generation from Organic Waste with Plasma Steam Reforming

    NASA Astrophysics Data System (ADS)

    Diaz, G.; Leal-Quiros, E.; Smith, R. A.; Elliott, J.; Unruh, D.

    2014-05-01

    A plasma steam reforming system to process waste is in the process of being set up at the University of California, Merced. The proposed concept will use two different plasma regimes, i.e. glow discharge and arc torches to process a percentage of the total liquid waste stream generated at the campus together with shredded local organic solid waste. One of the main advantages of the plasma technology to be utilized is that it uses graphite electrodes that can be fed to the reactor to achieve continuous operation, thus, electrode or nozzle life is not a concern. The waste to energy conversion process consists of two stages, one where a mixture of steam and hydrogen is generated from the liquid in a glow-discharge cell, and a second stage where the mixture of exhaust gases coming out of the first device are mixed with solid waste in a reactor operating in steam reforming mode interacting with a plasma torch to generate high-quality syngas. In this paper, the results of a thermodynamic model developed for the two stages are shown. The syngas composition obtained indicates that the fraction of CO2 present decreases with increasing temperature and the molar fractions of hydrogen and carbon monoxide become dominant. The fraction of water vapour present in the product gases coming out of the second stage needs to be condensed before the syngas can be utilized in a prime mover.

  7. Thermodynamic evaluation of hydrogen production via bioethanol steam reforming

    SciTech Connect

    Tasnadi-Asztalos, Zsolt; Cormos, Ana-Maria; Imre-Lucaci, Árpád; Cormos, Călin C.

    2013-11-13

    In this article, a thermodynamic analysis for bioethanol steam reforming for hydrogen production is presented. Bioethanol is a newly proposed renewable energy carrier mainly produced from biomass fermentation. Reforming of bioethanol provides a promising method for hydrogen production from renewable resources. Steam reforming of ethanol (SRE) takes place under the action of a metal catalyst capable of breaking C-C bonds into smaller molecules. A large domain for the water/bioethanol molar ratio as well as the temperature and average pressure has been used in the present work. The interval of investigated temperature was 100-800°C, the pressure was in the range of 1-10 bar and the molar ratio was between 3-25. The variations of gaseous species concentration e.g. H{sub 2}, CO, CO{sub 2}, CH{sub 4} were analyzed. The concentrations of the main products (H{sub 2} and CO) at lower temperature are smaller than the ones at higher temperature due to by-products formation (methane, carbon dioxide, acetylene etc.). The concentration of H2 obtained in the process using high molar ratio (>20) is higher than the one at small molar ratio (near stoichiometric). When the pressure is increased the hydrogen concentration decreases. The results were compared with literature data for validation purposes.

  8. Thermodynamic evaluation of hydrogen production via bioethanol steam reforming

    NASA Astrophysics Data System (ADS)

    Tasnadi-Asztalos, Zsolt; Cormos, Ana-Maria; Imre-Lucaci, Árpád; Cormos, Cǎlin C.

    2013-11-01

    In this article, a thermodynamic analysis for bioethanol steam reforming for hydrogen production is presented. Bioethanol is a newly proposed renewable energy carrier mainly produced from biomass fermentation. Reforming of bioethanol provides a promising method for hydrogen production from renewable resources. Steam reforming of ethanol (SRE) takes place under the action of a metal catalyst capable of breaking C-C bonds into smaller molecules. A large domain for the water/bioethanol molar ratio as well as the temperature and average pressure has been used in the present work. The interval of investigated temperature was 100-800°C, the pressure was in the range of 1-10 bar and the molar ratio was between 3-25. The variations of gaseous species concentration e.g. H2, CO, CO2, CH4 were analyzed. The concentrations of the main products (H2 and CO) at lower temperature are smaller than the ones at higher temperature due to by-products formation (methane, carbon dioxide, acetylene etc.). The concentration of H2 obtained in the process using high molar ratio (>20) is higher than the one at small molar ratio (near stoichiometric). When the pressure is increased the hydrogen concentration decreases. The results were compared with literature data for validation purposes.

  9. Self-assembly of highly efficient, broadband plasmonic absorbers for solar steam generation

    PubMed Central

    Zhou, Lin; Tan, Yingling; Ji, Dengxin; Zhu, Bin; Zhang, Pei; Xu, Jun; Gan, Qiaoqiang; Yu, Zongfu; Zhu, Jia

    2016-01-01

    The study of ideal absorbers, which can efficiently absorb light over a broad range of wavelengths, is of fundamental importance, as well as critical for many applications from solar steam generation and thermophotovoltaics to light/thermal detectors. As a result of recent advances in plasmonics, plasmonic absorbers have attracted a lot of attention. However, the performance and scalability of these absorbers, predominantly fabricated by the top-down approach, need to be further improved to enable widespread applications. We report a plasmonic absorber which can enable an average measured absorbance of ~99% across the wavelengths from 400 nm to 10 μm, the most efficient and broadband plasmonic absorber reported to date. The absorber is fabricated through self-assembly of metallic nanoparticles onto a nanoporous template by a one-step deposition process. Because of its efficient light absorption, strong field enhancement, and porous structures, which together enable not only efficient solar absorption but also significant local heating and continuous stream flow, plasmonic absorber–based solar steam generation has over 90% efficiency under solar irradiation of only 4-sun intensity (4 kW m−2). The pronounced light absorption effect coupled with the high-throughput self-assembly process could lead toward large-scale manufacturing of other nanophotonic structures and devices. PMID:27152335

  10. Self-assembly of highly efficient, broadband plasmonic absorbers for solar steam generation.

    PubMed

    Zhou, Lin; Tan, Yingling; Ji, Dengxin; Zhu, Bin; Zhang, Pei; Xu, Jun; Gan, Qiaoqiang; Yu, Zongfu; Zhu, Jia

    2016-04-01

    The study of ideal absorbers, which can efficiently absorb light over a broad range of wavelengths, is of fundamental importance, as well as critical for many applications from solar steam generation and thermophotovoltaics to light/thermal detectors. As a result of recent advances in plasmonics, plasmonic absorbers have attracted a lot of attention. However, the performance and scalability of these absorbers, predominantly fabricated by the top-down approach, need to be further improved to enable widespread applications. We report a plasmonic absorber which can enable an average measured absorbance of ~99% across the wavelengths from 400 nm to 10 μm, the most efficient and broadband plasmonic absorber reported to date. The absorber is fabricated through self-assembly of metallic nanoparticles onto a nanoporous template by a one-step deposition process. Because of its efficient light absorption, strong field enhancement, and porous structures, which together enable not only efficient solar absorption but also significant local heating and continuous stream flow, plasmonic absorber-based solar steam generation has over 90% efficiency under solar irradiation of only 4-sun intensity (4 kW m(-2)). The pronounced light absorption effect coupled with the high-throughput self-assembly process could lead toward large-scale manufacturing of other nanophotonic structures and devices. PMID:27152335

  11. Fuel cell hydrogen production by catalytic ethanol-steam reforming

    SciTech Connect

    Amphlett, J.C.; Leclerc, S.; Mann, R.F.; Peppley, B.A.; Roberge, P.R.

    1998-07-01

    It is clear that the reaction network that results from catalytic reaction of ethanol, with and without steam, is very complex and involves over a dozen potential products. Reactions to avoid are any that lead to CP{sub 4} species and ethylene, the former representing a more difficult challenge for subsequent steam reforming and the latter providing what is probably the major route to carbon production and coking of the catalyst. Dehydration reactions, therefore, should generally be avoided. Dehydrogenation catalysts would seem to be most appropriate, especially since the production of hydrogen is the main goal. Copper-based catalysts have been long-established for this function so that they are commercially available and therefore lower cost. CuO/ZnO, CuO/SiO{sub 2}, CuO/Cr{sub 2}O{sub 3} or CuO/NiO/SiO{sub 2} may be the best catalyst candidates. Reaction pressures should be relatively low (1 to a few atm) and the best reaction temperature could be in the range 350 to 450 C. Insufficient experimental work has been reported to give a clear idea of the required water-to-ethanol mole ratio. The stoichiometric value of this ratio is three and it is likely that excess water, although presenting some process complications, will be necessary to minimize yields of CO and CH{sub 4}. A major new aspect of catalyst selection and operation, when comparing ethanol to methanol steam reforming, will be catalyst deactivation due to temperature. The methanol process works well on CuO/ZnO around 250 to 260 C, just on the threshold of fairly rapid catalyst deactivation. If the ethanol process is to work at or above 300 C, the present CuO/ZnO catalysts will be operating at an activity well below that obtainable in methanol-steam reformers. This means that larger reformers (i.e. more catalyst) will be necessary or that Cu-based (or other) catalysts with slower deactivation in the 300 C-plus range will have to be developed.

  12. A 400-kWe high-efficiency steam turbine for industrial cogeneration

    NASA Technical Reports Server (NTRS)

    Leibowitz, H. M.

    1982-01-01

    An advanced state-of-the-art steam turbine-generator developed to serve as the power conversion subsystem for the Department of Energy's Sandia National Laboratories' Solar Total-Energy Project (STEP) is described. The turbine-generator, which is designed to provide 400-kW of net electrical power, represents the largest turbine-generator built specifically for commercial solar-powered cogeneration. The controls for the turbine-generator incorporate a multiple, partial-arc entry to provide efficient off-design performance, as well as an extraction control scheme to permit extraction flow regulation while maintaining 110-spsig pressure. Normal turbine operation is achieved while synchronized to a local utility and in a stand-alone mode. In both cases, the turbine-generator features automatic load control as well as remote start-up and shutdown capability. Tests totaling 200 hours were conducted to confirm the integrity of the turbine's mechanical structure and control function. Performance tests resulted in a measured inlet throttle flow of 8,450 pounds per hour, which was near design conditions.

  13. A 400-kWe high-efficiency steam turbine for industrial cogeneration

    NASA Astrophysics Data System (ADS)

    Leibowitz, H. M.

    1982-07-01

    An advanced state-of-the-art steam turbine-generator developed to serve as the power conversion subsystem for the Department of Energy's Sandia National Laboratories' Solar Total-Energy Project (STEP) is described. The turbine-generator, which is designed to provide 400-kW of net electrical power, represents the largest turbine-generator built specifically for commercial solar-powered cogeneration. The controls for the turbine-generator incorporate a multiple, partial-arc entry to provide efficient off-design performance, as well as an extraction control scheme to permit extraction flow regulation while maintaining 110-spsig pressure. Normal turbine operation is achieved while synchronized to a local utility and in a stand-alone mode. In both cases, the turbine-generator features automatic load control as well as remote start-up and shutdown capability. Tests totaling 200 hours were conducted to confirm the integrity of the turbine's mechanical structure and control function. Performance tests resulted in a measured inlet throttle flow of 8,450 pounds per hour, which was near design conditions.

  14. Modified Ni-Cu catalysts for ethanol steam reforming

    SciTech Connect

    Dan, M.; Mihet, M.; Almasan, V.; Borodi, G.; Katona, G.; Muresan, L.; Lazar, M. D.

    2013-11-13

    Three Ni-Cu catalysts, having different Cu content, supported on γ-alumina were synthesized by wet co-impregnation method, characterized and tested in the ethanol steam reforming (ESR) reaction. The catalysts were characterized for determination of: total surface area and porosity (N{sub 2} adsorption - desorption using BET and Dollimer Heal methods), Ni surface area (hydrogen chemisorption), crystallinity and Ni crystallites size (X-Ray Diffraction), type of catalytic active centers (Hydrogen Temperature Programmed Reduction). Total surface area and Ni crystallites size are not significantly influenced by the addition of Cu, while Ni surface area is drastically diminished by increasing of Cu concentration. Steam reforming experiments were performed at atmospheric pressure, temperature range 150-350°C, and ethanol - water molar ration of 1 at 30, using Ar as carrier gas. Ethanol conversion and hydrogen production increase by the addition of Cu. At 350°C there is a direct connection between hydrogen production and Cu concentration. Catalysts deactivation in 24h time on stream was studied by Transmission Electron Microscopy (TEM) and temperature-programmed reduction (TPR) on used catalysts. Coke deposition was observed at all studied temperatures; at 150°C amorphous carbon was evidenced, while at 350°C crystalline, filamentous carbon is formed.

  15. Modified Ni-Cu catalysts for ethanol steam reforming

    NASA Astrophysics Data System (ADS)

    Dan, M.; Mihet, M.; Almasan, V.; Borodi, G.; Katona, G.; Muresan, L.; Lazar, M. D.

    2013-11-01

    Three Ni-Cu catalysts, having different Cu content, supported on γ-alumina were synthesized by wet co-impregnation method, characterized and tested in the ethanol steam reforming (ESR) reaction. The catalysts were characterized for determination of: total surface area and porosity (N2 adsorption - desorption using BET and Dollimer Heal methods), Ni surface area (hydrogen chemisorption), crystallinity and Ni crystallites size (X-Ray Diffraction), type of catalytic active centers (Hydrogen Temperature Programmed Reduction). Total surface area and Ni crystallites size are not significantly influenced by the addition of Cu, while Ni surface area is drastically diminished by increasing of Cu concentration. Steam reforming experiments were performed at atmospheric pressure, temperature range 150-350°C, and ethanol - water molar ration of 1 at 30, using Ar as carrier gas. Ethanol conversion and hydrogen production increase by the addition of Cu. At 350°C there is a direct connection between hydrogen production and Cu concentration. Catalysts deactivation in 24h time on stream was studied by Transmission Electron Microscopy (TEM) and temperature-programmed reduction (TPR) on used catalysts. Coke deposition was observed at all studied temperatures; at 150°C amorphous carbon was evidenced, while at 350°C crystalline, filamentous carbon is formed.

  16. High Efficiency Solar-based Catalytic Structure for CO{sub 2} Reforming

    SciTech Connect

    Menkara, Hisham

    2013-09-30

    Throughout this project, we developed and optimized various photocatalyst structures for CO{sub 2} reforming into hydrocarbon fuels and various commodity chemical products. We also built several closed-loop and continuous fixed-bed photocatalytic reactor system prototypes for a larger-scale demonstration of CO{sub 2} reforming into hydrocarbons, mainly methane and formic acid. The results achieved have indicated that with each type of reactor and structure, high reforming yields can be obtained by refining the structural and operational conditions of the reactor, as well as by using various sacrificial agents (hole scavengers). We have also demonstrated, for the first time, that an aqueous solution containing acid whey (a common bio waste) is a highly effective hole scavenger for a solar-based photocatalytic reactor system and can help reform CO{sub 2} into several products at once. The optimization tasks performed throughout the project have resulted in efficiency increase in our conventional reactors from an initial 0.02% to about 0.25%, which is 10X higher than our original project goal. When acid whey was used as a sacrificial agent, the achieved energy efficiency for formic acid alone was ~0.4%, which is 16X that of our original project goal and higher than anything ever reported for a solar-based photocatalytic reactor. Therefore, by carefully selecting sacrificial agents, it should be possible to reach energy efficiency in the range of the photosynthetic efficiency of typical crop and biofuel plants (1-3%).

  17. Development of Technologies on Innovative-Simplified Nuclear Power Plant Using High-Efficiency Steam Injectors (9) System Outline and Endurance Test of Low-Pressure Steam Injectors

    SciTech Connect

    Shuichi Ohmori; Michitsugu Mori; Shoji Goto; Tadashi Narabayashi; Chikako Iwaki; Yutaka Asanuma

    2006-07-01

    A Steam Injector (SI) is a simple, compact and passive pump and also acts as a high-performance direct-contact compact heater. This provides SI with capability to serve also as a direct-contact feedwater heater that heats up feedwater by using extracted steam from the turbine. We are developing technology for 'Innovative Simplified Nuclear Power Plants' in order to further improve the economy and safety of nuclear power plants. Our technology development aims to significantly simplify equipment and reduce physical quantities by applying 'High-Efficiency SI', which are applicable to a wide range of operation regimes beyond the performance and applicable range of existing SIs and enables unprecedented multistage and parallel operation, to the low-pressure feedwater heaters and Emergency Core Cooling Systems (ECCS) of nuclear power plants, as well as achieve high inherent safety to prevent severe accidents by keeping the core covered with water (a Severe Accident-Free Concept). The innovative-simplified nuclear power plant consists of a simplified feedwater heating system, a passive core injection system and a passive containment cooling system. This report describes the results of the endurance and performance tests of low-pressure SIs for feedwater heaters with Jet-deaerator and core injection system. A part of this report are fruits of research which is carried out by Tokyo Electric Power Company (TEPCO), Toshiba, and 7 Universities in Japan, funded from the Ministry of Economy, Trade and Industry (METI) of Japan as the national public research-funded program. (authors)

  18. In silico search for novel methane steam reforming catalysts

    NASA Astrophysics Data System (ADS)

    Xu, Yue; Lausche, Adam C.; Wang, Shengguang; Khan, Tuhin S.; Abild-Pedersen, Frank; Studt, Felix; Nørskov, Jens K.; Bligaard, Thomas

    2013-12-01

    This paper demonstrates a method for screening transition metal and metal alloy catalysts based on their predicted rates and stabilities for a given catalytic reaction. This method involves combining reaction and activation energies (available to the public via a web-based application ‘CatApp’) with a microkinetic modeling technique to predict the rates and selectivities of a prospective material. This paper illustrates this screening technique using the steam reforming of methane to carbon monoxide and hydrogen as a test reaction. While catalysts are already commercially available for this process, the method demonstrated in this paper is very general and could be applied to a wide range of catalytic reactions. Following the steps outlined herein, such an analysis could potentially enable researchers to understand reaction mechanisms on a fundamental level and, on this basis, develop leads for new metal alloy catalysts.

  19. Catalytic deactivation on methane steam reforming catalysts. 2. Kinetic study

    SciTech Connect

    Agnelli, M.E.; Ponzi, E.N.; Yeramian, A.A.

    1987-08-01

    The kinetics of methane steam reforming reaction over an alumina-supported nickel catalyst was investigated at a temperature range of 640-740/sup 0/C in a flow reactor at atmospheric pressure. The experiments were performed varying the inlet concentration of methane, hydrogen, and water. A kinetic scheme of the Houghen-Watson type was satisfactorily proposed assuming the dissociative adsorption of CH/sub 4/ as the rate-limiting step, but this kinetic scheme can be easily replaced by a first-order kinetics (r/sub CH/4/sub / = kapparho/sub CH/4/sub /) for engineering purposes. Catalyst activation with H/sub 2/ and N/sub 2/ mixtures or with the reactant mixture results in the same extent of reaction.

  20. Evaluation of dissociated and steam-reformed methanol as automotive engine fuels

    NASA Technical Reports Server (NTRS)

    Lalk, T. R.; Mccall, D. M.; Mccanlies, J. M.

    1984-01-01

    Dissociated and steam reformed methanol were evaluated as automotive engine fuels. Advantages and disadvantages in using methanol in the reformed rather than liquid state were discussed. Engine dynamometer tests were conducted with a four cylinder, 2.3 liter, spark ignition automotive engine to determine performance and emission characteristics operating on simulated dissociated and steam reformed methanol (2H2 + CO and 3H2 + CO2 respectively), and liquid methanol. Results are presented for engine performance and emissions as functions of equivalence ratio, at various throttle settings and engine speeds. Operation on dissociated and steam reformed methanol was characterized by flashback (violent propagation of a flame into the intake manifold) which limited operation to lower power output than was obtainable using liquid methanol. It was concluded that: an automobile could not be operated solely on dissociated or steam reformed methanol over the entire required power range - a supplementary fuel system or power source would be necessary to attain higher powers; the use of reformed mechanol, compared to liquid methanol, may result in a small improvement in thermal efficiency in the low power range; dissociated methanol is a better fuel than steam reformed methanol for use in a spark ignition engine; and use of dissociated or steam reformed methanol may result in lower exhaust emissions compared to liquid methanol.

  1. Integrated solar thermochemical reaction system for steam methane reforming

    SciTech Connect

    Zheng, Feng; Diver, Rich; Caldwell, Dustin D.; Fritz, Brad G.; Cameron, Richard J.; Humble, Paul H.; TeGrotenhuis, Ward E.; Dagle, Robert A.; Wegeng, Robert S.

    2015-06-05

    Solar-aided upgrade of the energy content of fossil fuels, such as natural gas, can provide a near-term transition path towards a future solar-fuel economy and reduce carbon dioxide emission from fossil fuel consumption. Both steam and dry reforming a methane-containing fuel stream have been studied with concentrated solar power as the energy input to drive the highly endothermic reactions but the concept has not been demonstrated at a commercial scale. Under a current project with the U.S. Department of Energy, PNNL is developing an integrated solar thermochemical reaction system that combines solar concentrators with micro- and meso-channel reactors and heat exchangers to accomplish more than 20% solar augment of methane higher heating value. The objective of our three-year project is to develop and prepare for commercialization such solar reforming system with a high enough efficiency to serve as the frontend of a conventional natural gas (or biogas) combined cycle power plant, producing power with a levelized cost of electricity less than 6¢/kWh, without subsidies, by the year 2020. In this paper, we present results from the first year of our project that demonstrated a solar-to-chemical energy conversion efficiency as high as 69% with a prototype reaction system.

  2. Integrated solar thermochemical reaction system for steam methane reforming

    DOE PAGESBeta

    Zheng, Feng; Diver, Rich; Caldwell, Dustin D.; Fritz, Brad G.; Cameron, Richard J.; Humble, Paul H.; TeGrotenhuis, Ward E.; Dagle, Robert A.; Wegeng, Robert S.

    2015-06-05

    Solar-aided upgrade of the energy content of fossil fuels, such as natural gas, can provide a near-term transition path towards a future solar-fuel economy and reduce carbon dioxide emission from fossil fuel consumption. Both steam and dry reforming a methane-containing fuel stream have been studied with concentrated solar power as the energy input to drive the highly endothermic reactions but the concept has not been demonstrated at a commercial scale. Under a current project with the U.S. Department of Energy, PNNL is developing an integrated solar thermochemical reaction system that combines solar concentrators with micro- and meso-channel reactors and heatmore » exchangers to accomplish more than 20% solar augment of methane higher heating value. The objective of our three-year project is to develop and prepare for commercialization such solar reforming system with a high enough efficiency to serve as the frontend of a conventional natural gas (or biogas) combined cycle power plant, producing power with a levelized cost of electricity less than 6¢/kWh, without subsidies, by the year 2020. In this paper, we present results from the first year of our project that demonstrated a solar-to-chemical energy conversion efficiency as high as 69% with a prototype reaction system.« less

  3. Fuel Chemistry and Bed Performance in a Black Liquor Steam Reformer

    SciTech Connect

    2006-04-01

    The objective of this research is to address critical issues that inhibit successful commercialization of low-temperature BLG systems, including the steam reforming technology developed by Manufacturing and Technology Conversion International, Inc.

  4. Durability Testing of Fluidized Bed Steam Reforming Products

    SciTech Connect

    JANTZEN, CAROL M.; PAREIZS, JOHN M.; LORIER, TROY H.; MARRA, JAMES C.

    2005-07-01

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of radioactive wastes but especially aqueous high sodium wastes at the Hanford site, at the Idaho National Laboratory (INL), and at the Savannah River Site (SRS). The FBSR technology converts organic compounds to CO{sub 2} and H{sub 2}O, converts nitrate/nitrite species to N{sub 2}, and produces a solid residue through reactions with superheated steam, the fluidizing media. If clay is added during processing a ''mineralized'' granular waste form can be produced. The mineral components of the waste form are primarily Na-Al-Si (NAS) feldspathoid minerals with cage-like and ring structures and iron bearing spinel minerals. The cage and ring structured minerals atomically bond radionuclides like Tc{sup 99} and Cs{sup 137} and anions such as SO{sub 4}, I, F, and Cl. The spinel minerals appear to stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Durability testing of the FBSR products was performed using ASTM C1285 (Product Consistency Test) and the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP). The FBSR mineral products (bed and fines) evaluated in this study were found to be two orders of magnitude more durable than the Hanford Low Activity Waste (LAW) glass requirement of 2 g/m{sup 2} release of Na{sup +}. The PCT responses for the FBSR samples tested were consistent with results from previous FBSR Hanford LAW product testing. Differences in the response can be explained by the minerals formed and their effects on PCT leachate chemistry.

  5. Steam Reforming on Transition-metal Carbides from Density-functional Theory

    SciTech Connect

    Vojvodic, Aleksandra

    2012-05-11

    A screening study of the steam reforming reaction on clean and oxygen covered early transition-metal carbides surfaces is performed by means of density-functional theory calculations. It is found that carbides provide a wide spectrum of reactivities, from too reactive via suitable to too inert. Several molybdenum-based systems are identified as possible steam reforming catalysts. The findings suggest that carbides provide a playground for reactivity tuning, comparable to the one for pure metals.

  6. Solid oxide fuel cell steam reforming power system

    DOEpatents

    Chick, Lawrence A.; Sprenkle, Vincent L.; Powell, Michael R.; Meinhardt, Kerry D.; Whyatt, Greg A.

    2013-03-12

    The present invention is a Solid Oxide Fuel Cell Reforming Power System that utilizes adiabatic reforming of reformate within this system. By utilizing adiabatic reforming of reformate within the system the system operates at a significantly higher efficiency than other Solid Oxide Reforming Power Systems that exist in the prior art. This is because energy is not lost while materials are cooled and reheated, instead the device operates at a higher temperature. This allows efficiencies higher than 65%.

  7. Enviro-Friendly Hydrogen Generation from Steel Mill-Scale via Metal-Steam Reforming

    ERIC Educational Resources Information Center

    Azad, Abdul-Majeed; Kesavan, Sathees

    2006-01-01

    An economically viable and environmental friendly method of generating hydrogen for fuel cells is by the reaction of certain metals with steam, called metal-steam reforming (MSR). This technique does not generate any toxic by-products nor contributes to the undesirable greenhouse effect. From the standpoint of favorable thermodynamics, total…

  8. HIGH EFFICIENCY SYNGAS GENERATION

    SciTech Connect

    Robert J. Copeland; Yevgenia Gershanovich; Brian Windecker

    2005-02-01

    This project investigated an efficient and low cost method of auto-thermally reforming natural gas to hydrogen and carbon monoxide. Reforming is the highest cost step in producing products such as methanol and Fisher Tropsch liquids (i.e., gas to liquids); and reducing the cost of reforming is the key to reducing the cost of these products. Steam reforming is expensive because of the high cost of the high nickel alloy reforming tubes (i.e., indirectly fired reforming tubes). Conventional auto-thermal or Partial Oxidation (POX) reforming minimizes the size and cost of the reformers and provides a near optimum mixture of CO and hydrogen. However POX requires pure oxygen, which consumes power and significantly increases the cost to reforming. Our high efficiency process extracts oxygen from low-pressure air with novel oxygen sorbent and transfers the oxygen to a nickel-catalyzed reformer. The syngas is generated at process pressure (typically 20 to 40 bar) without nitrogen dilution and has a 1CO to 2H{sub 2} ratio that is near optimum for the subsequent production of Fisher-Tropsch liquid to liquids and other chemicals (i.e., Gas to Liquids, GTL). Our high process efficiency comes from the way we transfer the oxygen into the reformer. All of the components of the process, except for the oxygen sorbent, are commonly used in commercial practice. A process based on a longlived, regenerable, oxygen transfer sorbent could substantially reduce the cost of natural gas reforming to syngas. Lower cost syngas (CO + 2H{sub 2}) that is the feedstock for GTL would reduce the cost of GTL and for other commercial applications (e.g., methanol, other organic chemicals). The vast gas resources of Alaska's North Slope (ANS) offer more than 22 Tcf of gas and GTL production in this application alone, and could account for as much as 300,000 to 700,000 bpd for 20 to 30+ years. We developed a new sorbent, which is an essential part of the High Efficiency Oxygen Process (HOP). We tested the

  9. DURABILITY TESTING OF FLUIDIZED BED STEAM REFORMER (FBSR) WASTE FORMS

    SciTech Connect

    Jantzen, C

    2006-01-06

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium aqueous radioactive wastes. The addition of clay and a catalyst as co-reactants converts high sodium aqueous low activity wastes (LAW) such as those existing at the Hanford and Idaho DOE sites to a granular ''mineralized'' waste form that may be made into a monolith form if necessary. Simulant Hanford and Idaho high sodium wastes were processed in a pilot scale FBSR at Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low-activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium-bearing waste (SBW). The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The durability of the FBSR waste form products was tested in order to compare the measured durability to previous FBSR waste form testing on Hanford Envelope C waste forms that were made by THOR Treatment Technologies (TTT) and to compare the FBSR durability to vitreous LAW waste forms, specifically the Hanford low activity waste (LAW) glass known as the Low-activity Reference Material (LRM). The durability of the FBSR waste form is comparable to that of the LRM glass for the test responses studied.

  10. Steam reforming of low-level mixed waste

    SciTech Connect

    Voelker, G.E.; Steedman, W.G.; Chandran, R.R.

    1996-12-31

    The U.S. department of Energy (DOE) is responsible for the treatment and disposal of an inventory of approximately 160,000 tons of Low-Level Mixed Waste (LLMW). Most of this LLMW is stored in drums, barrels and steel boxes at 20 different sites throughout the DOE complex. The basic objective of low-level mixed waste treatment systems is to completely destroy the hazardous constituents and to simultaneously isolate and capture the radionuclides in a superior final waste form such as glass. The DOE is sponsoring the development of advanced technologies that meet this objective while achieving maximum volume reduction, low-life cycle costs and maximum operational safety. ThermoChem, Inc. is in the final stages of development of a steam-reforming system capable of treating a wide variety of DOE low-level mixed waste that meets these objectives. The design, construction, and testing of a nominal 1 ton/day Process Development Unit is described.

  11. FLUIDIZED BED STEAM REFORMING ENABLING ORGANIC HIGH LEVEL WASTE DISPOSAL

    SciTech Connect

    Williams, M

    2008-05-09

    Waste streams planned for generation by the Global Nuclear Energy Partnership (GNEP) and existing radioactive High Level Waste (HLW) streams containing organic compounds such as the Tank 48H waste stream at Savannah River Site have completed simulant and radioactive testing, respectfully, by Savannah River National Laboratory (SRNL). GNEP waste streams will include up to 53 wt% organic compounds and nitrates up to 56 wt%. Decomposition of high nitrate streams requires reducing conditions, e.g. provided by organic additives such as sugar or coal, to reduce NOX in the off-gas to N2 to meet Clean Air Act (CAA) standards during processing. Thus, organics will be present during the waste form stabilization process regardless of the GNEP processes utilized and exists in some of the high level radioactive waste tanks at Savannah River Site and Hanford Tank Farms, e.g. organics in the feed or organics used for nitrate destruction. Waste streams containing high organic concentrations cannot be stabilized with the existing HLW Best Developed Available Technology (BDAT) which is HLW vitrification (HLVIT) unless the organics are removed by pretreatment. The alternative waste stabilization pretreatment process of Fluidized Bed Steam Reforming (FBSR) operates at moderate temperatures (650-750 C) compared to vitrification (1150-1300 C). The FBSR process has been demonstrated on GNEP simulated waste and radioactive waste containing high organics from Tank 48H to convert organics to CAA compliant gases, create no secondary liquid waste streams and create a stable mineral waste form.

  12. Steam reforming as a method to treat Hanford underground storage tank (UST) wastes

    SciTech Connect

    Miller, J.E.; Kuehne, P.B.

    1995-07-01

    This report summarizes a Sandia program that included partnerships with Lawrence Livermore National Laboratory and Synthetica Technologies, Inc. to design and test a steam reforming system for treating Hanford underground storage tank (UST) wastes. The benefits of steam reforming the wastes include the resolution of tank safety issues and improved radionuclide separations. Steam reforming destroys organic materials by first gasifying, then reacting them with high temperature steam. Tests indicate that up to 99% of the organics could be removed from the UST wastes by steam exposure. In addition, it was shown that nitrates in the wastes could be destroyed by steam exposure if they were first distributed as a thin layer on a surface. High purity alumina and nickel alloys were shown to be good candidates for materials to be used in the severe environment associated with steam reforming the highly alkaline, high nitrate content wastes. Work was performed on designing, building, and demonstrating components of a 0.5 gallon per minute (gpm) system suitable for radioactive waste treatment. Scale-up of the unit to 20 gpm was also considered and is feasible. Finally, process demonstrations conducted on non-radioactive waste surrogates were carried out, including a successful demonstration of the technology at the 0.1 gpm scale.

