US3144312A - Catalytic conversion plant for the continuous generation of gases of any kind out of ydrocarbons - Google Patents

Catalytic conversion plant for the continuous generation of gases of any kind out of ydrocarbons Download PDF

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US3144312A
US3144312A US150605A US15060561A US3144312A US 3144312 A US3144312 A US 3144312A US 150605 A US150605 A US 150605A US 15060561 A US15060561 A US 15060561A US 3144312 A US3144312 A US 3144312A
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/06Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes
    • B01J8/062Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes being installed in a furnace
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/382Multi-step processes
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10GCRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G11/00Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/10Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with stationary catalyst bed
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10GCRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G11/00Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • C10G11/20Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils by direct contact with inert heated gases or vapours
    • C10G11/22Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils by direct contact with inert heated gases or vapours produced by partial combustion of the material to be cracked
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00Technologies relating to chemical industry
    • Y02P20/10Process efficiency
    • Y02P20/129Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Definitions

  • This invention relates to a catalytic conversion plant for the continuous generation of industrial gases of any kind for further chemical treatment, town gas, synthetic gases or gases rich in olefine from hydrocarbons with reactants such as air, oxygen and water vapour, which have been added singly or in a definite ratio.
  • Orthodox plants of this type sufler from the disadvantage of requiring great amounts of heat for pre-heating the charging mixture and for executing the reaction, as well as necessitating long contact pipes.
  • This invention is based on the idea of creating a catalytic conversion plant which combines a compact construction and a minimum supply of heat with a high efficiency in operation.
  • this problem is solved by the arrangement of a conversion element, a heat exchanger, an operative air preheater, and a burner in one unit, which is detachably connected with a steam generator by means of a flange connection.
  • a further advantage of this arrangement lies in the fact that the conversion element can be easily exchanged and any repair work or renewal of parts can be effected without any trouble to adjoining plants.
  • the pipes of the conversion element may have a ribbed or corrugated finish in order to increase the heating surface.
  • FIG. 1 shows the plant in elevation
  • FIG. 2 shows a cross-section on the line AA' of FIG. 1;
  • FIG. 3 shows a cross-section on the line B-B of FIG. 1.
  • the catalytic conversion plant of this invention consists of the conversion element 1, the heat exchanger 2, the air preheater 3, the burner 4, and the steam generator 5.
  • the conversion element 1, the heat exchanger 2, the air preheater 3 and the burner 4 forms one unit which is detachably connected with the steam generator 5 by means of a flange connection 6.
  • the conversion element 1 consists of three concentrically arranged pipes 7, 8, and 9 which form two annular spaces 10 and 11.
  • the annular spaces 10 and 11 are connected at their bottom and are filled with a catalytic agent.
  • the heat exchanger 2 consists of two concentric pipes 12 and 13 forming the annulus 14 which is closed at its top and connected with the annulus 10 in its lower part; it is provided with a connecting piece 15.
  • pipes 16 in circular arrangement. They are in their lower part connected with the annulus 11 and on top they are connected with a chamber 17 having a circular section.
  • the heat exchanger 2 is surrounded by the air preheater 3.
  • the burner 4 in which a suitable fuel is burnt with air, producing flue gas.
  • the air preheater 3 consists of three concentrically arranged pipes 18, 19, and 20, being closed in their upper and lower parts. They form two annular spaces 21 and 22 which are in connection with each other and provided with inlet and outlet pipe connections 23 and 24.
  • the steam generator 5 consists of four concentrically arranged pipes 25, 26, 27, and 28 which are 3,144,312 Patented Aug. 11, 1964 closed at their top and bottom. They form three annular spaces 29, 30 and 31.
  • the conversion element 1 projects into the inner pipe 28.
  • the external annulus 29 is provided with a connecting piece 32 for the outlet of the flue gases.
  • the annulus 30 in the middle has a connecting piece for the intake of the feed water.
  • a connecting piece 36 in the bottom of the pipe 26 serves for the elutriation of the steam generator 5.
  • air for the reaction passes through the tangentially placed connecting piece 23 and enters the air preheater 3 at a temperature of 20 to 35 C. It leaves it, preheated to a temperature of approximately 200 C. through the connecting piece 24 and is mixed with the steam for the reactions that is discharged through the connecting piece 33.
  • the amount of hydrocarbon is fed to this mixture in measured quantities.
  • the reactive mixture air-water vapour-hydrocarbon passes through the connecting piece 15 and enters the annulus 14 of the heat exchanger 2 in order to be preheated to a temperature of 450 to 500 C. by the conversion gases which flow as countercurrents through the pipes 16.
  • the conversion mixture enters the external annulus 10 of the conversion element 1 and transforms, first of all, especially With the reactive air and some water vapour conversion partly into conversion gases.
