DE1009165B - Process for the flameless conversion of gaseous hydrocarbons with insufficient amounts of oxygen for complete combustion to carbon oxide and hydrogen - Google Patents

Process for the flameless conversion of gaseous hydrocarbons with insufficient amounts of oxygen for complete combustion to carbon oxide and hydrogen

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Publication number
DE1009165B
DE1009165B DEB36807A DEB0036807A DE1009165B DE 1009165 B DE1009165 B DE 1009165B DE B36807 A DEB36807 A DE B36807A DE B0036807 A DEB0036807 A DE B0036807A DE 1009165 B DE1009165 B DE 1009165B
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DE
Germany
Prior art keywords
oxygen
hydrogen
conversion
flameless
complete combustion
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.)
Pending
Application number
DEB36807A
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German (de)
Inventor
Dr Ernst Bartholome
Dr Alfred Helms
Dr Otto Frey
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
BASF SE
Original Assignee
BASF SE
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by BASF SE filed Critical BASF SE
Priority to DEB36807A priority Critical patent/DE1009165B/en
Publication of DE1009165B publication Critical patent/DE1009165B/en
Pending legal-status Critical Current

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Classifications

    • 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
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/28—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using moving solid particles
    • C01B3/30—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using moving solid particles using the fluidised bed technique
    • 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
    • C01B3/386—Catalytic partial combustion
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0261—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a catalytic partial oxidation step [CPO]
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1052—Nickel or cobalt catalysts
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1276—Mixing of different feed components

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Description

DEUTSCHESGERMAN

Das Hauptpatent 938 610 betrifft ein Verfahren zur flammenlosen Umsetzung von gasförmigen Kohlenwasserstoffen an fest angeordneten Katalysatoren unter Wasserdampfzusatz mit einer zur vollständigen Verbrennung unzureichenden Menge Sauerstoff zu Kohlenoxyd und Wasserstoff. Die Gase werden vor der Einführung in den Reaktionsofen in einer oder mehreren Mischvorrichtungen zusammengeführt, nachdem zuvor dem sauerstoffhaltigen Gas Wasserdampf in einer Menge zugeführt wurde, die ausreicht, eine durch Zündung an der Mischstelle auftretende Flamme aus der Mischvorrichtung hinauszutragen und zu löschen, wobei das sauerstoffhaltige Gas, in Volumprozent gerechnet, mehr Wasserdampf enthält als das kohlenwasserstoffhaltige Gas.The main patent 938 610 relates to a method for the flameless conversion of gaseous hydrocarbons on fixed catalysts with the addition of steam with a complete Combustion of insufficient amount of oxygen to carbon dioxide and hydrogen. The gases are in front after being introduced into the reaction furnace in one or more mixing devices previously the oxygen-containing gas was supplied water vapor in an amount sufficient to a to carry out the flame occurring at the mixing point by ignition from the mixing device and to extinguish, whereby the oxygen-containing gas, calculated as a percentage by volume, contains more water vapor than that hydrocarbon-containing gas.

Es wurde nun gefunden, daß man dieses Verfahren mit Vorteil auch in der Weise durchführen kann, daß man die Katalysatoren statt in fest angeordneter Form in Wirbelschicht verwendet.It has now been found that this process can also be carried out with advantage in such a way that the catalysts are used in a fluidized bed instead of in a fixed form.

Die Erzeugung der Wirbelschicht geschieht in der üblichen Weise. Im übrigen arbeitet man, wie es im Hauptpatent beschrieben ist.The fluidized bed is generated in the usual way. Otherwise one works as it does in the Main patent is described.

