US2173984A - Apparatus and process for catalytic reactions - Google Patents
Apparatus and process for catalytic reactions Download PDFInfo
- Publication number
- US2173984A US2173984A US161715A US16171537A US2173984A US 2173984 A US2173984 A US 2173984A US 161715 A US161715 A US 161715A US 16171537 A US16171537 A US 16171537A US 2173984 A US2173984 A US 2173984A
- Authority
- US
- United States
- Prior art keywords
- tubes
- furnace
- catalyst
- tube
- gas
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/02—Chemical 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
- B01J8/06—Chemical 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
- B01J8/062—Chemical 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
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production 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
- C01B3/34—Production 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
- C01B3/38—Production 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
- C01B3/384—Production 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 the catalyst being continuously externally heated
Definitions
- 'Ihis invention relates to improved apparatus and process for catalytic reactions involving the application of heat to gases and vapors, particularly adapted to the art of producing gas rich in 5' free hydrogen from hydrocarbon gas with steam or other compounds containing oxygen, which may react with the carbon of the hydrocarbons.
- Another special method heretofore in use has 40 been the use of high proportions of excess air in the combustion gases, in order to reduce the temi perature of the gases to a suitable point.
- the exit temperatures are all below the melting point of the alloy tube.
- the thermal eihciency is then about 2li-35%, a very low value.
- the temperature differential for heating the hot end of the tube and furnace wall is low, 500 F. maximum at 28% thermal elciency.
- the construction and design of such old apparatus necessitates a substantial temperature difference (250 F.500 F.) between the furnace wall and the metal tube, making high operating temperature diiiicult to obtain. It is therefore evident that the old apparatus design, including provision for parallel flow, represents a common and specific state in the artV and one not meeting thedemand for cheap hydrogen.
- I may use counter-ciment flow with the combustion gases containing a minimum of excess air, and by the use of high temperature combustion gases, without endangering the metal alloy catalyst tubes. Such I accomplish by the use of a heating furnace containing the catalyst tubes hereinafter more fully described.
- My improved apparatus enables not only higher thermal efficiency to be obtained, but higher chemical eficiency. This is due to the fact that the tube wall temperature can be very close to the refractory wall temperature, and for any specified thermal efficiency for the furnace, as compared to a parallel flow operated furnace, the tube operating temperatures will be higher, which gives directly higher chemical efliciency.
- I represents a furnace. constructed preferably of fire: brick, containing metal alloy catalyst tubes 2, placed vertically in planes parallel to the side walls of the furnace. Any number of such tubes may be used, arranged, for example, as is more fully described in connection with Figure 2.
- the tubes are constructed of a nickel-chromium-iron alloy adapted to withstand high temperatures.
- the tubes 2 project through the top and bottom of the furnace, passing through tiles 3.
- the projecting ends of the tubes and the outer surface of the furnace may, if desired, be covered with insulating material (not shown to enhance clarity).
- Tubes 2 are supported by means of any suitable support at the top of each tube, e.
- the upper flange 5 of tube 2 rests upon a short collar 6, through which tube 2 may pass freely.
- Collar 6 is supported by and fastened to steel beam l, supported in any suitable manner upon the furnace housing. Any of tubes 2 may be readily removed from the furnace by disconnecting it at the :flange and lifting it vertically from the furnace.
- Tubes 2 are filled with a suitable catalytic material 8, supported by a perforated alloy plate 9. Suitable catalysts are hereinafter disclosed. Plate 9 is removable, and rests upon support I0, attached to the inner surface of the tube.
- the tubes 2 may be removed and replaced, even when filled with catalyst, in the manner already described, and the catalyst may be placed in the tubes, or removed therefrom, both while the tubes are in the furnace or at other places remote from.
- gases or vapors are supplied through convenient pipes, which may differ from those shown in the accompanying drawings as circumstances and process may require.
- a mixture of hydrocarbon gas and steam is forced through line II, controlled by valve I2, into tubes 2.
