Including Decomposing Water Patents (Class 423/652)
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Publication number: 20020041842Abstract: Provided is a trap and method for removing hydrogen sulfide from a gas stream. The hydrogen sulfide trap includes a monolith substrate on which is disposed zinc oxide, and a second metal or oxide thereof. In some aspects, the hydrogen sulfide trap is advantageously incorporated into systems for producing hydrogen for PEM fuel cells.Type: ApplicationFiled: September 26, 2001Publication date: April 11, 2002Applicant: ENGELHARD CORPORATIONInventors: Wolfgang F. Ruettinger, Robert J. Farrauto, Lawrence Shore
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Publication number: 20020031471Abstract: The present invention is a method and apparatus (vessel) for providing a heat transfer rate from a reaction chamber through a wall to a heat transfer chamber substantially matching a local heat transfer rate of a catalytic thermal chemical reaction. The key to the invention is a thermal distance defined on a cross sectional plane through the vessel inclusive of a heat transfer chamber, reaction chamber and a wall between the chambers. The cross sectional plane is perpendicular to a bulk flow direction of the reactant stream, and the thermal distance is a distance between a coolest position and a hottest position on the cross sectional plane. The thermal distance is of a length wherein the heat transfer rate from the reaction chamber to the heat transfer chamber substantially matches the local heat transfer rate.Type: ApplicationFiled: July 27, 1998Publication date: March 14, 2002Inventors: ANNA LEE Y. TONKOVICH, YONG WANG, ROBERT S. WEGENG, YUFEI GAO
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Patent number: 6348278Abstract: The present invention provides a method and system for efficiently producing hydrogen that can be supplied to a fuel cell. The method and system of the present invention produces hydrogen in a reforming reactor using a hydrocarbon stream and water vapor stream as reactants. The hydrogen produced is purified in a hydrogen separating membrane to form a retentate stream and purified hydrogen stream. The purified hydrogen can then be fed to a fuel cell where electrical energy is produced and a fuel cell exhaust stream containing water vapor and oxygen depleted air is emitted. In one embodiment of the present invention, a means and method is provided for recycling a portion of the retentate stream to the reforming reactor for increased hydrogen yields. In another embodiment, a combustor is provided for combusting a second portion of the retentate stream to provide heat to the reforming reaction or other reactants.Type: GrantFiled: June 1, 1999Date of Patent: February 19, 2002Assignee: Mobil Oil CorporationInventors: Rene B. LaPierre, Randall D. Partridge
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Patent number: 6342197Abstract: The present invention relates to an improvement of integrated fuel processor and fuel cell systems which improves stability of operation, simplifies control, and improves the heat recovery. According to the invention, a reforming zone is heated by indirect heat exchange with a first combustion effluent stream and provides a cooled first combustion effluent stream. The cooled combustion effluent stream is reheated in at least an additional combustion zone with at least a portion of the anode waste gas from the fuel cell to provide a reheated combustion effluent stream. The reheated combustion effluent stream is employed to further heat the reforming zone.Type: GrantFiled: March 29, 2000Date of Patent: January 29, 2002Assignee: UOP LLCInventors: John J. Senetar, Gavin P. Towler, John R. Harness
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Patent number: 6340437Abstract: Disclosed is a process for producing a synthesis gas by an autothermal reforming method including a step of partially oxidizing a carbon-containing organic compound to produce a high temperature mixed gas, and a synthesis producing step of reacting the unreacted carbon-containing organic compound contained in the high temperature mixed gas with carbon dioxide and/or steam, wherein a catalyst having a considerably suppressed carbon deposition activity is used as a catalyst for the synthesis gas producing step. The catalyst is characterized in that the catalyst comprises a carrier formed of a metal oxide, and at least one catalytic metal selected from rhodium, ruthenium, iridium, palladium and platinum and supported on the carrier, in that the catalyst has a specific surface area of 25 m2/g or less, in that metal ion of the carrier metal oxide has electronegativity of 13.0 or less, and in that the amount of the catalytic metal supported is 0.0005-0.Type: GrantFiled: March 11, 1999Date of Patent: January 22, 2002Assignee: Chiyoda CorporationInventors: Fuyuki Yagi, Atsuro Nagumo, Yukitaka Wada, Mitsunori Shimura, Sachio Asaoka, Shuhei Wakamatsu
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Patent number: 6338833Abstract: Process for the preparation of a hydrogen and/or carbon monoxide rich gas from a hydrocarbon feedstock comprising partial oxidation of the feedstock with an oxidant supplied by permeation through a membrane and steam reforming of the feedstock in presence of a steam reforming catalyst being arranged on permeation side of the membrane, wherein steam reforming activity of catalyst is reduced at inlet region of the catalyst bed.Type: GrantFiled: February 23, 2000Date of Patent: January 15, 2002Assignee: Haldor Topsoe A/SInventor: Kim Aasberg-Petersen
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Publication number: 20010055559Abstract: Process for the production of hydrogen consisting in subjecting a solid to oxidation and treating, in a different zone, the oxidized form thus produced with a reducing stream, preferably a hydrocarbon.Type: ApplicationFiled: March 19, 2001Publication date: December 27, 2001Applicant: Snamprogetti S.p.A.Inventors: Domenico Sanfilippo, Alberto Paggini, Valerio Piccoli, Roberta Miglio, Stefano Rossini