Die katalytische Erzeugung von Kohlenoxyd und Wasserstoff aus Kohlenwasserstoffen und Sauerstoff unter Zugabe von Dampf im Wirbelschichtverfahren ist an sich bereits bekannt. Bei keinem dieser bekannten Verfahren bestand jedoch die durch die vorliegende Erfindung gelöste Aufgabe, eine durch Zündung an der Mischstelle auftretende Flamme aus der Mischvorrichtung hinauszutragen und zu löschen. Bei dem Verfahren der USA.-Patentschrift 2 681 272 werden die zu spaltenden Kohlenwasserstoffe getrennt dem Reaktionsgefäß zugeführt, wogegen die Mischung der umzusetzenden Kohlenwasserstoffe mit Sauerstoff vor Eintritt in den Reaktionsraum die Vorteile einer beschleunigten Umsetzung und besserer Wärmeausnutzung bietet. Bei dem Verfahren der USA.-Patentschrift 2 697 655 wird ein Gemisch von Kohlenwasserstoffen und Wasserdampf zusammen mit einer zuvor durch partielle Verbrennung von Kohlenwasserstoffen erzeugten, hauptsächlich aus Kohlenoxyd und Wasserstoff bestehenden heißen Gasmischung in die Wirbelschicht eingeführt. In beiden Fällen kann von einer Gefahr einer Flammenbildung an einer Mischstelle nicht gesprochen werden, und somit konnte aus diesen Veröffentlichungen auch nicht entnommen werden, wie sich eine Flammenbildung an der Mischstelle vermeiden oder unschädlich machen läßt.The catalytic production of carbon monoxide and hydrogen from hydrocarbons and oxygen with the addition of steam in the fluidized bed process is already known per se. None of these known methods, however, the problem solved by the present invention was one by Carry out ignition of the flame occurring at the mixing point from the mixing device and extinguish it. In the process of US Pat. No. 2,681,272, the hydrocarbons to be cleaved are separated fed to the reaction vessel, whereas the mixture of the hydrocarbons to be converted with oxygen the advantages of accelerated conversion and better heat utilization before entering the reaction chamber offers. In the process of U.S. Patent 2,697,655, a mixture of hydrocarbons and water vapor together with a pre-partial combustion of hydrocarbons produced, consisting mainly of carbon oxide and hydrogen, hot gas mixture into the fluidized bed introduced. In both cases, there is a risk of flame formation at a mixing point cannot be spoken, and therefore it could not be inferred from these publications how a flame formation at the mixing point can be avoided or rendered harmless.

Beispielexample

In einer Wirbelschichtkammer von einer lichten Weite von 2,5 m und einer Wirbelschichthöhe von etwa 1,5 m wird ein Kokereigas mit etwa 3O°/o Methangehalt mit Sauerstoff bei 950° und gewöhn-Verfahren zur flammenlos en Umsetzung von gasförmigen KohlenwasserstoffenIn a fluidized bed chamber with a clear width of 2.5 m and a fluidized bed height of About 1.5 m a coke oven gas with about 30% methane content with oxygen at 950 ° and habitual process for the flameless conversion of gaseous hydrocarbons

mit zur vollständigen Verbrennungwith for complete combustion

unzureichenden Mengen Sauerstoffinsufficient amounts of oxygen

zu Kohlenoxyd und Wasserstoffto carbon dioxide and hydrogen

Zusatz zum Patent 938 610Addendum to patent 938 610

Anmelder:Applicant:

Badische Anilin- & Soda-Fabrik
Aktiengesellschaft, Ludwigshafen/RheinAniline & Soda Factory in Baden
Aktiengesellschaft, Ludwigshafen / Rhein

Dr. Ernst Bartholome, Heidelberg, Dr. Alfred Helms und Dr. Otto Frey, Ludwigshafen/Rhein,Dr. Ernst Bartholome, Heidelberg, Dr. Alfred Helms and Dr. Otto Frey, Ludwigshafen / Rhine,

sind als Erfinder genannt wordenhave been named as inventors

lichem Druck zu Synthesegas umgesetzt. Die Wirbelschichtkammer ist mit einem feinkörnigen Katalysator aus Magnesit mit einem Gehalt von etwa 3 Gewichtsprozent Nickel gefüllt. Die Mischung der Gase erfolgt in einer aus zwei konzentrischen Rohren bestehenden Vorrichtung, wobei das innere kürzere Rohr für die Sauerstoffzuführung dient, während das Kokereigas durch den von beiden Rohren gebildeten Ringkanal zuströmt.Lich pressure converted to synthesis gas. The fluidized bed chamber is with a fine-grained catalyst made of magnesite with a content of about 3 percent by weight Nickel filled. The gases are mixed in a tube consisting of two concentric tubes Device, the inner shorter tube for the oxygen supply, while the coke oven gas flows through the annular channel formed by the two tubes.

Werden das Kokereigas und der Sauerstoff vor der Vermischung bei 70° mit Wasserdampf gesättigt, wobei also beide Gase, in Volumprozent gerechnet, gleiche Mengen Wasserdampf enthalten, so führen gelegentliche im technischen Betrieb unvermeidliche Vorzündungen bei den in der Wirbelschicht üblichen Belastungen von etwa 700 m3 feuchtem Endgas je m2 Fläche des Reaktionsofens und Stunde zu einer an der Sauerstoffdüse haftenden, bleibenden Flamme.If the coke oven gas and the oxygen are saturated with water vapor at 70 ° before they are mixed, so both gases contain the same amount of water vapor, calculated as a percentage by volume, then occasional pre-ignition, which is unavoidable in technical operation, leads to the loads of around 700 m 3 that are common in the fluidized bed moist end gas per m 2 of area of the reaction furnace and hour to a permanent flame adhering to the oxygen nozzle.