- Burners I5 are located in the side wall of furnace I at various levels. Suitable burners are those giving a short flame, such as inspirator type N571-A, made by the Surface Combustion Corporation. Gas is supplied to the burners through gas pipes I6, the pressure being indicated by gauge I'I. The combustion gases from the burners pass into the furnace substantially tangentlally to tubes 2. and pas: upward around the tubes with a circulatory motion, at the same time heating the inner furnace walls to a high temperature and radiating heat from said walls to tubes 2. The gases of combustion finally escape from the furnace in a flue Il, connecting with a stack (not shown). Suitable heat exchange equipment or waste heat boilers'may be used to recover heat remaining in said flue gas.
- a mixture of steam and hydrocarbon gas is passed down through pipes 2 and through catalyst mass 8, where it is heated rapidly to a temperature of about 1600 to about 2000" F.
- a temperature of about 1600 to about 2000" F At such temperatures there' is a marked decrease in the strength of alloys used for the catalyst tubes, and serious bending and distortion occur if said tubes are supported at the bottom. Suspension of the tubes at the top, leaving the bottom and connections thereto free to move with thermal expansion of the tube, prevents this distortion.
- each chamber of which contains catalyst tubes having the herein defined relation of tube surface to vertical wail surface, preferably about 3 inches to about 8 inches in diameter, but not exceeding 12 inches in diameter, and preferably about 25 feet long, but not exceeding 50 feet4 in length.
- Suitable catalysts for the production of hydrogen by cracking hydrocarbon gases possess high activity and physical strength, and shrink very little at the operating temperatures employed.
- Calcium and magnesium oxides and silica may be added to produce catalysts of greater strength at high temperatures.
- Phosphoric acid with alumina and nickel oxide produce a very active catalyst, which shrinks very little at high tempera tures.
- a particularly suitable catalyst is prepared from nickel oxides, magnesia and kaolin. The catalyst is usually prepared in the form of a paste, cut into small cubes, dried slowly, then heated slowly in the presence of steam to a temperature of about 500 F.
- my catalyst in my furnace comprising diaspore impregnated with nickel nitrate so as to contain about 6% by weight of nickel, and heating to about 500 F. to decompose the nitrate, then reduced by passing therethrough hot reducing gases.
- my catalyst mass comprises particles from about to about in diameter.
- the gas may be cooled immediately after leaving the furnace, if a hydrogen-carbon monoxide mixture is desired for the production of synthetic alcohol, or, if a. gas containing almost entirely hydrogen is desired, it is preferable to pass the exist gas, with added steam over iron oxides or other suitable catalyst in the known manner, for conversion of carbon monoxide to carbon dioxide, then cool the gas, scrub out the carbon dioxide by known means, leaving a hydrogen oi about 95% purity.
- My appl'atus may be Operated at any desired pressure above or below atmospheric, limited only by strength of materials at the operating temperature employed.
- a process for preparing hydrogen which comprises passing reactants comprising gaseous hydrocarbons and steam downwardly through elongate ⁇ vertical tubes contained in a heating zone, simultaneously heating said reactants indirectly by introducing hot flaming gases into said heating zone at a plurality of vertically spaced points along and adjacent to said tubes and substantially tangentially to saidtubes, and withdrawing the resulting combustion gases at a. point adjacent the top oi' said zone, whereby said flaming gases follow an upwardly ascending rotary path around said tubes, Vwhich are thereby uniformly heated without substantial flame impingement thereon.
- a process for preparing hydrogen which comprises passing reactants comprising gaseous hydrocarbons and steam downwardly through elongate vertical catalyst tubes contained in a heating zone, heating said ,reactants indirectly by introducing hot combustion gases into said heating zone at a plurality of vertically spaced points along and adjacent to said tubes and substantially tangentially to said tubes, withdrawing the treated reactants from adjacent the bottom of the said tubes and withdrawing the combustion gases at a point adjacent the top of said heating zone, whereby said hot combustion gases follow an upwardly ascending rotary path around said tubes, which are thereby uniformly heated without substantial flame impingement thereon.
- a process for preparing hydrogen which comprises passing reactants comprising gaseous hydrocarbons and steam downwardly through a bank oi' substantially vertically disposed catalyst tubes contained in a heating zone, heating said 'flame impingement thereon.