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Patent number: 6331283Abstract: A process of producing hydrogen by autothermal steam reformation of a hydrocarbon comprises the steps of providing a reactor vessel having a fluidized catalyst bed, introducing steam and a gaseous hydrocarbon, introducing oxygen, maintaining the bed temperature below the spontaneous combustion temperature of the hydrocarbon in a fluidized bed, and withdrawing hydrogen by means of a perm selective membrane. An apparatus for producing hydrogen comprises a reactor vessel, steam and hydrocarbon inlets, an oxygen inlet, a fluidized bed of catalyst within the reactor vessel and a perm selective membrane for withdrawing hydrogen from the reactor.Type: GrantFiled: September 16, 1999Date of Patent: December 18, 2001Assignee: University Technologies International Inc.Inventors: Surajit Roy, Barry Pruden, Alaa Adris, John Grace
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Patent number: 6328945Abstract: A process for producing carbon monoxide (CO) by reforming methane and steam in the presence of a reforming catalyst to produce a reformate product enriched in CO, carbon dioxide (CO2) and hydrogen. CO2 in the enriched reformate is shifted to CO in an integrated sorption enhanced reaction (SER) cycle which employs a series of cyclic steps to facilitate reaction of CO2 and hydrogen at high conversion and to produce a CO-enriched product obtained at reactor feed pressure and at essentially constant flow rate. A series of adsorbent regeneration step including depressurization, purging and product pressurization are used to desorb water which is selectively adsorbed by the adsorbent during the shift reaction and to prepare the reactor for a subsequent process cycle.Type: GrantFiled: April 8, 1996Date of Patent: December 11, 2001Assignee: Air Products and Chemicals, Inc.Inventors: Jeffrey Raymond Hufton, Shivaji Sircar, William Frederick Baade, Joseph Michael Abrardo, Madhu Anand
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Patent number: 6315973Abstract: A cyclic process for operating an equilibrium controlled reaction in a plurality of reactors containing an admixture of an adsorbent and a reaction catalyst suitable for performing the desired reaction which is operated in a predetermined timed sequence wherein the heating and cooling requirements in a moving reaction mass transfer zone within each reactor are provided by indirect heat exchange with a fluid capable of phase change at temperatures maintained in each reactor during sorpreaction, depressurization, purging and pressurization steps during each process cycle.Type: GrantFiled: April 8, 1996Date of Patent: November 13, 2001Assignee: Air Products and Chemicals, Inc.Inventors: Shankar Nataraj, Brian Thomas Carvill, Jeffrey Raymond Hufton, Steven Gerard Mayorga, Thomas Richard Gaffney, Jeffrey Richard Brzozowski
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Patent number: 6312660Abstract: Disclosed is a process for producing a synthesis gas by reacting a carbon-containing organic compound with steam and/or carbon dioxide using a catalyst whose carbon deposition activity is considerably suppressed. The catalyst is characterized in that it comprises a carrier formed of a metal oxide, and at least one catalytic metal selected from rhodium, ruthenium, iridium, palladium and platinum and supported on the carrier, in that the catalyst has a specific surface area of 25 m2/g or less, in that the electronegativity of the metal ion of the carrier metal oxide is 13.0 or less and in that the amount of the catalytic metal is 0.0005-0.1 mole %, in terms of metal, based on the carrier metal oxide.Type: GrantFiled: March 11, 1999Date of Patent: November 6, 2001Assignee: Chiyoda CorporationInventors: Fuyuki Yagi, Atsuro Nagumo, Yukitaka Wada, Mitsunori Shimura, Sachio Asaoka, Shuhei Wakamatsu
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Patent number: 6303089Abstract: The invention is a process to recover a high pressure hydrogen-rich gas stream from a purge gas stream taken from a hydrotreater. This purge gas stream is admixed with synthesis gas that was the original source of the hydrogen to form a gaseous mixture. This mixed gas comprising purge gas and synthesis gas is advantageously treated to remove acid gases and possibly other impurities. The mixed gas is then treated to extract a hydrogen-rich gas and a hydrogen-depleted gas using, for example, a membrane. At least a portion of the hydrogen-rich gas is then heated and compressed as necessary and is recycled to the hydrotreater.Type: GrantFiled: January 11, 2000Date of Patent: October 16, 2001Assignee: Texaco Inc.Inventors: Paul S. Wallace, Kay Anderson Johnson
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Patent number: 6299853Abstract: A system for generating hydrogen-rich gas has a reformer for catalytic water vapor reforming of a water vapor/fuel mixture by an input supply of thermal energy, and a CO oxidation stage for removing carbon monoxide from the hydrogen-rich gas while emitting heat, with the reformer and the CO oxidation stage being thermally coupled. An oxygen quantity fed to the CO oxidation stage is adjusted as a function of the gas temperature in or at the output of the reformer/oxidation stage. This can take place by an automatic (feedback) control, a combination of open loop control and automatic control or by an adaptive characteristic diagram.Type: GrantFiled: October 13, 1999Date of Patent: October 9, 2001Assignee: Xcellsis GmbHInventors: Stefan Boneberg, Stefan Brauchle, Dirk Georg, Joachim Guertler, Martin Schaefer, Martin Schuessler, Matthias Wolfsteiner