  • the heating is effected by means of flue gases which rise as a countercurrent in the annulus 37, formed by the pipes 7 and 28.
  • the flue gases interchange heat there, having a temperature of about 900 C. at the bottom and up to 750 C. at the top. Practically all of the heat of the flue gases is eliminated in the annulus 10 by means of the external pipe 7 of the conversion element 1, in order to facilitate the conversion.
  • the conversion gases and the undecomposed hydrocarbons mixed with water vapour pass for the final decomposition of the still undecomposed hydrocarbons with water vapour from the annulus 10 into the annulus 11, which is also filled with a catalytic agent.
  • This reaction consumes a great amount of heat which is for the greater part compensated by the direct heating of the internal pipe 9 with radiation heat of the flue gases that leave the burner 4.
  • the finished conversion gas leaves the annulus 11 and enters the concentrically arranged pipes of the heat exchanger 2. There the greater part of the heat is indirectly dissipated to the heat exchanger 2 for raising the temperature of the charging mixture.
  • the cooled conversion gas is tangentially discharged at 38.
  • the flue gases generated by the burner 4 radiate the heat required for the conversion, especially for that required in the water vapour reaction, to the annulus 11 which is filled with the catalytic agent. This is done in a countercurrent.
  • the gases reverse their direction in the lower part in order to radiate in the annulus 37 the required heat in countercurrent to the charging mixture indirectly to the charge in the annulus 10.
  • the flue gases enter the annulus 31 to dissipate part of their heat to the steam generator 5.
  • this steam generator flue gas flows around it to eflect the vaporization of the water in annulus 30.
  • Catalytic conversion plant for the continuous genera tion of gases, comprising a container, a plurality of coaxial vertical pipes one within the other Within the container and including an outer pipe, an intermediate pipe and an inner pipe forming outer and inner annular catalyst spaces, means extending between the outer and inner pipes closing oil such spaces from their outside, such spaces communicating adjacent their lower ends, a catalytic material in said spaces, means closing off a first of said catalyst spaces at the top, inner and outer pipe sections coaxial with said pipes extending upwardly from the top ends of the pipes and providing an annular heat-exchange space therebetween, said heat exchange space communicating with the other of said catalyst spaces, said heat exchange space having an inlet opening from outside the container, a plurality of tubes extending upwardly through said heat exchange space having their lower ends open to said first catalyst space, a collector connected to the upper ends of said tubes and having an outlet to the outside of the container therefrom, a burner in the space within the inner pipe section, means in the container to direct upwardly on the outside of the outer pipe gases flowing downwardly through the inner pipe

Description

Aug. 11, 1964 c. MERTENS 3,144,312
CATALYTIC CONVERSION PLANT FOR THE CONTINUOUS GENERATION OF GASES OF ANY KIND ou'r or HYDROCARBONS Filed June 6. 1961 I NVENTOR W M E A w m M L J m .w J B m H Elihu i LFILLV\\\ \1 United States Patent CATALYTIC CUNVERSION PLANT FOR THE CQN- TINUOUS GENERATION 9F GASES OF ANY KIND OUT OF hYDRQCAREONS Carl Mertens, Am Holzwege 15, Bochum- Linden, Germany Filed June 6, 1961, Ser. No. 150,605 1 Claim. (Cl. 48-95) This invention relates to a catalytic conversion plant for the continuous generation of industrial gases of any kind for further chemical treatment, town gas, synthetic gases or gases rich in olefine from hydrocarbons with reactants such as air, oxygen and water vapour, which have been added singly or in a definite ratio. Orthodox plants of this type sufler from the disadvantage of requiring great amounts of heat for pre-heating the charging mixture and for executing the reaction, as well as necessitating long contact pipes.
This invention is based on the idea of creating a catalytic conversion plant which combines a compact construction and a minimum supply of heat with a high efficiency in operation.
In terms of the invention this problem is solved by the arrangement of a conversion element, a heat exchanger, an operative air preheater, and a burner in one unit, which is detachably connected with a steam generator by means of a flange connection. A further advantage of this arrangement lies in the fact that the conversion element can be easily exchanged and any repair work or renewal of parts can be effected without any trouble to adjoining plants.
In compliance with this invention, the pipes of the conversion element may have a ribbed or corrugated finish in order to increase the heating surface.
Further features and details of the invention are shown in the following description with reference to the drawing in which a form of construction is demonstrated.
FIG. 1 shows the plant in elevation;
FIG. 2 shows a cross-section on the line AA' of FIG. 1;
FIG. 3 shows a cross-section on the line B-B of FIG. 1.