  13. FLUIDIZED BED STEAM REFORMER (FBSR) PRODUCT: MONOLITH FORMATION AND CHARACTERIZATION

    SciTech Connect

    Jantzen, C

    2006-09-13

    The most important requirement for Hanford's low activity waste (LAW) form for shallow land disposal is the chemical durability of the product. A secondary, but still essential specification, is the compressive strength of the material with regards to the strength of the material under shallow land disposal conditions, e.g. the weight of soil overburden and potential intrusion by future generations, because the term ''near-surface disposal'' indicates disposal in the uppermost portion, or approximately the top 30 meters, of the earth's surface. The THOR{reg_sign} Treatment Technologies (TTT) mineral waste form for LAW is granular in nature because it is formed by Fluidized Bed Steam Reforming (FBSR). As a granular product it has been shown to be as durable as Hanford's LAW glass during testing with ASTM C-1285-02 known as the Product Consistency Test (PCT) and with the Single Pass Flow Through Test (SPFT). Hanford Envelope A and Envelope C simulants both performed well during PCT and SPFT testing and during subsequent performance assessment modeling. This is partially due to the high aluminosilicate content of the mineral product which provides a natural aluminosilicate buffering mechanism that inhibits leaching and is known to occur in naturally occurring aluminosilicate mineral analogs. In order for the TTT Na-Al-Si (NAS) granular mineral product to meet the compressive strength requirements (ASTM C39) for a Hanford waste form, the granular product needs to be made into a monolith or disposed of in High Integrity Containers (HIC's). Additionally, the Hanford intruder scenario for disposal in the Immobilized Low Activity Waste (ILAW) trench is mitigated as there is reduced intruder exposure when a waste form is in a monolithic form. During the preliminary testing of a monolith binder for TTT's FBSR mineral product, four parameters were monitored: (1) waste loading (not optimized for each waste form tested); (2) density; (3) compressive strength; and (4) durability

  14. Production of synthetic fuels using syngas from a steam hydrogasification and reforming process

    NASA Astrophysics Data System (ADS)

    Raju, Arun Satheesh Kumar

    This thesis is aimed at the research, optimization and development of a thermo-chemical process aimed at the production of synthesis gas (mixture of H2 and CO) with a flexible H2 to CO ratio using coupled steam hydrogasification and steam reforming processes. The steam hydrogasification step generates a product gas containing significant amounts of methane by gasifying a carbonaceous feed material with steam and internally generated H2. This product gas is converted to synthesis gas with an excess H2 to CO using the steam reformer. Research involving experimental and simulation work has been conducted on steam hydrogasification, steam reforming and the Fischer-Tropsch reaction. The Aspen Plus simulation tool has been used to develop a process model that can perform heat and mass balance calculations of the whole process using built-in reactor modules and an empirical FT model available in the literature. This model has been used to estimate optimum feed ratios and process conditions for specific feedstocks and products. Steam hydrogasification of coal and wood mixtures of varying coal to wood ratios has been performed in a stirred batch reactor. The carbon conversion of the feedstocks to gaseous products is around 60% at 700°C and 80% at 800°C. The coal to wood ratio of the feedstock does not exert a significant influence on the carbon conversion. The rates of formation of CO, CO 2 and CH4 during gasification have been calculated based on the experimental results using a simple kinetic model. Experimental research on steam reforming has been performed. It has been shown that temperature and the feed CO2/CH4 ratio play a dominant role in determining the product gas H2/CO ratio. Reforming of typical steam hydrogasification product-gas stream has been investigated over a commercial steam reforming catalyst. The results demonstrate that the combined use of steam hydrogasification process with a reformer can generate a synthesis gas with a predetermined H2/CO ratio

  15. Steam reforming of tar model compound using Pd catalyst on alumina tube.

    PubMed

    Nisamaneenate, Jurarat; Atong, Duangduen; Sricharoenchaikul, Viboon

    2012-12-01

    Gasification processing of biomass as a renewable energy source generates tar in the product gas. Tar leads to foul-up of the process equipment by corrosion and deposit formation. Catalytic elimination of tars is a crucial step to improve fuel gas quality from the process. In this study, a palladium catalyst on alumina (Pd/Al2O3) was used in steam reforming of benzene as a biomass gasification tar model compound. The reaction was carried out in a laboratory-scale tube reactor made of stainless steel to study the effect of reaction temperature, catalyst loading, quantity of palladium catalyst tubes, steam to carbon ratio (S/C), and residence time on catalytic performance and stability. Pd/Al2O3 showed high efficiency ofbenzene decomposition and enhanced the formation of fuel gas. Hydrogen and carbon conversions increased with reaction temperature. Although the benzene concentration increased from 2000 to 5000 mg/l, the catalytic performance at 600 degrees C and 800 degrees C was similar. 1.0 wt% Pd/Al2O3 showed excellent catalytic activity with the highest hydrogen and carbon conversions of 83% and 81%, respectively at 800 degrees C. This result is attributed to the smooth surface of the palladium, as noted from scanning electron microscopy imaging. An S/C of 2 provided the highest conversion. The addition of catalyst from four and seven tubes did not result in any great difference in terms of benzene cracking efficiency. The fourth cyclic usage of 1.0 wt% Pd/Al2O3 exhibited a higher conversion than that of 0.5 wt%. PMID:23437646

  16. New Insights into Reaction Mechanisms of Ethanol Steam Reforming on Co-ZrO2

    SciTech Connect

    Sun, Junming; Karim, Ayman M.; Mei, Donghai; Engelhard, Mark H.; Bao, Xinhe; Wang, Yong

    2015-01-01

    The reaction pathway of ethanol steam reforming on Co-ZrO2 has been identified and the active sites associated with each step are proposed. Ethanol is converted to acetaldehyde and then to acetone, followed by acetone steam reforming. More than 90% carbon was found to follow this reaction pathway. N2-Sorption, X-ray Diffraction (XRD), Temperature Programmed Reduction (TPR), in situ X-ray Photoelectron Spectroscopy (XPS), Transmission Electron Microscopy, as well as theoretical Density Functional Theory (DFT) calculations have been employed to identify the structure and functionality of the catalysts, which was further used to correlate their performance in ESR. It was found that metallic cobalt is mainly responsible for the acetone steam reforming reactions; while, CoO and basic sites on the support play a key role in converting ethanol to acetone via dehydrogenation and condensation/ketonization reaction pathways. The current work provides fundamental understanding of the ethanol steam reforming reaction mechanisms on Co-ZrO2 catalysts and sheds light on the rational design of selective and durable ethanol steam reforming catalysts.

  17. In-Space Propulsion, Logistics Reduction, and Evaluation of Steam Reformer Kinetics: Problems and Prospects

    NASA Technical Reports Server (NTRS)

    Jaworske, D. A.; Palaszewski, B. A.; Kulis, M. J.; Gokoglu, S. A.

    2015-01-01

    Human space missions generate waste materials. A 70-kg crewmember creates a waste stream of 1 kg per day, and a four-person crew on a deep space habitat for a 400+ day mission would create over 1600 kg of waste. Converted into methane, the carbon could be used as a fuel for propulsion or power. The NASA Advanced Exploration Systems (AES) Logistics Reduction and Repurposing (LRR) project is investing in space resource utilization with an emphasis on repurposing logistics materials for useful purposes and has selected steam reforming among many different competitive processes as the preferred method for repurposing organic waste into methane. Already demonstrated at the relevant processing rate of 5.4 kg of waste per day, high temperature oxygenated steam consumes waste and produces carbon dioxide, carbon monoxide, and hydrogen which can then be converted into methane catalytically. However, the steam reforming process has not been studied in microgravity. Data are critically needed to understand the mechanisms that allow use of steam reforming in a reduced gravity environment. This paper reviews the relevant literature, identifies gravity-dependent mechanisms within the steam gasification process, and describes an innovative experiment to acquire the crucial kinetic information in a small-scale reactor specifically designed to operate within the requirements of a reduced gravity aircraft flight. The experiment will determine if the steam reformer process is mass-transport limited, and if so, what level of forced convection will be needed to obtain performance comparable to that in 1-g.

  18. Steam-Reforming Characteristics of Heavy and Light Tars Derived from Cellulose

    NASA Astrophysics Data System (ADS)

    Watanabe, Hirotatsu; Morinaga, Yosuke; Okazaki, Ken

    In this study, tar formation and steam-reforming mechanisms are discussed by separating the tars into heavy, middle, and light tars. Cellulose was heated in a drop-tube furnace under an Ar or Ar/steam atmosphere. After the tars were passed through the furnace for thermal cracking and polymerization, they were trapped by filters set at different temperatures (573, 393, and 273 K), and were respectively defined as heavy, middle, and light tars. Incondensable volatiles and gaseous products were measured using gas chromatography with thermal conductivity (GC-TCD), and flame ionization (GC-FID) detectors. The middle and light tars obtained under an Ar atmosphere were first characterized using time-of-flight mass spectrometry (TOF-MS). The analysis showed that the middle tar did not contain any low-boiling-point light tar components, while the light tar did contain them. It was also found that complex species in the tars were separated to a certain degree by changing the trap temperature. Moreover, the formation of heavy tar was quite different from that of the light tar. With increasing temperature, the formation of heavy tar was inhibited, while that of the light tar was enhanced during pyrolysis. The steam-reforming characteristics of these tars were also different. The heavy tar was barely reformed at a low temperature of 873 K, even with a long residence time, while the middle tar was well reformed by steam. While it was difficult to describe the tar formation and steam-reforming characteristics when the tar was considered as a single condensable matter, the tar formation and steam-reforming characteristics were clarified by separating the tars. This study shows that, to prevent tar emissions, the formation of heavy tar, which barely reacts with steam, should be inhibited during pyrolysis by controlling the heating.

  19. Developing an energy efficient steam reforming process to produce hydrogen from sulfur-containing fuels

    NASA Astrophysics Data System (ADS)

    Simson, Amanda

    Hydrogen powered fuel cells have the potential to produce electricity with higher efficiency and lower emissions than conventional combustion technology. In order to realize the benefits of a hydrogen fuel cell an efficient method to produce hydrogen is needed. Currently, over 90% of hydrogen is produced from the steam reforming of natural gas. However, for many applications including fuel cell vehicles, the use of a liquid fuel rather than natural gas is desirable. This work investigates the feasibility of producing hydrogen efficiently by steam reforming E85 (85% ethanol/15% gasoline), a commercially available sulfur-containing transportation fuel. A Rh-Pt/SiO2-ZrO2 catalyst has demonstrated good activity for the E85 steam reforming reaction. An industrial steam reforming process is often run less efficiently, with more water and at higher temperatures, in order to prevent catalyst deactivation. Therefore, it is desirable to develop a process that can operate without catalyst deactivation at more energy efficient conditions. In this study, the steam reforming of a sulfur-containing fuel (E85) was studied at near stoichiometric steam/carbon ratios and at 650C, conditions at which catalyst deactivation is normally measured. At these conditions the catalyst was found to be stable steam reforming a sulfur-free E85. However, the addition of low concentrations of sulfur significantly deactivated the catalyst. The presence of sulfur in the fuel caused catalyst deactivation by promoting ethylene which generates surface carbon species (coke) that mask catalytic sites. The amount of coke increased during time on stream and became increasingly graphitic. However, the deactivation due to both sulfur adsorption and coke formation was reversible with air treatment at 650°C. However, regenerations were found to reduce the catalyst life. Air regenerations produce exotherms on the catalyst surface that cause structural changes to the catalyst. During regenerations the

  20. High efficiency, quasi-instantaneous steam expansion device utilizing fossil or nuclear fuel as the heat source

    SciTech Connect

    Claudio Filippone, Ph.D.

    1999-06-01

    Thermal-hydraulic analysis of a specially designed steam expansion device (heat cavity) was performed to prove the feasibility of steam expansions at elevated rates for power generation with higher efficiency. The steam expansion process inside the heat cavity greatly depends on the gap within which the steam expands and accelerates. This system can be seen as a miniaturized boiler integrated inside the expander where steam (or the proper fluid) is generated almost instantaneously prior to its expansion in the work-producing unit. Relatively cold water is pulsed inside the heat cavity, where the heat transferred causes the water to flash to steam, thereby increasing its specific volume by a large factor. The gap inside the heat cavity forms a special nozzle-shaped system in which the fluid expands rapidly, accelerating toward the system outlet. The expansion phenomenon is the cause of ever-increasing fluid speed inside the cavity system, eliminating the need for moving parts (pumps, valves, etc.). In fact, the subsequent velocity induced by the sudden fluid expansion causes turbulent conditions, forcing accelerating Reynolds and Nusselt numbers which, in turn, increase the convective heat transfer coefficient. When the combustion of fossil fuels constitutes the heat source, the heat cavity concept can be applied directly inside the stator of conventional turbines, thereby greatly increasing the overall system efficiency.

  1. HIGH EFFICIENCY, QUASI-INSTANTANEOUS STEAM EXPANSION DEVICE UTILIZING FOSSIL OR NUCLEAR FUEL AS THE HEAT SOURCE

    SciTech Connect

    Claudio Filippone, Ph.D.

    1999-06-01

    Thermal-hydraulic analysis of a specially designed steam expansion device (heat cavity) was performed to prove the feasibility of steam expansions at elevated rates for power generation with higher efficiency. The steam expansion process inside the heat cavity greatly depends on the gap within which the steam expands and accelerates. This system can be seen as a miniaturized boiler integrated inside the expander where steam (or the proper fluid) is generated almost instantaneously prior to its expansion in the work-producing unit. Relatively cold water is pulsed inside the heat cavity, where the heat transferred causes the water to flash to steam, thereby increasing its specific volume by a large factor. The gap inside the heat cavity forms a special nozzle-shaped system in which the fluid expands rapidly, accelerating toward the system outlet. The expansion phenomenon is the cause of ever-increasing fluid speed inside the cavity system, eliminating the need for moving parts (pumps, valves, etc.). In fact, the subsequent velocity induced by the sudden fluid expansion causes turbulent conditions, forcing accelerating Reynolds and Nusselt numbers which, in turn, increase the convective heat transfer coefficient. When the combustion of fossil fuels constitutes the heat source, the heat cavity concept can be applied directly inside the stator of conventional turbines, thereby greatly increasing the overall system efficiency.

  2. Heterogeneous Reactor Model for Steam Reforming of Methane in a Microchannel Reactor with Microstructured Catalysts

    SciTech Connect

    Cao, Chunshe; Wang, Yong; Rozmiarek, Robert T.

    2005-12-15

    Microstructured catalysts used for methane steam reforming in microchannel reactors are mathematically described and experimentally demonstrated under realistic process conditions. A heterogeneous model has been developed with a graphical interface to represent the three dimensions of the microchannel reactor. Porous metal substrates (FeCrAlY) were used to form engineered catalysts with active precious metal (Rh) for methane steam reforming. Two types of structures were evaluated in the microchannel reactors and simulated with the developed heterogeneous reactor model. Local temperature and methane concentration profiles within the structures are illustrated to show the correlation of the catalyst structure and its performance. Such a modeling technique provides a convenient and flexible method to evaluate variables in designing more efficient catalysts for the highly endothermic steam reforming reactions, as the desired mass and heat transfer characteristics are achieved.

  3. DATA QUALITY OBJECTIVES FOR SELECTING WASTE SAMPLES FOR THE BENCH STEAM REFORMER TEST

    SciTech Connect

    BANNING DL

    2010-08-03

    This document describes the data quality objectives to select archived samples located at the 222-S Laboratory for Fluid Bed Steam Reformer testing. The type, quantity and quality of the data required to select the samples for Fluid Bed Steam Reformer testing are discussed. In order to maximize the efficiency and minimize the time to treat Hanford tank waste in the Waste Treatment and Immobilization Plant, additional treatment processes may be required. One of the potential treatment processes is the fluid bed steam reformer (FBSR). A determination of the adequacy of the FBSR process to treat Hanford tank waste is required. The initial step in determining the adequacy of the FBSR process is to select archived waste samples from the 222-S Laboratory that will be used to test the FBSR process. Analyses of the selected samples will be required to confirm the samples meet the testing criteria.

  4. Steam Reforming Technology for Denitration and Immobilization of DOE Tank Wastes

    SciTech Connect

    Mason, J. B.; McKibbin, J.; Ryan, K.; Schmoker, D.

    2003-02-26

    THOR Treatment Technologies, LLC (THOR) is a joint venture formed in June 2002 by Studsvik, Inc. (Studsvik) and Westinghouse Government Environmental Services Company LLC to further develop, market, and deploy Studsvik's patented THORSM non-incineration, steam reforming waste treatment technology. This paper provides an overview of the THORSM steam reforming process as applied to the denitration and conversion of Department of Energy (DOE) tank wastes to an immobilized mineral form. Using the THORSM steam reforming technology to treat nitrate containing tank wastes could significantly benefit the DOE by reducing capital and life-cycle costs, reducing processing and programmatic risks, and positioning the DOE to meet or exceed its stakeholder commitments for tank closure. Specifically, use of the THORSM technology can facilitate processing of up to 75% of tank wastes without the use of vitrification, yielding substantial life-cycle cost savings.

  5. The Effects of PdZn Crystallite Size on Methanol Steam Reforming

    SciTech Connect

    Dagle, Robert A.; Chin, Ya-Huei; Wang, Yong

    2007-11-30

    Exceptional activity and selectivity of Pd/ZnO catalysts for methanol steam reforming have been attributed to the formation of PdZn alloy. In this paper, we evaluated the crystallite size effects of PdZn alloy on methanol steam reforming. An organic preparation method was used to avoid the complexity from the alteration of ZnO morphology typically associated with the conventional aqueous preparation method. Both Pd loading and reduction temperature (>350ºC) were used to vary the crystallite size of PdZn alloy. Experimental activity studies and transmission electron microscope (TEM) characterizations indicated that formation of large sized PdZn crystallites exhibit high reactivity and low CO selectivity during methanol steam reforming.

  6. Fluidized Bed Steam Reforming of Hanford LAW Using THORsm Mineralizing Technology

    SciTech Connect

    Olson, Arlin L.; Nicholas R Soelberg; Douglas W. Marshall; Gary L. Anderson

    2004-11-01

    The U.S. Department of Energy (DOE) documented, in 2002, a plan for accelerating cleanup of the Hanford Site, located in southeastern Washington State, by at least 35 years. A key element of the plan was acceleration of the tank waste program and completion of ''tank waste treatment by 2028 by increasing the capacity of the planned Waste Treatment Plant (WTP) and using supplemental technologies for waste treatment and immobilization.'' The plan identified steam reforming technology as a candidate for supplemental treatment of as much as 70% of the low-activity waste (LAW). Mineralizing steam reforming technology, offered by THOR Treatment Technologies, LLC would produce a denitrated, granular mineral waste form using a high-temperature fluidized bed process. A pilot scale demonstration of the technology was completed in a 15-cm-diameter reactor vessel. The pilot scale facility was equipped with a highly efficient cyclone separator and heated sintered metal filters for particulate removal, a thermal oxidizer for reduced gas species and NOx destruction, and a packed activated carbon bed for residual volatile species capture. The pilot scale equipment is owned by the DOE, but located at the Science and Technology Applications Research (STAR) Center in Idaho Falls, ID. Pilot scale testing was performed August 2–5, 2004. Flowsheet chemistry and operational parameters were defined through a collaborative effort involving Idaho National Engineering and Environmental Laboratory, Savannah River National Laboratory (SRNL), and THOR Treatment Technologies personnel. Science Application International Corporation, owners of the STAR Center, personnel performed actual pilot scale operation. The pilot scale test achieved a total of 68.7 hrs of cumulative/continuous processing operation before termination in response to a bed de-fluidization condition. 178 kg of LAW surrogate were processed that resulted in 148 kg of solid product, a mass reduction of about 17%. The process

  7. On-board reforming of biodiesel and bioethanol for high temperature PEM fuel cells: Comparison of autothermal reforming and steam reforming

    NASA Astrophysics Data System (ADS)

    Martin, Stefan; Wörner, Antje

    2011-03-01

    In the 21st century biofuels will play an important role as alternative fuels in the transportation sector. In this paper different reforming options (steam reforming (SR) and autothermal reforming (ATR)) for the on-board conversion of bioethanol and biodiesel into a hydrogen-rich gas suitable for high temperature PEM (HTPEM) fuel cells are investigated using the simulation tool Aspen Plus. Special emphasis is placed on thermal heat integration. Methyl-oleate (C19H36O2) is chosen as reference substance for biodiesel. Bioethanol is represented by ethanol (C2H5OH). For the steam reforming concept with heat integration a maximum fuel processing efficiency of 75.6% (76.3%) is obtained for biodiesel (bioethanol) at S/C = 3. For the autothermal reforming concept with heat integration a maximum fuel processing efficiency of 74.1% (75.1%) is obtained for biodiesel (bioethanol) at S/C = 2 and λ = 0.36 (0.35). Taking into account the better dynamic behaviour and lower system complexity of the reforming concept based on ATR, autothermal reforming in combination with a water gas shift reactor is considered as the preferred option for on-board reforming of biodiesel and bioethanol. Based on the simulation results optimum operating conditions for a novel 5 kW biofuel processor are derived.

  8. Hydrogen production from the steam reforming of Dinethyl Ether and Methanol

    SciTech Connect

    Semelsberger, T. A.; Borup, R. L.

    2004-01-01

    This study investigates dimethyl ether (DME) steam reforming for the generation of hydrogen rich fuel cell feeds for fuel cell applications. Methanol has long been considered as a fuel for the generation of hydrogen rich fuel cell feeds due to its high energy density, low reforming temperature, and zero impurity content. However, it has not been accepted as the fuel of choice due its current limited availability, toxicity and corrosiveness. While methanol steam reforming for the generation of hydrogen rich fuel cell feeds has been extensively studied, the steam reforming of DME, CH{sub 3}OCH{sub 3} + 3H{sub 2}O = 2CO{sub 2} + 6H{sub 2}, has had limited research effort. DME is the simplest ether (CH{sub 3}OCH{sub 3}) and is a gas at ambient conditions. DME has physical properties similar to those of LPG fuels (i.e. propane and butane), resulting in similar storage and handling considerations. DME is currently used as an aerosol propellant and has been considercd as a diesel substitute due to the reduced NOx, SOx and particulate emissions. DME is also being considered as a substitute for LPG fuels, which is used extensively in Asia as a fuel for heating and cooking, and naptha, which is used for power generation. The potential advantages of both methanol and DME include low reforming temperature, decreased fuel proccssor startup energy, environmentally benign, visible flame, high heating value, and ease of storage and transportation. In addition, DME has the added advantages of low toxicity and being non-corrosive. Consequently, DME may be an ideal candidate for the generation of hydrogen rich fuel cell feeds for both automotive and portable power applications. The steam reforming of DME has been demonstrated to occur through a pair of reactions in series, where the first reaction is DME hydration followed by MeOH steam reforming to produce a hydrogen rich stream.

  9. Intrinsic reaction kinetics of methane steam reforming on a nickel/zirconia anode

    NASA Astrophysics Data System (ADS)

    Dicks, A. L.; Pointon, K. D.; Siddle, A.

    For the purposes of optimising important system parameters in direct internally reforming (DIR) solid oxide fuel cell (SOFC) systems, a detailed knowledge of the methane steam reforming rate on the anode is needed. In order to shed light on the present poorly understood kinetics, a study of the methane steam reforming rate given by a typical thin electrolyte-supported nickel/zirconia SOFC anode has been carried out using a tubular plug flow differential reactor. These tests were essentially gradientless. The reaction rate was studied as a function of temperature (700-1000°C) and the partial pressure of methane (2-40 kPa), hydrogen (10-70 kPa) and steam (10-70 kPa). The total pressure was nominally 1 atm. The reaction was first order in methane with a weak positive effect of hydrogen, and a stronger negative effect of steam. The kinetics were complicated by the fact that reaction orders in hydrogen and steam were either temperature dependent and/or depended on the partial pressures of other components in the gas mixture. Furthermore, Arrhenius-type plots gave gradients which were dependent on the steam partial pressure. It is clear from this study that the reaction cannot be represented as simply as is generally attempted in the literature. An improved rate equation has been derived.

  10. Steam reforming of fuel to hydrogen in fuel cell

    DOEpatents

    Young, J.E.; Fraioli, A.V.

    1983-07-13

    A fuel cell is described capable of utilizing a hydrocarbon such as methane as fuel and having an internal dual catalyst system within the anode zone, the dual catalyst system including an anode catalyst supporting and in heat conducting relationship with a reforming catalyst with heat for the reforming reaction being supplied by the reaction at the anode catalyst.

  11. Steam reforming of fuel to hydrogen in fuel cells

    DOEpatents

    Fraioli, Anthony V.; Young, John E.

    1984-01-01

    A fuel cell capable of utilizing a hydrocarbon such as methane as fuel and having an internal dual catalyst system within the anode zone, the dual catalyst system including an anode catalyst supporting and in heat conducting relationship with a reforming catalyst with heat for the reforming reaction being supplied by the reaction at the anode catalyst.

  12. CATALYTIC STEAM REFORMING OF CHLOROCARBONS: TRICHLOROETHANE, TRICHLOROETHYLENE AND PERCHLOROETHYLENE. (R826694C633)

    EPA Science Inventory

    The effective destruction of trichloroethane, trichloroethylene and perchloroethylene by steam reforming with a commercial nickel catalyst has been demonstrated. Conversion levels of up to 0.99999 were attained in both laboratory and semi-pilot experiments, with the products c...

  13. FLUIDIZED BED STEAM REFORMING FOR TREATMENT AND IMMOBILIZATION OF LOW-ACTIVITY WASTE

    SciTech Connect

    HEWITT WM

    2011-04-08

    This report is one of four reports written to provide background information regarding immobilization technologies remaining under consideration for supplemental immobilization of Hanford's low-activity waste. This paper provides the reader a general understanding of fluidized bed steam reforming and its possible application to treat and immobilize Hanford low-activity waste.

  14. CATALYTIC STEAM REFORMING OF CHLOROCARBONS: POLYCHLORINATED BIPHENYLS (PCBS). (R826694C633)

    EPA Science Inventory

    Experiments with commercial askarals (Aroclors 1221, 1248 and 1254) have confirmed the feasibility of catalytic steam reforming as a method for destroying polychlorinated biphenyls (PCBs). Rhodium, platinum and nickel supported on CATALYTIC STEAM REFORMING OF CHLOROCARBONS: CATALYST COMPARISONS. (R822721C633)

    EPA Science Inventory

    Catalyst candidates for steam reforming chlorocarbons have been screened for activity using methyl chloride as a model reactant. At 500°C, a H2O/C ratio of about 10 and a GHSV of 254 000 h-1, catalysts comprising 0.5% loading of the metals o...

  15. CATALYTIC STEAM REFORMING OF CHLOROCARBONS: CATALYST DEACTIVATION. (R826694C633)

    EPA Science Inventory

    Deactivation of 0.5 wt.% Pt/small gamma, Greek-Al2O3 catalysts during trichloroethylene (TCE)–steam reforming was studied with experiments at 700°C, H

  16. CATALYTIC STEAM REFORMING OF CHLOROCARBONS: CATALYST COMPARISONS. (R826694C633)

    EPA Science Inventory

    Catalyst candidates for steam reforming chlorocarbons have been screened for activity using methyl chloride as a model reactant. At 500°C, a H2O/C ratio of about 10 and a GHSV of 254 000 h-1, catalysts comprising 0.5% loading of the metals ...

  17. Thermal analysis of cylindrical natural-gas steam reformer for 5 kW PEMFC

    NASA Astrophysics Data System (ADS)

    Jo, Taehyun; Han, Junhee; Koo, Bonchan; Lee, Dohyung

    2016-01-01

    The thermal characteristics of a natural-gas based cylindrical steam reformer coupled with a combustor are investigated for the use with a 5 kW polymer electrolyte membrane fuel cell. A reactor unit equipped with nickel-based catalysts was designed to activate the steam reforming reaction without the inclusion of high-temperature shift and low-temperature shift processes. Reactor temperature distribution and its overall thermal efficiency depend on various inlet conditions such as the equivalence ratio, the steam to carbon ratio (SCR), and the fuel distribution ratio (FDR) into the reactor and the combustor components. These experiments attempted to analyze the reformer's thermal and chemical properties through quantitative evaluation of product composition and heat exchange between the combustor and the reactor. FDR is critical factor in determining the overall performance as unbalanced fuel injection into the reactor and the combustor deteriorates overall thermal efficiency. Local temperature distribution also influences greatly on the fuel conversion rate and thermal efficiency. For the experiments, the operation conditions were set as SCR was in range of 2.5-4.0 and FDR was in 0.4-0.7 along with equivalence ratio of 0.9-1.1; optimum results were observed for FDR of 0.63 and SCR of 3.0 in the cylindrical steam reformer.

  18. On the origin of reactivity of steam reforming of ethylene glycol on supported Ni catalysts.

    PubMed

    Li, Shuirong; Zhang, Chengxi; Zhang, Peng; Wu, Gaowei; Ma, Xinbin; Gong, Jinlong

    2012-03-28

    This paper describes a strategy for producing hydrogen via steam reforming of ethylene glycol over supported nickel catalysts. Nickel plays a crucial role in conversion of ethylene glycol and production of hydrogen, while oxide supports affect product distribution of carbonaceous species. A plausible reaction pathway is proposed based on our results and the literature. PMID:22246195

  19. Production of hydrogen from biomass by catalytic steam reforming of fast pyrolysis oil

    SciTech Connect

    Czernik, S.; Wang, D.; Chornet, E.

    1998-08-01

    Hydrogen is the prototype of the environmentally cleanest fuel of interest for power generation using fuel cells and for transportation. The thermochemical conversion of biomass to hydrogen can be carried out through two distinct strategies: (a) gasification followed by water-gas shift conversion, and (b) catalytic steam reforming of specific fractions derived from fast pyrolysis and aqueous/steam processes of biomass. This paper presents the latter route that begins with fast pyrolysis of biomass to produce bio-oil. This oil (as a whole or its selected fractions) can be converted to hydrogen via catalytic steam reforming followed by a water-gas shift conversion step. Such a process has been demonstrated at the bench scale using model compounds, poplar oil aqueous fraction, and the whole pyrolysis oil with commercial Ni-based steam reforming catalysts. Hydrogen yields as high as 85% have been obtained. Catalyst initial activity can be recovered through regeneration cycles by steam or CO{sub 2} gasification of carbonaceous deposits.

  1. Process and apparatus for the production of hydrogen by steam reforming of hydrocarbon

    DOEpatents

    Sircar, Shivaji; Hufton, Jeffrey Raymond; Nataraj, Shankar

    2000-01-01

    In the steam reforming of hydrocarbon, particularly methane, under elevated temperature and pressure to produce hydrogen, a feed of steam and hydrocarbon is fed into a first reaction volume containing essentially only reforming catalyst to partially reform the feed. The balance of the feed and the reaction products of carbon dioxide and hydrogen are then fed into a second reaction volume containing a mixture of catalyst and adsorbent which removes the carbon dioxide from the reaction zone as it is formed. The process is conducted in a cycle which includes these reactions followed by countercurrent depressurization and purge of the adsorbent to regenerate it and repressurization of the reaction volumes preparatory to repeating the reaction-sorption phase of the cycle.

  2. Thermodynamics of Hydrogen Production from Dimethyl Ether Steam Reforming and Hydrolysis

    SciTech Connect

    T.A. Semelsberger

    2004-10-01

    The thermodynamic analyses of producing a hydrogen-rich fuel-cell feed from the process of dimethyl ether (DME) steam reforming were investigated as a function of steam-to-carbon ratio (0-4), temperature (100 C-600 C), pressure (1-5 atm), and product species: acetylene, ethanol, methanol, ethylene, methyl-ethyl ether, formaldehyde, formic acid, acetone, n-propanol, ethane and isopropyl alcohol. Results of the thermodynamic processing of dimethyl ether with steam indicate the complete conversion of dimethyl ether to hydrogen, carbon monoxide and carbon dioxide for temperatures greater than 200 C and steam-to-carbon ratios greater than 1.25 at atmospheric pressure (P = 1 atm). Increasing the operating pressure was observed to shift the equilibrium toward the reactants; increasing the pressure from 1 atm to 5 atm decreased the conversion of dimethyl ether from 99.5% to 76.2%. The order of thermodynamically stable products in decreasing mole fraction was methane, ethane, isopropyl alcohol, acetone, n-propanol, ethylene, ethanol, methyl-ethyl ether and methanol--formaldehyde, formic acid, and acetylene were not observed. The optimal processing conditions for dimethyl ether steam reforming occurred at a steam-to-carbon ratio of 1.5, a pressure of 1 atm, and a temperature of 200 C. Modeling the thermodynamics of dimethyl ether hydrolysis (with methanol as the only product considered), the equilibrium conversion of dimethyl ether is limited. The equilibrium conversion was observed to increase with temperature and steam-to-carbon ratio, resulting in a maximum dimethyl ether conversion of approximately 68% at a steam-to-carbon ratio of 4.5 and a processing temperature of 600 C. Thermodynamically, dimethyl ether processed with steam can produce hydrogen-rich fuel-cell feeds--with hydrogen concentrations exceeding 70%. This substantiates dimethyl ether as a viable source of hydrogen for PEM fuel cells.

