EP2076332A1 - Hydrogen production method by direct decomposition of natural gas and lpg - Google Patents

Hydrogen production method by direct decomposition of natural gas and lpg

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Publication number
EP2076332A1
EP2076332A1 EP07826782A EP07826782A EP2076332A1 EP 2076332 A1 EP2076332 A1 EP 2076332A1 EP 07826782 A EP07826782 A EP 07826782A EP 07826782 A EP07826782 A EP 07826782A EP 2076332 A1 EP2076332 A1 EP 2076332A1
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EP
European Patent Office
Prior art keywords
catalyst
natural gas
lpg
hydrogen production
direct decomposition
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.)
Ceased
Application number
EP07826782A
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German (de)
French (fr)
Inventor
Rafig Alibeyli
Beycan Ibrahimoglu
Sadig Guliyev
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.)
Vestel Elektronik Sanayi ve Ticaret AS
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Vestel Elektronik Sanayi ve Ticaret AS
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Publication of EP2076332A1 publication Critical patent/EP2076332A1/en
Ceased legal-status Critical Current

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    • 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; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/22—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/26—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts
    • 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
    • B01J23/74—Iron group metals
    • B01J23/755—Nickel
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0201—Impregnation
    • B01J37/0205—Impregnation in several steps
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • 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
    • B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
    • B01J21/02—Boron or aluminium; Oxides or hydroxides thereof
    • B01J21/04—Alumina
    • 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
    • C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
    • C01B2203/0277—Processes for making hydrogen or synthesis gas containing a decomposition step containing a catalytic decomposition 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
    • C01B2203/10—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
    • C01B2203/1058—Nickel 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
    • 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