The catalytic conversion plant of this invention consists of the conversion element 1, the heat exchanger 2, the air preheater 3, the burner 4, and the steam generator 5. The conversion element 1, the heat exchanger 2, the air preheater 3 and the burner 4 forms one unit which is detachably connected with the steam generator 5 by means of a flange connection 6. The conversion element 1 consists of three concentrically arranged pipes 7, 8, and 9 which form two annular spaces 10 and 11. The annular spaces 10 and 11 are connected at their bottom and are filled with a catalytic agent. On top of the annular spaces 10 and 11 there is the heat exchanger 2 annexed to them. The heat exchanger 2 consists of two concentric pipes 12 and 13 forming the annulus 14 which is closed at its top and connected with the annulus 10 in its lower part; it is provided with a connecting piece 15. In the annulus 14 there are pipes 16 in circular arrangement. They are in their lower part connected with the annulus 11 and on top they are connected with a chamber 17 having a circular section. The heat exchanger 2 is surrounded by the air preheater 3. In its interior there is the burner 4 in which a suitable fuel is burnt with air, producing flue gas. The air preheater 3 consists of three concentrically arranged pipes 18, 19, and 20, being closed in their upper and lower parts. They form two annular spaces 21 and 22 which are in connection with each other and provided with inlet and outlet pipe connections 23 and 24. The steam generator 5 consists of four concentrically arranged pipes 25, 26, 27, and 28 which are 3,144,312 Patented Aug. 11, 1964 closed at their top and bottom. They form three annular spaces 29, 30 and 31. The conversion element 1 projects into the inner pipe 28. The external annulus 29 is provided with a connecting piece 32 for the outlet of the flue gases. The annulus 30 in the middle has a connecting piece for the intake of the feed water. At the bottom of the pipes 26 and 27 there are connections 35 between the internal annulus 31 and the external annulus 29. A connecting piece 36 in the bottom of the pipe 26 serves for the elutriation of the steam generator 5.
When the plant is in operation, air for the reaction passes through the tangentially placed connecting piece 23 and enters the air preheater 3 at a temperature of 20 to 35 C. It leaves it, preheated to a temperature of approximately 200 C. through the connecting piece 24 and is mixed with the steam for the reactions that is discharged through the connecting piece 33. The amount of hydrocarbon is fed to this mixture in measured quantities. The reactive mixture air-water vapour-hydrocarbon passes through the connecting piece 15 and enters the annulus 14 of the heat exchanger 2 in order to be preheated to a temperature of 450 to 500 C. by the conversion gases which flow as countercurrents through the pipes 16. At this temperature the conversion mixture enters the external annulus 10 of the conversion element 1 and transforms, first of all, especially With the reactive air and some water vapour conversion partly into conversion gases. The heating is effected by means of flue gases which rise as a countercurrent in the annulus 37, formed by the pipes 7 and 28. The flue gases interchange heat there, having a temperature of about 900 C. at the bottom and up to 750 C. at the top. Practically all of the heat of the flue gases is eliminated in the annulus 10 by means of the external pipe 7 of the conversion element 1, in order to facilitate the conversion. The conversion gases and the undecomposed hydrocarbons mixed with water vapour pass for the final decomposition of the still undecomposed hydrocarbons with water vapour from the annulus 10 into the annulus 11, which is also filled with a catalytic agent. This reaction consumes a great amount of heat which is for the greater part compensated by the direct heating of the internal pipe 9 with radiation heat of the flue gases that leave the burner 4. The finished conversion gas leaves the annulus 11 and enters the concentrically arranged pipes of the heat exchanger 2. There the greater part of the heat is indirectly dissipated to the heat exchanger 2 for raising the temperature of the charging mixture. The cooled conversion gas is tangentially discharged at 38.
The flue gases generated by the burner 4 radiate the heat required for the conversion, especially for that required in the water vapour reaction, to the annulus 11 which is filled with the catalytic agent. This is done in a countercurrent. The gases reverse their direction in the lower part in order to radiate in the annulus 37 the required heat in countercurrent to the charging mixture indirectly to the charge in the annulus 10. After covering the whole amount of conversion heat and the appropriate part of the reactive air preheating, the flue gases enter the annulus 31 to dissipate part of their heat to the steam generator 5. At two sides of this steam generator flue gas flows around it to eflect the vaporization of the water in annulus 30. Through the connections 35 the flue gases pass from the annulus 31 into the annulus 29, heating the annulus 30, and discharge through the connecting piece into the atmosphere. The steam leaves the steam generator 5 through the connecting piece 33. The reactive air enters the air preheater through the connecting piece 23, flows through the annulus 21 and in countercurrent also through the annulus 22 and leaves the preheater 3 through the connecting piece 24.
In spite of the high temperatures a refractory lining is not necessary because the upper parts in the air preheater 3 are kept cool.