  3. The Engine of Reform Gathers Steam: Kentucky Starts from Scratch.

    ERIC Educational Resources Information Center

    Harrington-Lueker, Donna

    1990-01-01

    Charged with overhauling the state's educational system, the Kentucky General Assembly last spring devised a landmark reform scheme that mandates site-based management, abolishes the existing state board of education, and institutes an ambitious system of rewards and sanctions aimed at holding schools accountable for student performance. A sidebar…

  4. Evaluation of the feasibility of ethanol steam reforming in a molten carbonate fuel cell

    SciTech Connect

    Cavallaro, S.; Passalacqua, E.; Maggio, G.; Patti, A.; Freni, S.

    1996-12-31

    The molten carbonate fuel cells (MCFCs) utilizing traditional fuels represent a suitable technological progress in comparison with pure hydrogen-fed MCFCs. The more investigated fuel for such an application is the methane, which has the advantages of low cost and large availability; besides, several authors demonstrated the feasibility of a methane based MCFC. In particular, the methane steam-reforming allows the conversion of the fuel in hydrogen also inside the cell (internal reforming configuration), utilizing the excess heat to compensate the reaction endothermicity. In this case, however, both the catalyst and the cell materials are subjected to thermal stresses due to the cold spots arising near to the reaction sites MCFC. An alternative, in accordance with the recent proposals of other authors, may be to produce hydrogen from methane by the partial oxidation reaction, rather than by steam reforming. This reaction is exothermic ({Delta}H{degrees}=-19.1 kJ/mol H{sub 2}) and it needs to verify the possibility to obtain an acceptable distribution of the temperature inside the cell. The alcohols and, in particular, methanol shows the gas reformed compositions as a function of the steam/ethanol molar ratio, ranging from 1.0 to 3.5. The hydrogen production enhances with this ratio, but it presents a maximum at S/EtOH of about 2.0. Otherwise, the increase of S/EtOH depresses the production of CO and CH{sub 4}, and ethanol may be a further solution for the hydrogen production inside a MCFC. In this case, also, the reaction in cell is less endothermic compared with the methane steam reforming with the additional advantage of a liquid fuel more easily storable and transportable. Aim of the present work is to perform a comparative evaluation of the different solutions, with particular reference to the use of ethanol.

  5. Biomass gasification with air in fluidized bed: Reforming of the gas composition with commercial steam reforming catalysts

    SciTech Connect

    Corella, J.; Orio, A.; Aznar, P.

    1998-12-01

    Four commercial catalysts for steam reforming of higher hydrocarbons (naphthas) and three for steam reforming of light hydrocarbons are tested for hot gas clean up and upgrading in biomass gasification with air in fluidized bed. The catalysts used originate from four manufacturers: BASF, AG, ICI-Katalco, Haldor Topsoe a/s, and United Catalysts Inc. The work is performed in a small pilot plant (1--2 kg of biomass fed/h) with three reactors in series: gasifier, guard bed of dolomite, and full flow catalytic bed. Samples of gas are taken before and after the catalytic bed at different times-on-stream. It is shown how the H{sub 2}, CO, CO{sub 2}, CH{sub 4} and steam contents in the flue gas change because of the catalytic bed approaching contents near to the ones corresponding to the equilibrium state. Variations in the heating value of the gas and gas yield as a result of the catalytic bed are also reported.

  6. Biomass-to-hydrogen via fast pyrolysis and catalytic steam reforming

    SciTech Connect

    Chornet, E.; Wang, D.; Czernik, S.

    1996-10-01

    Pyrolysis of lignocellulosic biomass and reforming the pyroligneous oils is being studied as a strategy for producing hydrogen. Novel technologies for the rapid pyrolysis of biomass have been developed in the past decade. They provide compact and efficient systems to transform biomass into vapors that are condensed to oils, with yields as high as 75-80 wt.% of the anhydrous biomass. This {open_quotes}bio-oil{close_quotes} is a mixture of aldehydes, alcohols, acids, oligomers from the constitutive carbohydrates and lignin, and some water derived from the dehydration reactions. Hydrogen can be produced by reforming the bio-oil or its fractions with steam. A process of this nature has the potential to be cost competitive with conventional means of producing hydrogen. The reforming facility can be designed to handle alternate feedstocks, such as natural gas and naphtha, if necessary. Thermodynamic modeling of the major constituents of the bio-oil has shown that reforming is possible within a wide range of temperatures and steam-to-carbon ratios. Existing catalytic data on the reforming of oxygenates have been studied to guide catalyst selection. Tests performed on a microreactor interfaced with a molecular beam mass spectrometer showed that, by proper selection of the process variables: temperature, steam-to-carbon ratio, gas hourly space velocity, and contact time, almost total conversion of carbon in the feed to CO and CO{sub 2} could be obtained. These tests also provided possible reaction mechanisms where thermal cracking competes with catalytic processes. Bench-scale, fixed bed reactor tests demonstrated high hydrogen yields from model compounds and carbohydrate-derived pyrolysis oil fractions. Reforming bio-oil or its fractions required proper dispersion of the liquid to avoid vapor-phase carbonization of the feed in the inlet to the reactor. A special spraying nozzle injector was designed and successfully tested with an aqueous fraction of bio-oil.

  7. Glycerol Steam Reforming Over Ni-Fe-Ce/Al2O3 Catalyst: Effect of Cerium.

    PubMed

    Go, Gwang-Sub; Go, Yoo-Jin; Lee, Hong-Joo; Moon, Dong-Ju; Park, Nam-Cook; Kim, Young-Chul

    2016-02-01

    In this work, hydrogen production from glycerol by steam reforming was studied using Ni-metal oxide catalysts. Ni-based catalyst becomes deactivated during steam reforming reactions because of coke deposits and sintering. Therefore, the aim of this study was to reduce carbon deposits and sintering on the catalyst surface by adding a promoter. Ni-metal oxide catalysts supported on Al2O3 were prepared via impregnation method, and the calcined catalyst was reduced under H2 flow for 2 h prior to the reaction. The characteristics of the catalysts were examined by XRD, TPR, TGA, and SEM. The Ni-Fe-Ce/Al2O3 catalyst, which contained less than 2 wt% Ce, showed the highest hydrogen selectivity and glycerol conversion. Further analysis of the catalysts revealed that the Ni-Fe-Ce/Al2O3 catalyst required a lower reduction temperature and produced minimum carbon deposit. PMID:27433687

  8. Steam reforming of ethanol on Ni/MgO catalysts: H 2 production for MCFC

    NASA Astrophysics Data System (ADS)

    Freni, S.; Cavallaro, S.; Mondello, N.; Spadaro, L.; Frusteri, F.

    H 2 production by ethanol steam reforming in simulating molten carbonate fuel cell (MCFC) conditions was explored. Ni/MgO catalysts exhibit very high selectivity to H 2 and CO 2 as a consequence of their low tendency to promote carbon monoxide methanation and ethanol decomposition reactions. Coke formation is strongly depressed due to the benefits induced by the use of basic carrier which positively modify the electronic properties of supported Ni.

  9. Hydrogen production from glucose and sorbitol by sorption-enhanced steam reforming: challenges and promises.

    PubMed

    He, Li; Chen, De

    2012-03-12

    Concerning energy and environmental sustainability, it is appealing to produce hydrogen from sugars or sugar alcohols that are readily obtained from the hydrolysis of cellulosic biomass. Nevertheless, the conversion of such compounds for hydrogen production poses great technical challenges. In this paper, we report that hydrogen purity and yield can be significantly improved by integrating in situ CO(2) capture into the steam reforming reaction of the model compounds-glucose and sorbitol. The experimental assessment was conducted at a steam-to-carbon ratio of 1.8 for sorbitol and 6 for glucose from 450-625 °C. As predicted by thermodynamic analysis, combining CO(2) capture and reforming reactions at favorable operating conditions yielded very high purity hydrogen, for instance, 98.8 mol % from sorbitol and 99.9 mol % from glucose. However, there are trade-offs between hydrogen purity and yield in practice. The lower operating temperatures in the examined range helped to increase the hydrogen purity and reduce the CO content in the gas product, whereas a high hydrogen yield was more likely to be obtained at higher temperatures. Coupling CO(2) capture lowered the risk of coke formation during the steam reforming of glucose. Coke accumulated in the reactor for the sorption-enhanced steam reforming of glucose was mostly from the slow pyrolysis of glucose before it came into contact with the catalyst-acceptor bed. This problem may be solved by improving heat transfer or reconstructing the reactor, for instance, by using a fluidized-bed reactor. PMID:22378630

  10. Development and life evaluation of a steam reforming process for PAFC

    SciTech Connect

    Nagase, S.; Takami, S.; Masuda, M.

    1996-12-31

    This paper reports a life evaluation method for a carbon monoxide (CO) shift process in the steam reforming process for PAFC. A CO shift reactor simulation was developed to evaluate the whole performance of the CO shift process. The calculation results of the simulation almost coincide with the experimental data obtained from a demonstration plant. By evaluating and grasping the sintering trend of the catalyst, and by simulation calculation of the reactor, it became possible to evaluate the performance at targeted operation hours.

  11. Studies of potassium-promoted nickel catalysts for methane steam reforming: Effect of surface potassium location

    NASA Astrophysics Data System (ADS)

    Borowiecki, Tadeusz; Denis, Andrzej; Rawski, Michał; Gołębiowski, Andrzej; Stołecki, Kazimierz; Dmytrzyk, Jaromir; Kotarba, Andrzej

    2014-05-01

    The effect of potassium addition to the Ni/Al2O3 steam reforming catalyst has been investigated on several model systems, including K/Al2O3 with various amounts of alkali promoters (1-4 wt% of K2O), a model catalyst 90%NiO-10%Al2O3 promoted with potassium and a commercial catalyst. The potassium surface state and stability were investigated by means of the Species Resolved Thermal Alkali Desorption method (SR-TAD). The activity of the catalysts in the steam reforming of methane and their coking-resistance were also evaluated. The results reveal that the beneficial effect of potassium addition is strongly related to its location in the catalysts. The catalyst surface should be promoted with potassium in order to obtain high coking-resistant catalysts. Moreover, the catalyst preparation procedure should ensure a direct interaction of potassium with the Al2O3 support surface. Due to the low stability of potassium on θ-Al2O3 this phase is undesirable during the preparation of a stable steam reforming catalyst.

  12. Heat-transfer simulation in a furnace for steam reformer

    SciTech Connect

    Kudo, K.; Taniguchi, H.; Guo, K. . Faculty of Engineering); Katayama, T.; Nagata, T. )

    1991-01-01

    This paper discusses three-dimensional combined radiative and convective heat-transfer process in a furnace for LPG reforming which is simulated by introducing the radiosity concept into the radiative heat ray method for accurate radiative heat-transfer analysis. Together with an analysis of the chemical reaction in the reactor tubes of the furnace, the heat-transfer simulation gives the three-dimensional profile of the combustion gas temperature in the furnace, the tube-surface heat-flux distribution and the composition of the product gas obtained from the forming. The results obtained are as follows: increasing the jet angle of the heating burner raises the gas temperature and the tube surface heat flux near the burner entrance; the flame shape is the most important factor for deciding the heat flux distribution of the tube surface because the heat transferred by flame radiation is much more than they by convection of the combustion gas.

  13. INVESTIGATION OF FUEL CHEMISTRY AND BED PERFORMANCE IN A FLUIDIZED BED BLACK LIQUOR STEAM REFORMER

    SciTech Connect

    Kevin Whitty

    2003-12-01

    The University of Utah project ''Investigation of Fuel Chemistry and Bed Performance in a Fluidized Bed Black Liquor Steam Reformer'' (DOE award number DE-FC26-02NT41490) was developed in response to a solicitation for projects to provide technical support for black liquor and biomass gasification. The primary focus of the project is to provide support for a DOE-sponsored demonstration of MTCI's black liquor steam reforming technology at Georgia-Pacific's paper mill in Big Island, Virginia. A more overarching goal is to improve the understanding of phenomena that take place during low temperature black liquor gasification. This is achieved through five complementary technical tasks: (1) construction of a fluidized bed black liquor gasification test system, (2) investigation of bed performance, (3) evaluation of product gas quality, (4) black liquor conversion analysis and modeling and (5) computational modeling of the Big Island gasifier. Four experimental devices have been constructed under this project. The largest facility, which is the heart of the experimental effort, is a pressurized fluidized bed gasification test system. The system is designed to be able to reproduce conditions near the black liquor injectors in the Big Island steam reformer, so the behavior of black liquor pyrolysis and char gasification can be quantified in a representative environment. The gasification test system comprises five subsystems: steam generation and superheating, black liquor feed, fluidized bed reactor, afterburner for syngas combustion and a flue gas cooler/condenser. The three-story system is located at University of Utah's Industrial Combustion and Gasification Research Facility, and all resources there are available to support the research.

  14. Plasma steam reforming of E85 for hydrogen rich gas production

    NASA Astrophysics Data System (ADS)

    Zhu, Xinli; Hoang, Trung; Lobban, Lance L.; Mallinson, Richard G.

    2011-07-01

    E85 (85 vol% ethanol and 15 vol% gasoline) is a partly renewable fuel that is increasing in supply availability. Hydrogen production from E85 for fuel cell or internal combustion engine applications is a potential method for reducing CO2 emissions. Steam reforming of E85 using a nonthermal plasma (pulse corona discharge) reactor has been exploited at low temperature (200-300 °C) without external heating, diluent gas, oxidant or catalyst in this work. Several operational parameters, including the discharge current, E85 concentration and feed flow rate, have been investigated. The results show that hydrogen rich gases (63-67% H2 and 22-29% CO, with small amounts of CO2, C2 hydrocarbons and CH4) can be produced by this method. A comparison with ethanol reforming and gasoline reforming under identical conditions has also been made and the behaviour of E85 reforming is found to be close to that of ethanol reforming with slightly higher C2 hydrocarbons yields.

  15. Hydrogen production by ethanol steam reforming on Ni/oxide catalysts

    NASA Astrophysics Data System (ADS)

    Lazar, Mihaela D.; Dan, Monica; Mihet, Maria; Borodi, George; Almasan, Valer

    2012-02-01

    Hydrogen production from bio-fuels such as bio-ethanol provides significant environmental benefits since the resulted CO2 is consumed again for biomass growth, offering a carbon dioxide neutral energy source. In the actual conditions of increasing energy demand and atmosphere pollution, clean produced hydrogen can be an alternative option for a clean energy vector. In this paper we present the results obtained in hydrogen production by steam reforming of ethanol using oxide supported nickel catalysts. Although Ni is not the most active catalyst for this process, economically is the most attractive one, due to the high price and low availability of noble metals. Ni was dispersed on several oxides: ZrO2, Al2O3, Cr2O3, SiO2 with a target metal concentration of 8 wt%. using impregnation method. The catalysts were characterized using several techniques: N2 adsorption desorption isotherms to determine total surface area and porosity, XRD to determine oxide crystallinity and Ni crystallite size. Each catalyst was tested in steam reforming of ethanol at temperatures ranging from 150 to 350°C, at atmospheric pressure and a ethanol: steam ratio of 1:9. The best ethanol conversion and catalyst stability was obtained for Ni/Al2O3. The catalyst selectivity for H2 production depends on the support nature. The best H2 selectivity was obtained for Ni/ZrO2 catalyst.

  16. Process Options Description for Steam Reforming Flowsheet Model of INEEL Tank Farm Waste

    SciTech Connect

    Taylor, D.D.; Barnes, C.M.; Nichols, T.T.

    2002-05-21

    Technical information is provided herein that is required for development of a steady-state process simulation of a baseline steam reforming treatment train for Tank Farm waste at the Idaho National Engineering and Environmental Laboratory (INEEL). This document supercedes INEEL/EXT-2001-173, produced in FY2001 to support simulation of the direct vitrification treatment train which was the previous process baseline. A process block flow diagram for steam reforming is provided, together with a list of unit operations which constitute the process. A detailed description of each unit operation is given which includes its purpose, principal phenomena present, expected pressure and temperature ranges, key chemical species in the inlet steam, and the proposed manner in which the unit operation is to be modeled in the steady state process simulation. Models for the unit operations may be mechanistic (based on first principles), empirical (based solely on pilot test data without extrapolation) , or by correlations (based on extrapolative or statistical schemes applied to pilot test data). Composition data for the expected process feed streams is provided.

  17. Diesel steam reforming with a nickel-alumina spinel catalyst for solid oxide fuel cell application

    NASA Astrophysics Data System (ADS)

    Fauteux-Lefebvre, Clémence; Abatzoglou, Nicolas; Braidy, Nadi; Achouri, Ines Esma

    Liquid hydrocarbons (LC) are considered as fuel cells feed and, more particularly, as solid oxide fuel cell feed. Cost-effective LC-reforming catalysts are critically needed for the successful commercialization of such technologies. An alternative to noble metal catalysts, proposed by the authors in a previous publication, has been proven efficient for diesel steam reforming (SR). Nickel, less expensive and more readily available than noble metals, was used in a form that prevents deactivation. The catalyst formulation is a Ni-alumina spinel (NiAl 2O 4) supported on alumina (Al 2O 3) and yttria-stabilized zirconia (YSZ). SR of commercial diesel was undertaken for more than 15 h at high gas hourly space velocities and steam-to-carbon ratios lower than 2. Constant diesel conversion and high hydrogen concentrations were obtained. Ni catalyst characterization revealed no detectable amounts of carbon on the spinel catalyst surface Ni. The effect of catalyst composition (Ni concentration and YSZ presence) was studied to understand and optimize the developed catalyst. Two phenomena were found to be influenced by relative catalyst composition: water-gas-shift vs reforming reaction extent, and concentration of light hydrocarbons in products.

  18. Bio-ethanol steam reforming: Insights on the mechanism for hydrogen production

    NASA Astrophysics Data System (ADS)

    Benito, M.; Sanz, J. L.; Isabel, R.; Padilla, R.; Arjona, R.; Daza, L.

    New catalysts for hydrogen production by steam reforming of bio-ethanol have been developed. Catalytic tests have been performed at laboratory scale, with the reaction conditions demanded in a real processor: i.e. ethanol and water feed, without a diluent gas. Catalyst ICP0503 has shown high activity and good resistance to carbon deposition. Reaction results show total conversion, high selectivity to hydrogen (70%), CO 2, CO and CH 4 being the only by-products obtained. The reaction yields 4.25 mol of hydrogen by mol of ethanol fed, close to the thermodynamic equilibrium prediction. The temperature influence on the catalytic activity for this catalyst has been studied. Conversion reaches 100% at temperature higher than 600 °C. In the light of reaction results obtained, a reaction mechanism for ethanol steam reforming is proposed. Long-term reaction experiments have been performed in order to study the stability of the catalytic activity. The excellent stability of the catalyst ICP0503 indicates that the reformed stream could be fed directly to a high temperature fuel cell (MCFC, SOFC) without a further purification treatment. These facts suggest that ICP0503 is a good candidate to be implemented in a bio-ethanol processor for hydrogen production to feed a fuel cell.

  19. Structure and Reactivity Investigations on Supported Bimetallic Au-Ni Catalysts Used for Hydrocarbon Steam Reforming

    SciTech Connect

    Chin, Ya-Huei; King, David L.; Roh, Hyun-Seog; Wang, Yong; Heald, S.

    2006-12-10

    The addition of small quantities of gold to the surface of supported nickel catalysts has been described as a means to retard carbon formation during hydrocarbon steam reforming. Calculations by others have indicated that gold locates at the most catalytically active (step and edge) sites that also serve as nucleation sites for carbon formation. In this paper we describe experiments to characterize the Ni-Au interactions on bimetallic Au-Ni/MgAl2O4 catalysts at various Ni and Au loadings. The catalyst structure was investigated using EXAFS/XANES spectroscopy and adsorption-desorption measurements with H2 and N2O. Evidence for surface alloy formation is provided in the Ni K and Au LIII edge EXAFS measurements of Au-promoted 8.8%Ni/MgAl2O4, especially at Au loadings ?0.2 wt.%. At higher Au concentrations, there is evidence for a combination of alloy and segregated Au species. H2 chemisorption and N2O temperature programmed desorption (TPD) measurements showed a significant decrease in total surface sites, or surface site reactivity, on Au modified Ni/MgAl2O4 catalyst. The XANES structure is consistent with perturbation of the electronic structure of both the Ni and Au atoms as a result of alloy formation. TGA studies with steam/n-butane feed confirmed the ability of Au to retard coke deposition under low S/C reforming conditions, although carbon formation was not fully suppressed. When testing for methane steam reforming, a lower initial activity and deactivation rate resulted from Au promotion of the Ni catalyst. However, both catalysts showed a declining activity with time. The lack of a direct correlation between the surface characterization results and catalytic activity is most likely a result of decreasing effectiveness of the surface alloy with increasing temperature.

  20. Investigation of Fuel Chemistry and Bed Performance in a Fluidized Bed Black Liquor Steam Reformer

    SciTech Connect

    Kevin Whitty

    2007-06-30

    University of Utah's project entitled 'Investigation of Fuel Chemistry and Bed Performance in a Fluidized Bed Black Liquor Steam Reformer' (DOE Cooperative Agreement DE-FC26-02NT41490) was developed in response to a solicitation released by the U.S. Department of Energy in December 2001, requesting proposals for projects targeted towards black liquor/biomass gasification technology support research and development. Specifically, the solicitation was seeking projects that would provide technical support for Department of Energy supported black liquor and biomass gasification demonstration projects under development at the time.

  1. Metal catalysts for steam reforming of tar derived from the gasification of lignocellulosic biomass.

    PubMed

    Li, Dalin; Tamura, Masazumi; Nakagawa, Yoshinao; Tomishige, Keiichi

    2015-02-01

    Biomass gasification is one of the most important technologies for the conversion of biomass to electricity, fuels, and chemicals. The main obstacle preventing the commercial application of this technology is the presence of tar in the product gas. Catalytic reforming of tar appears a promising approach to remove tar and supported metal catalysts are among the most effective catalysts. Nevertheless, improvement of catalytic performances including activity, stability, resistance to coke deposition and aggregation of metal particles, as well as catalyst regenerability is greatly needed. This review focuses on the design and catalysis of supported metal catalysts for the removal of tar in the gasification of biomass. The recent development of metal catalysts including Rh, Ni, Co, and their alloys for steam reforming of biomass tar and tar model compounds is introduced. The role of metal species, support materials, promoters, and their interfaces is described. PMID:25455089

  2. STEAM REFORMING TECHNOLOGY DEMONSTRATION FOR THE DESTRUCTION OF ORGANICS ON ACTUAL DOE SAVANNAH RIVER SITE TANK 48H WASTE 9138

    SciTech Connect

    Burket, P

    2009-02-24

    This paper describes the design of the Bench-scale Steam Reformer (BSR); a processing unit for demonstrating steam reforming technology on actual radioactive waste [1]. It describes the operating conditions of the unit used for processing a sample of Savannah River Site (SRS) Tank 48H waste. Finally, it compares the results from processing the actual waste in the BSR to processing simulant waste in the BSR to processing simulant waste in a large pilot scale unit, the Fluidized Bed Steam Reformer (FBSR), operated at Hazen Research Inc. in Golden, CO. The purpose of this work was to prove that the actual waste reacted in the same manner as the simulant waste in order to validate the work performed in the pilot scale unit which could only use simulant waste.

  3. Kinetics, simulation and optimization of methanol steam reformer for fuel cell applications

    NASA Astrophysics Data System (ADS)

    Choi, Yongtaek; Stenger, Harvey G.

    To evaluate reaction rates for making hydrogen from methanol, kinetic studies of methanol decomposition, methanol steam reforming, the water gas shift reaction, and CO selective oxidation have been performed. These reactions were studied in a microreactor testing unit using a commercial Cu-ZnO/Al 2O 3 catalyst for the first three reactions and Pt-Fe/γ-alumina catalyst for the last reaction. The activity tests were performed between 120 and 325 °C at atmospheric pressure with a range of feed rates and compositions. For methanol decomposition, a simplified reaction network of five elementary reactions was proposed and parameters for all five rate expressions were obtained using non-linear least squares optimization, numerical integration of a one-dimensional PFR model, and extensive experimental data. Similar numerical analysis was carried out to obtain the rate expressions for methanol steam reaction, the water gas shift reaction, and CO selective oxidation. Combining the three reactors with several heat exchange options, an integrated methanol reformer system was designed and simulated using MATLAB. Using this simulation, the product distribution, the effects of reactor volume and temperature, and the options of water and air injection rates were studied. Also, a series of optimization tests were conducted to give maximum hydrogen yield and/or maximum economic profit.

  4. Bimetallic PtSn/C catalysts obtained via SOMC/M for glycerol steam reforming.

    PubMed

    Pastor-Pérez, Laura; Merlo, Andrea; Buitrago-Sierra, Robison; Casella, Mónica; Sepúlveda-Escribano, Antonio

    2015-12-01

    A detailed study on the preparation of bimetallic PtSn/C catalysts using surface-controlled synthesis methods, and on their catalytic performance in the glycerol steam reforming reaction has been carried out. In order to obtain these well-defined bimetallic phases, techniques derived from Surface Organometallic Chemistry on Metals (SOMC/M) were used. The preparation process involved the reaction between an organometallic compound ((C4H9)4Sn) and a supported transition metal (Pt) in a H2 atmosphere. Catalysts with Sn/Pt atomic ratios of 0.2, 0.3, 0.5, and 0.7 were obtained, and characterized using several techniques: ICP, H2 chemisorption, TEM and XPS. These systems were tested in the glycerol steam reforming varying the reaction conditions (glycerol concentration and reaction temperature). The best performance was observed for the catalysts with the lowest tin contents (PtSn0.2/C and PtSn0.3/C). It was observed that the presence of tin increased the catalysts' stability when working under more severe reaction conditions. PMID:26283100

  5. Phase 2 THOR Steam Reforming Tests for Sodium Bearing Waste Treatment

    SciTech Connect

    Nicholas R. Soelberg

    2004-01-01

    About one million gallons of acidic, hazardous, and radioactive sodium-bearing waste is stored in stainless steel tanks at the Idaho Nuclear Technology and Engineering Center (INTEC), which is a major operating facility of the Idaho National Engineering and Environmental Laboratory. Steam reforming is a candidate technology being investigated for converting the waste into a road ready waste form that can be shipped to the Waste Isolation Pilot Plant in New Mexico for interment. A steam reforming technology patented by Studsvik, Inc., and licensed to THOR Treatment Technologies has been tested in two phases using a Department of Energy-owned fluidized bed test system located at the Science Applications International Corporation (SAIC) Science and Technology Applications Research Center located in Idaho Falls, Idaho. The Phase 1 tests were reported earlier in 2003. The Phase 2 tests are reported here. For Phase 2, the process feed rate, stoichiometry, and chemistry were varied to identify and demonstrate process operation and product characteristics under different operating conditions. Two test series were performed. During the first series, the process chemistry was designed to produce a sodium carbonate product. The second series was designed to produce a more leach-resistant, mineralized sodium aluminosilicate product. The tests also demonstrated the performance of a MACT-compliant off-gas system.

  6. Phase 2 TWR Steam Reforming Test for Sodium-Bearing Waste Treatment

    SciTech Connect

    Nicholas R. Soelberg; Doug Marshall; Dean Taylor; Steven Bates

    2004-01-01

    About one million gallons of acidic, hazardous, and radioactive sodium-bearing waste (SBW) is stored in stainless steel tanks a the Idaho Nuclear Technology and Engineering Center (INTEC), which is a major operating facility of the Idaho National Engineering and Environmental Laboratory (INEEL). Steam reforming is a candidate technology being investigated for converting the SBW into a road ready waste form that can be shipped to the Waste Isolation Pilot Plant in New Mexico for interment. Fluidized bed steam reforming technology, licensed to ThermoChem Waste Remediation, LLC (TWR) by Manufacturing Technology Conversion International, was tested in two phases using an INEEL (Department of Energy) fluidized bed test system located at the Science Applications International Corporation (SAIC) Science and Technology Applications Research Center in Idaho Falls, Idaho. The Phase 1 tests were reported earlier. The Phase 2 tests are reported here. For Phase 2, the process feed rate, reductant stoichiometry, and process temperature were varied to identify and demonstrate how the process might be optimized to improve operation and product characteristics. The first week of testing was devoted primarily to process chemistry and the second week was devoted more toward bed stability and particle size control.

  7. Characterization of the activity and stability of supported cobalt catalysts for the steam reforming of ethanol

    NASA Astrophysics Data System (ADS)

    Batista, Marcelo S.; Santos, Rudye K. S.; Assaf, Elisabete M.; Assaf, José M.; Ticianelli, Edson A.

    This paper reports results of studies of the catalytic activity and stability of supported cobalt catalysts for steam reforming of ethanol. Co/Al 2O 3, Co/SiO 2, and Co/MgO catalysts were prepared by an impregnation method and characterized by X-ray diffraction, atomic absorption spectroscopy, Raman spectroscopy, and temperature programmed reduction with hydrogen. The results showed the presence of Co 3O 4 and CoO x species interacting with Al 2O 3 or MgO and formed after a calcination step. It was evident that only Co 0 sites are active for the steam reforming of ethanol. All materials showed high levels of ethanol conversion, with molar yields of about 70% of hydrogen and 30% of CO+CO 2+CH 4 in the gaseous mixture. The Co/Al 2O 3 catalyst also produced ethylene through a dehydration reaction of ethanol. It is proposed that the methane formation on Co/SiO 2 catalysts occurs by methanation of CO and by ethanol decomposition. After 9 h of reaction, 14-24% (w/w) of carbon was deposited on all catalysts, indicating that a well characterized deactivation of the materials is due to coke deposition.

  8. Steam Reforming Application for Treatment of DOE Sodium Bearing Tank Wastes at INL for ICP

    SciTech Connect

    J. Bradley Mason; Kevin Ryan; Scott Roesener; Michael Cowen; Duane Schmoker; Pat Bacala; Bill Landman

    2006-03-01

    The patented THOR® steam reforming waste treatment technology has been selected as the technology of choice for treatment of Sodium Bearing Waste (SBW) at the Idaho National Laboratory (INL) for the Idaho Cleanup Project (ICP). SBW is an acidic tank waste at the Idaho Nuclear Technology and Engineering Center (INTEC) at INL. It consists primarily of waste from decontamination activities and laboratory wastes. SBW contains high concentrations of nitric acid, alkali and aluminum nitrates, with minor amounts of many inorganic compounds including radionuclides, mainly cesium and strontium. The THOR® steam reforming process will convert the SBW tank waste feed into a dry, solid, granular product. The THOR® technology was selected to treat SBW, in part, because it can provide flexible disposal options to accommodate the final disposition path selected for SBW. THOR® can produce a final end-product that will meet anticipated requirements for disposal as Remote-Handled TRU (RH-TRU) waste; and, with modifications, THOR® can also produce a final endproduct that could be qualified for disposal as High Level Waste (HLW). SBW treatment will be take place within the Integrated Waste Treatment Unit (IWTU), a new facility that will be located at the INTEC. This paper provides an overview of the THOR® process chemistry and process equipment being designed for the IWTU.