Definitions

  • the present invention relates to producing hydrogen in the petrochemistry field, particularly from natural gas or LPG (Liquefied Petroleum Gas) or from other gas mixtures containing the C 1 -C 4 hydrocarbons.
  • the hydrogen production approach according to the present invention is achieved by making use of Ni-Fe/ ⁇ -AI 2 O 3 type catalysts with a higher activity and a special preparation method.
  • Both of such methods are conducted at temperatures ranging from 750 0 C to 800 0 C and under low pressure levels. Both such methods bring about the following significant drawbacks: conducting the process at high temperatures; formation of CO besides H 2 in the process; provision of a special catalytic conversion system to completely convert CO to CO 2 .
  • the approach of the background art closest to the present invention is the process whereby methane is catalytically decomposed directly to hydrogen and carbon.
  • the basic drawback of this process is the high temperature (700-750 0 C) requirement to provide a high CH 4 conversion yield, whereas the others may be listed as following: - higher energy costs; material selection difficulty for the reactor; an increase in the amount of coke that forms and a decrease in the fixed working period without oxidative regeneration of the catalysts; shortening of the general working life of catalysts.
  • the present invention provides a high-yield hydrogen production approach at relatively lower temperatures by means of direct decomposition of natural gas, LPG, or other gas mixtures having a C r C 4 -hydrocarbon content.
  • This approach is achieved by making use of Ni-Fe/ ⁇ - AI 2 O 3 type catalysts with a higher activity and a special preparation method.
  • the subject process is as following.
  • the catalyst for the direct decomposition of methane is prepared according to the subject process.
  • industrial-type Y-AI 2 O 3 is used as the catalyst carrier, and Ni and Fe are employed as active metals.
  • concentrations of Ni and Fe each vary between 5% and 20% on the catalyst's surface.
  • the catalysts are prepared by adsorbing on the carrier surface the aqueous solutions of metal salts (typically the nitrate salts) in a multi-step method.
  • the adsorption phase is conducted at the room temperature.
  • the carrier is subjected to adsorption, the solution is evaporated and the catalyst dried under air.
  • the calcination of catalyst is carried out in an oven under air.
  • Ni-Fe/ ⁇ -AI 2 O 3 catalyst used in this invention has the following advantages as compared to known catalysts used for the direct decomposition of natural gas (or methane): the aqueous solutions of Ni and Fe salts are adsorbed in a multi-step manner on the carrier in order to have a more homogeneous distribution of such active metals on the carrier surface;
  • Ni and Fe salts are adsorbed together onto the carrier surface; and the catalyst is subjected to calcination after each interim adsorption step conducted on the carrier surface.
  • Any such prepared catalysts are used in the direct decomposition process of natural gas or LPG according to the present invention.
  • the process is conducted under atmosphere pressure and at 550-650 0 C temperature.
  • the volumetric flow rate of natural gas or LPG used as raw materials in this process varies between 720 hour “1 and 4320 hour “1 .
  • the conversion rate of methane in the natural gas to hydrogen varies between 66 to 91% according to the conditions of this process.
  • the contents of the natural gas and LPG used as inputs in the process, and the gaseous products as the output of the process are analyzed by means of Gas Chromatography.
  • the amount and character of the coke formed on the catalyst surface as a result of directly decomposing CH 4 according to this process are studied by the Differential Thermal-Gravimetric Analysis method.
  • Ni + 5% Fe/ ⁇ -AI 2 O 3 catalyst is prepared for use in the subject process. For this reason, 3.12 g Ni(NO 3 ) 2 .6H 2 O and 4.56 g Fe(NO 3 ) 3 .9H 2 O salts are dissolved in 10 ml distilled water and the resulting solution is adsorbed in two steps under mixing for 12 hours on the surface of Y-AI 2 O 3 (10 g), which is previously dried under 150 0 C for 4 hours.
  • the solution is evaporated and the catalyst is dried under air at 150 0 C for 6 hours and subjected to calcination at 500°C for 4 hours, then in the second step following adsorption, the solution is evaporated again and the catalyst dried under air at 15O 0 C. Then, the catalyst is subjected to the final calcination step under air at 75O 0 C for 4 hours. In the calcination steps, the temperature is raised by 150°C/hour "1 starting from 150°C.
  • a 2.5 g aliquot is taken from the prepared catalyst and used for directly decomposing the natural gas.
  • the content of the natural gas used as raw material in this process is as following (% by volume): H 2 - 0.14, CH 4 - 87.84, C 2 H 6 - 4.16, C 3 - 1.19, C 4 -C 5 - 0.03, N 2 - 5.6, O 2 - 0.51 , CO 2 - 0.43.
  • the process is conducted in a continuous experiment system with a fixed bed quarts reactor under atmosphere pressure at 65O 0 C and 30 ml/min gas flow rate (720 hour "1 ).
  • the reactor's inner diameter and length are 2.2 cm and 20 cm, respectively. After the gaseous products are put out of the reactor, they are cooled in a water cooler and analyzed by means of GC. The result is as following:
  • Ni + 10% Fe/ ⁇ -AI 2 O 3 catalyst is prepared for use in this process. Respectively 6.24 g and 9.12 g of Ni(NO 3 ) 2 .6H 2 O and Fe(NO 3 ) 3 .9H 2 O salts are used in the catalyst's synthesis. The adsorption of aqueous solutions of metal salts on the catalyst surface is conducted at three steps.
  • Ni + 20% Fe/ ⁇ -AI 2 O 3 catalyst is prepared for use in this process. Respectively 12.48 g and 18.24 g of Ni(NO 3 ) 2 .6H 2 O and Fe(NO 3 ) 3 .9H 2 O salts are used in the catalyst's synthesis. The adsorption of aqueous solutions of metal salts on the catalyst surface is conducted at four steps in the preparation of the catalyst.
  • 20% Ni + 20% Fe/ ⁇ -Al 2 O 3 catalyst is prepared for use in this process.
  • the preparation of the catalyst is conducted by means of a 4-step adsorption method.
  • the direct decomposition process is conducted at 550°C temperature.
  • 20% Ni + 20% Fe/ ⁇ -AI 2 O 3 catalyst is prepared for use in the subject process.
  • LPG with the following content (% by volume) is used as the raw material in this process: H 2 - 0.2, CH 4 - 0.6, C 2 H 6 - 15.99, C 3 - 50.98, C 4 - 29.15, C 5 - 0.19, N 2 - 1.78, O 2 - 1.11.
  • the temperature of the direct decomposition process is 650 0 C and the flow rate of the natural gas is 30 ml/min (720 hour "1 ).

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

Abstract

A nickel-iron catalyst on gamma-aluminum oxide which is prepared by means of a multi- step adsorption approach in a hydrogen production method by direct decomposition of natural gas and LPG is used. Aqueous solutions of nickel and iron nitrate salts are adsorbed together on the gamma-aluminum surface in preparing the catalyst used in this method, wherein the weight ratio of nickel and iron on the catalyst surface is 1 :1 and their total weight is 20-40% by weight. The temperature of this method varies between 550°C to 650°C.

