WO1996004201A1 - Catalyseur pour le reformage a la vapeur de methane et/ou l'oxydation methanique - Google Patents

Catalyseur pour le reformage a la vapeur de methane et/ou l'oxydation methanique Download PDF

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Publication number
WO1996004201A1
WO1996004201A1 PCT/EP1995/003101 EP9503101W WO9604201A1 WO 1996004201 A1 WO1996004201 A1 WO 1996004201A1 EP 9503101 W EP9503101 W EP 9503101W WO 9604201 A1 WO9604201 A1 WO 9604201A1
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WO
WIPO (PCT)
Prior art keywords
catalyst
methane
nickel
cerium
steam reforming
Prior art date
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PCT/EP1995/003101
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German (de)
English (en)
Inventor
Jürgen Ladebeck
Karl Kochloefl
Original Assignee
Süd-Chemie AG
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 Süd-Chemie AG filed Critical Süd-Chemie AG
Publication of WO1996004201A1 publication Critical patent/WO1996004201A1/fr

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    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
    • B01J23/8933—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/894—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with rare earths or actinides
    • 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
    • C01B3/025—Preparation or purification of gas mixtures for ammonia synthesis
    • 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
    • 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
    • C01B3/40—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 characterised by the catalyst
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/153—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases characterised by the catalyst used
    • C07C29/156—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases characterised by the catalyst used containing iron group metals, platinum group metals or compounds thereof
    • 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
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
    • 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
    • C01B2203/1005—Arrangement or shape of catalyst
    • C01B2203/1011—Packed bed of catalytic structures, e.g. particles, packing elements
    • 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
    • C01B2203/1064—Platinum group metal catalysts
    • C01B2203/107—Platinum 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
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1082—Composition of support materials
    • 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
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/50—Improvements relating to the production of bulk chemicals
    • Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts

