Temperature Control Or Regulation Of The Fischer-tropsch Reaction Patents (Class 518/712)
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Patent number: 5520891Abstract: Disclosed are a fixed-bed, cross-flow catalytic reactor wherein reaction heat can be exchanged against a heat exchange medium circulating indirectly through the catalyst bed, and a catalytic process comprising operation of the cross-flow reactor. The reactor comprises a catalyst bed having internally embedded banks of heat exchange tubes. An inlet distributor distributes reactants along the axial length of the bed. The distributed fluid passes through the bed in a cross-flow path wherein a catalytic reaction occurs. The reaction effluent is then collected from the bed by an outlet product collector. A heat exchange medium circulated through the internal heat exchange tubes adds or removes reaction heat as required for enhanced conversion in the reactor. Multiple heat exchange tubes can be used, and inlet and discharge manifolds are provided for distributing the circulating heat exchange medium.Type: GrantFiled: February 1, 1994Date of Patent: May 28, 1996Inventor: Jing M. Lee
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Patent number: 5455281Abstract: Method of direct cooling synthesis gas in a catalytic reactor with one or more catalyst beds of a metal oxide catalyst being loaded on gas permeable partitions with distribution means, which method comprises admixing the synthesis gas during its passage through the reactor with a cooling gas being introduced into a mixing zone beneath each partition, wherein the mixing zones are obtained by passing a reducing gas through the catalyst bed, so that the catalyst volume shrinks during reduction of the catalyst particles, and, thereby, providing necessary cavities for the mixing zones beneath each partition.Type: GrantFiled: December 7, 1993Date of Patent: October 3, 1995Assignee: Haldor Topsoe A/SInventor: Haldor F. A. Topsoe
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Patent number: 5449696Abstract: A process for the continuous production of methanol through contacting at least one feed stream containing at least carbon monoxide and hydrogen, and optionally carbon dioxide, with a simulated moving bed acting as a catalyst for methanol synthesis and an adsorbent for the methanol formed has been developed. The carbon monoxide and hydrogen are catalytically reacted to form methanol which is separated from the carbon monoxide and hydrogen by concurrent adsorption. The methanol is desorbed using a carbon dioxide or hydrogen desorbent and collected. A specific embodiment is one where the feed stream is introduced to the simulated moving bed at a temperature from about 210.degree. to about 270.degree. C. and the desorbent is introduced to the simulated moving bed at a temperature of about 150.degree. to about 250.degree. C.Type: GrantFiled: August 1, 1994Date of Patent: September 12, 1995Assignee: UOPInventors: Hemant W. Dandekar, Gregory A. Funk
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Patent number: 5409960Abstract: Pentane (or similar light hydrocarbon) is used in a gas conversion process to consume the exothermic heat of reaction in the Fischer-Tropsch process, and expanded to produce the energy to drive the air plant compressors.Type: GrantFiled: June 15, 1994Date of Patent: April 25, 1995Assignee: Exxon Research and Engineering CompanyInventor: Thomas M. Stark
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Patent number: 5219891Abstract: A process for the production of methanol by reacting a gaseous mixture comprising hydrogen and carbon monoxide in the presence of a catalyst composition in the form of a fluidized bed whilst cooling, characterized in that the catalyst composition is present in a plurality of interconnected fluidized bed sections whereby each section is cooled by at least one heat exchanger and whereby the temperature in the highest section is reduced to below the highest temperature in a lower section.Type: GrantFiled: October 28, 1991Date of Patent: June 15, 1993Assignee: Shell Oil CompanyInventor: Swan T. Sie
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Patent number: 5152977Abstract: In a process for exothermic and heterogeneous synthesis, for example of ammonia, in which the synthesis gas is reacted in several catalytic beds with axial-radial or only radial flow, the reaction gas is collected at the outlet from the last catalytic bed but one and is transferred to a system for heat recovery external to the reactor, and is re-introduced into the last catalytic bed.Type: GrantFiled: September 5, 1991Date of Patent: October 6, 1992Assignees: Ammonia Casale S.A., Umberto ZardiInventors: Umberto Zardi, Giorgio Pagani