I claim:
Catalytic conversion plant for the continuous genera tion of gases, comprising a container, a plurality of coaxial vertical pipes one within the other Within the container and including an outer pipe, an intermediate pipe and an inner pipe forming outer and inner annular catalyst spaces, means extending between the outer and inner pipes closing oil such spaces from their outside, such spaces communicating adjacent their lower ends, a catalytic material in said spaces, means closing off a first of said catalyst spaces at the top, inner and outer pipe sections coaxial with said pipes extending upwardly from the top ends of the pipes and providing an annular heat-exchange space therebetween, said heat exchange space communicating with the other of said catalyst spaces, said heat exchange space having an inlet opening from outside the container, a plurality of tubes extending upwardly through said heat exchange space having their lower ends open to said first catalyst space, a collector connected to the upper ends of said tubes and having an outlet to the outside of the container therefrom, a burner in the space within the inner pipe section, means in the container to direct upwardly on the outside of the outer pipe gases flowing downwardly through the inner pipe and out of the open bottom thereof, an air preheater around the outer pipe section, said air preheater comprising three pipe elements coaxial with the pipe sections to form two air heating spaces, an inlet into one of said air heating spaces and an outlet from the other near one end thereof, said air heating spaces communicating near the other end only, a doublewalled steam generator in said container on the outside of said directing means, and means to guide gases from said burner from the outside of the outer pipe to flow in heat exchange relation with said steam generator.
References Cited in the file of this patent UNITED STATES PATENTS 1,335,891 Greenwood et a1. Apr. 6, 1920 1,424,142 Hill July 25, 1922 1,689,684 Reed Oct. 30, 1928 1,809,291 Williams June 9, 1931 1,832,972 Ernst Nov. 24, 1931 1,839,738 Casale Jan. 5, 1932 2,032,652 Du Chaffaut Mar. 3, 1936 3,031,274 Schober Apr. 24, 1962
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US3366461A (en) * 1964-05-11 1968-01-30 Chemical Construction Corp Apparatus for exothermic catalytic reactions
US3909299A (en) * 1973-10-01 1975-09-30 United Technologies Corp Fuel cell system including reform reactor
US4026675A (en) * 1974-07-01 1977-05-31 Friedrich Uhde Gmbh Heat exchanger for nuclear reactor installations
US4071330A (en) * 1976-12-22 1978-01-31 United Technologies Corporation Steam reforming process and apparatus therefor
FR2374948A1 (en) * 1976-12-22 1978-07-21 United Technologies Corp IMPROVEMENT OF ENDOTHERMAL CATALYTIC REACTION EQUIPMENT WITH MULTIPLE REACTORS
FR2374946A1 (en) * 1976-12-22 1978-07-21 United Technologies Corp APPARATUS FOR CARRYING OUT ENDOTHERMAL CATALYTIC REACTIONS
FR2374947A1 (en) * 1976-12-22 1978-07-21 United Technologies Corp COMPACT MULTI-REACTOR APPARATUS FOR CATALYTIC REACTIONS
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US4746329A (en) * 1986-11-26 1988-05-24 Energy Research Corporation Methanol fuel reformer
US4830834A (en) * 1985-03-21 1989-05-16 Epri Electric Power Research Institute Reactor for the catalytic reforming of hydrocarbons
US4861347A (en) * 1986-12-29 1989-08-29 International Fuel Cells Corporation Compact chemical reaction vessel
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US6375906B1 (en) 1999-08-12 2002-04-23 Idatech, Llc Steam reforming method and apparatus incorporating a hydrocarbon feedstock
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US6494937B1 (en) 2001-09-27 2002-12-17 Idatech, Llc Hydrogen purification devices, components and fuel processing systems containing the same
US6537352B2 (en) 1996-10-30 2003-03-25 Idatech, Llc Hydrogen purification membranes, components and fuel processing systems containing the same
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US7195663B2 (en) 1996-10-30 2007-03-27 Idatech, Llc Hydrogen purification membranes, components and fuel processing systems containing the same
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US20080175770A1 (en) * 2007-01-19 2008-07-24 Paul Steven Wallace Methods and apparatus to facilitate cooling syngas in a gasifier
US7601302B2 (en) 2005-09-16 2009-10-13 Idatech, Llc Self-regulating feedstock delivery systems and hydrogen-generating fuel processing assemblies and fuel cell systems incorporating the same
US7682718B2 (en) 2001-06-26 2010-03-23 Idatech, Llc Fuel processor feedstock delivery system
US7939051B2 (en) 2006-05-23 2011-05-10 Idatech, Llc Hydrogen-producing fuel processing assemblies, heating assemblies, and methods of operating the same
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US8262752B2 (en) 2007-12-17 2012-09-11 Idatech, Llc Systems and methods for reliable feedstock delivery at variable delivery rates
US10476093B2 (en) 2016-04-15 2019-11-12 Chung-Hsin Electric & Machinery Mfg. Corp. Membrane modules for hydrogen separation and fuel processors and fuel cell systems including the same
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