- a process for preparing hydrogen which comprises passing reactants comprising gaseous hydrocarbons and steam downwardly through a bank of substantially vertically disposed catalyst tubes contained in a refractorywalled heating zone, maintaining a ratio of from 1 to 10 square feet of refractory wall surface to each square foot of catalyst tube surface, heating said reactants indirectlyby introducing hot combustion gases into said heating zone substantially tangentially to said bank of tubes and at a plurality of vertically spaced points along and adjacent to said bank, withdrawing the treated reactants from adjacent the bottom of the tubes and withdrawing combustion gases at a point adjacent the top of said heating zone, whereby said hot combustion gases follow an upwardly ascending rotary lpath around said bank of tubes, which is thereby uniformly heated without substantial flame impingement thereon.
- a process for preparing hydrogen which comprises passing reactants comprising gaseous hydrocarbons and steam downwardly through a bank of substantially vertically disposed catalyst tubes contained in a refractory-walled heating zone, maintaining a ratio of from 2 to 6 square feet of refractory wall surface to each square foot of catalyst tube surface, heating said reactants indirectly by introducing hot combustion gases into said heating zone substantially ta'ngentially to said bank of tubes and at a plurality of vertically spaced points along and adjacent ,to said bank, withdrawing the treated reactants from adjacent the bottom of the tubes and withdrawing combustion gases at a point adjacent the top of said heating zone, whereby said hot combustion gases follow an upwardly ascending rotary path around said bank of tubes, which is thereby uniformly heated without substantial flame impingement thereon.
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Engineering & Computer Science (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
Priority Applications (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US21521D USRE21521E (en) | 1937-08-30 | Process for catalytic reaction | |
BE429915D BE429915A (de) | 1937-08-30 | ||
US161715A US2173984A (en) | 1937-08-30 | 1937-08-30 | Apparatus and process for catalytic reactions |
DEH3052D DE887801C (de) | 1937-08-30 | 1938-08-18 | Kontaktofen zur Herstellung von wasserstoffreichen Gasen aus gasfoermigen Kohlenwasserstoffen und Wasserdampf |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US161715A US2173984A (en) | 1937-08-30 | 1937-08-30 | Apparatus and process for catalytic reactions |
Publications (1)
Publication Number | Publication Date |
---|---|
US2173984A true US2173984A (en) | 1939-09-26 |
Family
ID=22582393
Family Applications (2)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US21521D Expired USRE21521E (en) | 1937-08-30 | Process for catalytic reaction | |
US161715A Expired - Lifetime US2173984A (en) | 1937-08-30 | 1937-08-30 | Apparatus and process for catalytic reactions |
Family Applications Before (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US21521D Expired USRE21521E (en) | 1937-08-30 | Process for catalytic reaction |
Country Status (3)
Country | Link |
---|---|
US (2) | US2173984A (de) |
BE (1) | BE429915A (de) |
DE (1) | DE887801C (de) |
Cited By (22)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US2571953A (en) * | 1947-09-19 | 1951-10-16 | Hercules Powder Co Ltd | Manufacture of hydrogen |
US2638407A (en) * | 1949-12-31 | 1953-05-12 | Standard Oil Dev Co | Apparatus for close temperature control of catalyzed gas reactions |