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Patent number: 5045568Abstract: The invention concerns a process and an apparatus for performing chemical reactions under pressure in the presence of a solid catalyst in a multi-stage reaction zone, after external intermediary thermal conditioning. This process may be used for the synthesis of ammonia or methanol or for gasoline reforming. It is characterized in that at least one reaction fluid is introduced into at least one compartment, a first reaction effluent is recovered, a heat exchange takes place, outside the reaction zone, between a first effluent and an external heat exchange medium, then said first effluent is introduced into at least one subsequent compartment and a second reaction effluent is recovered from said subsequent compartment.Type: GrantFiled: January 21, 1988Date of Patent: September 3, 1991Assignee: Institut Francais du PetroleInventors: Dang V. Quang, Pierre Ham, Daniel Gelas, Christian Legrand
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Patent number: 4963338Abstract: Improved process for heterogeneous synthesis and related reactors according to which the synthesis catalyst is distributed in three catalytic beds either axial-radial or radial, control of the temperature between beds being effected by means of fresh quench gas between the first and the second bed and by means of indirect cooling with an exchanger between the second and the third bed of the gas leaving the second bed, using fresh gas which is heated inside the tubes of said exchanger.Type: GrantFiled: June 30, 1988Date of Patent: October 16, 1990Assignees: Ammonia Casale, S.A., Umberto ZardiInventors: Umberto Zardi, Giorgio Pagani
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Patent number: 4956392Abstract: A process for producing methanol or mixed alcohol which comprises reacting a synthesis gas containing hydrogen and carbon monoxide and/or carbon dioxide in a fluidized catalyst bed.Catalyst particles having an average particle diameter of not more than 150 microns and a particle density of at least 1.7 g/cm.sup.3 are used as the fluidized catalyst.The catalyst particles are contacted with the synthesis gas at a superficial linear velocity of at least 0.2 m/sec. under a pressure of 40 to 200 atmospheres.Type: GrantFiled: November 17, 1989Date of Patent: September 11, 1990Assignee: Mitsubishi Gas Chemical Company, Inc.Inventors: Yoshihiko Saito, Osamu Hashimoto, Masaaki Kuwa, Takashi Kojima, Kinya Tsuji
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Patent number: 4839391Abstract: A single stage methanization reactor and process are made to yield a product gas of high methane content as well as useful superheated steam without overheating the catalyst bed in which a synthesis gas containing, CO, CO.sub.2 and H.sub.2 is converted into product gas. A variety of dispositions of vaporizer and superheater portions of the cooling system in the catalyst bed, for which the temperature profiles of gas and coolant along the reactor length are shown and compared, illustrate the principles governing the cooling system for such a reactor. A small portion of the superheated steam is mixed with preheated synthesis gas for elimination of all or part of the carbon monoxide content before the synthesis gas is introduced into the methanization reactor.Type: GrantFiled: June 13, 1988Date of Patent: June 13, 1989Assignees: Kernforschungsanlage Julich GmbH, Rheinische Braunkohlenwerke AGInventors: Jochen Range, Bernd Hohlein, Hans Niessen, Volker Vau, H. J. R. Schiebahn, Horst Hoffmann, Manfred Vorwerk
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Patent number: 4767791Abstract: A process for synthesizing material uses an exothermic reactor which comprises a coolant shell, two concentric pipes provided within the shell, a catalyst bed packed between inner and outer ones of the concentric pipes, an introduction tube connected to the inner pipe through which a starting fluid is introduced, and a communication path enabling the fluid after the passage of the inner pipe to be passed through the catalyst bed in a direction opposite to the direction of the passage through the inner pipe, the coolant shell having an inlet and an outlet for a coolant arranged in such a way that the flow of the coolant is parallel to the flow of the fluid within the catalyst bed. The coolant on the outside and the starting fluid on the inside of the catalyst bed cools the bed in such a way as to produce a temperature distribution along the bed that follows a maximum reaction rate line (M in FIG. 1) relating the concentration of the methanol to the temperature of the starting fluid.Type: GrantFiled: November 6, 1986Date of Patent: August 30, 1988Assignee: Mitsubishi Jukogyo Kabushiki KaishaInventors: Yoshimitsu Nakajima, Kensuke Niwa, Kazuhiro Morita, Hiroshi Makihara
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Patent number: 4732918Abstract: For conducting exothermic catalytic reactions, e.g., production of methane from CO.sub.x and H.sub.2, a reactor is cooled internally by indirect heat exchange with a single heat exchanger provided in the reactor feed inlet region with a gradually increasing surface intensity (defined as the product of the overall coefficient of thermal conductivity, (h), of the tube wall times the cooling surface density, m.sup.2 /m.sup.3) reaching a maximum intensity at a central zone of the heat exchanger where the preponderant cooling occurs. A zone of gradually decreasing cooling surface intensity may also be provided at the outlet end of the reactor, and uncooled adiabatic zones may be incorporated in the zones immediate the inlet and outlet ends of the reactor.Type: GrantFiled: April 18, 1985Date of Patent: March 22, 1988Assignee: Linde AktiengesellschaftInventors: Reiner Lohmueller, Ulrich Lahne, Michael Heisel, Helmut Schneider, Markus Raab, Karl Hobel