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Patent number: 6299994Abstract: Hydrogen generation and fuel cell operation are integrated through the use of a low-cost hydrogen generation zone which comprises a pre-reforming zone, a partial oxidation zone, a reforming zone, and a water gas shift zone. Anode waste gas from the fuel cell is burned to provide heat to pre-reform the feed to the hydrogen generation zone while the burner exit temperature and the reforming zone exit temperatures are controlled to eliminate thermal cycling in the hydrogenation zone. This simplified control of the hot side temperatures in the hydrogen generation zone below about 700° C. combined with use of the pre-reforming zone, surprisingly permits the use of carbon steel and/or stainless steel for construction of the hydrogenation zone while providing an efficient system which does not require external fuel and offers a high degree of feedstock flexibility at low cost.Type: GrantFiled: June 18, 1999Date of Patent: October 9, 2001Assignee: UOP LLCInventors: Gavin P. Towler, Kishore J. Doshi, Kurt M. Vanden Bussche, John J. Senetar
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Patent number: 6299995Abstract: Disclosed is a hydrogen generation process for use with fuel cells which includes a preferential oxidation step to reduce the concentration of carbon monoxide. The preferential oxidation step includes contacting a fuel stream comprising hydrogen and carbon monoxide in the presence of an oxygen at a preferential oxidation temperature of between about 70° and about 160° C. with preferential oxidation catalyst for reducing the concentration of carbon monoxide to produce a treated fuel gas stream comprising less than about 50 ppm-vol carbon monoxide. The preferential oxidation catalyst comprises ruthenium metal disposed on an alumina carrier having a low density and a high porosity. Superior performance at low preferential oxidation temperatures below 130° C. was observed when the alumina carrier contained a bimodal pore distribution with an average pore distribution of from about 20 to about 3000 angstroms.Type: GrantFiled: May 31, 2000Date of Patent: October 9, 2001Assignee: UOP LLCInventors: Suheil F. Abdo, Cynthia A. DeBoy, Geralyn F. Schroeder
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Patent number: 6298652Abstract: The invention is directed to a method of fueling gas turbines from natural gas reserves with relatively low methane concentrations. The invention uses such reserves to generate electric power. The invention permits the use of these reserves at significantly lower cost than by producing pipeline natural gas to fuel gas turbines to generate electric power. These reserves currently generally are used only after the removal of impurities to produce pipeline natural gas quality turbine fuel. The latter current technology is capital intensive, and at current natural gas prices, economically unattractive. The process of the invention can remove the impurities from the gas from the natural gas reserve necessary for protection of the environment, and leaves inert gasses in the fuel in an amount which will increase the output of a gas turbine for the generation of power by about 5 to about 20%.Type: GrantFiled: December 13, 1999Date of Patent: October 9, 2001Assignee: Exxon Mobil Chemical Patents Inc.Inventors: Frank F. Mittricker, Donald J. Victory
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Publication number: 20010025010Abstract: A hydrocarbon-based fuel reforming catalyst that suffers less capability deterioration and has excellent heat resistance and excellent durability is disclosed. The reforming catalyst includes CuOx/ZnO/ZrO2/MnOx or CuOx/ZnO/ZrO2/Y2O3 formed by adding manganese or yttrium to a reforming catalyst composed of copper, zinc and zirconium. If manganese is added, the ratio of manganese to the sum of manganese and zirconium (n/(Mn+Zr)) is from about 0.1 to about 0.62 and, preferably, about 0.17 to about 0.5, and the ratio of copper to the sum of copper and zinc (Cu/(Cu+Zn)) is from about 0.2 to about 0.6 and, preferably, about 0.3 to about 0.48. The reforming catalyst exhibits less capability deterioration and good durability in the steam reforming reaction of methanol.Type: ApplicationFiled: February 12, 2001Publication date: September 27, 2001Applicant: TOYOTA JIDOSHA KABUSHIKI KAISHAInventor: Takeshi Hirabayashi
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Patent number: 6294149Abstract: The invention relates to a process for operating a system for the water vapor reforming of a hydrocarbon. The system includes a reactor which is suitable for POX operation as well as for a reforming operation, an evaporator, a hydrogen separating stage, and a catalytic burner device. A first part of the catalytic burner device is in thermal contact with the reforming reactor, and a second part of the burner device is in thermal contact with the evaporator. An air/hydrocarbon intermediate feeding pipe for the reactor and a pressure maintaining valve are provided for changing the reactor between the POX operation and the reforming operation. According to the process, during cold start of the system, a heating operation is carried out during which the reactor is first used in the POX operation at a lower pressure and subsequently is used for the reforming operation and simultaneously the pressure is increased to the normal operating pressure.Type: GrantFiled: December 16, 1998Date of Patent: September 25, 2001Assignee: Xcellsis GmbHInventors: Rainer Autenrieth, Stefan Boneberg, Thomas Poschmann, Martin Schuebler, Steffen Wieland