US2645566A (en) * | 1949-12-12 | 1953-07-14 | Gas Machinery Co | High-temperature reactor |
US2660519A (en) * | 1948-04-23 | 1953-11-24 | Chemical Construction Corp | Fluid heater |
US2667410A (en) * | 1950-01-04 | 1954-01-26 | Phillips Petroleum Co | Apparatus for reforming hydrocarbons |
US2730434A (en) * | 1950-05-01 | 1956-01-10 | Oxy Catalyst Inc | Catalytic contacting unit |
US2743171A (en) * | 1950-08-23 | 1956-04-24 | United Gas Improvement Co | Method for making gas rich in hydrogen |
US2788266A (en) * | 1951-10-13 | 1957-04-09 | Stirnemann Ernst | Catalytic reactor furnace |
US2852358A (en) * | 1954-06-10 | 1958-09-16 | Commercial Solvents Corp | Process for reforming hydrocarbons |
US2860959A (en) * | 1954-06-14 | 1958-11-18 | Inst Gas Technology | Pressure hydrogasification of natural gas liquids and petroleum distillates |
US2867516A (en) * | 1954-08-18 | 1959-01-06 | Du Pont | Process for burning gaseous fuels |
US2982797A (en) * | 1957-09-25 | 1961-05-02 | Phillips Petroleum Co | Catalyst regeneration and apparatus |
US3055745A (en) * | 1952-11-07 | 1962-09-25 | Vulcan Cincinnati Inc | Catalytic reactor |
US3062197A (en) * | 1959-07-23 | 1962-11-06 | Selas Corp Of America | Tube heater |
US3069348A (en) * | 1959-07-22 | 1962-12-18 | Socony Mobil Oil Co Inc | Multi-stage, multi-zone static bed reforming process and apparatus therefor |
US3190812A (en) * | 1960-01-22 | 1965-06-22 | Ruetgerswerke Ag | Device for the continuous production of hard pitch |
US3198727A (en) * | 1960-05-25 | 1965-08-03 | Socony Mobil Oil Co Inc | Quasi-isothermal hydrocarbon conversion and reactor therefor |
US3285847A (en) * | 1963-05-06 | 1966-11-15 | Phillips Petroleum Co | Fast thermal cracking of heavy carbonaceous materials |
US4101376A (en) * | 1974-03-18 | 1978-07-18 | Metallgesellschaft Aktiengesellschaft | Tubular heater for cracking hydrocarbons |
US4454839A (en) * | 1982-08-02 | 1984-06-19 | Exxon Research & Engineering Co. | Furnace |
WO2015028123A1 (de) * | 2013-08-26 | 2015-03-05 | Thyssenkrupp Industrial Solutions Ag | Sammlerleitung zur gemeinsamen abfuhr von aus mehreren reformerrohren zugeleiteten prozessgasen eines reformers |
WO2015075124A1 (de) * | 2013-11-21 | 2015-05-28 | Basf Se | Verfahren und vorrichtung zur durchführung endothermer reaktionen unter bildung einer wirbelschicht in reaktionsrohren |
Families Citing this family (11)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US2456554A (en) * | 1945-10-12 | 1948-12-14 | United Carr Fastener Corp | Connector for cords or cables |
US2628890A (en) * | 1946-06-20 | 1953-02-17 | Hercules Powder Co Ltd | Process for the decomposition of hydrocarbons |
US2707147A (en) * | 1948-02-07 | 1955-04-26 | Hercules Powder Co Ltd | Production of domestic gas |
US2680061A (en) * | 1951-02-07 | 1954-06-01 | Columbian Carbon | Carbon black |
GB792827A (en) * | 1954-02-19 | 1958-04-02 | Hercules Powder Co Ltd | Improvements in or relating to process for catalytic treatment of hydrocarbons |
US2914386A (en) * | 1954-12-20 | 1959-11-24 | Hercules Powder Co Ltd | Tubular furnace |
FR2045712B1 (de) * | 1969-06-25 | 1973-11-16 | Onia Gegi | |
DE10023410A1 (de) * | 2000-05-12 | 2001-11-15 | Linde Gas Ag | Verfahren zur Erzeugung eines CO- und H2-haltigen Behandlungsgases für die Wärmebehandlung von metallischem Gut, Gasgenerator und Wärmebehandlungsanlage |
DE10023409A1 (de) * | 2000-05-12 | 2001-11-15 | Linde Gas Ag | Gasgenerator und Verfahren zur Erzeugung eines CO- und H2-haltigen Behandlungsgases für die Wärmebehandlung von metallischem Gut sowie Wärmebehandlungsanlage mit einem Gasgenerator |