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Patent number: 4670473Abstract: Conversion of syn gas to methanol and higher alkanols wherein alkanols are added to a syn gas reactor. Lower alkanols are homologated to higher alkanols. Liquid methanol is added as an interstage quench.Type: GrantFiled: August 9, 1985Date of Patent: June 2, 1987Assignee: Amoco CorporationInventors: Robert H. Walker, David A. Palmer, Donna M. Salvatore, Edward J. Bernier
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Patent number: 4626552Abstract: A process for the start-up of a reactor which utilizes a feed comprising hydrogen and carbon monoxide for the synthesis of hydrocarbons. The feed is contacted with a bed of hydrocarbon synthesis catalyst in which perturbations of the temperature profile across the bed can develop, and which, at start-up is particularly acute. In practicing the process the feed is introduced into the reactor at a rate ranging up to about 100 percent of the total flow rate at which the feed is introduced to the reactor at line-out. Hydrogen is introduced into the reactor as a portion of said feed at a molar feed rate generally well below the feed rate in which the hydrogen is employed in the reactor at line-out, the molar ratio of hydrogen:carbon monoxide of the feed generally not exceeding about 90 percent, preferably 75 percent, of the molar ratio of hydrogen:carbon monoxide at line-out.Type: GrantFiled: January 6, 1986Date of Patent: December 2, 1986Assignee: Exxon Research and Engineering CompanyInventor: Kym B. Arcuri
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Patent number: 4559207Abstract: A reactor is provided for producing methanol by the reaction of synthesis gases containing carbon oxides and hydrogen in contact with a copper containing catalyst positioned in the reactor in catalyst tubes surrounded by boiling water under pressure. The catalyst tubes are made from a metallic material which is catalytically inactive with respect to the methanol synthesis gas and have approximately the same coefficient of thermal expansion as the shell of the reactor. The catalyst tubes are made of a steel composed of mixed austeniticferritic structure and containing 10-30% by weight chromium.Type: GrantFiled: November 28, 1983Date of Patent: December 17, 1985Assignee: Metallgesellschaft AGInventors: Heinz Hiller, Emil Supp, Friedemann Marschner, Hans Kupfer, Lutz Weidemann
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Patent number: 4539016Abstract: In methanizing CO and H.sub.2 containing charge gases, the charge gas is passed upwardly through a vertically extending fluidized bed reactor flowing, in turn, through a fluidized bed zone, a dust bed zone and a separation zone. From the separation zone, the gas is conveyed out of the reactor to a point of use. Coolant tubes are positioned in the reactor passing vertically through the fluidized bed zone, the dust bed zone and the separation zone for removing the heat generated in the reaction. An evaporable coolant, preferably water, is circulated through the coolant tubes. In a separate steam drum, the vapor pressure of the coolant is set for maintaining constant the temperature of the vaporizing coolant.Type: GrantFiled: April 24, 1981Date of Patent: September 3, 1985Assignees: Thyssengas G.m.b.H., Didier EngineeringInventors: Claus Flockenhaus, Erich Hackler, Werner Lommerzheim
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Patent number: 4525482Abstract: This invention provides an improved, simple and energy saving process for producing a gas containing methane, which process utilizes a reactor having a catalyst bed of a structure wherein a synthesis gas is allowed to pass perpendicularly to the longitudinal directions of a plurality of cooling tubes installed vertically within the catalyst bed. Within the cooling tubes, a liquid coolant at its boiling temperature is flowed upwardly under pressure. A portion of the reaction product gas leaving the catalyst bed is mixed, without cooling, with fresh feed gas and is recirculated to the catalyst bed. The amount of the recycled gas is less than 5 times the amount of fresh feed gas. The foregoing process produces a product gas containing methane from a feed gas containing carbon monoxide and hydrogen.Type: GrantFiled: March 22, 1984Date of Patent: June 25, 1985Assignee: Toyo Engineering CorporationInventors: Kozo Ohsaki, Katsutoshi Kikuchi, Yoshitsugu Hirota
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Patent number: 4503264Abstract: A process is disclosed for producing methyl tert.-butyl ether wherein n-butane is isomerized to isobutane which is then catalytically dehydrogenated to form an isobutane/isobutene mixture, while natural gas is reformed to form synthesis gas containing CO and H.sub.2 which is in turn converted to methanol, the resulting methanol and isobutene in the isobutane/isobutene mixture being etherified to form methyl tert.-butyl ether. Isobutane is then separated from the resulting etherification mixture and is recycled to the dehydrogenation stage.Type: GrantFiled: August 16, 1982Date of Patent: March 5, 1985Assignee: Davy McKee AGInventor: Ghazi R. Al-Muddarris