Definitions

  • the invention relates to a catalyst for methane vapor reforming and / or methane oxidation, containing platinum on an aluminum oxide support.
  • the production of various synthesis gases or of hydrogen from methane is one of the most important processes in chemical technology as the basis for the synthesis of methanol, Fischer-Tropsch hydrocarbons, oxo alcohols and ammonia.
  • the technically preferred production process is methane steam reforming according to equations 1 and 2.
  • the first reaction is endothermic and the heat required for this must be supplied to the reaction system.
  • the basic information on methane steam reforming is contained in numerous references (see, for example, "Catalytic Steam Reforming” in “Catalysis” Science and Technology, Vol. 5, Springer Verlag, Berlin, 1985 or “Catalysis” Vol. 3, Specialist Periodical Reports , London 1980, The Chemical Society).
  • a technically important variant is the autothermal methane steam reforming, in which the required heat is not supplied from the outside, but is generated directly in the reformer reactor. This is achieved by adding oxygen to a mixture of methane and water vapor.
  • Partial methane oxidation is a technically important alternative for synthesis gas production.
  • a mechanical destruction of the shaped catalyst articles and the loss of activity, in particular the upper catalyst layer in the reformer, are mostly caused by a strong mechanical-thermal load.
  • the result is a reduced ignitability of the catalyst, which should initiate the catalytic combustion of the methane component, and thereby an increased risk of explosion.
  • noble metal catalysts Pt, Pd, Rh on aluminum oxide
  • Ru, Pd, Rh on aluminum oxide are known which are used to initiate methane oxidation (equation 3) in the upper part of a reformer, the lower part of the reactor being coated with a commercial nickel -Reforming catalyst is filled.
  • these noble metal catalysts initiate methane oxidation, they have the disadvantage that the heat of reaction builds up in the first catalyst zone before it is removed by the subsequent reforming reaction (equation 1). The The consequence of this is overheating of the precious metal catalyst and its damage, or a significantly shortened service life.
  • the invention was based on the object of developing a catalyst which, in addition to the high methane oxidation activity, also has a corresponding steam reforming activity.
  • a catalyst for methane steam reforming and / or methane oxidation which contains platinum on an aluminum oxide support and which is characterized in that the support 2 to 12 wt .-%, preferably 5 to 8 wt .-% nickel and 1 to 10 wt .-%, preferably 3 to 6 wt .-% cerium (each calculated as metals and based on the total catalyst).
  • the catalyst according to the invention is surprisingly mechanically and catalytically very stable at temperatures above 850 ° C. and enables a reliable mode of operation in the case of autothermal methane vapor reforming, its oxidation activity (ignitability) remaining constant over longer periods of time.
  • the catalyst according to the invention initiates methane oxidation, and the heat of reaction developed in this way (equation 3) is simultaneously consumed by the reforming reaction taking place on the catalyst (equation 1).
  • the catalyst according to the invention without acting as a reforming catalyst, can be used as a catalyst for partial methane oxidation (equation 5).
  • the nickel is preferably present as nickel oxide or partly as nickel aluminate and cerium as cerium dioxide in an X or O_-Al 2 O 3 matrix.
  • the catalyst according to the invention generally contains about 0.01 to 1.0% by weight, preferably about 0.03 to 0.8% by weight. Platinum.
  • the carrier is preferably in the form of tablets, spheres, in particular rings or multi-hole tablets or wagon wheels. It can also be used in differently shaped articles.
  • the hollow bodies which are preferably used have a lower gas flow resistance than the solid molded bodies.
  • the catalyst according to the invention is preferably prepared by impregnating support bodies made of (- or ⁇ -Al 03 with aqueous nickel and cerium salt solution and thermally decomposing these salts to nickel oxide and cerium dioxide, whereupon an impregnation is carried out with an aqueous platinum salt solution.
  • Aqueous nickel and cerium salts Ce 3+ and Ni 2+ nitrate are preferably used, and H PtClg as the platinum salt.
  • the support impregnated with the nickel and cerium salt solutions is dried at about 100 to 180 ° C., in particular at about 130 ° C., and then calcined at about 400 to 1300 ° C., preferably at about 450 to 1200 ° C.
  • the aqueous hexachloroplatinic acid (H 2 PtClg) solution drying at about 100 to 180 ° C., in particular at about 130 ° C., and a final calcination at about 400 to 500 ° C., in particular at about 450 ° C.
  • the invention furthermore relates to the use of the catalyst indicated above in the autothermal methane reforming to initiate the methane oxidation and to the methane steam reforming which takes place in parallel therewith.
  • Another use of the catalyst comprises the initiation of methane oxidation in the upper part of a reformer reactor which is filled with a nickel-supported catalyst known per se is.
  • a third use of the catalyst involves partial methane oxidation to produce synthesis gas (Equation 5).
  • 500 g of a shaped ⁇ -Al 2 03 carrier are dissolved in 200 ml of deionized in 200 ml of aqueous cerium and nickel nitrate solution (75 g of Ce (NO3) 3 -6H 2 0 and 160 g of Ni ( ⁇ 3) 2 -6H 2 0 Water and made up to a volume of 200 ml) at 45 ° C.
  • the Al 2 ⁇ 3 support impregnated with cerium and nickel is first dried at 130 ° C. for 12 hours and then calcined at 450 ° C. for 3 hours.
  • Example 2 570 g of the cerium- and nickel-containing catalyst precursor from Example 2 are immersed in 200 ml of aqueous hexachloroplatinic acid solution (6 g of 10% H 2 PtClg, dissolved in deionized water and made up to a volume of 200 ml) at 25 ° C. Further processing is carried out as in Example 2.
  • aqueous hexachloroplatinic acid solution (6 g of 10% H 2 PtClg, dissolved in deionized water and made up to a volume of 200 ml
  • the "ignition temperature” was determined as a measure of the catalyst activity;
  • the composition of the reaction products was as Selekti ⁇ vticianshackstab by gas chromatography at temperatures Zvi ⁇ rule 300 and 700 ° C.
  • the test gas was composed of 2 6 V ol -% CH 4, 8 V ol .-% 0 2 and 66 vol .-% N 2 together.
  • the space ⁇ speed of the test gas was 10000 "l.
  • the catalyst temperature was a b 250 ° C at a rate of l ° C / min. increased to determine the ignition temperature.
  • the other catalysts according to the invention such as K-2, K-3 and K-4, also showed practically identical behavior in the methane oxidation and gave similar compositions of the reaction products.
  • the dry test gas had the following composition:

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

Abstract

L'invention concerne un catalyseur utilisé pour le reformage à la vapeur de méthane et/ou l'oxydation méthanique, contenant du platine sur un support en oxyde d'aluminium, qui se caractérise en ce que le support contient entre 2 et 12 % en poids, de préférence entre 5 et 8 % en poids de nickel et entre 1 et 10 % en poids, de préférence entre 3 et 6 % en poids de Cer (chacun de ces pourcentages étant calculé en tant que métal et étant rapporté à l'ensemble du catalyseur).
PCT/EP1995/003101 1994-08-04 1995-08-03 Catalyseur pour le reformage a la vapeur de methane et/ou l'oxydation methanique WO1996004201A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE4427665A DE4427665A1 (de) 1994-08-04 1994-08-04 Katalysator für die Methandampfreformierung und/oder Methanoxidation
DEP4427665.6 1994-08-04