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Patent number: 6290877Abstract: The present invention presents: (1) a starting method that is capable of quickly switching to the reforming process after warming up a catalyst; (2) a fuel supplying apparatus that is capable of maintaining a stable supply of a mixed water-methanol solution while preventing water from freezing in a cold climate, and is also capable of immediately supplying a mixed water-methanol gas that has a composition which is outside of the high-rate reaction region during the starting/stopping operation of the reformer when the control tends to be unstable; (3) a method to quickly cool down a catalyst layer without causing thermal runaway when stopping the operation of the methanol reforming apparatus; and (4) a method to quickly cool down the catalyst layer while preventing thermal runaway from occurring and removing residual fuel when stopping the operation of the methanol reforming apparatus.Type: GrantFiled: November 30, 2000Date of Patent: September 18, 2001Assignees: Honda Giken Kogyo Kabushiki Kaisha, Mitsubishi Gas Chemical Co., Inc.Inventors: Takahiro Naka, Hideaki Sumi, Masataka Furuyama, Shoji Isobe, Yasushi Hiramatsu, Mikio Yoneoka
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Patent number: 6284157Abstract: In a discharge reactor with a low-current gas discharge, an inlet gas made of a CH4—CO2 gas mixture is converted into a synthesis gas having an H2—CO gas mixture which has a higher energy content than the inlet gas. For a predeterminable synthesis gas volume ratio R=H2/CO, the requisite CO2 proportion in the inlet gas can be derived from a function curve (f) or calculated according to V=−4.76·R3+37.57·R2−99.13·R+105.39.Type: GrantFiled: December 28, 1998Date of Patent: September 4, 2001Assignee: ABB Research Ltd.Inventors: Baldur Eliasson, Ulrich Kogelschatz, Li-Ming Zhou
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Patent number: 6280864Abstract: Hydrogen generation and fuel cell operation are integrated through the use of a low-cost hydrogen generation zone which comprises a pre-reforming zone, a partial oxidation zone, a reforming zone, and a water gas shift zone. Anode waste gas from the fuel cell is burned to provide heat to pre-reform the feed to the hydrogen generation zone while the burner exit temperature and the reforming zone exit temperatures are controlled using a simplified control system to eliminate thermal cycling in the hydrogenation zone. This simplified control of the hot side temperatures in the hydrogen generation zone below about 700° C. combined with use of the pre-reforming zone, surprisingly permits the use of carbon steel and/or stainless steel for construction of the hydrogenation zone while providing an efficient system which does not require external fuel and offers a high degree of feedstock flexibility at low cost.Type: GrantFiled: June 18, 1999Date of Patent: August 28, 2001Assignee: UOP LLCInventors: Gavin P. Towler, Kishore J. Doshi, Kurt M. Vanden Bussche, John J. Senetar
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Patent number: 6280701Abstract: A method for the treatment of a methanol reforming catalyst includes pre-aging the catalyst by baking it out in a dry atmosphere in order thereby to complete its inherent initial loss of volume before the start of the methanol reforming reaction. The method may be used for methanol reforming reactors in fuel-cell-operated motor vehicles.Type: GrantFiled: May 11, 2000Date of Patent: August 28, 2001Assignees: Xcellsis GmbH, BASF AktiengesellschaftInventors: Rainer Autenrieth, Otto Krumberger
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Patent number: 6268075Abstract: The invention relates to a process for operating a system for the water vapor reforming of a hydrocarbon, having an evaporator, a reforming reactor, a membrane module connected behind, and a catalytic burner device. According to the invention, a first part of the catalytic burner device is in thermal contact with the reforming reactor, and a second part of the burner device is in thermal contact with the evaporator. According to the process, a heating operation is carried out during the cold start of the system, in which, in a first operating phase, at least the evaporator and the reforming reactor are heated by the catalytic burner device, and in a second operating phase, a hydrocarbon/water vapor mixture is prepared in the evaporator at a water/hydrocarbon ratio which is higher than in the normal operation and is fed to the reactor, the substance mixture emerging from the reactor being fed by way of the membrane module to the catalytic burner device.Type: GrantFiled: December 16, 1998Date of Patent: July 31, 2001Assignee: Xcellsis GmbHInventors: Rainer Autenrieth, Stefan Boneberg, Dietmar Heil, Thomas Poschmann, Steffen Wieland
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Patent number: 6264856Abstract: A reforming reactor, particularly for the water vapor reforming of methanol, with three serially arranged reactor steps, each of which is charged with a catalyst pellet fill. According to the invention, the center reactor step is maintained at a temperature which is suitable for the reforming reaction, while the two other reactor steps remain unheated. The present invention may be used as a reforming reactor for the water vapor reforming of methanol for the purpose of producing hydrogen in a fuel-cell operated motor vehicle.Type: GrantFiled: December 30, 1999Date of Patent: July 24, 2001Assignee: DaimlerChrysler AGInventors: Rainer Autenrieth, Josef Haenfling, Dietmar Heil, Heinz Steinke, Norbert Wiesheu
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Patent number: 6254848Abstract: A system for generating a high-hydrogen gas comprises a reformer for the catalytic water vapor reforming of a water vapor/fuel mixture while supplying thermal energy; a gas purification stage for removing carbon monoxide from the high-hydrogen gas while releasing heat; and devices for transmitting thermal energy from the gas purification stage into the reformer. The reaction rates in the reformer and in the gas purification stage are designed such that a defined temperature level is set automatically by the coupling of the two reactions.Type: GrantFiled: December 30, 1999Date of Patent: July 3, 2001Assignee: Xcellsis GmbHInventors: Rainer Autenrieth, Barbara Strobel