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Patent number: 4496666Abstract: Catalysts comprising the mixed oxides of ruthenium, palladium or platinum and alkali metals are provided which are useful in the subject process for the upgrading of synthesis gas, particularly for obtaining alkanes and alcohols having at least two carbon atoms, in addition to methane and methanol. Also provided is a temperature gradient reactor useful in synthesis gas upgrading reactions for increasing selectivity to higher carbon number products.Type: GrantFiled: December 2, 1983Date of Patent: January 29, 1985Assignee: The Standard Oil CompanyInventors: Frederick A. Pesa, Anne M. Graham
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Patent number: 4431751Abstract: Only a part of the synthesis gas supply is passed through a first internally cooled catalytic reactor (1) and the hotter gas coming out of it is reunited with the remaining gas supply for passing through an adiabatic reactor (2) that is followed by a heat exchanger (3) on its way to a second internally cooled reactor (4) in which the methanization reaction is completed. Water is heated up to practically the saturated steam temperature in the cooling system of the last mentioned reactor and is converted to saturated steam in the cooling system of the first internally cooled reactor. The saturated steam is superheated in the above-mentioned heat exchanger. To make the process run more smoothly a steam drum is provided through which the hot water piping between the cooling systems of the two internally cooled reactors runs and the saturated steam is brought into the steam drum and from it to the heat exchanger before it is superheated.Type: GrantFiled: May 26, 1982Date of Patent: February 14, 1984Assignee: Kernforschungsanlage Julich GmbHInventors: Bernd Hohlein, Manfred Vorwerk, Udo Boltendahl
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Patent number: 4424282Abstract: Methane is produced by passing hydrogen, carbon monoxide and an aqueous liquid phase downwardly through a fixed bed of a catalyst containing ruthenium on a carrier such as alumina, separating and externally coolng in a heat exchanger the resultant aqueous phase before recycling, thereby limiting the reaction temperature within a range from 200.degree. to 320.degree. C.Type: GrantFiled: February 16, 1982Date of Patent: January 3, 1984Assignee: Institut Francais du PetroleInventors: Yves Chauvin, Dominique Commereuc, Andre Sugier, Jean-Francois Le Page
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Patent number: 4423022Abstract: Processes for carrying out catalytic exothermic and endothermic high-pressure gas reactions with a single-walled pressure vessel or shell containing cross-flow (e.g., radial flow) heat transfer exchangers, a continuous catalytic bed having at least two stages, and means for effecting "cross-over" material flows from "outside" to "inside" (for exothermic reactions) and vice versa (for endothermic reactions), whereby conditions of: maximum gas temperature always being in the core of said vessel or shell, minimal pressure drop, and minimal compression of catalyst particles are achieved, along with significant economic savings in cost of the pressure vessel or shell and catalyst (through extension of catalyst life).Type: GrantFiled: April 21, 1983Date of Patent: December 27, 1983Assignee: The Lummus CompanyInventors: John V. Albano, George Friedman
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Patent number: 4407974Abstract: A method of catalytic conversion of feed gases, particularly of a low-sulphur gas mixture rich in carbon monoxide and hydrogen, into a product gas mixture containing methane and/or higher hydrocarbons under high pressure includes the step of removing heat of reaction from the catalytic conversion from a reaction zone by feeding both water and steam to form a cooling medium through a pipe coil in the reaction zone. This forms superheated steam in the pipe coil and the superheated steam is then converted into another form of energy, for example in a turbo-generator. Preferably the reaction zone is a fluidized bed. For carrying out this method a reactor is used, which is preferably a fluidized bed reactor and in this reactor the piping system forming the superheater is disposed in the lower part of the reaction zone. The superheater is connected to a feedwater line and to a steam inlet line and a steam turbine is connected to a steam output line leading from the superheater.Type: GrantFiled: April 23, 1982Date of Patent: October 4, 1983Assignees: Thyssengas GmbH, Didier Engineering GmbHInventors: Claus Flockenhaus, Erich Hackler, Werner Lommerzheim