Publications (1)

Publication Number Publication Date
WO1996004201A1 true WO1996004201A1 (fr) 1996-02-15

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PCT/EP1995/003101 WO1996004201A1 (fr) 1994-08-04 1995-08-03 Catalyseur pour le reformage a la vapeur de methane et/ou l'oxydation methanique

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DE (1) DE4427665A1 (fr)
WO (1) WO1996004201A1 (fr)
ZA (1) ZA956493B (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1110362C (zh) * 1996-11-17 2003-06-04 中国石化齐鲁石油化工公司 节能型烃类水蒸汽转化催化剂及用途
CN110026201A (zh) * 2019-05-10 2019-07-19 大连大学 一种用于甲烷催化燃烧的催化剂及其制备方法

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WO1998035908A1 (fr) * 1997-02-14 1998-08-20 Shell Internationale Research Maatschappij B.V. Oxydation catalytique partielle d'hydrocarbures
DE10025032A1 (de) * 2000-05-20 2001-11-29 Dmc2 Degussa Metals Catalysts Verfahren zur autothermen, katalytischen Dampfreformierung von Kohlenwasserstoffen
US6557342B2 (en) * 2000-09-19 2003-05-06 Nissan Motor Co., Ltd. Exhaust gas purifying system
US6729125B2 (en) 2000-09-19 2004-05-04 Nissan Motor Co., Ltd. Exhaust gas purifying system
WO2002038268A1 (fr) * 2000-11-08 2002-05-16 Idemitsu Kosan Co., Ltd. Catalyseur de reformage pour hydrocarbures et procede de reformage correspondant
US7067453B1 (en) 2001-07-13 2006-06-27 Innovatek, Inc. Hydrocarbon fuel reforming catalyst and use thereof
DE10157155A1 (de) * 2001-11-22 2003-06-12 Omg Ag & Co Kg Verfahren zur katalytischen autothermen Dampfreformierung von höheren Alkoholen, insbesondere Ethanol

Citations (1)

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Publication number Priority date Publication date Assignee Title
JPH05270803A (ja) * 1992-03-24 1993-10-19 Toyo Eng Corp メタンと二酸化炭素および水蒸気を原料とする合成ガスの製造方法

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DE3539127C1 (de) * 1985-11-05 1987-01-02 Hoechst Ag Verfahren zur Herstellung eines Traegerkatalysators
GB9028034D0 (en) * 1990-12-24 1991-02-13 Isis Innovation Improved processes for the conversion of methane to synthesis gas
JP3226558B2 (ja) * 1991-03-12 2001-11-05 日石三菱株式会社 炭化水素の高温水蒸気改質用触媒
US5321160A (en) * 1991-07-31 1994-06-14 Tosoh Corporation Process for producing an ethylenamine
EP0582004B1 (fr) * 1992-07-29 1997-01-29 Council of Scientific and Industrial Research Catalyseurs et leur utilisation dans la conversion par oxydation de méthane ou de gaz naturel en gaz de synthèse

Patent Citations (1)

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Publication number Priority date Publication date Assignee Title
JPH05270803A (ja) * 1992-03-24 1993-10-19 Toyo Eng Corp メタンと二酸化炭素および水蒸気を原料とする合成ガスの製造方法

Non-Patent Citations (2)

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DATABASE WPI Week 9346, Derwent World Patents Index; AN 364927 *
S. S. MAHMOUD: "Hydrogenation of phenylacetylene over (Pt-Ni)/Al2O3 and (Pt-Ni-Ce)/Al2O3 alloys", INDIAN JOURNAL OF TECHNOLOGY, vol. 31, INDIA, pages 709 - 712 *

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1110362C (zh) * 1996-11-17 2003-06-04 中国石化齐鲁石油化工公司 节能型烃类水蒸汽转化催化剂及用途
CN110026201A (zh) * 2019-05-10 2019-07-19 大连大学 一种用于甲烷催化燃烧的催化剂及其制备方法
CN110026201B (zh) * 2019-05-10 2022-05-17 大连大学 一种用于甲烷催化燃烧的催化剂及其制备方法

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ZA956493B (en) 1996-03-15
DE4427665A1 (de) 1996-02-08

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