DE10333854A1 (de) * | 2003-07-24 | 2005-02-17 | Uhde Gmbh | Röhrenspaltofen |
DE102007019830B3 (de) * | 2007-04-25 | 2008-07-31 | Uhde Gmbh | Primärreformer mit brennerzuführenden Sekundäreinlasskanälen |
-
0
- BE BE429915D patent/BE429915A/xx unknown
- US US21521D patent/USRE21521E/en not_active Expired
-
1937
- 1937-08-30 US US161715A patent/US2173984A/en not_active Expired - Lifetime
-
1938
- 1938-08-18 DE DEH3052D patent/DE887801C/de not_active Expired
Cited By (24)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US2571953A (en) * | 1947-09-19 | 1951-10-16 | Hercules Powder Co Ltd | Manufacture of hydrogen |
US2660519A (en) * | 1948-04-23 | 1953-11-24 | Chemical Construction Corp | Fluid heater |
US2645566A (en) * | 1949-12-12 | 1953-07-14 | Gas Machinery Co | High-temperature reactor |
US2638407A (en) * | 1949-12-31 | 1953-05-12 | Standard Oil Dev Co | Apparatus for close temperature control of catalyzed gas reactions |
US2667410A (en) * | 1950-01-04 | 1954-01-26 | Phillips Petroleum Co | Apparatus for reforming hydrocarbons |
US2730434A (en) * | 1950-05-01 | 1956-01-10 | Oxy Catalyst Inc | Catalytic contacting unit |
US2743171A (en) * | 1950-08-23 | 1956-04-24 | United Gas Improvement Co | Method for making gas rich in hydrogen |
US2788266A (en) * | 1951-10-13 | 1957-04-09 | Stirnemann Ernst | Catalytic reactor furnace |
US3055745A (en) * | 1952-11-07 | 1962-09-25 | Vulcan Cincinnati Inc | Catalytic reactor |
US2852358A (en) * | 1954-06-10 | 1958-09-16 | Commercial Solvents Corp | Process for reforming hydrocarbons |
US2860959A (en) * | 1954-06-14 | 1958-11-18 | Inst Gas Technology | Pressure hydrogasification of natural gas liquids and petroleum distillates |
US2867516A (en) * | 1954-08-18 | 1959-01-06 | Du Pont | Process for burning gaseous fuels |
US2982797A (en) * | 1957-09-25 | 1961-05-02 | Phillips Petroleum Co | Catalyst regeneration and apparatus |
US3069348A (en) * | 1959-07-22 | 1962-12-18 | Socony Mobil Oil Co Inc | Multi-stage, multi-zone static bed reforming process and apparatus therefor |
US3062197A (en) * | 1959-07-23 | 1962-11-06 | Selas Corp Of America | Tube heater |
US3190812A (en) * | 1960-01-22 | 1965-06-22 | Ruetgerswerke Ag | Device for the continuous production of hard pitch |
US3198727A (en) * | 1960-05-25 | 1965-08-03 | Socony Mobil Oil Co Inc | Quasi-isothermal hydrocarbon conversion and reactor therefor |
US3285847A (en) * | 1963-05-06 | 1966-11-15 | Phillips Petroleum Co | Fast thermal cracking of heavy carbonaceous materials |
US4101376A (en) * | 1974-03-18 | 1978-07-18 | Metallgesellschaft Aktiengesellschaft | Tubular heater for cracking hydrocarbons |
US4454839A (en) * | 1982-08-02 | 1984-06-19 | Exxon Research & Engineering Co. | Furnace |
WO2015028123A1 (de) * | 2013-08-26 | 2015-03-05 | Thyssenkrupp Industrial Solutions Ag | Sammlerleitung zur gemeinsamen abfuhr von aus mehreren reformerrohren zugeleiteten prozessgasen eines reformers |
CN105492378A (zh) * | 2013-08-26 | 2016-04-13 | 蒂森克虏伯工业解决方案股份公司 | 用于共同除去来自通过多个重整器管道供应的重整器的工艺气体的收集器导管 |
CN105492378B (zh) * | 2013-08-26 | 2018-10-16 | 蒂森克虏伯工业解决方案股份公司 | 用于共同除去来自通过多个重整器管道供应的重整器的工艺气体的收集器导管 |
WO2015075124A1 (de) * | 2013-11-21 | 2015-05-28 | Basf Se | Verfahren und vorrichtung zur durchführung endothermer reaktionen unter bildung einer wirbelschicht in reaktionsrohren |
Also Published As
Publication number | Publication date |
---|---|
DE887801C (de) | 1953-08-27 |
USRE21521E (en) | 1940-07-30 |
BE429915A (de) |
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