  9. Non-syngas direct steam reforming of methanol to hydrogen and carbon dioxide at low temperature.

    PubMed

    Yu, Kai Man Kerry; Tong, Weiyi; West, Adam; Cheung, Kevin; Li, Tong; Smith, George; Guo, Yanglong; Tsang, Shik Chi Edman

    2012-01-01

    A non-syngas direct steam reforming route is investigated for the conversion of methanol to hydrogen and carbon dioxide over a CuZnGaO(x) catalyst at 150-200 °C. This route is in marked contrast with the conventional complex route involving steam reformation to syngas (CO/H2) at high temperature, followed by water gas shift and CO cleanup stages for hydrogen production. Here we report that high quality hydrogen and carbon dioxide can be produced in a single-step reaction over the catalyst, with no detectable CO (below detection limit of 1 ppm). This can be used to supply proton exchange membrane fuel cells for mobile applications without invoking any CO shift and cleanup stages. The working catalyst contains, on average, 3-4 nm copper particles, alongside extremely small size of copper clusters stabilized on a defective ZnGa2O4 spinel oxide surface, providing hydrogen productivity of 393.6 ml g(-1)-cat h(-1) at 150 °C. PMID:23187630

  10. Methanol steam reforming in microreactor with constructal tree-shaped network

    NASA Astrophysics Data System (ADS)

    Chen, Yongping; Zhang, Chengbin; Wu, Rui; Shi, Mingheng

    2011-08-01

    The construcal tree-shaped network is introduced into the design of a methanol steam microreactor in the context of optimization of the flow configuration. A three-dimensional model for methanol steam reaction in this designed microreactor is developed and numerically analyzed. The methanol conversion, CO concentration in the product and the total pressure drop of the gases in the microreactor with constructal tree-shaped network are evaluated and compared with those in the serpentine reactor. It is found that the reaction of methanol steam reforming is enhanced in the constructal tree-shaped microreactor, since the tree-shaped reactor configuration, which acts an optimizer for the reactant distribution, provides a reaction space with larger surface-to-volume ratio and the reduction of reactant velocities in the branches. Compared with the serpentine microreactor, the constructal reactor possesses a higher methanol conversion rate accompanied with a higher CO concentration. The conversion rate of the constructal microreactor is more than 10% over that of serpentine reactor. More particularly, the reduction of flow distance makes the constructal microreactor still possess almost the same pressure drop as the corresponding serpentine reactor, despite that the bifurcations induce extra local pressure loss, and the reduction of channel size in branches also causes pressure losses.

  11. Engineering Study for a Full Scale Demonstration of Steam Reforming Black Liquor Gasification at Georgia-Pacific's Mill in Big Island, Virginia

    SciTech Connect

    Robert De Carrera; Mike Ohl

    2002-03-19

    Georgia-Pacific Corporation performed an engineering study to determine the feasibility of installing a full-scale demonstration project of steam reforming black liquor chemical recovery at Georgia-Pacific's mill in Big Island, Virginia. The technology considered was the Pulse Enhanced Steam Reforming technology that was developed and patented by Manufacturing and Technology Conversion, International (MTCI) and is currently licensed to StoneChem, Inc., for use in North America. Pilot studies of steam reforming have been carried out on a 25-ton per day reformer at Inland Container's Ontario, California mill and on a 50-ton per day unit at Weyerhaeuser's New Bern, North Carolina mill.

  12. Hydrogen generation for fuel-cell power systems by high-pressure catalytic methanol-steam reforming

    SciTech Connect

    Peppley, B.A.; Amphlett, J.C.; Kearns, L.M.; Mann, R.F.; Roberge, P.R.

    1997-12-31

    Results of kinetic studies of methanol-steam reforming on a commercial low-temperature shift catalyst, BASF K3-110, are reported. A comprehensive Langmuir-Hinshelwood kinetic model of methanol-steam reforming on Cu/ZnO/Al{sub 2}O{sub 3} catalyst was used to simulate a methanol-steam reformer operating at pressures up to 45 bar. At constant temperature and steam-to-methanol ratio, increasing the pressure results in an increase in the initial rate of the reaction and a corresponding improvement in reformer performance. This is partially offset as the equilibrium conversion decreases with increasing pressure. The rate of reaction is highest at low conversion. The result is that there is a large heat demand near the entrance of the catalyst bed which causes a strong endothermic effect and a corresponding temperature minimum. In the worst case, this temperature minimum can be below the dewpoint temperature of the operating fluid causing a loss in reformer performance due to condensation in the pores of the catalyst. The situation is exacerbated by the potential for thermal damage to other regions of the catalyst bed if the heating temperature is increased to overcome the endothermic effect. Catalyst deactivation at elevated pressures was also studied in an 80 hour experiment at 260 C. Increasing the operating pressure did not accelerate the rate of deactivation for the typical gas compositions encountered during normal reformer operation. No catalyst fouling was observed for experimental pressures as high as 40 bar at steam-to-methanol ratios greater than unity even though the tendency for carbon formation increases with pressure. Catalyst selectivity improved at lower conversion due to kinetic effects. The equilibrium CO concentration, however, does not vary significantly with pressure because of the stoichiometry of the water-gas shift reaction.

  13. Steam Reforming of Ethylene Glycol over MgAl₂O₄ Supported Rh, Ni, and Co Catalysts

    SciTech Connect

    Mei, Donghai; Lebarbier, Vanessa M.; Xing, Rong; Albrecht, Karl O.; Dagle, Robert A.

    2015-11-25

    Steam reforming of ethylene glycol (EG) over MgAl₂O₄ supported metal (15 wt.% Ni, 5 wt.% Rh, and 15 wt.% Co) catalysts were investigated using combined experimental and theoretical methods. Compared to highly active Rh and Ni catalysts with 100% conversion, the steam reforming activity of EG over the Co catalyst is comparatively lower with only 42% conversion under the same reaction conditions (500°C, 1 atm, 119,000 h⁻¹, S/C=3.3 mol). However, CH₄ selectivity over the Co catalyst is remarkably lower. For example, by varying the gas hour space velocity (GHSV) such that complete conversion is achieved for all the catalysts, CH₄ selectivity for the Co catalyst is only 8%, which is much lower than the equilibrium CH₄ selectivity of ~ 24% obtained for both the Rh and Ni catalysts. Further studies show that varying H₂O concentration over the Co catalyst has a negligible effect on activity, thus indicating zero-order dependence on H₂O. These experimental results suggest that the supported Co catalyst is a promising EG steam reforming catalyst for high hydrogen production. To gain mechanistic insight for rationalizing the lower CH₃ selectivity observed for the Co catalyst, the initial decomposition reaction steps of ethylene glycol via C-O, O-H, C-H, and C-C bond scissions on the Rh(111), Ni(111) and Co(0001) surfaces were investigated using density functional theory (DFT) calculations. Despite the fact that the bond scission sequence in the EG decomposition on the three metal surfaces varies, which leads to different reaction intermediates, the lower CH₄ selectivity over the Co catalyst, as compared to the Rh and Ni catalysts, is primarily due to the higher barrier for CH₄ formation. The higher S/C ratio enhances the Co catalyst stability, which can be elucidated by the facile water dissociation and an alternative reaction path to remove the CH species as a coking precursor via the HCOH formation. This work was financially supported by the United

  14. Fluidized Bed Steam Reforming of INEEL SBW Using THORsm Mineralizing Technology

    SciTech Connect

    Arlin L. Olson; Nicholas R. Soelberg; Douglas W. Marshall; Gary L. Anderson

    2004-12-01

    Sodium bearing waste (SBW) disposition is one of the U.S. Department of Energy (DOE) Idaho Operation Office’s (NE-ID) and State of Idaho’s top priorities at the Idaho National Engineering and Environmental Laboratory (INEEL). Many studies have resulted in the identification of five treatment alternatives that form a short list of perhaps the most appropriate technologies for the DOE to select from. The alternatives are (a) calcination with maximum achievable control technology (MACT) upgrade, (b) steam reforming, (c) cesium ion exchange (CsIX) with immobilization, (d) direct evaporation, and (e) vitrification. Each alternative has undergone some degree of applied technical development and preliminary process design over the past four years. DOE desired further experimental data, with regard to steam reforming technology, to make informed decisions concerning selection of treatment technology for SBW. Mineralizing steam reforming technology, offered by THOR Treatment Technologies, LLC would produce a denitrated, granular mineral waste form using a high-temperature fluidized bed process. A pilot scale demonstration of the technology was performed in a 15-cm-diameter reactor vessel September 27 through October 1, 2004. The pilot scale equipment is owned by the DOE, and located at the Science and Technology Applications Research (STAR) Center in Idaho Falls, ID. Flowsheet chemistry and operational parameters were defined through a collaborative effort involving Idaho National Engineering and Environmental Laboratory, Savannah River National Laboratory (SRNL), and THOR Treatment Technologies personnel. Personnel from Science Applications International Corporation, owners of the STAR Center, operated the pilot plant. The pilot scale test was terminated as planned after achieving a total of 100 hrs of cumulative/continuous processing operation. About 230 kg of SBW surrogate were processed that resulted in about 88 kg of solid product, a mass reduction of about 62

  15. Hydrogen Production by Low-temperature Steam Reforming of Bio-oil over Ni/HZSM-5 Catalyst

    NASA Astrophysics Data System (ADS)

    Qiu, Song-bai; Gong, Lu; Liu, Lu; Hong, Cheng-gui; Yuan, Li-xia; Li, Quan-xin

    2011-04-01

    We investigated high catalytic activity of Ni/HZSM-5 catalysts synthesized by the impregnation method, which was successfully applied for low-temperature steam reforming of bio-oil. The influences of the catalyst composition, reforming temperature and the molar ratio of steam to carbon fed on the stream reforming process of bio-oil over the Ni/HZSM-5 catalysts were investigated in the reforming reactor. The promoting effects of current passing through the catalyst on the bio-oil reforming were also studied using the electrochemical catalytic reforming approach. By comparing Ni/HZSM-5 with commonly used Ni/Al2O3 catalysts, the Ni20/ZSM catalyst with Ni-loading content of about 20% on the HZSM-5 support showed the highest catalytic activity. Even at 450 °C, the hydrogen yield of about 90% with a near complete conversion of bio-oil was obtained using the Ni20/ZSM catalyst. It was found that the performance of the bio-oil reforming was remarkably enhanced by the HZSM-5 supporter and the current through the catalyst. The features of the Ni/HZSM-5 catalysts were also investigated via X-ray diffraction, inductively coupled plasma and atomic emission spectroscopy, hydrogen temperature-programmed reduction, and Brunauer-Emmett-Teller methods.

  16. An attempt to minimize the temperature gradient along a plug-flow methane/steam reforming reactor by adopting locally controlled heating zones

    NASA Astrophysics Data System (ADS)

    Mozdzierz, M.; Brus, G.; Sciazko, A.; Komatsu, Y.; Kimijima, S.; Szmyd, J. S.

    2014-08-01

    Plug flow reactors are very common in the chemical process industry, including methane/steam reforming applications. Their operation presents many challenges, such as a strong dependence of temperature and composition distribution on the inlet conditions. The strongly endothermic methane/steam reforming reaction might result in a temperature drop at the inlet of the reactor and consequently the occurrence of large temperature gradients. The strongly non-uniform temperature distribution due to endothermic chemical reaction can have tremendous consequences on the operation of the reactor, such as catalyst degradation, undesired side reactions and thermal stresses. To avoid such unfavorable conditions, thermal management of the reactor becomes an important issue. To carry out thermal management properly, detailed modeling and corresponding numerical analyses of the phenomena occurring inside the reforming system is required. This paper presents experimental and numerical studies on the methane/steam reforming process inside a plug-flow reactor. To optimize the reforming reactors, detailed data about the entire reforming process is required. In this study the kinetics of methane/steam reforming on the Ni/YSZ catalyst was experimentally investigated. Measurements including different thermal boundary conditions, the fuel flow rate and the steam- to-methane ratios were performed. The reforming rate equation derived from experimental data was used in the numerical model to predict gas composition and temperature distribution along the steam-reforming reactor. Finally, an attempt was made to control the temperature distribution by adopting locally controlled heating zones.

  17. Fluidized bed steam reformed mineral waste form performance testing to support Hanford Supplemental Low Activity Waste Immobilization Technology Selection

    SciTech Connect

    Jantzen, C. M.; Pierce, E. M.; Bannochie, C. J.; Burket, P. R.; Cozzi, A. D.; Crawford, C. L.; Daniel, W. E.; Fox, K. M.; Herman, C. C.; Miller, D. H.; Missimer, D. M.; Nash, C. A.; Williams, M. F.; Brown, C. F.; Qafoku, N. P.; Neeway, J. J.; Valenta, M. M.; Gill, G. A.; Swanberg, D. J.; Robbins, R. A.; Thompson, L. E.

    2015-10-01

    This report describes the benchscale testing with simulant and radioactive Hanford Tank Blends, mineral product characterization and testing, and monolith testing and characterization. These projects were funded by DOE EM-31 Technology Development & Deployment (TDD) Program Technical Task Plan WP-5.2.1-2010-001 and are entitled “Fluidized Bed Steam Reformer Low-Level Waste Form Qualification”, Inter-Entity Work Order (IEWO) M0SRV00054 with Washington River Protection Solutions (WRPS) entitled “Fluidized Bed Steam Reforming Treatability Studies Using Savannah River Site (SRS) Low Activity Waste and Hanford Low Activity Waste Tank Samples”, and IEWO M0SRV00080, “Fluidized Bed Steam Reforming Waste Form Qualification Testing Using SRS Low Activity Waste and Hanford Low Activity Waste Tank Samples”. This was a multi-organizational program that included Savannah River National Laboratory (SRNL), THOR® Treatment Technologies (TTT), Pacific Northwest National Laboratory (PNNL), Oak Ridge National Laboratory (ORNL), Office of River Protection (ORP), and Washington River Protection Solutions (WRPS). The SRNL testing of the non-radioactive pilot-scale Fluidized Bed Steam Reformer (FBSR) products made by TTT, subsequent SRNL monolith formulation and testing and studies of these products, and SRNL Waste Treatment Plant Secondary Waste (WTP-SW) radioactive campaign were funded by DOE Advanced Remediation Technologies (ART) Phase 2 Project in connection with a Work-For-Others (WFO) between SRNL and TTT.

  18. A Ni@ZrO2 nanocomposite for ethanol steam reforming: enhanced stability via strong metal-oxide interaction.

    PubMed

    Li, Shuirong; Zhang, Chengxi; Huang, Zhiqi; Wu, Gaowei; Gong, Jinlong

    2013-05-14

    This communication describes the synthesis of a nanocomposite Ni@ZrO2 catalyst with enhanced metal-support interaction by introducing metal nanoparticles into the framework of the oxide support. The catalyst shows high catalytic activity and stability for hydrogen production via steam reforming of ethanol. PMID:23124111

  19. Superior reactivity of skeletal Ni-based catalysts for low-temperature steam reforming to produce CO-free hydrogen.

    PubMed

    Zhang, Chengxi; Zhang, Peng; Li, Shuirong; Wu, Gaowei; Ma, Xinbin; Gong, Jinlong

    2012-03-14

    This paper describes the utilization of skeletal Ni-based catalysts for steam reforming of ethanol to produce CO-free hydrogen, which could be superior in the application of fuel cells. Assistant metals play different roles in the reaction; Pt and Cu suppress the methanation and enhance H(2) production, while Co promotes the methanation. PMID:22297434

  20. Steam reforming of glycerol for hydrogen production over supported nickel catalysts on alumina.

    PubMed

    Choi, Ga Young; Kim, Young Chul; Moon, Dong Ju; Seo, Gon; Park, Nam Cook

    2013-01-01

    The experiment was carried out to produce hydrogen through steam reforming of glycerol over nano-sized Ni catalysts supported on alumina (Al2O3). The catalysts were characterized by BET surface area, metal dispersion, XRD, TPR, NH3-TPD and SEM. 15 wt% Ni/Al2O3 catalysts presented carbon nano fiber after the catalyst was used. However, when the Ni loading was higher than that of 15 wt%, the catalytic activity reduced, and the increase of the Ni particle size and the formation of graphitic carbon occurred. The Ni/SiO2(70)-Al2O3 with the high surface area and the small Ni particle size promoted the catalytic activity and could easily reduce from NiO to Ni, inhibiting the formation of NiAl2O4. PMID:23646792

  1. MTCI/ThermoChem steam reforming process for solid fuels for combined cycle power generation

    SciTech Connect

    Mansour, M.N.; Voelker, G.; Dural-Swamy, K.

    1995-12-31

    Manufacturing and Technology Conversion International, Inc. (MTCI) has developed a novel technology to convert solid fuels including biomass, coal, municipal solid waste (MSW) and wastewater sludges into usable syngas by steam reforming in an indirectly heated, fluid-bed reactor. MTCI has licensed and patented the technology to ThermoChem, Inc. Both MTCI and ThermoChem have built two modular commercial-scale demonstration units: one for recycle paper mill rejects (similar to refuse-derived fuel [RDF]), and another for chemical recovery of black liquor. ThermoChem has entered into an agreement with Ajinkyatara Cooperative Sugar Factory, India, for building a 10 MW combined cycle power generation facility based on bagasse and agro-residue gasification.

  2. Stable hydrogen production by methane steam reforming in a two zone fluidized bed reactor: Experimental assessment

    NASA Astrophysics Data System (ADS)

    Pérez-Moreno, L.; Soler, J.; Herguido, J.; Menéndez, M.

    2013-12-01

    The Two Zone Fluidized Bed Reactor concept is proposed for hydrogen production via the steam reforming of methane (SRM) including integrated catalyst regeneration. In order to study the effect of the contact mode, the oxidative SRM has been carried out over a Ni/Al2O3 catalyst using a fixed bed reactor (fBR), a conventional fluidized-bed reactor (FBR) and the proposed two-zone fluidized bed reactor (TZFBR). The technical feasibility of these reactors has been studied experimentally, investigating their performance (CH4 conversion, CO and H2 selectivity, and H2 global yield) and stability under different operating conditions. Coke generation in the process has been verified by several techniques. A stable performance was obtained in the TZFBR, where coke formation was counteracted with continuous catalyst regeneration. The viability of the TZFBR for carrying out this process with a valuable global yield to hydrogen is demonstrated.

  3. Radioactive Demonstrations Of Fluidized Bed Steam Reforming (FBSR) With Hanford Low Activity Wastes

    SciTech Connect

    Jantzen, C. M.; Crawford, C. L.; Burket, P. R.; Bannochie, C. J.; Daniel, W. G.; Nash, C. A.; Cozzi, A. D.; Herman, C. C.

    2012-10-22

    Several supplemental technologies for treating and immobilizing Hanford low activity waste (LAW) are being evaluated. One immobilization technology being considered is Fluidized Bed Steam Reforming (FBSR) which offers a low temperature (700-750?C) continuous method by which wastes high in organics, nitrates, sulfates/sulfides, or other aqueous components may be processed into a crystalline ceramic (mineral) waste form. The granular waste form produced by co-processing the waste with kaolin clay has been shown to be as durable as LAW glass. The FBSR granular product will be monolithed into a final waste form. The granular component is composed of insoluble sodium aluminosilicate (NAS) feldspathoid minerals such as sodalite. Production of the FBSR mineral product has been demonstrated both at the industrial, engineering, pilot, and laboratory scales on simulants. Radioactive testing at SRNL commenced in late 2010 to demonstrate the technology on radioactive LAW streams which is the focus of this study.

  4. Steam reforming of glycerol over Pt-MCM-41 synthesized in a one-step process

    NASA Astrophysics Data System (ADS)

    Zhang, Xiao-Hui; Yan, Feng-Wen; Guo, Cun-Yue; Yuan, Guo-Qing

    2012-12-01

    Pt-MCM-41 materials were synthesized by a simple method via simultaneous self-assembling and Pt incorporation using cetyltrimethylammonium chloride (CTAC) as a structure directing agent. Structural characterization of the sample was carried out by N2 sorption, XRD and TEM measurements. The highly ordered structure of MCM-41 was not appreciably affected by the formation of the Pt particles. Unlike related results, the Pt nanoparticles were incorporated into the mesopores and embedded into the pore walls as framework. The Pt-MCM-41 sample was tested as a catalyst in the steam reforming of glycerol in which it exhibited moderate activity, high selectivity to hydrogen, and very low selectivity to light alkanes.

  5. Cu-Al spinel oxide as an efficient catalyst for methanol steam reforming.

    PubMed

    Xi, Hongjuan; Hou, Xiaoning; Liu, Yajie; Qing, Shaojun; Gao, Zhixian

    2014-10-27

    Cu-Al spinel oxide, which contains a small portion of the CuO phase, has been successfully used in methanol steam reforming (MSR) without prereduction. The omission of prereduction not only avoids the copper sintering prior to the catalytic reaction, but also slows down the copper-sintering rate in MSR. During this process, the CuO phase can initiate MSR at a lower temperature, and CuAl2O4 releases active copper gradually. The catalyst CA2.5-900, calcined at 900 °C with n(Al)/n(Cu) = 2.5, has a higher CuAl2O4 content, higher BET surface area, and smaller CuAl2O4 crystal size. Its activity first increases and then decreases during MSR. Furthermore, both fresh and regenerated CA2.5-900 showed better catalytic performance than the commercial Cu-Zn-Al catalyst. PMID:25213737

  6. Steam Reforming, 6-in. Bench-Scale Design and Testing Project -- Technical and Functional Requirements Description

    SciTech Connect

    Losinski, Sylvester John; Marshall, Douglas William

    2002-08-01

    Feasibility studies and technology development work are currently being performed on several processes to treat radioactive liquids and solids currently stored at the Idaho Nuclear Technology and Engineering Center (INTEC), located within the Idaho National Engineering and Environmental Laboratory (INEEL). These studies and development work will be used to select a treatment process for treatment of the radioactive liquids and solids to meet treatment milestones of the Settlement Agreement between the Department of Energy and the State of Idaho. One process under consideration for treating the radioactive liquids and solids, specifically Sodium-Bearing Waste (SBW) and tank heel solids, is fluid bed steam reforming (FBSR). To support both feasibility and development studies a bench-scale FBSR is being designed and constructed. This report presents the technical and functional requirements, experimental objectives, process flow sheets, and equipment specifications for the bench-scale FBSR.

  7. Disposition of Tank 48H Organics by Fluidized Bed Steam Reforming (FBSR)

    SciTech Connect

    Jantzen, C.M.

    2003-12-02

    In order to make space in the Savannah River Site Tank farm, the Tank 48H waste must be removed. Therefore, the Tank 48H waste must be processed to reduce or eliminate levels of nitrates, nitrites, and sodium tetraphenyl borate in order to reduce impacts of these species before it is vitrified. Fluidized Bed Steam Reforming is being considered as a candidate technology for destroying the nitrates and the NaTPB prior to melting. The Idaho National Engineering and Environmental Laboratory was tasked to perform a proof-of-concept steam reforming test to evaluate the technical feasibility for pretreating the Tank 48H waste. The crucible (bench scale) tests conducted at the Savannah River Technology Center were initiated to optimize and augment the parameters subsequently tested at the pilot scale at INEEL. The purposes of the current study, organic destruction and downstream processing of T48H waste slurry were fulfilled. TPB was destroyed in all 19 samples tested with the simulated FB SR process at operational temperatures 650-725 degrees Celsius. A test temperature of 650 degrees Celsius optimized NO3 destruction during the formation of an Na2CO3 FBSR product. A test temperature of 725 degrees Celsius optimized NO3 destruction during formation of a sodium silicate FBSR product. Destruction of nitrate at greater than 99 per cent was achieved with addition of sugar as a reductant at 1X stoichiometry and total organic carbon analyses indicated that excess reductant was not present in the FBSR product. The use of sugar at 1X stoichiometry appears to ensure that excess reductant is not contained in the FBSR product that would alter the REDuction/OXidation equilibrium of the DWPF melter, while simultaneously assuring that NO3 is destroyed adequately. Destruction of antifoam with the simulated FBSR process was also achieved at operating temperatures between 650-725 degrees Celsius. based on measured total organic carbon.

  8. Radioactive Bench-scale Steam Reformer Demonstration of a Monolithic Steam Reformed Mineralized Waste Form for Hanford Waste Treatment Plant Secondary Waste - 12306

    SciTech Connect

    Evans, Brent; Olson, Arlin; Mason, J. Bradley; Ryan, Kevin; Jantzen, Carol; Crawford, Charles

    2012-07-01

    Hanford currently has 212,000 m{sup 3} (56 million gallons) of highly radioactive mixed waste stored in the Hanford tank farm. This waste will be processed to produce both high-level and low-level activity fractions, both of which are to be vitrified. Supplemental treatment options have been under evaluation for treating portions of the low-activity waste, as well as the liquid secondary waste from the low-activity waste vitrification process. One technology under consideration has been the THOR{sup R} fluidized bed steam reforming process offered by THOR Treatment Technologies, LLC (TTT). As a follow-on effort to TTT's 2008 pilot plant FBSR non-radioactive demonstration for treating low-activity waste and waste treatment plant secondary waste, TTT, in conjunction with Savannah River National Laboratory, has completed a bench scale evaluation of this same technology on a chemically adjusted radioactive surrogate of Hanford's waste treatment plant secondary waste stream. This test generated a granular product that was subsequently formed into monoliths, using a geo-polymer as the binding agent, that were subjected to compressibility testing, the Product Consistency Test and other leachability tests, and chemical composition analyses. This testing has demonstrated that the mineralized waste form, produced by co-processing waste with kaolin clay using the TTT process, is as durable as low-activity waste glass. Testing has shown the resulting monolith waste form is durable, leach resistant, and chemically stable, and has the added benefit of capturing and retaining the majority of Tc-99, I-129, and other target species at high levels. (authors)

  9. Process for alternately steam reforming sulfur containing hydrocarbons that vary in oxygen content

    SciTech Connect

    Lesieur, R.R.; Setzer, H.J.; Hawkins, J.R.

    1980-01-01

    In the hydrotreating and steam reforming of an oxygen and sulfur bearing hydrocarbon fuel, the oxygen is first removed in an oxidizer containing a bed of platinum catalyst, the inlet temperature being well below 1000/sup 0/F and preferably on the order of 300/sup 0/F. The sulfur in the fuel does not harm the oxidizer catalyst and may be removed downstream by known hydrodesulfurization techniques prior to reforming. A process is described for removing oxygen from an oxygen and sulfur bearing hydrocarbon fuel, such as peak shared natural gas, upstream in the process so that sulfur can be removed later. The fuel and some hydrogen are introduced into an oxidizer at a temperature of 350/sup 0/F or less down to the minimum ignition temperature. The oxidizer consists of a platinum bed catalyst which catalyzes the oxidation of the oxygen to water with accompanying heat release to raise the exit gas temperature to less than 650/sup 0/F. The temperature desorbs the sulfur from the catalyst, and the exit gases are passed downstream to nickel subsulfide or molybdenum desfulfide catalysts where the hydrosulfurization process takes place. (BLM)

  10. Synthesis of highly efficient CaO-based, self-stabilizing CO2 sorbents via structure-reforming of steel slag.

    PubMed

    Tian, Sicong; Jiang, Jianguo; Yan, Feng; Li, Kaimin; Chen, Xuejing

    2015-06-16

    Capturing anthropogenic CO2 in a cost-effective and highly efficient manner is one of the most challenging issues faced by scientists today. Herein, we report a novel structure-reforming approach to convert steel slag, a cheap, abundant, and nontoxic calcium-rich industrial waste, as the only feedstock into superior CaO-based, self-stabilizing CO2 sorbents. The CO2 capture capacity of all the steel slag-derived sorbents was improved more than 10-fold compared to the raw slag, with the maximum uptake of CO2 achieving at 0.50 gCO2 gsorbent(-1). Additionally, the initial steel slag-derived sorbent could retain 0.25 gCO2 gsorbent(-1), that is, a decay rate of only 12% over 30 carbonation-calcination cycles, the excellent self-stabilizing property allowed it to significantly outperform conventional CaO, and match with most of the existing synthetic CaO-based sorbents. A synergistic effect that facilitated CO2 capture by CaO-based sorbents was clearly recognized when Mg and Al, the most common elements in steel slag, coexisted with CaO in the forms of MgO and Al2O3, respectively. During the calcium looping process, MgO served as a well spacer to increase the porosity of sorbents together with Al2O3 serving as a durable stabilizer to coresist the sintering of CaCO3 grains at high temperatures. PMID:25961319

  11. Twenty kW fuel cell units of compact design. Part 5: Hydrogen production by steam reforming of methanol

    NASA Astrophysics Data System (ADS)

    Grave, B.

    1980-09-01

    To assess its potential use in alkaline fuel cells, The production of hydrogen by steam reforming of methanol was studied analytically and experimentally. The reformer, the converter, and the purification system of a prototype installation were designed and the optimal operation parameters derived and experimentally confirmed. For comparison, hydrogen production by ammonia cracking was also studied. An estimate of the manufacturing costs for a fuel cell aggregate of 20 kW indicates economical operation only to be possible at very high duty cycles. As a result the project was terminated.

  12. Development of Technologies on Innovative Simplified Nuclear Power Plant Using High-Efficiency Steam Injectors (10) Application to a Small District-Heating Reactor

    SciTech Connect

    Tadashi Narabayashi; Yoichiro Shimadu; Toshiiro Murase; Masatoshi Nagai; Michitsugu Mori; Shuichi Ohmori

    2006-07-01

    A steam injector (SI) is a simple, compact and passive pump and also acts as a high-performance direct-contact compact heater. This provides SI with capability to use as a passive ECCS pump and also as a direct-contact feedwater heater that heats up feedwater by using extracted steam from the turbine. In order to develop a high reliability passive ECCS pump and a compact feedwater heater, it is necessary to quantify the characteristics between physical properties of the flow field. We carried out experiments to observe the internal behavior of the water jet as well as measure the velocity of steam jet using a laser Doppler velocimetry. Its performance depends on the phenomena of steam condensation onto the water jet surface and heat transfer in the water jet due to turbulence on to the phase-interface. The analysis was also conducted by using a CFD code with the separate two-phase flow models. With regard to the simplified feed-water system, size of four-stage SI system is almost the same as the model SI that had done the steam and water test that pressures were same as that of current ABWR. The authors also conducted the hot water supply system test in the snow for a district heating. With regard to the SI core cooling system, the performance tests results showed that the low-pressure SI core cooling system will decrease the PCT to almost the same as the saturation temperature of the steam pressure in a pressure vessel. As it is compact equipment, SI is expected to bring about great simplification and materials-saving effects, while its simple structure ensures high reliability of its operation, thereby greatly contributing to the simplification of the power plant for not only an ABWR power plant but also a small PWR/ BWR for district heating system. (authors)

  13. Fluidized Bed Steam Reformed (FBSR) Mineral Waste Forms: Characterization and Durability Testing

    SciTech Connect

    Jantzen, Carol M.; Lorier, Troy H.; Pareizs, John M.; Marra, James C.

    2007-07-01

    Fluidized Bed Steam Reforming (FBSR) is being considered as a mineralizing technology for the immobilization of a wide variety of wastes that are high in organics, nitrates-nitrites, halides, and/or sulfates. These wastes include the decontaminated High Level Waste (HLW) supernates referred to as low activity waste (LAW) at Department of Energy (DOE) sites in the United States and waste streams that may be generated by the advanced nuclear fuel cycle flowsheets that are being considered by the Global Nuclear Energy Partnership (GNEP) initiative. The organics are pyrolyzed into CO{sub 2} and steam in the absence of air. The FBSR mineral waste form is a granular but can subsequently be made into a monolith for disposal if necessary. The waste form is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals (sodalite, nosean, and nepheline) with cage and ring structures that sequester radionuclides like Tc-99 and Cs-137 and anions such as SO{sub 4}, I, F, and Cl. Iron bearing spinel minerals are also formed and these phases stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Dissolution rates ({eta}) and activation energies of dissolution are parameters needed for Performance Assessments (PA) to be completed on the FBSR mineral waste form. These parameters are defined in this study by Single Pass Flow Through (SPFT) testing. The dissolution rate ({eta}) and the activation energies for dissolution calculated in this study agree with the available rate and activation energy data for natural single crystal nepheline. (authors)

  14. FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING

    SciTech Connect

    Jantzen, C; Troy Lorier, T; John Pareizs, J; James Marra, J

    2006-12-06

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium low activity wastes (LAW) such as those existing at the Hanford site, at the Idaho National Laboratory (INL), and the Savannah River Site (SRS). The addition of clay, charcoal, and a catalyst as co-reactants with the waste denitrates the aqueous wastes and forms a granular mineral waste form that can subsequently be made into a monolith for disposal if necessary. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage and ring structures and iron bearing spinel minerals. The mineralization occurs at moderate temperatures between 650-750 C in the presence of superheated steam. The cage and ring structured feldspathoid minerals atomically bond radionuclides like Tc-99 and Cs-137 and anions such as SO{sub 4}, I, F, and Cl. The spinel minerals stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium bearing waste (SBW) in pilot scale facilities at the Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The results of the SPFT testing and the activation energies for dissolution are discussed in this study.