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Patent number: 6254839Abstract: A hydrocarbon fuel reformer (200) is disclosed suitable for producing synthesis hydrogen gas from reactions with hydrocarbons fuels, oxygen, and steam. The reformer (200) comprises first and second tubes (208,218). The first tube (208) includes a first catalyst (214) and receives a first mixture of steam and a first fuel. The second tube (218) is annularly disposed about the first tube (208) and receives a second mixture of an oxygen-containing gas and a second fuel. In one embodiment, a third tube (224) is annularly disposed about the second tube (218) and receives a first reaction reformate from the first tube (208) and a second reaction reformate from the second tube (218). A catalyst reforming zone (260) annularly disposed about the third tube (224) may be provided to subject reformate constituents to a shift reaction. In another embodiment, a fractionator is provided to distill first and second fuels from a fuel supply source.Type: GrantFiled: November 3, 1998Date of Patent: July 3, 2001Assignee: Arthur D. Little, Inc.Inventors: Lawrence G. Clawson, William L. Mitchell, Jeffrey M. Bentley, Johannes H. J. Thijssen
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Patent number: 6254807Abstract: A process for enhancing H2 or CO production in a partial oxidation reaction by feeding H2O or CO2 with the feed hydrocarbon and oxygen over a transition metal monolith catalyst such as unsupported Ni monolith or alternatively contacting the hydrocarbon/oxygen first with a noble metal then with a transition metal with the H2O or CO2 being added before or after the noble metal catalyst. The addition of H2O suppresses CO and enhances H2 production and the addition of CO2 suppresses H2 and enhances CO production. Little steam or CO2 reforming occurs with the addition of up to 32% H2O or CO2 respectively. Thus, the ratio of H2:CO which is about 2 in a conventional partial oxidation is manipulated by the addition of either water or CO2 to the partial oxidation.Type: GrantFiled: January 12, 1998Date of Patent: July 3, 2001Assignee: Regents of the University of MinnesotaInventors: Lanny D. Schmidt, Paul M. Witt
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Publication number: 20010005500Abstract: A process for generating a high-hydrogen, low-carbon monoxide gas comprises generating a product gas in a gas generating device. The product gas contains hydrogen and carbon monoxide that are generated from catalytic water vapor reforming of a water/fuel mixture and/or from partial oxidation of an oxygen/fuel mixture. In a gas purification stage, the carbon monoxide fraction in the product gas is reduced by selective CO oxidation on an oxidation catalyst. During a starting phase, oxygen is admixed to the supplied fuel and the flow direction is reversed such that the flow first takes place through the gas purification stage and only then through the gas generating device.Type: ApplicationFiled: February 21, 2001Publication date: June 28, 2001Applicant: XCELLSIS GmbHInventors: Martin Schuessler, Barbara Strobel, Detlef zur Megede
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Publication number: 20010002248Abstract: This specification discloses a hydrogen generating apparatus comprising a reformer, a heating section, a fuel supply section, a water supply section, a shift reactor with a shift catalyst layer, a first heat exchanger on the downstream side of the shift catalyst layer, and a temperature detector for the shift catalyst layer. It is the most notable feature of the hydrogen generating apparatus of the present invention that the temperature of the downstream portion of the shift catalyst layer is raised by the action of the heat exchanger compared with the temperature of the same before the amount of the reformed gas is increased. And, the temperature of the downstream portion is lowered compared with the temperature of the same before the amount of the reformed gas is reduced when reducing the amount of the reformed gas.Type: ApplicationFiled: September 9, 1999Publication date: May 31, 2001Inventors: KUNIHIRO UKAI, KIMIYASU HONDA, KIYOSHI TAGUCHI, TAKESHI TOMIZAWA, KOUICHIRO KITAGAWA, TOSHIYUKI SHONO
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Patent number: 6238816Abstract: A process and apparatus for steam reforming of hydrocarbons, using a sulfur-tolerant catalyst comprising an active phase and a support phase, and optionally a promoter, which provides substantially complete conversion of the hydrocarbon to a mixture of hydrogen, carbon monoxide, and carbon dioxide. The process comprises introducing steam and a hydrocarbon feed containing at least about 2 ppm sulfur species into the apparatus, and reacting said steam and hydrocarbon feed in the catalyst bed.Type: GrantFiled: January 13, 1999Date of Patent: May 29, 2001Assignee: Technology Management, Inc.Inventors: Thomas L. Cable, Adam B. Brakas, Robert C. Ruhl, Christopher E. Milliken
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Patent number: 6235262Abstract: A process for the production of hydrogen rich gas by soot free autothermal steam reforming of a hydrogen process gas, wherein the hydrogen rich gas being withdrawn from the autothermal steam reforming process at elevated pressure is depressurized in a gas turbine for generation of valuable power.Type: GrantFiled: April 15, 1999Date of Patent: May 22, 2001Assignee: Haldor Topsoe A/SInventor: Henrik Solgaard Andersen