Durch Vorversuche stellt man fest, daß gelegentliche Vorreaktionen in der Mischapparatur aus dieser herausgetragen werden, wenn dem Sauerstoff eine weitere Wasserdampfmenge zugeführt wird, die je Nm3 etwa gleich der Sauerstoffmenge ist. Unter diesen Bedingungen ist es möglich, betriebssicher ohne Bildung einer stationären Flamme in der Mischvorrichtung zu arbeiten. In der Mischvorrichtung erleidet das im Ringraum zuströmende Kokereigas einenPreliminary tests show that occasional preliminary reactions in the mixing apparatus are carried out of this when a further amount of water vapor is added to the oxygen which is approximately equal to the amount of oxygen per Nm 3. Under these conditions it is possible to work reliably without the formation of a stationary flame in the mixing device. In the mixing device, the coke oven gas flowing in in the annular space suffers from a

709 546/409709 546/409

Druckverlust von weniger als einem halben Meter Wassersäule, das im inneren Rohr strömende Gemisch von Sauerstoff und Wasserdampf einen Druckverlust von weniger als einem Meter Wassersäule.Pressure loss of less than half a meter of water, the mixture flowing in the inner pipe of oxygen and water vapor a pressure loss of less than a meter of water column.

Claims (1)

PATENTANSPRUCH:PATENT CLAIM: Abänderung des Verfahrens zur flammenlosen Umsetzung von gasförmigen Kohlenwasserstoffen an Katalysatoren unter Wasserdampfzusatz mit zur vollständigen Verbrennung unzureichendenModification of the process for the flameless conversion of gaseous hydrocarbons on catalysts with the addition of steam with insufficient for complete combustion Mengen Sauerstoff zu Kohlenoxyd und Wasserstoff, wobei die Gase vor der Einführung in den Reaktionsofen in einer oder mehreren Mischvorrichtungen zusammengeführt werden, nach Patent 938 610, dadurch gekennzeichnet, daß die Katalysatoren statt in fest angeordneter Form in Wirbelschicht verwendet werden.Amounts of oxygen to carbon and hydrogen, with the gases before introduction into the Reaction furnace are brought together in one or more mixing devices, according to patent 938 610, characterized in that the catalysts instead of in a fixed form in fluidized bed be used. In Betracht gezogene Druckschriften:
USA.-Patentschriften Nr. 2 681272, 2 697 655.Considered publications:
U.S. Patent Nos. 2,681,272, 2,697,655. © 709 5W409 5.© 709 5W409 5.
DEB36807A 1954-06-26 1955-08-10 Process for the flameless conversion of gaseous hydrocarbons with insufficient amounts of oxygen for complete combustion to carbon oxide and hydrogen Pending DE1009165B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
DEB36807A DE1009165B (en) 1954-06-26 1955-08-10 Process for the flameless conversion of gaseous hydrocarbons with insufficient amounts of oxygen for complete combustion to carbon oxide and hydrogen

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE777527X 1954-06-26
DEB36807A DE1009165B (en) 1954-06-26 1955-08-10 Process for the flameless conversion of gaseous hydrocarbons with insufficient amounts of oxygen for complete combustion to carbon oxide and hydrogen
DEB0056807 1955-08-10

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Publication Number Publication Date
DE1009165B true DE1009165B (en) 1957-05-29

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1098148B (en) * 1959-02-09 1961-01-26 Didier Werke Ag Gas generating furnace for the production of fuel gas by catalytic splitting of hydrocarbons at normal pressure
DE1144239B (en) * 1959-09-01 1963-02-28 Basf Ag Process for the conversion of gaseous and liquid, sulfur-containing hydrocarbons, especially minerals, to hydrogen and carbon oxide

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2681272A (en) * 1948-01-10 1954-06-15 Kellogg M W Co Method for manufacture of a gas rich in hydrogen
US2697655A (en) * 1947-12-31 1954-12-21 Kellogg M W Co Manufacture of a hydrogen-rich gas

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2697655A (en) * 1947-12-31 1954-12-21 Kellogg M W Co Manufacture of a hydrogen-rich gas
US2681272A (en) * 1948-01-10 1954-06-15 Kellogg M W Co Method for manufacture of a gas rich in hydrogen

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1098148B (en) * 1959-02-09 1961-01-26 Didier Werke Ag Gas generating furnace for the production of fuel gas by catalytic splitting of hydrocarbons at normal pressure
DE1144239B (en) * 1959-09-01 1963-02-28 Basf Ag Process for the conversion of gaseous and liquid, sulfur-containing hydrocarbons, especially minerals, to hydrogen and carbon oxide

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