  15. FLUIDIZED BED STEAM REFORMED MINERAL WASTE FORMS: CHARACTERIZATION AND DURABILITY TESTING

    SciTech Connect

    Jantzen, C; Troy Lorier, T; John Pareizs, J; James Marra, J

    2007-03-31

    Fluidized Bed Steam Reforming (FBSR) is being considered as a potential technology for the immobilization of a wide variety of high sodium low activity wastes (LAW) such as those existing at the Hanford site, at the Idaho National Laboratory (INL), and the Savannah River Site (SRS). The addition of clay, charcoal, and a catalyst as co-reactants with the waste denitrates the aqueous wastes and forms a granular mineral waste form that can subsequently be made into a monolith for disposal if necessary. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage and ring structures and iron bearing spinel minerals. The mineralization occurs at moderate temperatures between 650-750 C in the presence of superheated steam. The cage and ring structured feldspathoid minerals atomically bond radionuclides like Tc-99 and Cs-137 and anions such as SO4, I, F, and Cl. The spinel minerals stabilize Resource Conservation and Recovery Act (RCRA) hazardous species such as Cr and Ni. Granular mineral waste forms were made from (1) a basic Hanford Envelope A low-activity waste (LAW) simulant and (2) an acidic INL simulant commonly referred to as sodium bearing waste (SBW) in pilot scale facilities at the Science Applications International Corporation (SAIC) Science and Technology Applications Research (STAR) facility in Idaho Falls, ID. The FBSR waste forms were characterized and the durability tested via ASTM C1285 (Product Consistency Test), the Environmental Protection Agency (EPA) Toxic Characteristic Leaching Procedure (TCLP), and the Single Pass Flow Through (SPFT) test. The results of the SPFT testing and the activation energies for dissolution are discussed in this study.

  16. Stable hydrogen production from ethanol through steam reforming reaction over nickel-containing smectite-derived catalyst.

    PubMed

    Yoshida, Hiroshi; Yamaoka, Ryohei; Arai, Masahiko

    2015-01-01

    Hydrogen production through steam reforming of ethanol was investigated with conventional supported nickel catalysts and a Ni-containing smectite-derived catalyst. The former is initially active, but significant catalyst deactivation occurs during the reaction due to carbon deposition. Side reactions of the decomposition of CO and CH4 are the main reason for the catalyst deactivation, and these reactions can relatively be suppressed by the use of the Ni-containing smectite. The Ni-containing smectite-derived catalyst contains, after H2 reduction, stable and active Ni nanocrystallites, and as a result, it shows a stable and high catalytic performance for the steam reforming of ethanol, producing H2. PMID:25547495

  17. Stable Hydrogen Production from Ethanol through Steam Reforming Reaction over Nickel-Containing Smectite-Derived Catalyst

    PubMed Central

    Yoshida, Hiroshi; Yamaoka, Ryohei; Arai, Masahiko

    2014-01-01

    Hydrogen production through steam reforming of ethanol was investigated with conventional supported nickel catalysts and a Ni-containing smectite-derived catalyst. The former is initially active, but significant catalyst deactivation occurs during the reaction due to carbon deposition. Side reactions of the decomposition of CO and CH4 are the main reason for the catalyst deactivation, and these reactions can relatively be suppressed by the use of the Ni-containing smectite. The Ni-containing smectite-derived catalyst contains, after H2 reduction, stable and active Ni nanocrystallites, and as a result, it shows a stable and high catalytic performance for the steam reforming of ethanol, producing H2. PMID:25547495

  18. Hydrogen Permeability of Palladium Membrane for Steam-Reforming of Bio-Ethanol Using the Membrane Reactor

    NASA Astrophysics Data System (ADS)

    Kinouchi, Kouji; Katoh, Masahiro; Horikawa, Toshihide; Yoshikawa, Takushi; Wada, Mamoru

    A Palladium membrane was prepared by electro-less plating method on porous stainless steel. The catalytic hydrogen production by steam-reforming of biomass-derived ethanol (bio-ethanol) using a Pd membrane was analyzed by comparing it with those for the reaction using reagent ethanol (the reference sample). And the hydrogen permeability of the palladium membrane was investigated using the same palladium membrane (H2/He selectivity = 249, at ΔP = 0.10 MPa, 873 K). As a result, for bio-ethanol, deposited carbon had a negative influence on the hydrogen-permeability of the palladium membrane and hydrogen purity. The sulfur content in the bio-ethanol may have promoted carbon deposition. By using a palladium membrane, it was confirmed that H2 yield (%) was increased. It can be attributed that methane was converted from ethanol and produced more hydrogen by steam reforming, due to the in situ removal of hydrogen from the reaction location.

  19. Steam Reforming Solidification of Cesium and Strontium Separations Product from Advanced Aqueous Processing of Spent Nuclear Fuel

    SciTech Connect

    Julia L. Tripp; T. G. Garn; R. D. Boardman; J. D. Law

    2006-02-01

    The Advanced Fuel Cycle Initiative program is conducting research on aqueous separations processes for the nuclear fuel cycle. This research includes development of solvent extraction processes for the separation of cesium and strontium from dissolved spent nuclear fuel solutions to reduce the short-term decay heat load. The cesium/strontium strip solution from candidate separation processes will require treatment and solidification for managed storage. Steam reforming is currently being investigated for stabilization of these streams because it can potentially destroy the nitrates and organics present in these aqueous, nitrate-bearing solutions, while converting the cesium and strontium into leach-resistant aluminosilicate minerals, such as pollucite. These ongoing experimental studies are being conducted to evaluate the effectiveness of steam reforming for this application.

  20. Nickel-carbon nanocomposites prepared using castor oil as precursor: A novel catalyst for ethanol steam reforming

    NASA Astrophysics Data System (ADS)

    Carreño, Neftalí L. V.; Garcia, Irene T. S.; Raubach, Cristiane W.; Krolow, Mateus; Santos, Cláudia C. G.; Probst, Luiz F. D.; Fajardo, Humberto V.

    A novel and simple method to prepare nickel-based catalysts for ethanol steam reforming is proposed. The present method was developed using castor oil as a precursor. The results clarify that the nickel-carbon (Ni/C) catalyst has a high activity for ethanol steam reforming. It was observed that the catalytic behavior could be modified according to the experimental conditions employed. Moreover, it is interesting to note that the increase in the catalytic activity of the Ni/C nanocomposite over time, at 500 and 600 °C of reaction temperature, may be associated with the formation of filamentous carbon. The preliminary results indicate that the novel methodology used, led to the obtainment of materials with important properties that can be extended to applications in different catalytic process.

  1. Stabilization of Savannah River National Laboartory (SRNL) Aqueous Waste by Fluidized Bed Steam Reforming (FBSR)

    SciTech Connect

    Jantzen, C

    2004-11-01

    The Savannah River National Laboratory (SRNL) is a multidisciplinary laboratory operated by Westinghouse Savannah River Company (WSRC) in Aiken, South Carolina. Research and development programs have been conducted at SRNL for {approx}50 years generating non-radioactive (hazardous and non-hazardous) and radioactive aqueous wastes. Typically the aqueous effluents from the R&D activities are disposed of from each laboratory module via the High Activity Drains (HAD) or the Low Activity Drains (LAD) depending on whether they are radioactive or not. The aqueous effluents are collected in holding tanks, analyzed and shipped to either H-Area (HAD waste) or the F/H Area Effluent Treatment Facility (ETF) (LAD waste) for volume reduction. Because collection, analysis, and transport of LAD and HAD waste is cumbersome and since future treatment of this waste may be curtailed as the F/H-Area evaporators and waste tanks are decommissioned, SRNL laboratory operations requested several proof of principle demonstrations of alternate technologies that would define an alternative disposal path for the aqueous wastes. Proof of principle for the disposal of SRNL HAD waste using a technology known as Fluidized Bed Steam Reforming (FBSR) is the focus of the current study. The FBSR technology can be performed either as a batch process, e.g. in each laboratory module in small furnaces with an 8'' by 8'' footprint, or in a semi-continuous Bench Scale Reformer (BSR). The proof of principle experiments described in this study cover the use of the FBSR technology at any scale (pilot or full scale). The proof of principle experiments described in this study used a non-radioactive HAD simulant.

  2. Hydrogen production from steam reforming of acetic acid over Cu-Zn supported calcium aluminate.

    PubMed

    Mohanty, Pravakar; Patel, Madhumita; Pant, Kamal K

    2012-11-01

    Hydrogen can be produced by catalytic steam reforming (CSR) of biomass-derived oil. Typically bio oil contains 12-14% acetic acid; therefore, this acid was chosen as model compound for reforming of biooil with the help of a Cu-Zn/Ca-Al catalyst for high yield of H(2) with low CH(4) and CO content. Calcium aluminate support was prepared by solid-solid reaction at 1350°C. X-ray diffraction indicates 12CaO·7Al(2)O(3) as major, CaA(l4)O(7) and Ca(5)A(l6)O(14) as minor phases. Cu and Zn were loaded onto the support by wet-impregnation at 10 and 1wt.%, respectively. The catalysts were characterized by Brunauer-Emmett-Teller (BET), Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy TEM and the surface area for both support and Cu-Zn were 10.5 and 5.8m(2)/g, respectively. CSR was carried out in a tubular fixed bed reactor (I.D.=19mm) at temperatures between 600 and 800°C with 3-g loadings and (H(2)O/acetic acid) wt. ratio of 9:1. Significantly high (80%) yield of hydrogen was obtained over Cu-Zn/Ca-Al catalyst, as incorporation of Zn enhanced the H(2) yield by reducing deactivation of the catalyst. The coke formation on the support (Ca-12/Al-7) surface was negligible due to the presence of excess oxygen in the 12CaO·7Al(2)O(3) phase. PMID:22944490

  3. A highly active and coke-resistant steam reforming catalyst comprising uniform nickel-iron alloy nanoparticles.

    PubMed

    Koike, Mitsuru; Li, Dalin; Nakagawa, Yoshinao; Tomishige, Keiichi

    2012-12-01

    Doing fine with Ni-Fe: The calcination and reduction of a hydrotalcite precursor containing Ni and Fe ions gives uniform Ni-Fe alloy nanoparticles mixed with Mg(Ni, Fe, Al)O particles. The uniformity of the Ni-Fe alloy nanoparticles is connected to the catalyst's high activity and resistance to coke formation in toluene and phenol steam reforming reactions. PMID:23135797

  4. Model biogas steam reforming in a thin Pd-supported membrane reactor to generate clean hydrogen for fuel cells

    NASA Astrophysics Data System (ADS)

    Iulianelli, A.; Liguori, S.; Huang, Y.; Basile, A.

    2015-01-01

    Steam reforming of a model biogas mixture is studied for generating clean hydrogen by using an inorganic membrane reactor, in which a composite Pd/Al2O3 membrane separates part of the produced hydrogen through its selective permeation. The characteristics of H2 perm-selectivity of the fresh membrane is expressed in terms of H2/N2 ideal selectivity, in this case equal to 4300. Concerning biogas steam reforming reaction, at 380 °C, 2.0 bar H2O:CH4 = 3:1, GHSV = 9000 h-1 the permeate purity of the recovered hydrogen is around 96%, although the conversion (15%) and hydrogen recovery (>20%) are relatively low; on the contrary, at 450 °C, 3.5 bar H2O:CH4 = 4:1, GHSV = 11000 h-1 the conversion is increased up to more than 30% and the recovery of hydrogen to about 70%. This novel work constitutes a reference study for new developments on biogas steam reforming reaction in membrane reactors.

  5. Steam Reforming Application for Treatment of DOE Sodium Bearing Tank Wastes at Idaho National Laboratory for Idaho Cleanup Project

    SciTech Connect

    Landman, W.; Roesener, S.; Mason, B.; Wolf, K.; Amaria, N.

    2007-07-01

    The patented THOR{sup R} steam reforming waste treatment technology has been selected by the Department of Energy (DOE) as the technology of choice for treatment of about one million gallons of Sodium Bearing Waste (SBW) at the Idaho National Laboratory (INL). SBW is an acidic waste created primarily from cleanup of the fuel reprocessing equipment at the Idaho Nuclear Technology and Engineering Center (INTEC) at the INL. SBW contains high concentrations of nitric acid and alkali and aluminum nitrates with minor amounts of many inorganic compounds including radionuclides, mainly cesium. The steam reforming process will convert the SBW into dry, solid, carbonate and aluminate minerals supporting a preferred path for disposal as remote handled transuranic (RH-TRU) waste at the Waste Isolation Pilot Project (WIPP). The Idaho Cleanup Project (ICP) will design, build, and operate an Integrated Waste Treatment Unit (IWTU) that will comprise an integrated THOR{sup R} process system that will utilize dual fluidized bed steam reformers (FBSR) for treatment of the SBW. Design of the IWTU is nearing completion. The IWTU will be constructed at INTEC, immediately east of the New Waste Calcine Facility (NWCF), with planned fabrication and construction to start in early 2007 upon receipt of needed permits and completion of design and engineering. This paper provides a project and process overview of the IWTU and discusses the design and construction status. IWTU equipment and facility designs and bases will be presented. (authors)

  6. Mechanistic Insights into Catalytic Ethanol Steam Reforming Using Isotope-Labeled Reactants.

    PubMed

    Crowley, Stephen; Castaldi, Marco J

    2016-08-26

    The low-temperature ethanol steam reforming (ESR) reaction mechanism over a supported Rh/Pt catalyst has been investigated using isotope-labeled EtOH and H2 O. Through strategic isotope labeling, all nonhydrogen atoms were distinct from one another, and allowed an unprecedented level of understanding of the dominant reaction pathways. All combinations of isotope- and non-isotope-labeled atoms were detected in the products, thus there are multiple pathways involved in H2 , CO, CO2 , CH4 , C2 H4 , and C2 H6 product formation. Both the recombination of C species on the surface of the catalyst and preservation of the C-C bond within ethanol are responsible for C2 product formation. Ethylene is not detected until conversion drops below 100 % at t=1.25 h. Also, quantitatively, 57 % of the observed ethylene is formed directly through ethanol dehydration. Finally there is clear evidence to show that oxygen in the SiO2 -ZrO2 support constitutes 10 % of the CO formed during the reaction. PMID:27487203

  7. Carbon Deposition Onto Ni-Based Catalysts for Combined Steam/CO2 Reforming of Methane.

    PubMed

    Li, Peng; Park, Yoon Hwa; Moon, Dong Ju; Park, Nam Cook; Kim, Young Chul

    2016-02-01

    The present study was performed to suppress carbon deposition by Ce and Fe onto Ni-based catalysts in combined steam/CO2 reforming of methane (CSCRM), which is a process for producing synthesis gas (H2:CO = 2:1) for gas-to-liquids (GTL). The catalytic reaction was evaluated at 900 degrees C and 20 bar with a reactant feed ratio CH4:CO2:H20:Ar = 1:0.8:1.3:1 and gas hourly space velocity GHSV = 25,000 h(-1). The Ce and Fe modified Ni/gamma-A120, catalyst was characterized by BET surface area analysis, X-ray diffraction (XRD), H2 temperature-programmed reduction (TPR), H2 chemisorption, CO2 temperature-programmed desorption (TPD) and SEM. Ce- and Fe-modified Ni/Al2O3 catalysts exhibited remarkable activity and stability during the CSCRM over the course of 50 hours. It suggested that the Ni(12)-Ce(5)-Fe(5)/Al2O3 catalyst shows highly dispersed Ni particles with strong metal-to-support interaction (SMSI) as well as excellent catalytic activity. PMID:27433622

  8. Promotion effect of cobalt-based catalyst with rare earth for the ethanol steam reforming

    SciTech Connect

    Chiou, Josh Y. Z.; Chen, Ya-Ping; Yu, Shen-Wei; Wang, Chen-Bin

    2013-12-16

    Catalytic performance of ethanol steam reforming (ESR) was investigated on praseodymium (Pr) modified ceria-supported cobalt oxide catalyst. The ceria-supported cobalt oxide (Ce-Co) catalyst was prepared by co-precipitation-oxidation (CPO) method, and the doped Pr (5 and 10 wt% loading) catalysts (Pr{sub 5}−Ce−Co and Pr{sub 10}−Ce−Co) were prepared by incipient wetness impregnation method. The reduction pretreatment under 250 and 400 °C (H250 and H400) was also studied. All samples were characterized by XRD, TPR and TEM. Catalytic performance of ESR was tested from 250 to 500 °C in a fixed-bed reactor. The doping of Pr into the ceria lattice has significantly promoted the activity and reduced the coke formation. The products distribution also can be influenced by the different reduction pretreatment. The Pr{sub 10}−Ce−Co−H400 sample is a preferential ESR catalyst, where the hydrogen distribution approaches 73% at 475 °C with less amounts (< 2%) of CO and CH{sub 4}.

  9. Highly loaded Ni-based catalysts for low temperature ethanol steam reforming.

    PubMed

    Wang, Tuo; Ma, Hongyan; Zeng, Liang; Li, Di; Tian, Hao; Xiao, Shengning; Gong, Jinlong

    2016-05-21

    This paper describes the design of high-loading Ni/Al2O3 catalysts (78 wt% Ni) for low temperature ethanol steam reforming. The catalysts were synthesized via both co-precipitation (COP) and impregnation (IMP) methods. All the catalysts were measured by N2 adsorption-desorption, XRD, H2-TPR, and H2 pulse chemisorption. The characterization results demonstrated that the preparation method and the loading significantly affected the nickel particle size, active nickel surface area and catalytic performance. Over COP catalysts, large nickel particles were presented in nickel aluminum mixed oxides. In comparison, IMP catalysts gained more "free" NiO particles with weak interaction with the aluminum oxide. Consequently, COP catalysts yielded smaller nickel particles and larger active nickel surface areas than those of IMP catalysts. High loading is beneficial for obtaining sufficient active nickel sites when nickel particles are dispersed via COP, whereas excessive nickel content is not desired for catalysts prepared by IMP. Specifically, the 78 wt% nickel loaded catalyst synthesized by COP possessed small nickel particles (∼6.0 nm) and an abundant active nickel area (35.1 m(2) gcat(-1)). Consequently, COP-78 achieved superior stability with 92% ethanol conversion and ∼35% H2 selectivity at 673 K for 30 h despite the presence of a considerable amount of coke. PMID:27122228

  10. Steady-State Simulation of Steam Reforming of INEEL Tank Farm Waste

    SciTech Connect

    Nichols, Todd Travis; Taylor, Dean Dalton; Wood, Richard Arthur; Barnes, Charles Marshall

    2002-08-01

    A steady-state model of the Sodium-Bearing Waste steam reforming process at the Idaho National Engineering and Environmental Laboratory has been performed using the commercial ASPEN Plus process simulator. The preliminary process configuration and its representation in ASPEN are described. As assessment of the capability of the model to mechanistically predict product stream compositions was made, and fidelity gaps and opportunities for model enhancement were identified, resulting in the following conclusions: 1) Appreciable benefit is derived from using an activity coefficient model for electrolyte solution thermodynamics rather than assuming ideality (unity assumed for all activity coefficients). The concentrations of fifteen percent of the species present in the primary output stream were changed by more than 50%, relative to Electrolyte NRTL, when ideality was assumed; 2) The current baseline model provides a good start for estimating mass balances and performing integrated process optimization because it contains several key species, uses a mechanistic electrolyte thermodynamic model, and is based on a reasonable process configuration; and 3) Appreciable improvement to model fidelity can be realized by expanding the species list and the list of chemical and phase transformations. A path forward is proposed focusing on the use of an improved electrolyte thermodynamic property method, addition of chemical and phase transformations for key species currently absent from the model, and the combination of RGibbs and Flash blocks to simulate simultaneous phase and chemical equilibria in the off-gas treatment train.

  11. Inhibition of carbon formation during steam reforming of methane using thiol-coated nickel catalysts

    NASA Astrophysics Data System (ADS)

    Oudghiri-Hassani, H.; Rakass, S.; Abatzoglou, N.; Rowntree, P.

    n-Butanethiol-impregnated, micrometric, pristine Ni powder (Ni-C 4S) was tested as a catalyst for use in the steam reforming of methane, using X-Ray photoemission spectroscopy (XPS) and mass spectrometry (MS). The catalytic activities of both the pristine Ni and the Ni-C 4S powders were measured at 700 °C, under conditions that favoured (molar CH 4:H 2O ratio of 2:1), and did not favour (molar CH 4:H 2O ratio of 1:2) formation of surface carbon. The results show that: (a) Ni-C 4S demonstrates both high catalytic activity and stability during the 21 h duration test; (b) under conditions favouring the deposition of surface carbon, the Ni-C 4S retained both its efficiency and structural integrity, while the catalytic activity of the Ni was reduced by ∼70% and the catalyst pellets lost their integrity; (c) the amount of deposited carbon in the case of the Ni-C 4S catalyst was significantly lower than that observed for the Ni catalyst, in spite of the longer testing duration. It was concluded that the thiols pre-treatment of Ni surfaces, to be subsequently used in the production of catalysts supported SOFC anodes, can considerably increase their "active life span" this being a critical attribute in respect of their eventual commercialization.

  12. Characterization and Leaching Tests of the Fluidized Bed Steam Reforming (FBSR) Waste Form for LAW Immobilization

    SciTech Connect

    Neeway, James J.; Qafoku, Nikolla; Brown, Christopher F.; Peterson, Reid A.

    2013-10-01

    Several supplemental technologies for treating and immobilizing Hanford low activity waste (LAW) have been evaluated. One such immobilization technology is the Fluidized Bed Steam Reforming (FBSR) granular product. The FBSR granular product is composed of insoluble sodium aluminosilicate (NAS) feldspathoid minerals. Production of the FBSR mineral product has been demonstrated both at the industrial and laboratory scale. Pacific Northwest National Laboratory (PNNL) was involved in an extensive characterization campaign. This goal of this campaign was study the durability of the FBSR mineral product and the mineral product encapsulated in a monolith to meet compressive strength requirements. This paper gives an overview of results obtained using the ASTM C 1285 Product Consistency Test (PCT), the EPA Test Method 1311 Toxicity Characteristic Leaching Procedure (TCLP), and the ASTMC 1662 Single-Pass Flow-Through (SPFT) test. Along with these durability tests an overview of the characteristics of the waste form has been collected using Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD), microwave digestions for chemical composition, and surface area from Brunauer, Emmett, and Teller (BET) theory.

  13. Radionuclide and contaminant immobilization in the fluidized bed steam reforming waste products

    SciTech Connect

    Neeway, James J.; Qafoku, Nikolla; Westsik, Joseph H.; Brown, Christopher F.; Jantzen, Carol; Pierce, Eric M.

    2012-05-01

    The goal of this chapter is to introduce the reader to the Fluidized Bed Steam Reforming (FBSR) process and resulting waste form. The first section of the chapter gives an overview of the potential need for FBSR processing in nuclear waste remediation followed by an overview of the engineering involved in the process itself. This is followed by a description of waste form production at a chemical level followed by a section describing different process streams that have undergone the FBSR process. The third section describes the resulting mineral product in terms of phases that are present and the ability of the waste form to encapsulate hazardous and radioactive wastes from several sources. Following this description is a presentation of the physical properties of the granular and monolith waste form product including and contaminant release mechanisms. The last section gives a brief summary of this chapter and includes a section on the strengths associated with this waste form and the needs for additional data and remaining questions yet to be answered. The reader is directed elsewhere for more information on other waste forms such as Cast Stone (Lockrem, 2005), Ceramicrete (Singh et al., 1997, Wagh et al., 1999) and geopolymers (Kyritsis et al., 2009; Russell et al., 2006).

  14. Ethanol Steam Reforming on Co/CeO2: The Effect of ZnO Promoter

    SciTech Connect

    Davidson, Stephen; Sun, Junming; Wang, Yong

    2013-12-02

    A series of ZnO promoted Co/CeO2 catalysts were synthesized and characterized using XRD, TEM, H2-TPR, CO chemisorption, O2-TPO, IR-Py, and CO2-TPD. The effects of ZnO on the catalytic performances of Co/CeO2 were studied in ethanol steam reforming. It was found that the addition of ZnO facilitated the oxidation of Co0 via enhanced oxygen mobility of the CeO2 support which decreased the activity of Co/CeO2 in C–C bond cleavage of ethanol. 3 wt% ZnO promoted Co/CeO2 exhibited minimum CO and CH4 selectivity and maximum CO2 selectivity. This resulted from the combined effects of the following factors with increasing ZnO loading: (1) enhanced oxygen mobility of CeO2 facilitated the oxidation of CHx and CO to form CO2; (2) increased ZnO coverage on CeO2 surface reduced the interaction between CHx/CO and Co/CeO2; and (3) suppressed CO adsorption on Co0 reduced CO oxidation rate to form CO2. In addition, the addition of ZnO also modified the surface acidity and basicity of CeO2, which consequently affected the C2–C4 product distributions.

  15. Promotion effect of cobalt-based catalyst with rare earth for the ethanol steam reforming

    NASA Astrophysics Data System (ADS)

    Chiou, Josh Y. Z.; Chen, Ya-Ping; Yu, Shen-Wei; Wang, Chen-Bin

    2013-12-01

    Catalytic performance of ethanol steam reforming (ESR) was investigated on praseodymium (Pr) modified ceria-supported cobalt oxide catalyst. The ceria-supported cobalt oxide (Ce-Co) catalyst was prepared by co-precipitation-oxidation (CPO) method, and the doped Pr (5 and 10 wt% loading) catalysts (Pr5-Ce-Co and Pr10-Ce-Co) were prepared by incipient wetness impregnation method. The reduction pretreatment under 250 and 400 °C (H250 and H400) was also studied. All samples were characterized by XRD, TPR and TEM. Catalytic performance of ESR was tested from 250 to 500 °C in a fixed-bed reactor. The doping of Pr into the ceria lattice has significantly promoted the activity and reduced the coke formation. The products distribution also can be influenced by the different reduction pretreatment. The Pr10-Ce-Co-H400 sample is a preferential ESR catalyst, where the hydrogen distribution approaches 73% at 475 °C with less amounts (< 2%) of CO and CH4.

  16. Steady-State Simulation of Steam Reforming of INEEL Tank Farm Waste

    SciTech Connect

    Nichols, T.T.; Taylor, D.D.; Wood, R.A.; Barnes, C.M.

    2002-08-15

    A steady-state model of the Sodium-Bearing Waste steam reforming process at the Idaho National Engineering and Environmental Laboratory has been performed using the commercial ASPEN Plus process simulator. The preliminary process configuration and its representation in ASPEN are described. As assessment of the capability of the model to mechanistically predict product stream compositions was made, and fidelity gaps and opportunities for model enhancement were identified, resulting in the following conclusions: (1) Appreciable benefit is derived from using an activity coefficient model for electrolyte solution thermodynamics rather than assuming ideality (unity assumed for all activity coefficients). The concentrations of fifteen percent of the species present in the primary output stream were changed by more than 50%, relative to Electrolyte NRTL, when ideality was assumed; (2) The current baseline model provides a good start for estimating mass balances and performing integrated process optimization because it contains several key species, uses a mechanistic electrolyte thermodynamic model, and is based on a reasonable process configuration; and (3) Appreciable improvement to model fidelity can be realized by expanding the species list and the list of chemical and phase transformations. A path forward is proposed focusing on the use of an improved electrolyte thermodynamic property method, addition of chemical and phase transformations for key species currently absent from the model, and the combination of RGibbs and Flash blocks to simulate simultaneous phase and chemical equilibria in the off-gas treatment train.

  17. Highly loaded Ni-based catalysts for low temperature ethanol steam reforming

    NASA Astrophysics Data System (ADS)

    Wang, Tuo; Ma, Hongyan; Zeng, Liang; Li, Di; Tian, Hao; Xiao, Shengning; Gong, Jinlong

    2016-05-01

    This paper describes the design of high-loading Ni/Al2O3 catalysts (78 wt% Ni) for low temperature ethanol steam reforming. The catalysts were synthesized via both co-precipitation (COP) and impregnation (IMP) methods. All the catalysts were measured by N2 adsorption-desorption, XRD, H2-TPR, and H2 pulse chemisorption. The characterization results demonstrated that the preparation method and the loading significantly affected the nickel particle size, active nickel surface area and catalytic performance. Over COP catalysts, large nickel particles were presented in nickel aluminum mixed oxides. In comparison, IMP catalysts gained more ``free'' NiO particles with weak interaction with the aluminum oxide. Consequently, COP catalysts yielded smaller nickel particles and larger active nickel surface areas than those of IMP catalysts. High loading is beneficial for obtaining sufficient active nickel sites when nickel particles are dispersed via COP, whereas excessive nickel content is not desired for catalysts prepared by IMP. Specifically, the 78 wt% nickel loaded catalyst synthesized by COP possessed small nickel particles (~6.0 nm) and an abundant active nickel area (35.1 m2 gcat-1). Consequently, COP-78 achieved superior stability with 92% ethanol conversion and ~35% H2 selectivity at 673 K for 30 h despite the presence of a considerable amount of coke.

  18. Performance of the Fluidized Bed Steam Reforming Product Under Hydraulically Unsaturated Conditions

    SciTech Connect

    Neeway, James J.; Qafoku, Nikolla; Williams, Benjamin D.; Rod, Kenton A.; Bowden, Mark E.; Brown, Christopher F.; Pierce, Eric M.

    2014-05-01

    Currently, several candidates for secondary waste immobilization at the Hanford site in the State of Washington, USA are being considered. To demonstrate the durability of the product in the unsaturated Integrated Disposal Facility (IDF) at the site, a series of tests have been performed one of the candidate materials using the Pressurized Unsaturated Flow (PUF) system. The material that was tested was the Fluidized Bed Steam Reformer (FBSR) granular product and the granular product encapsulated in a geopolymer matrix. The FBSR product is composed primarily of an insoluble sodium aluminosilicate matrix with the dominant phases being feldspathoid minerals mostly nepheline, sodalite, and nosean. The PUF test method allows for the accelerated weathering of materials, including radioactive waste forms, under hydraulically unsaturated conditions, thus mimicking the open-flow and transport properties that most likely will be present at the IDF. The experiments show a trend of decreasing tracer release as a function of time for several of the elements released from the material including Na, Si, Al, and Cs. However, some of the elements, notably I and Re, show a steady release throughout the yearlong test. This result suggests that the release of these minerals from the sodalite cage occurs at a different rate compared with the dissolution of the predominant nepheline phase.

  19. Methanol steam reforming promoted by molten salt-modified platinum on alumina catalysts.

    PubMed

    Kusche, Matthias; Agel, Friederike; Ní Bhriain, Nollaig; Kaftan, Andre; Laurin, Mathias; Libuda, Jörg; Wasserscheid, Peter

    2014-09-01

    We herein describe a straight forward procedure to increase the performance of platinum-on-alumina catalysts in methanol steam reforming by applying an alkali hydroxide coating according to the "solid catalyst with ionic liquid layer" (SCILL) approach. We demonstrate by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and temperature-programmed desorption (TPD) studies that potassium doping plays an important role in the catalyst activation. Moreover, the hygroscopic nature and the basicity of the salt modification contribute to the considerable enhancement in catalytic performance. During reaction, a partly liquid film of alkali hydroxides/carbonates forms on the catalyst/alumina surface, thus significantly enhancing the availability of water at the catalytically active sites. Too high catalyst pore fillings with salt introduce a considerable mass transfer barrier into the system as indicated by kinetic studies. Thus, the optimum interplay between beneficial catalyst modification and detrimental mass transfer effects had to be identified and was found on the applied platinum-on-alumina catalyst at KOH loadings around 7.5 mass%. PMID:25124120

  20. Steam reforming of methanol over copper loaded anodized aluminum oxide (AAO) prepared through electrodeposition

    NASA Astrophysics Data System (ADS)

    Linga Reddy, E.; Karuppiah, J.; Lee, Hyun Chan; Kim, Dong Hyun

    2014-12-01

    In order to study the steam reforming of methanol (SRM) to produce hydrogen for fuel cells, porous γ-alumina support is developed on Al substrate using anodic oxidation process and copper catalyst particles are deposited homogeneously over anodic aluminum oxide (AAO) surface by electrodeposition method. We investigated the effect of electrodeposition time and hot water treatment (HWT) on the activity of catalysts for SRM reaction in the temperature range between 160 and 360 °C. The experimental results indicate that the SRM activity, CO2 and dimethyl ether (DME) selectivity's over Cu catalysts increased as the electrodeposition time increased from 30 to 120 s, further increment in deposition time of Cu have no significant effect on it. The rates of SRM conversion are found to be higher for the catalysts made from the supports obtained after HWT, which may be due to the enhancement in the surface area of AAO support. It is found that the SRM activity and CO2 selectivity strongly depended upon the free exposed copper sites available for methanol adsorption and reaction, and DME in products is mainly observed in the reaction temperature range between 300 and 350 °C and it is higher for the catalysts with low Cu content.