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Patent number: 6235417Abstract: A two-phase proton and electron conductor is described which comprises (a) a proton conductive oxides represented by the formula: ABO3 where A is selected from the group consisting of Ba, Ca, Mg and Sr and B is Ce1−xMx or Zr1−xMx, where x has a value greater than zero and less than one and M is an element selected from the group consisting of Y, Yb, In, Gd, Nd, Eu, Sm and Tb, in combination with (b) an electron conductor comprising palladium. The palladium may be coated on particles of the oxide in the form of an oxide powder. This novel two-phase conductor is particularly useful as a mixed hydrogen ion and electronic conducting membrane for separating hydrogen from a hydrogen-containing gas.Type: GrantFiled: April 30, 1999Date of Patent: May 22, 2001Assignee: Her Majesty the Queen in right of Canada, as represented by the Minister of Natural ResourcesInventors: Eric D. Wachsman, Naixiong Jiang
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Patent number: 6231831Abstract: A membrane for separating hydrogen from a gas mixture is provided on at least one side with a catalyst layer for a specific catalytic combustion process. A methanol reformation system so equipped can be brought rapidly to operating temperature, with the hydrogen-separating membrane being heated directly by performing the catalytic combustion process.Type: GrantFiled: December 16, 1998Date of Patent: May 15, 2001Assignee: Xcellsis GmbHInventors: Rainer Autenrieth, Thomas Poschmann, Steffen Wieland, Dietmar Heil, Stefan Boneberg
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Patent number: 6214314Abstract: Process for the co-production of hydrogen and methanol by steam reforming a hydrocarbon feedstock, condensing and separating steam from the reformed gas, synthesizing methanol from the resultant de-watered reformed gas without further compression, separating synthesized methanol and separating hydrogen from the residual gas, optionally after subjecting the residual gas to the shift reaction is disclosed.Type: GrantFiled: January 13, 2000Date of Patent: April 10, 2001Assignee: Imperial Chemical Industries PLCInventor: Peter Edward James Abbott
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Patent number: 6207132Abstract: An apparatus for producing hydrogen includes at least one reforming chamber containing a reforming catalyst bed for reforming a carbonaceous fuel into hydrogen, at least one hydrogen-permeable membrane tube disposed inside the reforming chamber to be surrounded by the reforming catalyst bed and to confine therein a hydrogen compartment, and at least one oxidation chamber provided adjacent to the reforming catalyst bed for burning the gas not permeable to the membrane tube and for supplying heat to the reforming chamber. The oxidation chamber has an oxidation catalyst bed. A process for producing hydrogen via the apparatus is also disclosed.Type: GrantFiled: December 4, 1998Date of Patent: March 27, 2001Assignee: Chinese Petroleum CorporationInventors: Yu-Ming Lin, Min-Hon Rei
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Patent number: 6180081Abstract: A reactor unit includes a monolithic block with several parallel reaction chamber lengthwise channels into which a reaction starting product can flow, which contain a suitable reaction catalyst material, and which are delimited externally by membrane walls for the selective separation of a desired reaction component from the reaction end product. A catalytic burner is accommodated in at least some of the lengthwise channels.Type: GrantFiled: March 25, 1999Date of Patent: January 30, 2001Assignee: Xcellsis GmbHInventors: Thomas Poschmann, Steffen Wieland
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Patent number: 6171992Abstract: A methanol reforming reactor includes a reforming reaction space into which a methanol reforming catalyst is charged. The methanol reforming catalyst is present at the start of the reforming reaction operation in a pre-aged state in the reforming reaction space. A process for pre-aging the methanol reforming catalyst comprises heating at a temperature of between approximately 240° C. and approximately 350° C. and at a load of between approximately 0.5 m3H2/h and approximately 50 m3H2/h per liter of catalyst material in a methanol/water atmosphere. The reactor may be used in fuel-cell-operated motor vehicles for generating hydrogen for the fuel cells by means of the water vapor reforming of methanol.Type: GrantFiled: June 15, 1998Date of Patent: January 9, 2001Assignee: XCELLSIS GmbHInventors: Rainer Autenrieth, Andreas Christen, Detlef zur Megede
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Patent number: 6165438Abstract: Apparatus and method for simultaneous recovery of hydrogen from water and from hydrocarbon feed material. The feed material is caused to flow over a heated catalyst which fosters the water-gas shift reaction (H.sub.2 O+COH.sub.2 +CO.sub.2) and the methane steam reforming reaction (CH.sub.4 +H.sub.2 O3 H.sub.2 +CO). Both of these reactions proceed only to partial completion. However, by use of a Pd/Ag membrane which is exclusively permeable to hydrogen isotopes in the vicinity of the above reactions and by maintaining a vacuum on the permeate side of the membrane, product hydrogen isotopes are removed and the reactions are caused to proceed further toward completion. A two-stage palladium membrane reactor was tested with a feed composition of 28% CQ.sub.4, 35% Q.sub.2 O (where Q=H, D, or T), and 31% Ar in 31 hours of continuous operation during which 4.5 g of tritium were processed. Decontamination factors were found to increase with decreasing inlet rate.Type: GrantFiled: January 6, 1999Date of Patent: December 26, 2000Assignee: The Regents of the University of CaliforniaInventors: R. Scott Willms, Stephen A. Birdsell