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Patent number: 4369255Abstract: A method of controlling the equilibrium conditions and of simultaneously producing steam under high pressure in the production of methanol by a reaction of oxides of carbon and of hydrogen-containing gases at temperatures of 200.degree. to 300.degree. C. under a pressure of 20 to 100 bars at a copper-containing catalyst, which is contained within the reactor in tubes, which are indirectly cooled by boiling water under pressure, wherein the resulting steam is withdrawn together with circulating water and is separated from the water, the water is recycled and the evaporated water is replaced by feed water. According to the invention the process is carried out in such a manner that a perforated thin intermediate bottom plate is provided in the reactor spaced 20 to 150 cm over the lower tube plate, the reactor is fed with the circulating water above that intermediate bottom and with feed water below that intermediate bottom, the gaseous reaction mixture is cooled by 20.degree. to 50.degree. C.Type: GrantFiled: July 27, 1981Date of Patent: January 18, 1983Assignee: Metallgesellschaft AktiengesellschaftInventor: Emil Supp
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Patent number: 4346179Abstract: Process for manufacturing a constituent for motor car gasoline from a synthesis gas containing essentially carbon dioxide, carbon monoxide and hydrogen, comprising producing methanol and its higher homologs by treatment of said synthesis gas in a first catalytic reaction zone at 230.degree.-350.degree. C., cooling and condensing the effluent therefrom, separating from the liquid condensate a gas fraction, treating the latter at 240.degree.-300.degree. C. in a second catalytic reaction zone to produce a liquid methanol fraction and admixing said methanol fraction with said liquid condensate to form said gasoline constituent.Type: GrantFiled: April 4, 1980Date of Patent: August 24, 1982Assignee: Institut Francais du PetroleInventors: Andre Sugier, Edouard Freund, Jean-Francois Le Page
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Patent number: 4326041Abstract: The invention relates to a process for the catalytic synthesis of methanol from a raw gas which mainly contains CO, CO.sub.2 and H.sub.2 and is obtained in a catalytic natural-gas cracking plant, the raw gas being compressed in several stages to the synthesis pressure of 50-150 bar and gas being purged from the synthesis loop in order to maintain a given inert gas level.Type: GrantFiled: August 11, 1980Date of Patent: April 20, 1982Assignee: UHDE GmbHInventor: Hans-Joachim Bahnisch
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Patent number: 4298694Abstract: The invention relates to an improved catalytic methanation process wherein a feed gas containing predominantly hydrogen and being rich in carbon oxides (CO and/or CO.sub.2) is divided into two part streams of which the first is methanated partially in an adiabatic methanation reactor by a methanation catalyst whereafter the effluent from the adiabatic methanation reactor is united after cooling with the second feed gas part stream and the thus-combined stream is methanated in a cooled methanation reactor by a methanation catalyst, preferably the same as that used in the adiabatic methanation reactor. It is possible, but not always necessary, to recycle part of the recycle gas to the adiabatic methanation reactor to keep the temperature therein at a moderate level. The process is useful in connection with transport of energy from a nuclear reactor. It is advantageous because it can be operated to produce superheated steam, for use, e.g.Type: GrantFiled: December 3, 1979Date of Patent: November 3, 1981Assignee: Haldor Topsoe A/SInventor: Allan Skov
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Patent number: 4294932Abstract: Strongly exothermic, catalytically induced or promoted chemical reactions, e.g. the production of methane by the reaction of hydrogen with carbon oxides, are carried out by passing the reactants through an isothermically operated reactor in addition to an adiabatic reactor.Type: GrantFiled: August 8, 1979Date of Patent: October 13, 1981Assignee: Linde AGInventors: Reiner Lohmuller, Helmut Schneider, Allan Watson
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Patent number: 4269783Abstract: A method is disclosed for the conversion of a syngas to a liquid hydrocarbon product having a boiling range of less than 400.degree. F. at a 90% overhead and being a predominantly olefinic product, wherein the olefins have substantially internal double bonds. The method for accomplishing this stated result involves an improvement in the method for the conversion of synthesis gas by contacting the same with a catalyst composite comprising a mixture of a Fischer-Tropsch catalyst and a volume excess of an acidic catalyst, e.g., silica-alumina or a crystalline aluminosilicate zeolite and wherein the activity of the acidic component is balanced with the activity of the Fischer-Tropsch component so as to maximize the yield of desired olefinic product.Type: GrantFiled: March 7, 1977Date of Patent: May 26, 1981Assignee: Mobil Oil CorporationInventors: James A. Brennan, Philip D. Caesar, Julius Ciric, William E. Garwood, Robert E. Holland