  1. Durable Cu composite catalyst for hydrogen production by high temperature methanol steam reforming

    NASA Astrophysics Data System (ADS)

    Matsumura, Yasuyuki

    2014-12-01

    Durable catalysts are necessitated for the high temperature methanol steam reforming in compact hydrogen processors. The high durability at 400 °C can be obtained with a composite Cu catalyst where a small amount of Cu-ZnO-ZrO2-Y2O3-In2O3 is coprecipitated on a zirconia support. The lifetime of the composite catalyst containing 3 wt.% Cu is estimated to be as long as 53 × 102 h at 400 °C to produce the full conversion at a contact time of 250 g h m-3. The deactivation rate empirically relates to the cube of the activity. The gradual deactivation is caused by the gradual reduction of the Cu surface amount and also by the reduction of the surface activity which is believed to decrease with an increase in the Cu particle size. The interaction between the thin layer of the coprecipitate and the support surface probably suppresses the aggregation of the coprecipitate leading to Cu sintering.

  2. Methanol Steam Reforming Promoted by Molten Salt-Modified Platinum on Alumina Catalysts

    PubMed Central

    Kusche, Matthias; Agel, Friederike; Ní Bhriain, Nollaig; Kaftan, Andre; Laurin, Mathias; Libuda, Jörg; Wasserscheid, Peter

    2014-01-01

    We herein describe a straight forward procedure to increase the performance of platinum-on-alumina catalysts in methanol steam reforming by applying an alkali hydroxide coating according to the “solid catalyst with ionic liquid layer” (SCILL) approach. We demonstrate by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and temperature-programmed desorption (TPD) studies that potassium doping plays an important role in the catalyst activation. Moreover, the hygroscopic nature and the basicity of the salt modification contribute to the considerable enhancement in catalytic performance. During reaction, a partly liquid film of alkali hydroxides/carbonates forms on the catalyst/alumina surface, thus significantly enhancing the availability of water at the catalytically active sites. Too high catalyst pore fillings with salt introduce a considerable mass transfer barrier into the system as indicated by kinetic studies. Thus, the optimum interplay between beneficial catalyst modification and detrimental mass transfer effects had to be identified and was found on the applied platinum-on-alumina catalyst at KOH loadings around 7.5 mass %. PMID:25124120

  3. Characterization of ZrO 2-promoted Cu/ZnO/nano-Al 2O 3 methanol steam reforming catalysts

    NASA Astrophysics Data System (ADS)

    Jones, Samuel D.; Neal, Luke M.; Everett, Michael L.; Hoflund, Gar B.; Hagelin-Weaver, Helena E.

    2010-10-01

    Three Cu/ZnO/ZrO 2/Al 2O 3 methanol reforming catalysts were investigated using X-ray photoelectron spectroscopy (XPS). The catalysts which contained ZrO 2 from a monoclinic nanoparticle ZrO 2 precursor exhibit both a higher activity toward the methanol steam reforming reaction and a lower CO production rate compared to catalysts composed of an XRD-amorphous ZrO 2 produced by impregnation using a Zr(NO 3) 2 precursor. The presence of a monoclinic phase appears to result in an increased charge transfer between the Zr and Cu species, as evidenced by a relatively electron-rich ZrO 2 phase and a partially oxidized Cu species on reduced catalysts. This electron deficient Cu species is more reactive toward the methanol reforming reaction and partially suppresses CO formation through the reverse water gas shift or methanol decomposition reactions.

  4. The application of inelastic neutron scattering to investigate the steam reforming of methane over an alumina-supported nickel catalyst

    NASA Astrophysics Data System (ADS)

    McFarlane, Andrew R.; Silverwood, Ian P.; Norris, Elizabeth L.; Ormerod, R. Mark; Frost, Christopher D.; Parker, Stewart F.; Lennon, David

    2013-12-01

    An alumina-supported nickel catalyst, previously used in methane reforming experiments employing CO2 as the oxidant, is applied here in the steam reforming variant of the process. Micro-reactor experiments are used to discern an operational window compatible with sample cells designed for inelastic neutron scattering (INS) experiments. INS spectra are recorded after 6 h reaction of a 1:1 mixture of CH4 and H2O at 898 K. Weak INS spectra are observed, indicating minimal hydrogen retention by the catalyst in this operational regime. Post-reaction, the catalyst is further characterised by powder X-ray diffraction, transmission electron microscopy and Raman scattering. In a comparable fashion to that seen for the ‘dry’ reforming experiments, the catalyst retains substantial quantities of carbon in the form of filamentous coke. The role for hydrogen incorporation by the catalyst is briefly considered.

  5. Bi-reforming of methane from any source with steam and carbon dioxide exclusively to metgas (CO-2H2) for methanol and hydrocarbon synthesis.

    PubMed

    Olah, George A; Goeppert, Alain; Czaun, Miklos; Prakash, G K Surya

    2013-01-16

    A catalyst based on nickel oxide on magnesium oxide (NiO/MgO) thermally activated under hydrogen is effective for the bi-reforming with steam and CO(2) (combined steam and dry reforming) of methane as well as natural gas in a tubular flow reactor at elevated pressures (5-30 atm) and temperatures (800-950 °C). By adjusting the CO(2)-to-steam ratio in the gas feed, the H(2)/CO ratio in the produced syn-gas could be easily adjusted in a single step to the desired value of 2 for methanol and hydrocarbon synthesis. PMID:23256664

  6. Performance and economic assessments of a solid oxide fuel cell system with a two-step ethanol-steam-reforming process using CaO sorbent

    NASA Astrophysics Data System (ADS)

    Tippawan, Phanicha; Arpornwichanop, Amornchai

    2016-02-01

    The hydrogen production process is known to be important to a fuel cell system. In this study, a carbon-free hydrogen production process is proposed by using a two-step ethanol-steam-reforming procedure, which consists of ethanol dehydrogenation and steam reforming, as a fuel processor in the solid oxide fuel cell (SOFC) system. An addition of CaO in the reformer for CO2 capture is also considered to enhance the hydrogen production. The performance of the SOFC system is analyzed under thermally self-sufficient conditions in terms of the technical and economic aspects. The simulation results show that the two-step reforming process can be run in the operating window without carbon formation. The addition of CaO in the steam reformer, which runs at a steam-to-ethanol ratio of 5, temperature of 900 K and atmospheric pressure, minimizes the presence of CO2; 93% CO2 is removed from the steam-reforming environment. This factor causes an increase in the SOFC power density of 6.62%. Although the economic analysis shows that the proposed fuel processor provides a higher capital cost, it offers a reducing active area of the SOFC stack and the most favorable process economics in term of net cost saving.

  7. Accelerated Weathering of Fluidized Bed Steam Reformation Material Under Hydraulically Unsaturated Conditions

    SciTech Connect

    Pierce, Eric M.

    2007-09-16

    To predict the long-term fate of low- and high-level waste forms in the subsurface over geologic time scales, it is important to understand the behavior of the corroding waste forms under conditions the mimic to the open flow and transport properties of a subsurface repository. Fluidized bed steam reformation (FBSR), a supplemental treatment technology option, is being considered as a waste form for the immobilization of low-activity tank waste. To obtain the fundamental information needed to evaluate the behavior of the FBSR waste form under repository relevant conditions and to monitor the long-term behavior of this material, an accelerated weathering experiment is being conducted with the pressurized unsaturated flow (PUF) apparatus. Unlike other accelerated weathering test methods (product consistency test, vapor hydration test, and drip test), PUF experiments are conducted under hydraulically unsaturated conditions. These experiments are unique because they mimic the vadose zone environment and allow the corroding waste form to achieve its final reaction state. Results from this on-going experiment suggest the volumetric water content varied as a function of time and reached steady state after 160 days of testing. Unlike the volumetric water content, periodic excursions in the solution pH and electrical conductivity have been occurring consistently during the test. Release of elements from the column illustrates a general trend of decreasing concentration with increasing reaction time. Normalized concentrations of K, Na, P, Re (a chemical analogue for 99Tc), and S are as much as 1 × 104 times greater than Al, Cr, Si, and Ti. After more than 600 days of testing, the solution chemistry data collected to-date illustrate the importance of understanding the long-term behavior of the FBSR product under conditions that mimic the open flow and transport properties of a subsurface repository.

  8. Pyrolysis/Steam Reforming Technology for Treatment of TRU Orphan Wastes

    SciTech Connect

    Mason, J. B.; McKibbin, J.; Schmoker, D.; Bacala, P.

    2003-02-27

    Certain transuranic (TRU) waste streams within the Department of Energy (DOE) complex cannot be disposed of at the Waste Isolation Pilot Plant (WIPP) because they do not meet the shipping requirements of the TRUPACT-II or the disposal requirements of the Waste Analysis Plan (WAP) in the WIPP RCRA Part B Permit. These waste streams, referred to as orphan wastes, cannot be shipped or disposed of because they contain one or more prohibited items, such as liquids, volatile organic compounds (VOCs), hydrogen gas, corrosive acids or bases, reactive metals, or high concentrations of polychlorinated biphenyl (PCB), etc. The patented, non-incineration, pyrolysis and steam reforming processes marketed by THOR Treatment Technologies LLC removes all of these prohibited items from drums of TRU waste and produces a dry, inert, inorganic waste material that meets the existing TRUPACT-II requirements for shipping, as well as the existing WAP requirements for disposal of TRU waste at WIPP. THOR Treatment Technologies is a joint venture formed in June 2002 by Studsvik, Inc. (Studsvik) and Westinghouse Government Environmental Services Company LLC (WGES) to further develop and deploy Studsvik's patented THORSM technology within the DOE and Department of Defense (DoD) markets. The THORSM treatment process is a commercially proven system that has treated over 100,000 cu. ft. of nuclear waste from commercial power plants since 1999. Some of this waste has had contact dose rates of up to 400 R/hr. A distinguishing characteristic of the THORSM process for TRU waste treatment is the ability to treat drums of waste without removing the waste contents from the drum. This feature greatly minimizes criticality and contamination issues for processing of plutonium-containing wastes. The novel features described herein are protected by issued and pending patents.

  9. FLUIDIZED BED STEAM REFORMING TECHNOLOGY FOR ORGANIC AND NITRATE SALT SUPERNATE

    SciTech Connect

    Jantzen, C; Michael02 Smith, M

    2007-03-30

    About two decades ago a process was developed at the Savannah River Site (SRS) to remove Cs137 from radioactive high level waste (HLW) supernates so the supernates could be land disposed as low activity waste (LAW). Sodium tetraphenylborate (NaTPB) was used to precipitate Cs{sup 137} as CsTPB. The flowsheet called for destruction of the organic TPB by acid hydrolysis so that the Cs{sup 137} enriched residue could be mixed with other HLW sludge, vitrified, and disposed of in a federal geologic repository. The precipitation process was demonstrated full scale with actual HLW waste and a 2.5 wt% Cs137 rich precipitate containing organic TPB was produced admixed with 240,000 gallons of salt supernate. Organic destruction by acid hydrolysis proved to be problematic and other disposal technologies were investigated. Fluidized Bed Steam Reforming (FBSR), which destroys organics by pyrolysis, is the current baseline technology for destroying the TPB and the waste nitrates prior to vitrification. Bench scale tests were designed and conducted at the Savannah River National Laboratory (SRNL) to reproduce the pyrolysis reactions. The formation of alkali carbonate phases that are compatible with DWPF waste pre-processing and vitrification were demonstrated in the bench scale tests. Test parameters were optimized for a pilot scale FBSR demonstration that was performed at the SAIC Science & Technology Application Research (STAR) Center in Idaho Falls, ID by Idaho National Laboratory (INL) and SRNL in 2003. An engineering scale demonstration was completed by THOR{reg_sign} Treatment Technologies (TTT) and SRNL in 2006 at the Hazen Research, Inc. test facility in Golden, CO. The same mineral carbonate phases, the same organic destruction (>99.99%) and the same nitrate/nitrite destruction (>99.99%) were produced at the bench scale, pilot scale, and engineering scale although different sources of carbon were used during testing.

  10. Corrosion of SiC and oxide-composite ceramics by a simulated steam-reformer atmosphere

    SciTech Connect

    Federer, J.I.; Kim, H.E.; Moorhead, A.J.

    1991-09-01

    To achieve higher process efficiency by using pressurized reactants and/or heat transfer fluids, the US DOE is promoting development of high-pressure heat exchanger systems under cost-sharing agreements with industrial contractors. The steam reformer would contain more than 600 tubes. Because the combination of high temperature and pressure differential of 12.7 kg/cm{sup 2} (180 psig) across the tube wall is too severe for metallic tubes, ceramic materials are being considered for reformer tubes. Their use is expected to increase the efficiency of steam reformers by about 19%. At ORNL, four SiC ceramics, a SiC-TiB{sub 2} composite, a Si{sub 3}N{sub 4}-bonded SiC ceramic, and two alumina-matrix composites were selected as candidate materials for heat exchanger/steam-reformer tubes. These commercially available materials were exposed to a simulated steam-reformer atmosphere for up to 2000 h at 1260{degrees}C to assess their corrosion behavior and the effect of the exposure on their flexure strength (in air) at 20 and 1260{degrees}C. The approximate partial pressures of the constituents of the gas mixture at 1 atm total pressure were 0.54 H{sub 2}, 0.13 CO, 0.03 CO{sub 2}m 0.004 CH{sub 4}, and 0.30 H{sub 2}O. All but one material had net weight gains during the exposure test. The flexure strengths of the SiC and Si{sub 3}N{sub 4} ceramics and the SiC-TiB{sub 2} composite at 20 and 1260{degrees}C were not changed significantly by corrosion. The strengths of the alumina-matrix composites were decreased by corrosion; however, the strength of one of these (reinforced with SiC whiskers) was still higher than that of any other material after 500 h. The other alumina composite (containing SiC particles) exhibited the largest strength decrease of any material. The strength retention of the SiC ceramics and the SiC-TiB{sub 2} composite and the strength loss of the composites were associated with surface layers caused by corrosion. 12 refs., 12 figs., 4 tabs.

  11. Comparative Investigation of Benzene Steam Reforming over Spinel Supported Rh and Ir Catalysts

    SciTech Connect

    Mei, Donghai; Lebarbier, Vanessa M.; Rousseau, Roger; Glezakou, Vassiliki-Alexandra; Albrecht, Karl O.; Kovarik, Libor; Flake, Matt; Dagle, Robert A.

    2013-06-07

    In a combined experimental and first-principles density functional theory (DFT) study, benzene steam reforming (BSR) over MgAl2O4 supported Rh and Ir catalysts was investigated. Experimentally, it has been found that both highly dispersed Rh and Ir clusters (1-2 nm) on the MgAl2O4 spinel support are stable during the BSR in the temperature range of 700-850°C. Compared to the Ir/MgAl2O4 catalyst, the Rh/MgAl2O4 catalyst is more active with higher benzene turnover frequency and conversion. At typical steam conditions with the steam-to-carbon ratio > 12, the benzene conversion is only a weak function of the H2O concentration in the feed. This suggests that the initial benzene decomposition step rather than the benzene adsorption is most likely the rate-determined step in BSR over supported Rh and Ir catalysts. In order to understand the differences between the two catalysts, we followed with a comparative DFT study of initial benzene decomposition pathways over two representative model systems for each supported metal (Rh and Ir) catalysts. A periodic terrace (111) surface and an amorphous 50-atom metal cluster with a diameter of 1.0 nm were used to represent the two supported model catalysts under low and high dispersion conditions. Our DFT results show that the decreasing catalyst particle size enhances the benzene decomposition on supported Rh catalysts by lowering both C-C and C-H bond scission. The activation barriers of the C-C and the C-H bond scission decrease from 1.60 and 1.61 eV on the Rh(111) surface to 1.34 and 1.26 eV on the Rh50 cluster. For supported Ir catalysts, the decreasing particle size only affects the C-C scission. The activation barrier of the C-C scission of benzene decreases from 1.60 eV on the Ir(111) surface to 1.35 eV on the Ir50 cluster while the barriers of the C-H scission are practically the same. The experimentally measured higher BSR

  12. A core-shell structured, metal-ceramic composite-supported Ru catalyst for methane steam reforming

    NASA Astrophysics Data System (ADS)

    Lee, Hyun Chul; Potapova, Yulia; Lee, Doohwan

    2012-10-01

    Methane steam reforming on a metal-ceramic composite-supported ruthenium catalyst is studied at high temperatures. The core-shell structured Al2O3@Al composite consisting primarily of an Al metal core with a high surface area γ-Al2O3 overlayer is obtained by hydrothermal oxidation. Under the synthesis condition, primary Al2O3@Al particles aggregate to form a hierarchal secondary structure with macrosize inter-pores. This core-shell composite support enhances the heat conductivity and provides a high surface area for fine dispersion of a catalytic Ru component on the γ-Al2O3 overlayer. The Ru/Al2O3@Al catalyst exhibits significantly higher CH4 conversion than the conventional Ru/Al2O3 catalyst, indicating its superior properties for methane steam reforming at high temperatures contributed due to the fine Ru dispersion and facilitated heat and mass transfer via the unique catalyst structure. This metal-ceramic composite catalyst is stable in the reforming reaction for an extended time, suggesting reasonable stability in its physicochemical properties.

  13. Mechanistic aspects of the ethanol steam reforming reaction for hydrogen production on Pt, Ni, and PtNi catalysts supported on gamma-Al2O3.

    PubMed

    Sanchez-Sanchez, Maria Cruz; Navarro Yerga, Rufino M; Kondarides, Dimitris I; Verykios, Xenophon E; Fierro, Jose Luis G

    2010-03-25

    Mechanistic aspects of ethanol steam reforming on Pt, Ni, and PtNi catalysts supported on gamma-Al(2)O(3) are investigated from the analysis of adsorbed species and gas phase products formed on catalysts during temperature-programmed desorption of ethanol and during ethanol steam reforming reaction. DRIFTS-MS analyses of ethanol decomposition and ethanol steam reforming reactions show that PtNi and Ni catalysts are more stable than the Pt monometallic counterpart. Ethanol TPD results on Ni, Pt, and NiPt catalysts point to ethanol dehydrogenation and acetaldehyde decomposition as the first reaction pathways of ethanol steam reforming over the studied catalysts. The active sites responsible for the acetaldehyde decomposition are easily deactivated in the first minutes on-stream by carbon deposits. For Ni and PtNi catalysts, a second reaction pathway, consisting in the decomposition of acetate intermediates formed over the surface of alumina support, becomes the main reaction pathway operating in steam reforming of ethanol once the acetaldehyde decomposition pathway is deactivated. Taking into account the differences observed in the mechanism of ethanol decomposition, the better stability observed for PtNi catalyst is proposed to be related with a cooperative effect between Pt and Ni activities together with the enhanced ability of Ni to gasify the methyl groups formed by decomposition of acetate species. On the contrary, monometallic catalysts are believed to dehydrogenate these methyl groups forming coke that leads to deactivation of metal particles. PMID:19824680

  14. NiW and NiRu Bimetallic Catalysts for Ethylene Steam Reforming: Alternative Mechanisms for Sulfur Resistance

    SciTech Connect

    Rangan, M.; Yung, M. M.; Medlin, J. W.

    2012-06-01

    Previous investigations of Ni-based catalysts for the steam reforming of hydrocarbons have indicated that the addition of a second metal can reduce the effects of sulfur poisoning. Two systems that have previously shown promise for such applications, NiW and NiRu, are considered here for the steam reforming of ethylene, a key component of biomass derived tars. Monometallic and bimetallic Al{sub 2}O{sub 3}-supported Ni and W catalysts were employed for ethylene steam reforming in the presence and absence of sulfur. The NiW catalysts were less active than Ni in the absence of sulfur, but were more active in the presence of 50 ppm H{sub 2}S. The mechanism for the W-induced improvements in sulfur resistance appears to be different from that for Ru in NiRu. To probe reasons for the sulfur resistance of NiRu, the adsorption of S and C{sub 2}H{sub 4} on several bimetallic NiRu alloy surfaces ranging from 11 to 33 % Ru was studied using density functional theory (DFT). The DFT studies reveal that sulfur adsorption is generally favored on hollow sites containing Ru. Ethylene preferentially adsorbs atop the Ru atom in all the NiRu (111) alloys investigated. By comparing trends across the various bimetallic models considered, sulfur adsorption was observed to be correlated with the density of occupied states near the Fermi level while C{sub 2}H{sub 4} adsorption was correlated with the number of unoccupied states in the d-band. The diverging mechanisms for S and C{sub 2}H{sub 4} adsorption allow for bimetallic surfaces such as NiRu that enhance ethylene binding without accompanying increases in sulfur binding energy. In contrast, bimetallics such as NiSn and NiW appear to decrease the affinity of the surface for both the reagent and the poison.

  15. Kinetics for Steam and CO2 Reforming of Methane Over Ni/La/Al2O3 Catalyst.

    PubMed

    Park, Myung Hee; Choi, Bong Kwan; Park, Yoon Hwa; Moon, Dong Ju; Park, Nam Cook; Kim, Young Chul

    2015-07-01

    Kinetic studies of mixed (steam and dry) reforming of methane on Ni/La/Al2O3 and Ni/La-Co (1, 3 wt%)/Al2O3 catalysts were performed in an atmospheric fixed-bed reactor. Kinetic parameters for the mixed reforming over these catalysts were obtained under reaction conditions free from heat and mass transfer limitations. Variables for the mixed reforming were the reaction temperature and partial pressure of reactants. The fitting of the experimental data for the rate of methane conversion, rCH4, using the power law rate equation rCH4 = k(PrCH4)α(PCO2)β(PH2O)γ showed that the reaction orders α, β, and γ are steady and obtained values equal to α = 1, β = 0, and γ = 0. In other words, among CH4, CO2, H2O, and H2, only CH4 reaction orders were not zero and they were affected by the promoters. The apparent activation energy on catalysts Ni/La/Al2O3, Ni/La-Co (1)/Al2O3 and Ni/La-Co (3)/Al2O3 is 85.2, 93.8, and 99.4 kJ/mol, respectively. The addition of Co to Ni/La/Al2O3 was increased the apparent activation energy of the mixed reforming reaction. And the Ni/La-Co (3 wt%)/Al2O3 catalyst showed the highest reforming activity and apparent activation energy. The Co promoters can increase the apparent activation energy of mixed reforming of methane. PMID:26373118

  16. Preparation and initial characterization of fluidized bed steam reforming pure-phase standards

    SciTech Connect

    Missimer, D. M.; Rutherford, R. L.

    2013-03-21

    Hanford is investigating the Fluidized Bed Steam Reforming (FBSR) process for their Low Activity Waste. The FBSR process offers a low-temperature continuous method by which liquid waste can be processed with the addition of clay into a sodium aluminosilicate (NAS) waste form. The NAS waste form is mainly comprised of nepheline (NaAlSiO{sub 4}), sodalite (Na{sub 8}[AlSiO{sub 4}]{sub 6}Cl{sub 2}), and nosean (Na{sub 8}[AlSiO{sub 4}]{sub 6}SO{sub 4}). Anions such as perrhenate (ReO{sub 4}{sup -}), pertechnetate (TcO{sub 4}{sup -}), and iodine (I{sup -}) are expected to replace sulfate in the nosean structure and/or chloride in the sodalite mineral structure (atomically bonded inside the aluminosilicate cages that these mineral structures possess). In the FBSR waste form, each of these phases can exist in a variety of solid solutions that differ from the idealized forms observed in single crystals in nature. The lack of understanding of the durability of these stoichiometric or idealized mineral phases complicates the ability to deconvolute the durability of the mixed phase FBSR product since it is a combination of different NAS phases. To better understand the behavior, fabrication and testing of the individual phases of the FBSR product is required. Analytical Development (AD) of the Science and Technology directorate of the Savannah River National Laboratory (SRNL) was requested to prepare the series of phase-pure standards, consisting of nepheline, nosean, and Cl, Re, and I sodalite. Once prepared, X-ray Diffraction (XRD) analyses were used to confirm the products were phase pure. These standards are being used for subsequent characterization studies consisting of the following: single-pass flow-through (SPFT) testing, development of thermodynamic data, and x-ray diffraction (XRD) calibration curves. In addition to the above mentioned phase-pure standards, AD was tasked with fabricating a mixed Tc-Re sodalite.

  17. Performance of the Fluidized Bed Steam Reforming product under hydraulically unsaturated conditions.

    PubMed

    Neeway, James J; Qafoku, Nikolla P; Williams, Benjamin D; Rod, Kenton; Bowden, Mark E; Brown, Christopher F; Pierce, Eric M

    2014-05-01

    Several candidates for supplemental low-activity waste (LAW) immobilization at the Hanford site in Washington State, USA are being considered. One waste sequestering technology considered is Fluidized Bed Steam Reforming (FBSR). The granular product resulting from the FBSR process is composed primarily of an insoluble sodium aluminosilicate matrix with the dominant phases being feldspathoid minerals with a 1:1:1 molar ratio of Na, Al and Si. To demonstrate the durability of the product, which can be disposed of at the unsaturated Integrated Disposal Facility (IDF) at Hanford, a series of tests has been performed using the Pressurized Unsaturated Flow (PUF) system, which allows for the accelerated weathering of the solid materials. The system maintains hydraulically unsaturated conditions, thus mimicking the open-flow and transport properties that will be present at the IDF. Two materials were tested using the system: 1) the FBSR granular product and 2) the FBSR granular product encapsulated in a geopolymer to form a monolith. Results of the experiments show a trend of relatively constant effluent concentration of Na, Si, Al, and Cs as a function of time from both materials. The elements I and Re show a steady release throughout the yearlong test from the granular material but their concentrations seem to be increasing at one year from the monolith material. This result suggests that these two elements may be present in the sodalite cage structure rather than in the predominant nepheline phase because their release occurs at a different rate compared to nepheline phase. Also, these elements to not seem to reprecipitate when released from the starting material. Calculated one-year release rates for Si are on the order of 10(-6) g/(m(2) d) for the granular material and 10(-5) g/(m(2) d) for the monolith material while Re release is seen to be two orders of magnitude higher than Si release rates. SEM imaging and XRD analysis show how the alteration of the two

  18. Performance of the Fluidized Bed Steam Reforming product under hydraulically unsaturated conditions

    SciTech Connect

    Neeway, James J; Rod, Kenton A.; Bowden, Mark E; Pierce, Eric M; Qafoku, Nikolla; Williams, Benjamin D; Brown, Christopher F

    2014-01-01

    Several candidates for supplemental low-activity waste (LAW) immobilization at the Hanford site in Washington State, USA are being considered. One waste sequestering technology considered is Fluidized Bed Steam Reforming (FBSR). The granular product resulting from the FBSR process is composed primarily of an insoluble sodium aluminosilicate matrix with the dominant phases being feldspathoid minerals with a 1:1:1 molar ratio of Na, Al and Si. To demonstrate the durability of the product, which can be disposed of at the unsaturated Integrated Disposal Facility (IDF) at Hanford, a series of tests has been performed using the Pressurized Unsaturated Flow (PUF) system, which allows for the accelerated weathering of the solid materials. The system maintains hydraulically unsaturated conditions, thus mimicking the open-flow and transport properties that will be present at the IDF. Two materials were tested using the system: 1) the FBSR granular product and 2) the FBSR granular product encapsulated in a geopolymer to form a monolith. Results of the experiments show a trend of relatively constant effluent concentration of Na, Si, Al, and Cs as a function of time from both materials. The elements I and Re show a steady release throughout the yearlong test from the granular material but their concentrations seem to be increasing at one year from the monolith material. This result suggests that these two elements may be present in the sodalite cage structure rather than in the predominant nepheline phase because their release occurs at a different rate compared to nepheline phase. Also, these elements to not seem to reprecipitate when released from the starting material. Calculated one-year release rates for Si are on the order of 10 6 g/(m2 d) for the granular material and 10 5 g/(m2 d) for the monolith material while Re release is seen to be two orders of magnitude higher than Si release rates. SEM imaging and XRD analysis show how the alteration of the two materials is

  19. Minimizing the formation of coke and methane on Co nanoparticles in steam reforming of biomass-derived oxygenates

    SciTech Connect

    Sun, Junming; Mei, Donghai; Karim, Ayman M.; Datye, Abhaya K.; Wang, Yong

    2013-06-01

    Fundamental understanding and control of chemical transformations are essential to the development of technically feasible and economically viable catalytic processes for efficient conversion of biomass to fuels and chemicals. Using an integrated experimental and theoretical approach, we report high hydrogen selectivity and catalyst durability of acetone steam reforming (ASR) on inert carbon supported Co nanoparticles. The observed catalytic performance is further elucidated on the basis of comprehensive first-principles calculations. Instead of being considered as an undesired intermediate prone for catalyst deactivation during bioethanol steam reforming (ESR), acetone is suggested as a key and desired intermediate in proposed two-stage ESR process that leads to high hydrogen selectivity and low methane formation on Co-based catalysts. The significance of the present work also sheds a light on controlling the chemical transformations of key intermediates in biomass conversion such as ketones. We gratefully acknowledge the financial support from U. S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, and the Laboratory directed research and development (LDRD) project of Pacific Northwest National Laboratory (PNNL). Computing time was granted by the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL). The EMSL is a U.S. DOE national scientific user facility located at PNNL, and sponsored by the U.S. DOE’s Office of Biological and Environmental Research.

  20. Polymer electrolyte membrane fuel cell grade hydrogen production by methanol steam reforming: A comparative multiple reactor modeling study

    NASA Astrophysics Data System (ADS)

    Katiyar, Nisha; Kumar, Shashi; Kumar, Surendra

    2013-12-01

    Analysis of a fuel processor based on methanol steam reforming has been carried out to produce fuel cell grade H2. Six reactor configurations namely FBR1 (fixed bed reactor), MR1 (H2 selective membrane reactor with one reaction tube), MR2 (H2 selective membrane reactor with two reaction tubes), FBR2 (FBR1 + preferential CO oxidation (PROX) reactor), MR3 (MR1 + PROX), and MR4 (MR2 + PROX) are evaluated by simulation to identify the suitable processing scheme. The yield of H2 is significantly affected by H2 selective membrane, residence time, temperature, and pressure conditions at complete methanol conversion. The enhancement in residence time in MR2 by using two identical reaction tubes provides H2 yield of 2.96 with 91.25 mol% recovery at steam/methanol ratio of 1.5, pressure of 2 bar and 560 K temperature. The exit retentate gases from MR2 are further treated in PROX reactor of MR4 to reduce CO concentration to 4.1 ppm to ensure the safe discharge to the environment. The risk of carbon deposition on reforming catalyst is highly reduced in MR4, and MR4 reactor configuration generates 7.4 NL min-1 of CO free H2 from 0.12 mol min-1 of methanol which can provide 470 W PEMFC feedstock requirement. Hence, process scheme in MR4 provides a compact and innovative fuel cell grade H2 generating unit.

  1. Steam Reforming Application for Treatment of DOE Sodium Bearing Tank Wastes at Idaho National Laboratory for Idaho Cleanup Project

    SciTech Connect

    Mason, J.B.; Wolf, K.; Ryan, K.; Roesener, S.; Cowen, M.; Schmoker, D.; Bacala, P.; Landman, B.

    2006-07-01

    The patented THOR{sup R} steam reforming waste treatment technology has been selected as the technology of choice for treatment of Sodium Bearing Waste (SBW) at the Idaho National Laboratory (INL) for the Idaho Cleanup Project (ICP). SBW is an acidic tank waste at the Idaho Nuclear Technology and Engineering Center (INTEC) at INL. It consists primarily of waste from decontamination activities and laboratory wastes. SBW contains high concentrations of nitric acid, alkali and aluminum nitrates, with minor amounts of many inorganic compounds including radionuclides, mainly cesium and strontium. The THOR{sup R} steam reforming process will convert the SBW tank waste feed into a dry, solid, granular product. The THOR{sup R} technology was selected to treat SBW, in part, because it can provide flexible disposal options to accommodate the final disposition path selected for SBW. THOR{sup R} can produce a final end-product that will meet anticipated requirements for disposal as Remote-Handled TRU (RH-TRU) waste; and, with modifications, THOR{sup R} can also produce a final end-product that could be qualified for disposal as High Level Waste (HLW). SBW treatment will be take place within the Integrated Waste Treatment Unit (IWTU), a new facility that will be located at the INTEC. This paper provides an overview of the THOR{sup R} process chemistry and process equipment being designed for the IWTU. (authors)

  2. Steam Reforming Technology Demonstration Program for Treatment of DOE Sodium Bearing Tank Wastes at Idaho National Laboratory

    SciTech Connect

    Ryan, K.; Mason, B.; Wolf, K.; Olson, A.