Description

DESCRIPTION
HYDROGEN PRODUCTION METHOD BY DIRECT DECOMPOSITION OF NATURAL
GAS AND LPG
TECHNICAL FIELD The present invention relates to producing hydrogen in the petrochemistry field, particularly from natural gas or LPG (Liquefied Petroleum Gas) or from other gas mixtures containing the C1-C4 hydrocarbons. The hydrogen production approach according to the present invention is achieved by making use of Ni-Fe/γ-AI2O3 type catalysts with a higher activity and a special preparation method. TECHNICAL PROBLEMS THE PRESENT INVENTION AIMS TO SOLVE
Nowadays, various methods are known for producing hydrogen from natural gas. One of such methods reported in the "Journal of Power Sources" (Alessandra Fonseka, Elisabete M. Assaf - Production of the hydrogen by methane steam reforming over nickel catalysts prepared from hydrotalcite precursors, 142 (2005), 154-159.) is based on reforming of natural gas, LPG, or other hydrocarbon gases with water stream, or as reported in the "Fuel Processing Technology" (Shan Xu, Rui Zhao, Xiaolai Wang - Highly coking resistant and stable Ni/AI2O3 catalysts prepared by W/O microemulsion for partial oxidation of methane, 86 (2004), 123-133.), based on the partial oxidation thereof. Both of such methods are conducted at temperatures ranging from 7500C to 8000C and under low pressure levels. Both such methods bring about the following significant drawbacks: conducting the process at high temperatures; formation of CO besides H2 in the process; provision of a special catalytic conversion system to completely convert CO to CO2.
In addition to the abovementioned methods, another method reported in Applied Catalysis A: General (Jiuling Chen, Yongdan Li, Zongquan Li, Xixiang Zhang - Production of COx- free hydrogen and nanocarbon by direct decomposition of undiluted methane on Ni-Cu- alumina catalysts, 269 (2004), 179-186.) is based on decomposing methane on the catalyst's surface directly to hydrogen and carbon:
CH4 → 2H2 + C. This method has a very significant advantage as compared to the methods given above. No CO formation takes place in this process. The direct decomposition process of methane is conducted on various solid catalysts. Such catalysts include various carriers such as zeolites, SiO2 , AI2O3, etc. and active metals (such as Ni, Zn, Cu, etc.). Various methods such as adsorption, cation exchange, deposition, etc. are employed to prepare these catalysts.
The approach of the background art closest to the present invention is the process whereby methane is catalytically decomposed directly to hydrogen and carbon. (Jiuling Chen, Yongdan Li, Zongquan Li, Xixiang Zhang - Production of COx-free hydrogen and nanocarbon by direct decomposition of undiluted methane on Ni-Cu-alumina catalysts, Applied Catalysis A: General, 269 (2004), 179-186.) The basic drawback of this process is the high temperature (700-750 0C) requirement to provide a high CH4 conversion yield, whereas the others may be listed as following: - higher energy costs; material selection difficulty for the reactor; an increase in the amount of coke that forms and a decrease in the fixed working period without oxidative regeneration of the catalysts; shortening of the general working life of catalysts. In order to eliminate the aforesaid drawbacks of the foregoing methods, the present invention provides a high-yield hydrogen production approach at relatively lower temperatures by means of direct decomposition of natural gas, LPG, or other gas mixtures having a CrC4-hydrocarbon content. This approach is achieved by making use of Ni-Fe/γ- AI2O3 type catalysts with a higher activity and a special preparation method. DESCRIPTION OF INVENTION
The subject process is as following.
At first, the catalyst for the direct decomposition of methane is prepared according to the subject process. For this purpose, industrial-type Y-AI2O3 is used as the catalyst carrier, and Ni and Fe are employed as active metals. The concentrations of Ni and Fe each vary between 5% and 20% on the catalyst's surface. The catalysts are prepared by adsorbing on the carrier surface the aqueous solutions of metal salts (typically the nitrate salts) in a multi-step method. The adsorption phase is conducted at the room temperature. After the carrier is subjected to adsorption, the solution is evaporated and the catalyst dried under air. The calcination of catalyst is carried out in an oven under air. The Ni-Fe/γ-AI2O3 catalyst used in this invention has the following advantages as compared to known catalysts used for the direct decomposition of natural gas (or methane): the aqueous solutions of Ni and Fe salts are adsorbed in a multi-step manner on the carrier in order to have a more homogeneous distribution of such active metals on the carrier surface;
Ni and Fe salts are adsorbed together onto the carrier surface; and the catalyst is subjected to calcination after each interim adsorption step conducted on the carrier surface.
Any such prepared catalysts are used in the direct decomposition process of natural gas or LPG according to the present invention. The process is conducted under atmosphere pressure and at 550-6500C temperature. The volumetric flow rate of natural gas or LPG used as raw materials in this process varies between 720 hour"1 and 4320 hour"1. The conversion rate of methane in the natural gas to hydrogen varies between 66 to 91% according to the conditions of this process.