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Patent number: 6129861Abstract: In a reactor and a method for the conversion of methanol to hydrogen wherein the reactor comprises first and second chambers divided by a membrane which is permeable for hydrogen and CO but not for CO.sub.2, the methanol is converted in the first chamber by a catalyst disposed therein to a gas mixture comprising hydrogen, carbon monoxide and carbon dioxide, and the hydrogen and carbon monoxide pass through the membrane into the second chamber wherein the CO is converted by another catalyst disposed therein to methane.Type: GrantFiled: November 3, 1998Date of Patent: October 10, 2000Assignee: Forschungszentrum Julich GmbHInventors: Josefin Meusinger, Lambertus Haart, Ulrich Stimming
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Patent number: 6123913Abstract: A method is disclosed for synthesizing hydrogen gas from hydrocarbon fuel. A first mixture of steam and a first fuel is directed into a first tube 208 to subject the first mixture to a first steam reforming reaction in the presence of a first catalyst 214. A stream of oxygen-containing gas is pre-heated by transferring heat energy from product gases. A second mixture of the pre-heated oxygen-containing gas and a second fuel is directed into a second tube 218 disposed about the first tube 208 to subject the second mixture to a partial oxidation reaction and to provide heat energy for transfer to the first tube 208. A first reaction reformate from the first tube 208 and a second reaction reformate from the second tube 218 are directed into a third tube 224 disposed about the second tube 218 to subject the first and second reaction reformates to a second steam reforming reaction, wherein heat energy is transferred to the third tube 224 from the second tube 218.Type: GrantFiled: November 3, 1998Date of Patent: September 26, 2000Assignee: Arthur D. Little, Inc.Inventors: Lawrence G. Clawson, William L. Mitchell, Jeffrey M. Bentley, Johannes H. J. Thijssen
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Patent number: 6113874Abstract: A furnace is provided having at least two regenerator beds for heat recovery. While a first bed is being heated by hot flue gases produced by combusting a fuel and an oxidant in the furnace, a second bed, heated during a previous cycle, is cooled through carrying out an endothermic chemical reaction therein, for example the reforming reaction of a hydrocarbon with water vapor and carbon dioxide and/or the dissociation of a hydrocarbon. Once the second bed is cooled by the endothermic reaction, the hot flue gases are redirected to it while the first bed, now hot, is used for carrying out the endothermic chemical reaction. Thereafter the cycle is repeated.Type: GrantFiled: April 29, 1998Date of Patent: September 5, 2000Assignee: Praxair Technology, Inc.Inventor: Hisashi Kobayashi
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Patent number: 6110979Abstract: Hydrocarbon feedstocks are converted into synthesis gas in a two-stage process comprising an initial steam reforming step followed by final conversion to synthesis gas in a mixed conducting membrane reactor. The steam reforming step converts a portion of the methane into synthesis gas and converts essentially all of the hydrocarbons heavier than methane into methane, hydrogen, and carbon oxides. The steam reforming step produces an intermediate feed stream containing methane, hydrogen, carbon oxides, and steam which can be processed without operating problems in a mixed conducting membrane reactor. The steam reforming and mixed conducting membrane reactors can be heat-integrated for maximum operating efficiency and produce synthesis gas with compositions suitable for a variety of final products. Synthesis gas produced by the methods of the invention is further reacted to yield liquid hydrocarbon or oxygenated organic liquid products.Type: GrantFiled: September 21, 1998Date of Patent: August 29, 2000Assignee: Air Products and Chemicals, Inc.Inventors: Shankar Nataraj, Steven Lee Russek
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Patent number: 6103143Abstract: 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.Type: GrantFiled: January 5, 1999Date of Patent: August 15, 2000Assignee: Air Products and Chemicals, Inc.Inventors: Shivaji Sircar, Jeffrey Raymond Hufton, Shankar Nataraj
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Patent number: 6090312Abstract: New process designs are presented for reforming reactions of steam with hydrocarbons (such as methane, natural gas, light hydrocarbon feedstocks with one to four carbon atoms in each molecule), also for the water gas shift reaction that is of steam with carbon monoxide; also for carbon dioxide reforming of hydrocarbons (such as methane, acidic natural gas, coal gas, landfill gas, light hydrocarbon feedstocks with one to four carbon atoms in each molecule), and the combined reaction of steam carbon dioxide with same hydrocarbons. The processes employ organic polymer, organic polymer-inorganic support, and inorganic membrane permeators for species separation, with the permeators placed after the reactors where the above named reactions take place. The membranes in permeators separate selectively the H.sub.2 and CO.sub.2 species exiting from the reactors from the non-permeated reactants and products.Type: GrantFiled: January 31, 1996Date of Patent: July 18, 2000Inventors: Zoe D. Ziaka, Savvas Vasileiadis