    2007-07-01

    The patented THOR{sup R} steam reforming waste treatment technology has been selected by the Department of Energy (DOE) for treatment of Sodium Bearing Waste (SBW) at the Idaho National Laboratory (INL). SBW is an acidic waste created primarily from cleanup of the fuel reprocessing equipment at the Idaho Nuclear Technology and Engineering Center (INTEC) at the INL. The SBW contains high concentrations of nitric acid and alkali and aluminum nitrates, along with many other inorganic compounds, including substantial levels of radionuclides. As part of the implementation of the THOR{sup R} process at INTEC, an engineering-scale test demonstration (ESTD) was conducted using a specially designed pilot plant located at Hazen Research, Inc. in Golden Colorado. The purpose of the ESTD was to confirm and optimize operation of the THOR{sup R} dual fluidized bed steam reforming (FBSR) process for treating the SBW. The performance of the integrated FBSR thermal and off-gas systems was demonstrated while treating waste simulants representative of the actual SBW. Simulants were utilized that consisted of highly acidic nitrate solutions, with both dissolved and undissolved solids (UDS). The SBW simulant solutions were converted into a dry, granular solid, consisting of carbonate and aluminate product compounds. The successful performance of the integrated FBSR system was verified and demonstrated. (authors)

  3. Hydrogen generation having CO2 removal with steam reforming

    SciTech Connect

    Kandaswamy, Duraiswamy; Chellappa, Anand S.; Knobbe, Mack

    2015-07-28

    A method for producing hydrogen using fuel cell off gases, the method feeding hydrocarbon fuel to a sulfur adsorbent to produce a desulfurized fuel and a spent sulfur adsorbent; feeding said desulfurized fuel and water to an adsorption enhanced reformer that comprises of a plurality of reforming chambers or compartments; reforming said desulfurized fuel in the presence of a one or more of a reforming catalyst and one or more of a CO2 adsorbent to produce hydrogen and a spent CO2 adsorbent; feeding said hydrogen to the anode side of the fuel cell; regenerating said spent CO2 adsorbents using the fuel cell cathode off-gases, producing a flow of hydrogen by cycling between said plurality of reforming chambers or compartments in a predetermined timing sequence; and, replacing the spent sulfur adsorbent with a fresh sulfur adsorbent at a predetermined time.

  4. Multifunctional Pd/Ni-Co catalyst for hydrogen production by chemical looping coupled with steam reforming of acetic acid.

    PubMed

    Fermoso, Javier; Gil, María V; Rubiera, Fernando; Chen, De

    2014-11-01

    High yield of high-purity H2 from acetic acid, a model compound of bio-oil obtained from the fast pyrolysis of biomass, was produced by sorption-enhanced steam reforming (SESR). An oxygen carrier was introduced into a chemical loop (CL) coupled to the cyclical SESR process to supply heat in situ for the endothermic sorbent regeneration to increase the energy efficiency of the process. A new multifunctional 1 %Pd/20 %Ni-20 %Co catalyst was developed for use both as oxygen carrier in the CL and as reforming catalyst in the SESR whereas a CaO-based material was used as CO2 sorbent. In the sorbent-air regeneration step, the Ni-Co atoms in the catalyst undergo strong exothermic oxidation reactions that provide heat for the CaO decarbonation. The addition of Pd to the Ni-Co catalyst makes the catalyst active throughout the whole SESR-CL cycle. Pd significantly promotes the reduction of Ni-Co oxides to metallic Ni-Co during the reforming stage, which avoids the need for a reduction step after regeneration. H2 yield above 90 % and H2 purity above 99.2 vol % were obtained. PMID:25209388

  5. High efficiency carbonate fuel cell/turbine hybrid power cycle

    SciTech Connect

    Steinfeld, G.; Maru, H.C.; Sanderson, R.A.

    1996-07-01

    The hybrid power cycle studies were conducted to identify a high efficiency, economically competitive system. A hybrid power cycle which generates power at an LHV efficiency > 70% was identified that includes an atmospheric pressure direct carbonate fuel cell, a gas turbine, and a steam cycle. In this cycle, natural gas fuel is mixed with recycled fuel cell anode exhaust, providing water for reforming fuel. The mixed gas then flows to a direct carbonate fuel cell which generates about 70% of the power. The portion of the anode exhaust which is not recycled is burned and heat transferred through a heat exchanger (HX) to the compressed air from a gas turbine. The heated compressed air is then heated further in the gas turbine burner and expands through the turbine generating 15% of the power. Half the exhaust from the turbine provides air for the anode exhaust burner. All of the turbine exhaust eventually flows through the fuel cell cathodes providing the O2 and CO2 needed in the electrochemical reaction. Exhaust from the cathodes flows to a steam system (heat recovery steam generator, staged steam turbine generating 15% of the cycle power). Simulation of a 200 MW plant with a hybrid power cycle had an LHV efficiency of 72.6%. Power output and efficiency are insensitive to ambient temperature, compared to a gas turbine combined cycle; NOx emissions are 75% lower. Estimated cost of electricity for 200 MW is 46 mills/kWh, which is competitive with combined cycle where fuel cost is > $5.8/MMBTU. Key requirement is HX; in the 200 MW plant studies, a HX operating at 1094 C using high temperature HX technology currently under development by METC for coal gassifiers was assumed. A study of a near term (20 MW) high efficiency direct carbonate fuel cell/turbine hybrid power cycle has also been completed.

  6. Catalytic roles of Co0 and Co2+ during steam reforming of ethanol on Co/MgO catalysts

    SciTech Connect

    Karim, Ayman M.; Su, Yu; Engelhard, Mark H.; King, David L.; Wang, Yong

    2011-02-25

    Abstract: The catalytic roles of Co0 and Co2+ during steam reforming of ethanol were investigated over Co/MgO catalysts. Catalysts with different Co0/(Co0+Co2+) fraction were prepared through calcination and/or reduction at different temperatures, and the Co0 fraction was quantified by TPR and in-situ XPS. High temperature calcination of Co/MgO allowed us to prepare catalysts with more non-reducible Co2+ incorporated in the MgO lattice, while lower calcination temperatures allowed for the preparation of catalysts with higher Co0/(Co0+Co2+) fractions. The catalytic tests on Co0, non-reducible Co2+, and reducible Co2+ indicated that Co0 is much more active than either reducible or non-reducible Co2+ for C-C cleavage and water gas shift reaction. In addition, catalysts with a higher Co0 surface fraction exhibited a lower selectivity to CH4.

  7. Ethanol steam reforming on Ni/Al2O3 catalysts: effect of the addition of Zn and Pt.

    PubMed

    Buitrago-Sierra, R; Ruiz-Martínez, J; Serrano-Ruiz, J C; Rodríguez-Reinoso, F; Sepúlveda-Escribano, A

    2012-10-01

    Ni-based catalysts supported on Zn-modified alumina were investigated in the ethanol steam reforming reaction. A commercial γ-alumina was impregnated with different amounts of zinc nitrate (0, 2, 5, 10, 15, 20 wt.% on Zn basis), calcined, and then impregnated with nickel nitrate aqueous solutions. The samples were characterized by a number of techniques: N(2) adsorption at 77 K, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray fluorescence (XRF), and temperature-programmed reduction (TPR). Their catalytic behavior in the ethanol steam reforming reaction was studied at 873 K, with a H(2)O/ethanol ratio of 5:1. Two effects of the presence of Zn were detected. On the one hand, zinc modifies the surface structure and the surface chemistry of the catalysts by formation of zinc aluminates, and on the other hand, zinc oxide can be reduced to metallic zinc under reaction conditions, thus modifying the catalytic properties of the active phase. The presence of Zn increases the ethanol conversion to gaseous compounds as compared with the catalyst supported on the Zn-free commercial alumina. The addition of a small amount of Pt (1 wt.%) causes a beneficial effect in the reaction. When Ni catalysts were used without a previous reduction treatment, ethylene was formed in high amounts; however, the Pt-Ni catalysts need no reduction pre-treatment to achieve high H(2) yields (close to 70%) and showed a high stability versus time on stream because of the control of the production of ethylene, a coke precursor. PMID:22796067

  8. The production of pure pressurised hydrogen by the reformer-steam iron process in a fixed bed reactor system

    NASA Astrophysics Data System (ADS)

    Nestl, Stephan; Voitic, Gernot; Lammer, Michael; Marius, Bernhard; Wagner, Julian; Hacker, Viktor

    2015-04-01

    In this paper a fixed bed chemical looping process for the decentralised production of pure pressurised hydrogen for fuel cell applications is described. CH4 is converted to a syngas using conventional steam reforming. The syngas is directly used for the reduction of an iron based oxygen carrier. A consecutive oxidation step using steam leads to the formation of pure pressurised hydrogen. A thermodynamic analysis was performed in order to investigate feasible conditions for the syngas generation and reduction step. Experiments using pure hydrogen as well as an artificial syngas mixture showed the feasibility of the process for the production of pressurised hydrogen. A stable hydrogen production at a pressure of 8-11 bar(g) was achieved and only minor impurities of 700 ppm of carbon dioxide but no signs of carbon monoxide were detected in the produced hydrogen. Although the active surface decreased from 7.5 m2 g-1 to 0.9 m2 g-1 only moderate losses of reactivity were measured in the fixed bed reactor. Thermogravimetric analysis showed a loss of 9% of reactive material over nine cycles, presumably due to sintering effects.

  9. A novel approach to the experimental study on methane/steam reforming kinetics using the Orthogonal Least Squares method

    NASA Astrophysics Data System (ADS)

    Sciazko, Anna; Komatsu, Yosuke; Brus, Grzegorz; Kimijima, Shinji; Szmyd, Janusz S.

    2014-09-01

    For a mathematical model based on the result of physical measurements, it becomes possible to determine their influence on the final solution and its accuracy. However, in classical approaches, the influence of different model simplifications on the reliability of the obtained results are usually not comprehensively discussed. This paper presents a novel approach to the study of methane/steam reforming kinetics based on an advanced methodology called the Orthogonal Least Squares method. The kinetics of the reforming process published earlier are divergent among themselves. To obtain the most probable values of kinetic parameters and enable direct and objective model verification, an appropriate calculation procedure needs to be proposed. The applied Generalized Least Squares (GLS) method includes all the experimental results into the mathematical model which becomes internally contradicted, as the number of equations is greater than number of unknown variables. The GLS method is adopted to select the most probable values of results and simultaneously determine the uncertainty coupled with all the variables in the system. In this paper, the evaluation of the reaction rate after the pre-determination of the reaction rate, which was made by preliminary calculation based on the obtained experimental results over a Nickel/Yttria-stabilized Zirconia catalyst, was performed.

  10. A passively-fed methanol steam reformer heated with two-stage bi-fueled catalytic combustor

    NASA Astrophysics Data System (ADS)

    Lo, Kai-Fan; Wong, Shwin-Chung

    2012-09-01

    This paper presents further progress on our simple novel passively-fed methanol steam reformer. The present study focuses on the development of a catalytic combustor workable with both hydrogen and methanol fuels. The aim is to reutilize the exhaust hydrogen from a fuel cell under stable operation but burn methanol during the start-up. On a copper plate, the catalytic combustor in a u-turn channel is integrally machined under a two-turn serpentine-channel reformer. To resolve the highly different fuel reactivities, a suitably diluted catalyst formula demonstrates uniform temperature distributions burning with either liquid methanol or an H2/CO2 mixture simulating the exhaust gas from a fuel cell. In a two-stage process, it first takes 25 min to reach 270 °C by burning methanol. After the fuel is switched to the H2/CO2 mixture, another 20 min is needed to attain an optimal steady state which yields a high methanol conversion of 95% and acceptably low CO fraction of 1.04% at a reaction temperature of 278 °C. The H2 and CO2 concentrations are 75.1% and 23.6%.

  11. Process And Apparatus To Accomplish Autothermal Or Steam Reforming Via A Reciprocating Compression Device

    DOEpatents

    Lyons, K. David; James, Robert; Berry, David A.; Gardner, Todd

    2004-09-21

    The invention provides a method and apparatus for producing a synthesis gas from a variety of hydrocarbons. The apparatus (device) consists of a semi-batch, non-constant volume reactor to generate a synthesis gas. While the apparatus feeds mixtures of air, steam, and hydrocarbons into a cylinder where work is performed on the fluid by a piston to adiabatically raise its temperature without heat transfer from an external source.

  12. Process to Accomplish Autothermal or Steam Reforming Via a Reciprocating Compression Device

    SciTech Connect

    Lyons, David K.; James, Robert; Berry, David A.; Gardern, Todd

    2004-09-21

    The invention provides a method and apparatus for producing a synthesis gas from a variety of hydrocarbons. The apparatus (device) consists of a semi-batch, non-constant volume reactor to generate a synthesis gas. While the apparatus feeds mixtures of air, steam, and hydrocarbons into a cylinder where work is performed on the fluid by a piston to adiabatically raise its temperature without heat transfer from an external source.

  13. Applications of solar reforming technology

    SciTech Connect

    Spiewak, I.; Tyner, C.E.; Langnickel, U.

    1993-11-01

    Research in recent years has demonstrated the efficient use of solar thermal energy for driving endothermic chemical reforming reactions in which hydrocarbons are reacted to form synthesis gas (syngas). Closed-loop reforming/methanation systems can be used for storage and transport of process heat and for short-term storage for peaking power generation. Open-loop systems can be used for direct fuel production; for production of syngas feedstock for further processing to specialty chemicals and plastics and bulk ammonia, hydrogen, and liquid fuels; and directly for industrial processes such as iron ore reduction. In addition, reforming of organic chemical wastes and hazardous materials can be accomplished using the high-efficiency destruction capabilities of steam reforming. To help identify the most promising areas for future development of this technology, we discuss in this paper the economics and market potential of these applications.

  14. Development of a novel ceramic microchannel reactor for methane steam reforming

    NASA Astrophysics Data System (ADS)

    Murphy, Danielle M.

    Microchannel heat exchanger and reactor technology has recently gained interest as an innovative way to improve heat-exchanger efficiency, reduce size and weight, and utilize thermal management capabilities to improve conversion, yield, selectivity, and catalyst life. Among many other possible applications, this technology is suitable for advanced recuperated engines, oxy-fired combustion processes for oxygen separation, gas-cooled nuclear reactors, recuperative heat exchanger and reformer units for solid oxide fuel cell systems, and chemical processing. This work presents the design, fabrication, and performance of novel ceramic microchannel reactors in heat-exchanger and fuel-reforming applications. Although most microchannel devices are made of metal materials, ceramics offer an alternative which enables significantly higher operating temperatures, improved tolerance to harsh chemical environments, and improved adherence of ceramic-based catalyst washcoats. Significant cost savings in materials and manufacturing methods for high-volume manufacturing can also be achieved. High-temperature performance of the ceramic microchannel reactor is measured through non-reactive heat-exchanger experiments within a dedicated test stand. Heat-exchanger effectiveness of up to 88% is experimentally established. After coating catalyst material over half of the reactor layers, use of the ceramic microchannel reactor in methane fuel-processing applications is demonstrated. As a fuel reformer, the ceramic microchannel reactor achieves process intensification by combining heat-exchanger and catalytic-reactor functions to produce syngas. Gas hourly space velocities (GHSV) up to 50,000 hr-1 with methane conversion higher than 85% are achieved. A complete computational fluid dynamics (CFD) model, as well as a geometrically simplified hybrid CFD/chemical kinetics model, is used in conjunction with experimentation to examine heat transfer, fluid flow, and chemical kinetics within the

  15. CO(2)-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy.

    PubMed

    Rameshan, Christoph; Lorenz, Harald; Mayr, Lukas; Penner, Simon; Zemlyanov, Dmitry; Arrigo, Rosa; Haevecker, Michael; Blume, Raoul; Knop-Gericke, Axel; Schlögl, Robert; Klötzer, Bernhard

    2012-11-01

    In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd-In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa.Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd(1)In(1) phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd(1)Zn(1) counterpart.Catalytic characterization of the multilayer Pd(1)In(1) phase in MSR yielded a CO(2)-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In(2)O(3)-supported PdIn nanoparticles and pure In(2)O(3), intermediate formaldehyde is only partially converted to CO(2) using this Pd(1)In(1) phase. Strongly correlated with PdZn, on an In-diluted PdIn intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed.To achieve CO(2)-TOF values on the isolated Pd(1)In(1) intermetallic phase as high as on supported PdIn/In(2)O(3), at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO(2) conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd(1)In(1) inhibited inverse water-gas-shift reaction on In(2)O(3) and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO(2)-selectivity of the supported catalyst. PMID:23226689

  16. CO2-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy

    PubMed Central

    Rameshan, Christoph; Lorenz, Harald; Mayr, Lukas; Penner, Simon; Zemlyanov, Dmitry; Arrigo, Rosa; Haevecker, Michael; Blume, Raoul; Knop-Gericke, Axel; Schlögl, Robert; Klötzer, Bernhard

    2012-01-01

    In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd–In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa. Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd1In1 phase exhibits a similar “Cu-like” electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd1Zn1 counterpart. Catalytic characterization of the multilayer Pd1In1 phase in MSR yielded a CO2-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In2O3-supported PdIn nanoparticles and pure In2O3, intermediate formaldehyde is only partially converted to CO2 using this Pd1In1 phase. Strongly correlated with PdZn, on an In-diluted PdIn intermetallic phase with “Pd-like” electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed. To achieve CO2-TOF values on the isolated Pd1In1 intermetallic phase as high as on supported PdIn/In2O3, at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO2 conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd1In1 inhibited inverse water–gas-shift reaction on In2O3 and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO2-selectivity of the supported catalyst. PMID:23226689

  17. MINERALIZING, STEAM REFORMING TREATMENT OF HANFORD LOW-ACTIVITY WASTE (a.k.a. INEEL/EXT-05-02526)

    SciTech Connect

    A. L. Olson; N. R. Soelberg; D. W. Marshall; G. L. Anderson

    2005-02-01

    The U.S. Department of Energy (DOE) documented, in 2002, a plan for accelerating cleanup of the Hanford Site, located in southeastern Washington State, by at least 35 years. A key element of the plan was acceleration of the tank waste program and completion of ''tank waste treatment by 2028 by increasing the capacity of the planned Waste Treatment Plant (WTP) and using supplemental technologies for waste treatment and immobilization.'' The plan identified steam reforming technology as a candidate for supplemental treatment of as much as 70% of the low-activity waste (LAW). Mineralizing steam reforming technology, offered by THOR Treatment Technologies, LLC would produce a denitrated, granular mineral waste form using a high-temperature fluidized bed process. A pilot scale demonstration of the technology was completed in a 15-cm-diameter reactor vessel. The pilot scale facility was equipped with a cyclone separator and heated sintered metal filters for particulate removal, a thermal oxidizer for reduced gas species and NOx destruction, and a packed activated carbon bed for residual volatile species capture. The pilot scale equipment is owned by the DOE, but located at the Science and Technology Applications Research (STAR) Center in Idaho Falls, ID. Pilot scale testing was performed August 2–5, 2004. Flowsheet chemistry and operational parameters were defined through a collaborative effort involving Idaho National Engineering and Environmental Laboratory (INEEL), Savannah River National Laboratory (SRNL), and THOR Treatment Technologies personnel. Science Application International Corporation, owners of the STAR Center, personnel performed actual pilot scale operation. The pilot scale test achieved a total of 68.4 hours of cumulative/continuous processing operation before termination in response to a bed de-fluidization condition. 178 kg of LAW surrogate were processed that resulted in 148 kg of solid product, a mass reduction of about 17%. The process achieved

  18. Statistical validation and an empirical model of hydrogen production enhancement found by utilizing passive flow disturbance in the steam-reformation process

    SciTech Connect

    Erickson, Paul A.; Liao, Chang-hsien

    2007-11-15

    A passive flow disturbance has been proven to enhance the conversion of fuel in a methanol-steam reformer. This study presents a statistical validation of the experiment based on a standard 2{sup k} factorial experiment design and the resulting empirical model of the enhanced hydrogen producing process. A factorial experiment design was used to statistically analyze the effects and interactions of various input factors in the experiment. Three input factors, including the number of flow disturbers, catalyst size, and reactant flow rate were investigated for their effects on the fuel conversion in the steam-reformation process. Based on the experimental results, an empirical model was developed and further evaluated with an uncertainty analysis and interior point data. (author)

  19. CESIUM REMOVAL FROM TANKS 241-AN-103 & 241-SX-105 & 241-AZ-101 & 241AZ-102 COMPOSITE FOR TESTING IN BENCH SCALE STEAM REFORMER

    SciTech Connect

    DUNCAN JB; HUBER HJ

    2011-04-21

    This report documents the preparation of three actual Hanford tank waste samples for shipment to the Savannah River National Laboratory (SRNL). Two of the samples were dissolved saltcakes from tank 241-AN-103 (hereafter AN-103) and tank 241-SX-105 (hereafter SX-105); one sample was a supernate composite from tanks 241-AZ-101 and 241-AZ-102 (hereafter AZ-101/102). The preparation of the samples was executed following the test plans LAB-PLAN-10-00006, Test Plan for the Preparation of Samples from Hanford Tanks 241-SX-105, 241-AN-103, 241-AN-107, and LAB-PLN-l0-00014, Test Plan for the Preparation of a Composite Sample from Hanford Tanks 241-AZ-101 and 241-AZ-102 for Steam Reformer Testing at the Savannah River National Laboratory. All procedural steps were recorded in laboratory notebook HNF-N-274 3. Sample breakdown diagrams for AN-103 and SX-105 are presented in Appendix A. The tank samples were prepared in support of a series of treatability studies of the Fluidized Bed Steam Reforming (FBSR) process using a Bench-Scale Reformer (BSR) at SRNL. Tests with simulants have shown that the FBSR mineralized waste form is comparable to low-activity waste glass with respect to environmental durability (WSRC-STI-2008-00268, Mineralization of Radioactive Wastes by Fluidized Bed Steam Reforming (FBSR): Comparisons to Vitreous Waste Forms and Pertinent Durability Testing). However, a rigorous assessment requires long-term performance data from FBSR product formed from actual Hanford tank waste. Washington River Protection Solutions, LLC (WRPS) has initiated a Waste Form Qualification Program (WP-5.2.1-2010-001, Fluidized Bed Steam Reformer Low-level Waste Form Qualification) to gather the data required to demonstrate that an adequate FBSR mineralized waste form can be produced. The documentation of the selection process of the three tank samples has been separately reported in RPP-48824, Sample Selection Process for Bench-Scale Steam Reforming Treatability Studies Using

  20. CESIUM REMOVAL FROM TANKS 241-AN-103 & 241-SX-105 & 241-AZ-101/102 COMPOSITE FOR TESTING IN BENCH SCALE STEAM REFORMER

    SciTech Connect

    DUNCAN JB; HUBER HJ

    2011-06-08

    This report documents the preparation of three actual Hanford tank waste samples for shipment to the Savannah River National Laboratory (SRNL). Two of the samples were dissolved saltcakes from tank 241-AN-103 (hereafter AN-103) and tank 241-SX-105 (hereafter SX-105); one sample was a supernate composite from tanks 241-AZ-101 and 241-AZ-102 (hereafter AZ-101/102). The preparation of the samples was executed following the test plans LAB-PLAN-10-00006, Test Plan for the Preparation of Samples from Hanford Tanks 241-SX-105, 241-AN-103, 241-AN-107, and LAB-PLN-10-00014, Test Plan for the Preparation of a Composite Sample from Hanford Tanks 241-AZ-101 and 241-AZ-102 for Steam Reformer Testing at the Savannah River National Laboratory. All procedural steps were recorded in laboratory notebook HNF-N-274 3. Sample breakdown diagrams for AN-103 and SX-105 are presented in Appendix A. The tank samples were prepared in support of a series of treatability studies of the Fluidized Bed Steam Reforming (FBSR) process using a Bench-Scale Reformer (BSR) at SRNL. Tests with simulants have shown that the FBSR mineralized waste form is comparable to low-activity waste glass with respect to environmental durability (WSRC-STI-2008-00268, Mineralization of Radioactive Wastes by Fluidized Bed Steam Reforming (FBSR): Comparisons to Vitreous Waste Forms and Pertinent Durability Testing). However, a rigorous assessment requires long-term performance data from FB SR product formed from actual Hanford tank waste. Washington River Protection Solutions, LLC (WRPS) has initiated a Waste Form Qualification Program (WP-S.2.1-20 1 0-00 1, Fluidized Bed Steam Reformer Low-level Waste Form Qualification) to gather the data required to demonstrate that an adequate FBSR mineralized waste form can be produced. The documentation of the selection process of the three tank samples has been separately reported in RPP-48824, 'Sample Selection Process for Bench-Scale Steam Reforming Treatability Studies Using

  1. Deactivation Studies of Rh/Ce0.8Zr0.2O2 Catalysts in Low Temperature Ethanol Steam Reforming

    SciTech Connect

    Platon, Alex; Roh, Hyun-Seog; King, David L.; Wang, Yong

    2007-10-30

    Rapid deactivation of Rh/Ce0.8Zr0.2O2 catalysts in low temperature ethanol steam reforming was studied. A significant build-up of carbonaceous intermediate, instead of carbon deposit, was observed at a lower reaction temperature which was attributed to the rapid catalyst deactivation. Co-feed experiments indicated that acetone and ethylene caused more severe catalyst deactivation than other oxygenates such as acidic acid and acetaldehyde.

  2. High Activity of Ce1-xNixO2-y for H2 Production through Ethanol Steam Reforming: Tuning Catalytic Performance through Metal-Oxide Interactions

    SciTech Connect

    G Zhou; L Barrio; S Agnoli; S Senanayake; J Evans; A Kubacka; M Estrella; J Hanson; A Martinez-Arias; et al.

    2011-12-31

    The importance of the oxide: Ce{sub 0.8}Ni{sub 0.2}O{sub 2-y} is an excellent catalyst for ethanol steam reforming. Metal-oxide interactions perturb the electronic properties of the small particles of metallic nickel present in the catalyst under the reaction conditions and thus suppress any methanation activity. The nickel embedded in ceria induces the formation of O vacancies, which facilitate cleavage of the OH bonds in ethanol and water.

  3. Effects of preparation method on the performance of Ni/Al(2)O(3) catalysts for hydrogen production by bio-oil steam reforming.

    PubMed

    Li, Xinbao; Wang, Shurong; Cai, Qinjie; Zhu, Lingjun; Yin, Qianqian; Luo, Zhongyang

    2012-09-01

    Steam reforming of bio-oil derived from the fast pyrolysis of biomass is an economic and renewable process for hydrogen production. The main objective of the present work has been to investigate the effects of the preparation method of Ni/Al(2)O(3) catalysts on their performance in hydrogen production by bio-oil steam reforming. The Ni/Al(2)O(3) catalysts were prepared by impregnation, co-precipitation, and sol-gel methods. XRD, XPS, H(2)-TPR, SEM, TEM, TG, and N(2) physisorption measurements were performed to characterize the texture and structure of the catalysts obtained after calcination and after their subsequent use. Ethanol and bio-oil model compound were selected for steam reforming to evaluate the catalyst performance. The catalyst prepared by the co-precipitation method was found to display better performance than the other two. Under the optimized reaction conditions, an ethanol conversion of 99% and a H(2) yield of 88% were obtained. PMID:21562805

  4. RADIOACTIVE DEMONSTRATION OF FINAL MINERALIZED WASTE FORMS FOR HANFORD WASTE TREATMENT PLANT SECONDARY WASTE BY FLUIDIZED BED STEAM REFORMING USING THE BENCH SCALE REFORMER PLATFORM

    SciTech Connect

    Crawford, C.; Burket, P.; Cozzi, A.; Daniel, W.; Jantzen, C.; Missimer, D.

    2012-02-02

    The U.S. Department of Energy's Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. In addition, the WTP LAW vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as {sup 137}Cs, {sup 129}I, {sup 99}Tc, Cl, F, and SO{sub 4} that volatilize at the vitrification temperature of 1150 C in the absence of a continuous cold cap (that could minimize volatilization). The current waste disposal path for the WTP-SW is to process it through the Effluent Treatment Facility (ETF). Fluidized Bed Steam Reforming (FBSR) is being considered for immobilization of the ETF concentrate that would be generated by processing the WTP-SW. The focus of this current report is the WTP-SW. FBSR offers a moderate temperature (700-750 C) continuous method by which WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline ceramic

  5. Effect of Bimetallic Ni-Cr Catalysts for Steam-CO2 Reforming of Methane at High Pressure.

    PubMed

    Choi, Bong Kwan; Park, Yoon Hwa; Moon, Dong Ju; Park, Nam Cook; Kim, Young Chul

    2015-07-01

    The present work was to carry out the development of high performance Ni-based catalyst for Steam-CO2 reforming of methane (SCR) which is suitable for Fischer-Tropsch synthesis of GTL- FPSO (floating, production, storage and offloading) process. The bimetallic Ni-Cr catalysts were prepared by co-impregnation method. The Ni and Cr loading amount were fixed at 12 wt% and 3~7 wt%, respectively. The catalytic reaction was conducted at 900 °C and 20 bar with reactant feed ratio of CH4:CO2:H2O:Ar = 1:0.8:1.3:1 and GHSV = 25,000 h(-1). The Cr-modified Ni/γ-Al2O3 catalyst was characterized by BET surface area analysis, X-ray diffraction (XRD), H2-temperature programmed reduction (TPR), H2-chmisorption, CO2-temperature programmed desorption (TPD) and Transmission electron microscopy(TEM). To confirm the amount and type of the carbon deposition, the used catalysts were examined by Thermogravitic analysis (TGA) and Field emission-scanning microscopy/Energy dispersive X-ray analysis (FE-SEM/EDX). It was found that the bimetallic Ni-Cr catalyst exhibits highly dispersed Ni particles with strong metal-to-support interaction (SMSI) as well as excellent catalytic activity, resulting in the suppression of Ni sintering and carbon deposition. PMID:26373119

  6. Secondary Waste Form Screening Test Results—THOR® Fluidized Bed Steam Reforming Product in a Geopolymer Matrix

    SciTech Connect

    Pires, Richard P.; Westsik, Joseph H.; Serne, R. Jeffrey; Mattigod, Shas V.; Golovich, Elizabeth C.; Valenta, Michelle M.; Parker, Kent E.

    2011-07-14

    Screening tests are being conducted to evaluate waste forms for immobilizing secondary liquid wastes from the Hanford Tank Waste Treatment and Immobilization Plant (WTP). Plans are underway to add a stabilization treatment unit to the Effluent Treatment Facility to provide the needed capacity for treating these wastes from WTP. The current baseline is to use a Cast Stone cementitious waste form to solidify the wastes. Through a literature survey, DuraLith alkali-aluminosilicate geopolymer, fluidized-bed steam reformation (FBSR) granular product encapsulated in a geopolymer matrix, and a Ceramicrete phosphate-bonded ceramic were identified both as candidate waste forms and alternatives to the baseline. These waste forms have been shown to meet waste disposal acceptance criteria, including compressive strength and universal treatment standards for Resource Conservation and Recovery Act (RCRA) metals (as measured by the toxicity characteristic leaching procedure [TCLP]). Thus, these non-cementitious waste forms should also be acceptable for land disposal. Information is needed on all four waste forms with respect to their capability to minimize the release of technetium. Technetium is a radionuclide predicted to be in the secondary liquid wastes in small quantities, but the Integrated Disposal Facility (IDF) risk assessment analyses show that technetium, even at low mass, produces the largest contribution to the estimated IDF disposal impacts to groundwater.

  7. Application of multisection packing concept to sorption-enhanced steam methane reforming reaction for high-purity hydrogen production

    NASA Astrophysics Data System (ADS)

    Lee, Chan Hyun; Mun, Sungyong; Lee, Ki Bong

    2015-05-01

    Hydrogen has been gaining popularity as a new clean energy carrier, and bulk hydrogen production is achieved through the steam methane reforming (SMR) reaction. Since hydrogen produced via the SMR reaction contains large amounts of impurities such as unreacted reactants and byproducts, additional purification steps are needed to produce high-purity hydrogen. By applying the sorption-enhanced reaction (SER), in which catalytic reaction and CO2 byproduct removal are carried out simultaneously in a single reactor, high-purity hydrogen can be directly produced. Additionally, the thermodynamic limitation of conventional SMR reaction is circumvented, and the SMR reaction process becomes simplified. To improve the performance of the SER, a multisection packing concept was recently proposed. In this study, the multisection packing concept is experimentally demonstrated by applying it to a sorption-enhanced SMR (SE-SMR) reaction. The experimental results show that the SE-SMR reaction is significantly influenced by the reaction temperature, owing to the conflicting dependence of the reaction rate and the CO2 sorption uptake on the reaction temperature. Additionally, it is confirmed that more high-purity hydrogen (<10 ppm of CO) can be produced by applying the multisection packing concept to the SE-SMR reactions operated at sufficiently high temperatures where the SMR reaction is not limited by rate.