The significant advantages of this process as compared to the known direct decomposition method of methane (Jiuling Chen, Yongdan Li, Zongquan Li, Xixiang Zhang - Production of COx-free hydrogen and nanocarbon by direct decomposition of undiluted methane on Ni-Cu-alumina catalysts, Applied Catalysis A:General, 269 (2004), 179-186.) are as following:
Advantages of the catalyst
A simple preparation technology; the use of commercial Y-AI2O3 as the catalyst carrier; - the use of inexpensive metals such Ni and particularly Fe as the active components; and inexpensive catalyst. Advantages of the method
Lower process temperatures; - High conversion of CH4 or C2 - C4 gases); H2 production with lower costs.
The contents of the natural gas and LPG used as inputs in the process, and the gaseous products as the output of the process are analyzed by means of Gas Chromatography. The amount and character of the coke formed on the catalyst surface as a result of directly decomposing CH4 according to this process are studied by the Differential Thermal-Gravimetric Analysis method.
The present invention can be acknowledged by means of the following examples: EXAMPLE 1
5% Ni + 5% Fe/γ-AI2O3 catalyst is prepared for use in the subject process. For this reason, 3.12 g Ni(NO3)2.6H2O and 4.56 g Fe(NO3)3.9H2O salts are dissolved in 10 ml distilled water and the resulting solution is adsorbed in two steps under mixing for 12 hours on the surface of Y-AI2O3 (10 g), which is previously dried under 1500C for 4 hours. In the first interim step following adsorption, the solution is evaporated and the catalyst is dried under air at 1500C for 6 hours and subjected to calcination at 500°C for 4 hours, then in the second step following adsorption, the solution is evaporated again and the catalyst dried under air at 15O0C. Then, the catalyst is subjected to the final calcination step under air at 75O0C for 4 hours. In the calcination steps, the temperature is raised by 150°C/hour"1 starting from 150°C.
A 2.5 g aliquot is taken from the prepared catalyst and used for directly decomposing the natural gas. The content of the natural gas used as raw material in this process is as following (% by volume): H2 - 0.14, CH4 - 87.84, C2H6 - 4.16, C3 - 1.19, C4-C5 - 0.03, N2 - 5.6, O2- 0.51 , CO2- 0.43.
The process is conducted in a continuous experiment system with a fixed bed quarts reactor under atmosphere pressure at 65O0C and 30 ml/min gas flow rate (720 hour"1).
The reactor's inner diameter and length are 2.2 cm and 20 cm, respectively. After the gaseous products are put out of the reactor, they are cooled in a water cooler and analyzed by means of GC. The result is as following:
CH4 conversion (%) - 80.6 EXAMPLE 2
10% Ni + 10% Fe/γ-AI2O3 catalyst is prepared for use in this process. Respectively 6.24 g and 9.12 g of Ni(NO3)2.6H2O and Fe(NO3)3.9H2O salts are used in the catalyst's synthesis. The adsorption of aqueous solutions of metal salts on the catalyst surface is conducted at three steps.
After the first and second interim adsorption steps, the catalyst's drying and calcination steps and the catalyst's preparation and other conditions of the process are identical with those of Example 1. The result is as following: CH4 conversion (%) - 84.8 EXAMPLE 3
20% Ni + 20% Fe/γ-AI2O3 catalyst is prepared for use in this process. Respectively 12.48 g and 18.24 g of Ni(NO3)2.6H2O and Fe(NO3)3.9H2O salts are used in the catalyst's synthesis. The adsorption of aqueous solutions of metal salts on the catalyst surface is conducted at four steps in the preparation of the catalyst.
After the first, second, and third interim adsorption steps, the catalyst's drying and calcination steps and the catalyst's preparation and other conditions of the process are identical with those of Example 1 and 2. The result is as following:
CH4 conversion (%) - 91.5 EXAMPLE 4
20% Ni + 20% Fe/γ-Al2O3 catalyst is prepared for use in this process. The preparation of the catalyst is conducted by means of a 4-step adsorption method. The direct decomposition process is conducted at 550°C temperature.
Other conditions of preparing the catalyst and of the process are identical with those of Example 1 to 4. The result is as following:
CH4 conversion (%) - 66.7 EXAMPLE 5 20% Ni + 20% Fe/γ-AI2O3 catalyst is prepared for use in this process. In preparing the catalyst, a four-step adsorption method is conducted with the metal salts of the carrier. The temperature of the direct decomposition process is 65O0C and the flow rate of the natural gas is 180 ml/min (4320 hour"1).
Other conditions of preparing the catalyst and of the process are identical with those of Example 1 to 4. The result is as following:
CH4 conversion (%) - 87.0 EXAMPLE 6
20% Ni + 20% Fe/γ-AI2O3 catalyst is prepared for use in the subject process. LPG with the following content (% by volume) is used as the raw material in this process: H2 - 0.2, CH4 - 0.6, C2H6 - 15.99, C3 - 50.98, C4 - 29.15, C5 - 0.19, N2 - 1.78, O2 - 1.11. The temperature of the direct decomposition process is 6500C and the flow rate of the natural gas is 30 ml/min (720 hour"1).
Other conditions of preparing the catalyst and of the process are identical with those of Example 1 to 5. The result is as following: Total conversion of C2-C4 gases (%) - 94.8