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Patent number: 6086839Abstract: A system for the water vapor reforming of a hydrocarbon includes an evaporator, a prereforming unit, a main reformer, a CO removal unit and at least one catalytic burner unit. A first burner unit is in a thermal contact with the evaporator and a second burner unit is in a thermal contact with the main reformer, and the prereforming unit is in a thermal contact with the CO removal unit by way of one heat conducting separating medium. In addition, the outlet of the CO removal unit is connected with the inlet of the at least one burner unit. During a cold start, a heating-up operation is carried out during which first the two burner units are activated with an external feeding of hydrogen or hydrocarbon, and the reforming operation is started with a hydrocarbon fraction that is lower than in the normal operation. The resulting reformate gas, instead of the externally fed hydrogen or hydrocarbon, is introduced as fuel into the burner units.Type: GrantFiled: December 7, 1998Date of Patent: July 11, 2000Assignee: DBB Fuel Cell Engines GmbHInventors: Rainer Autenrieth, Stefan Boneberg, Dietmar Heil, Martin Schuessler, Barbara Strobel, Steffen Wieland, Detlef zur Megede
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Patent number: 6083425Abstract: A method for converting hydrocarbon fuel into hydrogen gas and carbon dioxide within a reformer 10 is disclosed. According to the method, a stream including an oxygen-containing gas is directed adjacent to a first vessel 18 and the oxygen-containing gas is heated. A stream including unburned fuel is introduced into the oxygen-containing gas stream to form a mixture including oxygen-containing gas and fuel. The mixture of oxygen-containing gas and unburned fuel is directed tangentially into a partial oxidation reaction zone 24 within the first vessel 18. The mixture of oxygen-containing gas and fuel is further directed through the partial oxidation reaction zone 24 to produce a heated reformate stream including hydrogen gas and carbon monoxide. Steam may also be mixed with the oxygen-containing gas and fuel, and the reformate stream from the partial oxidation reaction zone 24 directed into a steam reforming zone 26.Type: GrantFiled: November 2, 1998Date of Patent: July 4, 2000Assignee: Arthur D. Little, Inc.Inventors: Lawrence G. Clawson, William L. Mitchell, Jeffrey M. Bentley, Johannes H. J. Thijssen
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Patent number: 6077459Abstract: Process and process unit for the preparation of ammonia synthesis gas from a hydrocarbon feedstock comprising sequentially primary and secondary catalytic steam reforming of the feedstock in a primary heat exchange steam reformer and in a subsequent secondary reformer, wherein an effluent stream of primary steam reformed gas is heated by indirect heat exchange with a hot product effluent of secondary reformed gas prior to introduction of the primary steam reformed gas into the secondary reformer.Type: GrantFiled: May 5, 1998Date of Patent: June 20, 2000Assignee: Haldor Topsoe A/SInventors: Carsten Lau Laursen, Henrik Otto Stahl
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Patent number: 6066307Abstract: A process for producing synthesis gas and hydrogen by passing a compressed and heated oxygen-containing gas mixture into a reactor having at least one solid electrolyte oxygen ion transport membrane to separate transported oxygen Organic fuel reacts with the oxygen to form synthesis gas. The resulting synthesis gas is separated into hydrogen gas through at least one solid electrolyte hydrogen transport membrane to separate the transported hydrogen in the same or different separator.Type: GrantFiled: September 15, 1999Date of Patent: May 23, 2000Inventors: Nitin Ramesh Keskar, Ravi Prasad, Christian Friedrich Gottzmann
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Patent number: 6048508Abstract: The present invention is directed to a process for simultaneously obtaining pure carbon monoxide and pure hydrogen in a steam reformer plant for hydrogen or ammonia generation, having a primary reformer, a secondary reformer and downstream thereof, a CO conversion stage. A part gas stream of the synthesis gas stream, which is discharged from the secondary reformer having a CO content of between 2 and 20 mol. % and is at a temperature of from 200 to 500.degree. C. and a pressure between 15 and 50 bar, is removed between the secondary reformer and the CO conversion stage. The part gas stream is then is cooled to a temperature below 100.degree. C., thereby condensing out the major part of the steam contained in the gas stream. The remaining raw synthesis gas stream is then guided by way of a multistage gas separation plant in which the gas components H.sub.2, residual steam, CH.sub.4, CO.sub.2 and optionally N.sub.2 are separated, either individually or together, from the CO.Type: GrantFiled: June 18, 1997Date of Patent: April 11, 2000Assignee: Bayer AktiengesellschaftInventors: Hans-Ulrich Dummersdorf, Hans-Joachim Muller, Dieter Grenner, Gerhard Moormann
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Patent number: 6048472Abstract: Hydrocarbon feedstocks are converted into synthesis gas in a two-stage process comprising an initial steam reforming step followed by final conversion to synthesis gas in a mixed conducting membrane reactor. The steam reforming step converts a portion of the methane into synthesis gas and converts essentially all of the hydrocarbons heavier than methane into methane, hydrogen, and carbon oxides. The steam reforming step produces an intermediate feed stream containing methane, hydrogen, carbon oxides, and steam which can be processed without operating problems in a mixed conducting membrane reactor. The steam reforming and mixed conducting membrane reactors can be heat-integrated for maximum operating efficiency and produce synthesis gas with compositions suitable for a variety of final products.Type: GrantFiled: December 23, 1997Date of Patent: April 11, 2000Assignee: Air Products and Chemicals, Inc.Inventors: Shankar Nataraj, Robert Byron Moore, Steven Lee Russek