  8. Effectiveness of heat-integrated methanol steam reformer and polymer electrolyte membrane fuel cell stack systems for portable applications

    NASA Astrophysics Data System (ADS)

    Lotrič, A.; Sekavčnik, M.; Hočevar, S.

    2014-12-01

    Efficiently combining proton exchange membrane fuel cell (PEMFC) stack with methanol steam reformer (MSR) into a small portable system is still quite a topical issue. Using methanol as a fuel in PEMFC stack includes a series of chemical processes where each proceeds at a unique temperature. In a combined MSR-PEMFC-stack system with integrated auxiliary fuel processors (vaporizer, catalytic combustor, etc.) the processes are both endothermic and exothermic hence their proper thermal integration can help raising the system efficiency. A concept of such fully integrated and compact system is proposed in this study. Three separate systems are designed based on different PEMFC stacks and MSR. Low-temperature (LT) and conventional high-temperature (cHT) PEMFC stack characteristics are based on available data from suppliers. Also, a novel high-temperature (nHT) PEMFC stack is proposed because its operating temperature coincides with that of MSR. A comparative study of modelled systems is performed using a mass and energy balances zero-dimensional model, which is interdependently coupled to a physical model based on finite element method (FEM). The results indicate that a system with nHT PEMFC stack is feasible and has the potential to reach higher system efficiencies than systems with LT or cHT PEMFC stacks.

  9. Carbon Deposition from the CO2-Steam Reforming of Methane Over Modified Ni/γ-Al2O3 Catalysts.

    PubMed

    Choi, Bong Kwan; Ok, Hye Jeong; Moon, Dong Ju; Kim, Jong Ho; Park, Nam Cook; Kim, Young Chul

    2015-01-01

    The aim of this work is to study the catalytic activity and suppression of carbon deposition in the CO2-Steam reforming of methane (SCR) to develop a high performance catalyst for GTL-FPSO application which is required to high pressure (20 bar) for F-T synthesis. Ni/La-X(6)/Al2O3 (X = Ce, Mg, Zr) catalysts were prepared by the impregnation method. The catalytic reaction was studied in a fixed bed reactor system at high pressure. X-ray diffraction (XRD), BET specific surface area and H2-temperature programmed reduction (TPR) were used to observe the characteristics of the prepared catalysts. The carbon deposition and the carbon amount in the used catalysts were examined by SEM and TGA, respectively. As a result, it was found that the Ni/La-Mg(6)/Al2O3 catalyst showed the highest activity and high carbon resistance. The highest activity in Ni/La-Mg(6)/Al2O3 was attributed to the proper Mg loading. It also had the lowest Ni particle and formed relatively stable MgAl2O4, which have an effect on the catalytic activity. PMID:26328367

  10. Thermodynamic analysis of Glycerol Steam Reforming for hydrogen production with in situ hydrogen and carbon dioxide separation

    NASA Astrophysics Data System (ADS)

    Silva, Joel M.; Soria, M. A.; Madeira, Luis M.

    2015-01-01

    A thermodynamic study of Glycerol Steam Reforming (GSR) for hydrogen production with in situ carbon dioxide and hydrogen (reaction products) simultaneous removal was performed. The sorption-enhanced membrane reactor (SEMR) was divided into multiple sub-Gibbs reactors and the Gibbs free energy minimization method was employed. The effects of temperature (600-800 K), molar water-to-glycerol feed ratio (WGFR) (3-9), pressure (1-5 atm) and fraction of hydrogen and carbon dioxide removal (f, 0-0.99) on the GSR process were target of investigation. A hydrogen yield (total moles of hydrogen produced/mole of reacted glycerol) very close to the stoichiometric value of 7 was obtained at 700 K, WGFR of 9, 1 atm and for fCO2 = 0.99 and fH2 = 0.80. This corresponds to an enhancement of 217%, 47% and 22% in terms of hydrogen yield comparatively to the traditional reactor (TR), sorption-enhanced reactor (SER) with carbon dioxide capture (fCO2 = 0.99) and membrane reactor (MR) with hydrogen separation (fH2 = 0.80) , respectively. In terms of coke, its formation was only observed under WGFRs below the stoichiometric value of 3.

  11. Structure and Activity of Pt-Ni Catalysts Supported on Modified Al2O3 for Ethanol Steam Reforming.

    PubMed

    Navarro, R M; Sanchez-Sanchez, M C; Fierro, J L G

    2015-09-01

    Modification of alumina with La-, Ce-, Zr- and Mg-oxides was studied with the aim to use them as supports of bimetallic Pt-Ni catalysts for the steam reforming of ethanol. Activity results showed that modifications of Al2O3 support with the incorporation of La, Ce, Zr or Mg oxides play an essential role in the catalytic behaviour of PtNi catalysts. Bimetallic PtNi catalyst supported on bare Al2O3 showed evolution of the reaction products with time on stream consisting in the increase of C2H4 production with concomitant decrease of CH4 and CO2 production. The addition of Mg or Zr to γ-A1203 did not inhibit the appearance of ethylene but delayed its production. In the case of Ce- or La-supported catalysts, the product selectivities were stable with time-on-stream, with no changes being observed in the product distribution for 24 h. Characterization results showed that La- and Ce-containing supports improves the Pt and Ni metal exposure values. The better stability achieved for Ce and La containing catalysts was inferred to be related with a participation/assistance of lanthanum and cerium entities in the gasification of coke deposits together with a modification of Pt and Ni dispersion which lower the probability of the nucleation of coke precursors on their surfaces. PMID:26716216

  12. Characterization and Leaching Tests of the Fluidized Bed Steam Reforming (FBSR) Waste Form for LAW Immobilization - 13400

    SciTech Connect

    Neeway, James J.; Qafoku, Nikolla P.; Peterson, Reid A.; Brown, Christopher F.

    2013-07-01

    Several supplemental technologies for treating and immobilizing Hanford low activity waste (LAW) have been evaluated. One such immobilization technology is the Fluidized Bed Steam Reforming (FBSR) granular product. The FBSR granular product is composed of insoluble sodium aluminosilicate (NAS) feldspathoid minerals. Production of the FBSR mineral product has been demonstrated both at the industrial and laboratory scale. Pacific Northwest National Laboratory (PNNL) was involved in an extensive characterization campaign. The goal of this campaign was to study the durability of the FBSR mineral product and the encapsulated FBSR product in a geo-polymer monolith. This paper gives an overview of results obtained using the ASTM C 1285 Product Consistency Test (PCT), the EPA Test Method 1311 Toxicity Characteristic Leaching Procedure (TCLP), and the ASTMC 1662 Single-Pass Flow-Through (SPFT) test. Along with these durability tests an overview of the characteristics of the waste form has been collected using Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD), microwave digestions for chemical composition, and surface area from Brunauer, Emmett, and Teller (BET) theory. (authors)

  13. Efficient utilization of greenhouse gases in a gas-to-liquids process combined with CO2/steam-mixed reforming and Fe-based Fischer-Tropsch synthesis.

    PubMed

    Zhang, Chundong; Jun, Ki-Won; Ha, Kyoung-Su; Lee, Yun-Jo; Kang, Seok Chang

    2014-07-15

    Two process models for carbon dioxide utilized gas-to-liquids (GTL) process (CUGP) mainly producing light olefins and Fischer-Tropsch (F-T) synthetic oils were developed by Aspen Plus software. Both models are mainly composed of a reforming unit, an F-T synthesis unit and a recycle unit, while the main difference is the feeding point of fresh CO2. In the reforming unit, CO2 reforming and steam reforming of methane are combined together to produce syngas in flexible composition. Meanwhile, CO2 hydrogenation is conducted via reverse water gas shift on the Fe-based catalysts in the F-T synthesis unit to produce hydrocarbons. After F-T synthesis, the unreacted syngas is recycled to F-T synthesis and reforming units to enhance process efficiency. From the simulation results, it was found that the carbon efficiencies of both CUGP options were successfully improved, and total CO2 emissions were significantly reduced, compared with the conventional GTL processes. The process efficiency was sensitive to recycle ratio and more recycle seemed to be beneficial for improving process efficiency and reducing CO2 emission. However, the process efficiency was rather insensitive to split ratio (recycle to reforming unit/total recycle), and the optimum split ratio was determined to be zero. PMID:24933030

  14. Studying the characteristics of a 5 kW power installation on solid-oxide fuel cells with steam reforming of natural gas

    NASA Astrophysics Data System (ADS)

    Munts, V. A.; Volkova, Yu. V.; Plotnikov, N. S.; Dubinin, A. M.; Tuponogov, V. G.; Chernishev, V. A.

    2015-11-01

    The results from tests of a 5 kW power plant on solid-oxide fuel cells (SOFCs), in which natural gas is used as fuel, are presented. The installation's process circuit, the test procedure, and the analysis of the obtained results are described. The characteristics of the power plant developed by the Ural Industrial Company are investigated in four steady-state modes of its operation: with the SOFC nominal power capacity utilized by 40% (2 kW), 60% (3 kW), 90% (4.5 kW) and 110% (5.4 kW) (the peaking mode). The electrical and thermodynamic efficiencies are calculated for all operating modes, and the most efficient mode, in which the electrical efficiency reached almost 70%, is determined. The air excess coefficient and heat loss with flue gases q 2 are determined, and it is revealed that the heat loss q 5 decreases from 40 to 25% with increasing the load. Thermal balances are drawn up for the following components of the system the reformer, the SOFC battery, the catalytic burner for afterburning anode gases, the heat exchanger for heating the cathode air and the mixture of natural gas and steam, and the actual fuel utilization rates in the electrochemical generator are calculated. An equation for the resulting natural gas steam reforming reaction was obtained based on the results from calculating the equilibrium composition of reforming products for the achieved temperatures at the reformer outlet t 3.

  15. Effect of variable conditions on steam reforming and aqueous phase reforming of n-butanol over Ni/CeO2 and Ni/Al2O3 catalysts

    NASA Astrophysics Data System (ADS)

    Roy, B.; Sullivan, H.; Leclerc, C. A.

    2014-12-01

    A comparison of aqueous phase reforming (APR) and steam reforming (SR) of n-butanol (n-BuOH) over Ni(20 wt%) loaded Al2O3 and CeO2 catalysts has been discussed in this paper. The BuOH conversion increases as the system pressure decreases in APR and SR. For both catalysts, the H2 and CO2 selectivity increased as the pressure increased in SR, reached a maximum at the bubble point pressure, and then decreased in the APR region. The Ni/CeO2 catalyst demonstrated higher selectivity for H2 and CO2than the Ni/Al2O3 catalyst during SR, which are consistent with the results of our previous publication on APR of n-butanol (n-BuOH) over similar catalysts. Unlike in APR, the Ni/CeO2 catalyst produced CO in SR. For both of the catalysts, the activation energies for H2 and CO2 production and BuOH conversion were lower in SR than that in APR. The proposed primary reaction pathway for reforming of BuOH on both catalysts is the same for APR and SR. The n-BuOH dehydrogenated to butaldehyde followed by decarbonylation to propane. Then the propane is steam reformed to hydrogen and carbon monoxide. The CO converts to CO2 mostly through water gas shift.

  16. The Effect of Fe in Perovskite Catalysts for Steam CO2 Reforming of Methane.

    PubMed

    Yang, Eun-Hyeok; Noh, Young-Su; Lim, Sung Soo; Ahn, Byoung Sung; Moon, Dong Ju

    2016-02-01

    In this work, La0.95Sr0.05Ni(1-x)Fe(x)O3 catalysts were prepared by modified EDTA-cellulose method and the catalysts were characterized by various techniques such as N2 physisorption, TPR, XRD, SEM, TEM-EDS and TG analysis. La00.95Sr0.05Ni0.5Fe0.5O3 catalyst showed better catalytic performance under the reaction conditions of 900 degrees C, 21 bar and feed molar ratio of CH4:CO2:H20 = 1:0.7:1.5. It is considered that the dilution effect on nickel prevented the formation of large monometallic ensembles that favour the carbon deposition in reforming reactions, and the mean metallic particle size of Ni decreased with increasing substitution rate in B site. Therefore, partial substitution of Fe in B site enhances the dilution effect and induces a reaction between CO2 and La2O3, thereby resisting the carbon deposition and increasing CO2 conversion. PMID:27433705

  17. Ethanol steam reforming in a molten carbonate fuel cell: a thermodynamic approach

    NASA Astrophysics Data System (ADS)

    Freni, S.; Maggio, G.; Cavallaro, S.

    The economy of the world energy sources is showing interest in the utilization of oxygenated products whose purpose is to improve the storage and the transfer of hydrogen as a non-polluting fuel with a high heat power density. An interesting field of utilization of these products is represented by the fuel cell systems for production of electricity. In this respect, the use of the water/ethanol mixture has been investigated as an alternative fuel for molten carbonate fuel cells. Some thermodynamic calculations have been carried out by a mathematical model to determine the energy and mass balances for a water/ethanol fuelled molten carbonate fuel cell. The thermodynamic efficiencies determined for this system have been correlated with the main operative parameters that give some interesting findings indicating encouraging aspects on the utilization of these systems to the production of electricity and heat. Lastly, attractive operative conditions have been determined and compared with that of a molten carbonate fuel cell with methane direct internal reforming.

  18. RADIOACTIVE DEMONSTRATIONS OF FLUIDIZED BED STEAM REFORMING AS A SUPPLEMENTARY TREATMENT FOR HANFORD'S LOW ACTIVITY WASTE AND SECONDARY WASTES

    SciTech Connect

    Jantzen, C.; Crawford, C.; Cozzi, A.; Bannochie, C.; Burket, P.; Daniel, G.

    2011-02-24

    The U.S. Department of Energy's Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. The Supplemental Treatment chosen will immobilize that portion of the retrieved LAW that is not sent to the WTP's LAW Vitrification facility into a solidified waste form. The solidified waste will then be disposed on the Hanford site in the Integrated Disposal Facility (IDF). In addition, the WTP LAW vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as Cs-137, I-129, Tc-99, Cl, F, and SO4 that volatilize at the vitrification temperature of 1150 C in the absence of a continuous cold cap. The current waste disposal path for the WTP-SW is to recycle it to the supplemental LAW treatment to avoid a large steady state accumulation in the pretreatment-vitrification loop. Fluidized Bed Steam Reforming (FBSR) offers a moderate temperature (700-750 C) continuous method by which LAW and/or WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates, sulfates/sulfides, chlorides

  19. Sustainable production of syngas from biomass-derived glycerol by steam reforming over highly stable Ni/SiC.

    PubMed

    Kim, Sung Min; Woo, Seong Ihl

    2012-08-01

    The production of syngas was investigated by steam reforming glycerol over Ni/Al(2)O(3), Ni/CeO(2), and Ni/SiC (which have acidic, basic, and neutral properties) at temperatures below 773 K. The complete and stable conversion of glycerol with a yield (higher than 90 %) of gaseous products (mainly syngas) was achieved over Ni/SiC during a 60 h reaction, whereas the conversion of glycerol continually decreases over Ni/Al(2)O(3) (by 49.8 %) and Ni/CeO(2) (by 77.1 %). The deactivation of Ni/Al(2)O(3) and Ni/CeO(2) is mainly caused by coke deposition because of the C-C cleavage of the byproducts produced by dehydration over acidic sites and condensation over basic sites. Gaseous products with a 1.0-1.9 syngas ratio (H(2)/CO) are produced over Ni/SiC. This ratio is required for the Fischer-Tropsch synthesis. However, a syngas ratio of more than 3.0 was observed over Ni/Al(2)O(3) and Ni/CeO(2) because of the high activity of the water-gas-shift reaction. Any dissociative or associative adsorption of water on Al(2)O(3) and CeO(2) promotes a water-gas-shift reaction and produces a higher syngas ratio. H(2) and CO were mainly produced by decomposition of glycerol through dehydrogenation and decarbonylation over Ni sites. Thus, SiC promotes an intrinsic contribution of nickel (dehydrogenation, and decarbonylation) without any byproducts from the dehydration and condensation. PMID:22753307

  20. RADIOACTIVE DEMONSTRATIONS OF FLUIDIZED BED STEAM REFORMING WITH ACUTAL HANFORD LOW ACTIVITY WASTES VERIFYING FBSR AS A SUPPLEMENTARY TREATMENT

    SciTech Connect

    Jantzen, C.; Crawford, C.; Burket, P.; Bannochie, C.; Daniel, G.; Nash, C.; Cozzi, A.; Herman, C.

    2012-01-12

    The U.S. Department of Energy's Office of River Protection is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level waste (HLW) and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the cleanup mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA). Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. Fluidized Bed Steam Reforming (FBSR) is one of the supplementary treatments being considered. FBSR offers a moderate temperature (700-750 C) continuous method by which LAW and other secondary wastes can be processed irrespective of whether they contain organics, nitrates/nitrites, sulfates/sulfides, chlorides, fluorides, and/or radio-nuclides like I-129 and Tc-99. Radioactive testing of Savannah River LAW (Tank 50) shimmed to resemble Hanford LAW and actual Hanford LAW (SX-105 and AN-103) have produced a ceramic (mineral) waste form which is the same as the non-radioactive waste simulants tested at the engineering scale. The radioactive testing demonstrated that the FBSR process can retain the volatile radioactive components that cannot be contained at vitrification temperatures. The radioactive and nonradioactive mineral waste forms that were produced by co-processing waste with kaolin clay in an FBSR process are shown to be as durable as LAW glass.

  1. Hierarchical copper-decorated nickel nanocatalysts supported on La2O3 for low-temperature steam reforming of ethanol.

    PubMed

    Liu, Jyong-Yue; Su, Wei-Nien; Rick, John; Yang, Sheng-Chiang; Cheng, Ju-Hsiang; Pan, Chun-Jern; Lee, Jyh-Fu; Hwang, Bing-Joe

    2014-02-01

    Copper/nickel nanocatalysts with a unique morphology were prepared by thermal reduction of a perovskite LaNix Cu1-x O3 precursor (x=1, 0.9, and 0.7). During thermal reduction, copper was first reduced and reacted with lanthanum to form metastable Cu5 La and Cu13 La. When the thermal reduction temperature was increased, the perovskite decomposed to Ni and La2 O3 , CuLa alloys disappeared, and Cu deposits on Ni nanoparticles were generated, thereby forming Cu/Ni nanocatalysts with hierarchical structures. Nanosized nickel, decorated with copper and supported on La2 O3 , could be produced at 520-550 °C. The steam reforming of ethanol was used as a model reaction to demonstrate the catalytic capability of the materials formed. The hierarchical structure of the Cu/Ni/La2 O3 catalysts confers synergetic effects that greatly favor the dehydrogenation of ethanol and which break the C-C bond to produce a higher yield of hydrogen at a low reaction temperature, whereas La2 O3 provides the required stability during the reaction. The reaction at 290 °C achieved almost 100 % conversion with a hydrogen yield reaching 2.21 molH2  mol(-1) EtOH thus indicating that this special structural feature can achieve high activity for the SRE at low temperatures. The proposed synthesis of nanocatalysts appears to be a good way to generate oxide-supported hierarchically structured nanoparticles that can also be applied to other reactions catalyzed by a heterogeneous metal oxide system. PMID:24307476

  2. Fluidized Bed Steam Reforming (FBSR) Mineralization for High Organic and Nitrate Waste Streams for the Global Nuclear Energy Partnership (GNEP)

    SciTech Connect

    Jantzen, C.M.; Williams, M.R.

    2008-07-01

    Waste streams that may be generated by the Global Nuclear Energy Partnership (GNEP) Advanced Energy Initiative may contain significant quantities of organics (0-53 wt%) and/or nitrates (0-56 wt%). Decomposition of high nitrate streams requires reducing conditions, e.g. organic additives such as sugar or coal, to reduce the NOx in the off-gas to N{sub 2} to meet the Clean Air Act (CAA) standards during processing. Thus, organics will be present during waste form stabilization regardless of which GNEP processes are chosen, e.g. organics in the feed or organics for nitrate destruction. High organic containing wastes cannot be stabilized with the existing HLW Best Developed Available Technology (BDAT) which is HLW vitrification (HLVIT) unless the organics are removed by preprocessing. Alternative waste stabilization processes such as Fluidized Bed Steam Reforming (FBSR) operate at moderate temperatures (650-750 deg. C) compared to vitrification (1150-1300 deg. C). FBSR converts organics to CAA compliant gases, creates no secondary liquid waste streams, and creates a stable mineral waste form that is as durable as glass. For application to the high Cs-137 and Sr-90 containing GNEP waste streams a single phase mineralized Cs-mica phase was made by co-reacting illite clay and GNEP simulated waste. The Cs-mica accommodates up to 30% wt% Cs{sub 2}O and all the GNEP waste species, Ba, Sr, Rb including the Cs-137 transmutation to Ba-137. For reference, the cesium mineral pollucite (CsAlSi{sub 2}O{sub 6}), currently being studied for GNEP applications, can only be fabricated at {>=}1000 deg. C. Pollucite mineralization creates secondary aqueous waste streams and NOx. Pollucite is not tolerant of high concentrations of Ba, Sr or Rb and forces the divalent species into different mineral host phases. The pollucite can accommodate up to 33% wt% Cs{sub 2}O. (authors)

  3. FLUIDIZED BED STEAM REFORMING MINERALIZATION FOR HIGH ORGANIC AND NITRATE WASTE STREAMS FOR THE GLOBAL NUCLEAR ENERGY PARTNERSHIP

    SciTech Connect

    Jantzen, C; Michael Williams, M

    2008-01-11

    Waste streams that may be generated by the Global Nuclear Energy Partnership (GNEP) Advanced Energy Initiative may contain significant quantities of organics (0-53 wt%) and/or nitrates (0-56 wt%). Decomposition of high nitrate streams requires reducing conditions, e.g. organic additives such as sugar or coal, to reduce the NO{sub x} in the off-gas to N{sub 2} to meet the Clean Air Act (CAA) standards during processing. Thus, organics will be present during waste form stabilization regardless of which GNEP processes are chosen, e.g. organics in the feed or organics for nitrate destruction. High organic containing wastes cannot be stabilized with the existing HLW Best Developed Available Technology (BDAT) which is HLW vitrification (HLVIT) unless the organics are removed by preprocessing. Alternative waste stabilization processes such as Fluidized Bed Steam Reforming (FBSR) operate at moderate temperatures (650-750 C) compared to vitrification (1150-1300 C). FBSR converts organics to CAA compliant gases, creates no secondary liquid waste streams, and creates a stable mineral waste form that is as durable as glass. For application to the high Cs-137 and Sr-90 containing GNEP waste streams a single phase mineralized Cs-mica phase was made by co-reacting illite clay and GNEP simulated waste. The Cs-mica accommodates up to 30% wt% Cs{sub 2}O and all the GNEP waste species, Ba, Sr, Rb including the Cs-137 transmutation to Ba-137. For reference, the cesium mineral pollucite (CsAlSi{sub 2}O{sub 6}), currently being studied for GNEP applications, can only be fabricated at {ge} 1000 C. Pollucite mineralization creates secondary aqueous waste streams and NO{sub x}. Pollucite is not tolerant of high concentrations of Ba, Sr or Rb and forces the divalent species into different mineral host phases. The pollucite can accommodate up to 33% wt% Cs{sub 2}O.

  4. Steam reforming of methanol over a Cu/ZnO/Al 2O 3 catalyst: a kinetic analysis and strategies for suppression of CO formation

    NASA Astrophysics Data System (ADS)

    Agrell, Johan; Birgersson, Henrik; Boutonnet, Magali

    Steam reforming of methanol (CH 3OH+H 2O→CO 2+3H 2) was studied over a commercial Cu/ZnO/Al 2O 3 catalyst for production of hydrogen onboard proton exchange membrane (PEM) fuel cell vehicles. A simple power-law rate expression was fitted to experimental data in order to predict the rates of CO 2 and H 2 formation under various reaction conditions. The apparent activation energy ( Ea) was estimated to be 100.9 kJ mol -1, in good agreement with values reported in the literature. Appreciable amounts of CO by-product were formed in the reforming process at low contact times and high methanol conversions. Being a catalyst poison that deactivates the electrocatalyst at the fuel cell anode at concentrations exceeding a few ppm, special attention was paid to the pathways for CO formation and strategies for its suppression. It was found that increasing the steam-methanol ratio effectively decreases CO formation. Likewise, addition of oxygen or air to the steam-methanol mixture minimises the production of CO. By shortening the contact time and lowering the maximum temperature in the reactor, CO production can be further decreased by suppressing the reverse water-gas shift reaction.

  5. 2009 PILOT SCALE FLUIDIZED BED STEAM REFORMING TESTING USING THE THOR (THERMAL ORGANIC REDUCTION) PROCESS: ANALYTICAL RESULTS FOR TANK 48H ORGANIC DESTRUCTION - 10408

    SciTech Connect

    Williams, M.; Jantzen, C.; Burket, P.; Crawford, C.; Daniel, G.; Aponte, C.; Johnson, C.

    2009-12-28

    The Savannah River Site (SRS) must empty the contents of Tank 48H, a 1.3 million gallon Type IIIA HLW storage tank, to return this tank to service. The tank contains organic compounds, mainly potassium tetraphenylborate that cannot be processed downstream until the organic components are destroyed. The THOR{reg_sign} Treatment Technologies (TTT) Fluidized Bed Steam Reforming (FBSR) technology, herein after referred to as steam reforming, has been demonstrated to be a viable process to remove greater than 99.9% of the organics from Tank 48H during various bench scale and pilot scale tests. These demonstrations were supported by Savannah River Remediation (SRR) and the Department of Energy (DOE) has concurred with the SRR recommendation to proceed with the deployment of the FBSR technology to treat the contents of Tank 48H. The Savannah River National Laboratory (SRNL) developed and proved the concept with non-radioactive simulants for SRR beginning in 2003. By 2008, several pilot scale campaigns had been completed and extensive crucible testing and bench scale testing were performed in the SRNL Shielded Cells using Tank 48H radioactive sample. SRNL developed a Tank 48H non-radioactive simulant complete with organic compounds, salt, and metals characteristic of those measured in a sample of the radioactive contents of Tank 48H. FBSR Pilot Scaled Testing with the Tank 48H simulant has demonstrated the ability to remove greater than 98% of the nitrites and greater than 99.5% of the nitrates from the Tank 48H simulant, and to form a solid product that is primarily alkali carbonate. The alkali carbonate is soluble and, thus, amenable to pumping as a liquid to downstream facilities for processing. The FBSR technology was demonstrated in October of 2006 in the Engineering Scale Test Demonstration (ESTD) pilot scale steam reformer at the Hazen Research Inc. (HRI) facility in Golden, CO. Additional ESTD tests were completed in 2008 and in 2009 that further demonstrated the

  6. Steam reforming of fast pyrolysis-derived aqueous phase oxygenates over Co, Ni, and Rh metals supported on MgAl2O4

    DOE PAGESBeta

    Xing, Rong; Dagle, Vanessa Lebarbier; Flake, Matthew; Kovarik, Libor; Albrecht, Karl O.; Deshmane, Chinmay; Dagle, Robert A.

    2016-02-03

    In this paper we examine the feasibility of steam reforming the mixed oxygenate aqueous fraction derived from fast pyrolysis bio-oils. Catalysts selective towards hydrogen formation and resistant to carbon formation utilizing feeds with relatively low steam-to-carbon (S/C) ratios are desired. Rh (5 wt%), Pt (5 wt%), Ru (5 wt%), Ir (5 wt%), Ni (15 wt%), and Co (15 wt%) metals supported on MgAl2O4 were evaluated for catalytic performance at 500 °C and 1 atm using a complex feed mixture comprising acids, polyols, cycloalkanes, and phenolic compounds. The Rh catalyst was found to be the most active and resistant to carbonmore » formation. The Ni and Co catalysts were found to be more active than the other noble metal catalysts investigated (Pt, Ru, and Ir).« less

  7. Kinetic Study on the Effect of Chromium Addition to Ni-Based Catalysts for the Steam-CO2 Reforming of Methane.

    PubMed

    Park, Yoon-Hwa; Li, Peng; Moon, Dong-Ju; Park, Nam-Cook; Kim, Young-Chul

    2016-02-01

    In the present work, the kinetic effects of Ni-based catalysts containing various amounts of Cr on the steam-CO2 reforming (SCR) of methane were studied. Kinetic expressions for the SCR of methane over the Ni-based catalysts have been proposed using the power-law rate expression, based on the kinetic data obtained. In addition, the Arrhenius equation was used for calculating the activation energy. Analysis of the data revealed four simple results. Firstly, the partial pressure of CH4 exerts a major influence on the CH4 conversion rates. Secondly, the CH4 conversion rate is inversely proportional to the partial pressure of CO2. Thirdly, the partial pressure of steam has a very slight effect on the reaction rates. Finally, all the catalysts studied have similar apparent activation energies. PMID:27433614

  8. Hydrogen production by steam reforming of liquefied natural gas (LNG) over nickel catalysts supported on cationic surfactant-templated mesoporous aluminas

    NASA Astrophysics Data System (ADS)

    Seo, Jeong Gil; Youn, Min Hye; Park, Sunyoung; Jung, Ji Chul; Kim, Pil; Chung, Jin Suk; Song, In Kyu

    Two types of mesoporous γ-aluminas (denoted as A-A and A-S) are prepared by a hydrothermal method under different basic conditions using cationic surfactant (cetyltrimethylammonium bromide, CTAB) as a templating agent. A-A and A-S are synthesized in a medium of ammonia solution and sodium hydroxide solution, respectively. Ni/γ-Al 2O 3 catalysts (Ni/A-A and Ni/A-S) are then prepared by an impregnation method, and are applied to hydrogen production by steam reforming of liquefied natural gas (LNG). The effect of a mesoporous γ-Al 2O 3 support on the catalytic performance of Ni/γ-Al 2O 3 is investigated. The identity of basic solution strongly affects the physical properties of the A-A and A-S supports. The high surface-area of the mesoporous γ-aluminas and the strong metal-support interaction of supported catalysts greatly enhance the dispersion of nickel species on the catalyst surface. The well-developed mesopores of the Ni/A-A and Ni/A-S catalysts prohibit the polymerization of carbon species on the catalyst surface during the reaction. In the steam reforming of LNG, both Ni/A-A and Ni/A-S catalysts give better catalytic performance than the nickel catalyst supported on commercial γ-Al 2O 3 (Ni/A-C). In addition, the Ni/A-A catalyst is superior to the Ni/A-S catalyst. The relatively strong metal-support interaction of Ni/A-A catalyst effectively suppresses the sintering of metallic nickel and the carbon deposition in the steam reforming of LNG. The large pores of the Ni/A-A catalyst also play an important role in enhancing internal mass transfer during the reaction.

  9. Steam reforming of n-hexane on pellet and monolithic catalyst beds. A comparative study on improvements due to heat transfer

    NASA Technical Reports Server (NTRS)

    1981-01-01

    Monolithic catalysts with higher available active surface areas and better thermal conductivity than conventional pellets beds, making possible the steam reforming of fuels heavier than naphtha, were examined. Performance comparisons were made between conventional pellet beds and honeycomb monolith catalysts using n-hexane as the fuel. Metal-supported monoliths were examined. These offer higher structural stability and higher thermal conductivity than ceramic supports. Data from two metal monoliths of different nickel catalyst loadings were compared to pellets under the same operating conditions. Improved heat transfer and better conversion efficiencies were obtained with the monolith having higher catalyst loading. Surface-gas interaction was observed throughout the length of the monoliths.

  10. Alleviating coking in ethanol steam reforming by co-loading binary oxides Ni-M (M=Ag, Cu, Mn) on peony-like ceria

    NASA Astrophysics Data System (ADS)

    Xian, C. N.; Li, J. G.; Li, H.; Chen, L. Q.; Sun, J.; Lee, J. S.

    2011-06-01

    Previously, hydrothermally prepared mesoporous peony-like ceria (PCO) material was shown to exhibit superior catalytic properties for CO oxidation and ethanol reforming. Ni supported PCO had been shown to have high activity for ethanol steam reforming at low temperature. In this work, Ag, Cu and Mn is co-loaded with Ni on PCO catalysts by impregnation method. The catalysts were studied by X-ray diffraction (XRD), scanning electron microscopy (SEM), and a combined thermogravimetry, differential scanning calorimetry, and mass spectrometry (TG-DSC-MS). It was found that all the catalysts gave 100% ethanol conversion above ca. 300°C and exhibited similar H2 yield. It is found that the severe coking problem for the Ni-loaded PCO catalyst was alleviated significantly if Ag, Cu or Mn is co-loaded. Among them, the addition of Mn is the most effective in reducing carbon formation.