Claims

1. A hydrogen production method by direct decomposition of natural gas and LPG, characterized in that a nickel-iron catalyst prepared by means of a multi-step adsorption approach on gamma-aluminum oxide is used.
2. A hydrogen production method according to Claim 1 , characterized in that aqueous solutions of nitrate salts of nickel and iron are adsorbed on gamma-aluminum oxide in 2 to 4 steps to prepare the catalyst used in this method, wherein the weight ratio of nickel and iron on the catalyst surface is 1 :1 and their total weight is 20- 40% by weight.
3. A hydrogen production method according to claims 1 and 2, characterized in that this method is conducted at a temperature range of 550-6500C.
EP07826782A 2006-10-19 2007-10-18 Hydrogen production method by direct decomposition of natural gas and lpg Ceased EP2076332A1 (en)

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TR2006/05865A TR200605865A2 (en) 2006-10-19 2006-10-19 Hydrogen production by direct decomposition of natural gas and lpg
PCT/IB2007/054240 WO2008047321A1 (en) 2006-10-19 2007-10-18 Hydrogen production method by direct decomposition of natural gas and lpg

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DE102010049957B4 (en) * 2010-10-04 2013-11-14 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Exhaust gas purification device, process for exhaust gas purification and pyrolysis reactor
RU2526040C1 (en) * 2013-06-20 2014-08-20 Федеральное государственное бюджетное учреждение "Национальный исследовательский центр "Курчатовский институт" Method of petrol obtaining
RU2559878C1 (en) * 2014-06-10 2015-08-20 Федеральное государственное бюджетное учреждение науки Институт химии твердого тела Уральского отделения Российской академии наук Nickel-aluminium spinel as methane partial oxidation catalyst and method for production thereof
RU2651195C1 (en) * 2017-03-10 2018-04-18 Федеральное государственное бюджетное образовательное учреждение высшего образования "Тюменский индустриальный университет" (ТИУ) Synthetic gas production method
EP3609615A1 (en) 2017-04-14 2020-02-19 King Abdullah University Of Science And Technology Treated iron ore catalysts for production of hydrogen and graphene
CN110721691B (en) * 2019-11-12 2020-07-24 中南大学 CFAN catalyst, preparation thereof and application thereof in methane hydrogen production
US11890596B2 (en) * 2021-09-07 2024-02-06 United Arab Emirates University Coking resistant NiFeAl catalyst for partial oxidation of methane to synthesis gas

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RU2204434C2 (en) * 2001-05-08 2003-05-20 Институт катализа им. Г.К. Борескова СО РАН Catalyst and a method for production of hydrogen/carbon monoxide mixture
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RU2009118631A (en) 2010-11-27
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WO2008047321B1 (en) 2008-07-24

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