Catalyst for methane reforming and method for producing same

Abstract

A method for producing a methane reforming catalyst according to one embodiment of the present application includes the steps of preparing a solution containing a precursor of a perovskite compound represented by Chemical Formula 1; and coating a support with the solution and then performing a heat treatment process to produce a catalyst, where the precursor of the perovskite compound represented by Chemical Formula 1 contains strontium hydroxide.

Description

[Technical Field]

[0001] This application claims the benefit of the filing date of Korean Patent Application No. 10-2024-0004616, filed with the Korean Intellectual Property Office on January 11, 2024, the entire contents of which are incorporated herein by reference.

[0002] The present application relates to a catalyst for methane reforming and a method for producing the same. [Background technology]

[0003] As part of efforts to reduce greenhouse gas emissions caused by global warming, much research is underway into carbon dioxide conversion technologies. One of these technologies, the carbon dioxide reforming reaction, is a technique for producing synthesis gas consisting of hydrogen and carbon monoxide by reacting methane with carbon dioxide.

[0004] Syngas is a valuable substance for development as a raw material for various downstream processes. Natural gas reforming reactions, which are methods for industrially obtaining syngas (H2 / CO), can be broadly classified into steam reforming, CO2 reforming, catalytic partial oxidation, autothermal reforming, and tri-reforming, as shown in the following reaction equations 1 to 5.

[0005] [Reaction Scheme 1] CH4+H2O → 3H2+CO △H=226kJ / mol [Reaction Scheme 2] CH4+CO2→ 2H2+2CO △H=261kJ / mol [Reaction Scheme 3] CH4+0.5O2→ 2H2+CO △H=-44kJ / mol [Reaction Scheme 4] Autothermal reforming: Reaction 1 + Reaction 3 [Reaction Scheme 5] Tri-reforming: Reaction 1 + Reaction 2 + Reaction 3

[0006] Meanwhile, various catalysts can be used in the reforming process for improving reforming activity. Among these, the use of a noble metal catalyst in the reforming process has the advantage of high efficiency in converting natural gas to hydrogen, but the high cost of the noble metal catalyst results in poor economic viability.

[0007] Therefore, nickel catalysts, which have high hydrogen conversion efficiency and are relatively inexpensive, are mainly used in the reforming process. However, in such cases, there is a problem that the nickel catalyst is deactivated by carbon that is inevitably generated on the surface of the nickel catalyst.

[0008] Therefore, there is a need in the art for the development of catalysts that are resistant to carbon deposition and can be effectively applied in methane reforming processes. Summary of the Invention [Problem to be solved by the invention]

[0009] The present application seeks to provide a catalyst for methane reforming and a method for producing the same. [Means for solving the problem]

[0010] One embodiment of the present application is preparing a solution containing a precursor of a perovskite compound represented by the following chemical formula 1; and and a step of coating the support with the solution and then carrying out a heat treatment process to prepare a catalyst. The present invention provides a method for producing a catalyst for methane reforming, wherein the precursor of the perovskite compound represented by the following chemical formula 1 contains strontium hydroxide. [Chemical formula 1] Sr 1-x A x Ti α B y O 3-δ In the above chemical formula 1, A is selected from Y, La and the lanthanide series elements; B is Ni, Co, Fe, Cr, Mo, Ru or Rh; x is a real number between 0 and 1, y is a real number greater than or equal to 0 and less than 0.3, δ is a real number between 0 and 1, α is a real number greater than 0.7 and less than or equal to 1, (x+y)>0.

[0011] Another embodiment of the present application provides a methane reforming catalyst produced by the above-mentioned method for producing a methane reforming catalyst. [Effects of the Invention]

[0012] The methane reforming catalyst according to one embodiment of the present application is prepared by using strontium hydroxide as a precursor of the perovskite compound represented by Chemical Formula 1 above, thereby suppressing the dissolution of components that may cause side reactions or coke from the metal support due to low pH.

[0013] In addition, the amount of hydroxycarboxylic acid and polyhydroxy compound used in the conventional methane reforming catalyst manufacturing process can be minimized, and the loss of active components of the catalyst can be minimized when the perovskite-based compound represented by Chemical Formula 1 is coated on the metal support. This makes it possible to manufacture a catalyst in which the perovskite-based compound represented by Chemical Formula 1 is uniformly coated on the surface of the metal support.

[0014] Therefore, when the methane reforming catalyst according to an embodiment of the present application is applied to a methane reforming reaction, it can exhibit high activity even at a high space velocity, and can be stably operated for a long period of time of 1,000 hours or more without causing carbon deposition or sintering. DETAILED DESCRIPTION OF THE INVENTION

[0015] The present specification will be explained in more detail below.

[0016] In this specification, when a member is said to be located "on" another member, this includes not only when the member is in contact with the other member, but also when there is another member between the two members.

[0017] In this specification, when a part is said to "comprise" a certain component, this does not mean that it can further include other components, unless otherwise specified.

[0018] Currently, catalysts widely used in the reformer field are generally powder catalysts and pellet-type support catalysts. Powder catalysts have excellent catalyst dispersion and performance, but are difficult to directly use in industrial applications. For example, when a reformer is operated using a powder catalyst, the catalyst is released along with the products produced after the reaction. However, the powder catalyst gradually accumulates in the outlet flow tube, eventually clogging the entire tube. Therefore, a drawback is that powder catalysts cannot be used in commercial reformers for industrial use.

[0019] Pellet-type support catalysts are currently widely used in industrial reformers. While their catalytic performance is inferior to that of powder-type catalysts due to mass transfer rate limitations, the use of a support offers the advantage of long-term use. However, γ-Al2O3 pellets, which are commonly used as pellet-type support catalysts, have the disadvantage of weak structural strength and prone to cracking, which can lead to differential pressure within the reactor. Furthermore, due to their large volume, pellet-type support catalysts require significant volume expansion when used in high-capacity reformers. Furthermore, while all reforming reactions are sensitive to reaction temperature, existing pellet-type catalysts have the disadvantage of significantly reduced thermal conductivity, resulting in inconsistent heat distribution throughout the reactor. Furthermore, because reforming reactions are very fast, pellet-type support catalysts and extruded catalysts have a catalyst effectiveness factor of less than 0.3, resulting in reduced catalyst utilization.

[0020] Furthermore, in the dry reforming reaction of methane, the lower the reactor pressure, the less coke is produced thermodynamically. Therefore, there are increasing cases of using a metal support as a catalyst support to reduce the pressure drop in the catalyst layer. However, due to the side reactions and coke production caused by the metal components of the metal support itself, there are currently no reported cases of commercialization.

[0021] Therefore, the present application aims to provide a methane reforming catalyst and a method for producing the same, which uses a metal support with high heat and mass transfer rates and can suppress side reactions and coke generation caused by the metal components of the metal support itself.

[0022] A method for producing a methane reforming catalyst according to one embodiment of the present application includes the steps of preparing a solution containing a precursor of a perovskite compound represented by the following Chemical Formula 1; and coating a support with the solution and then performing a heat treatment process to produce a catalyst, where the precursor of the perovskite compound represented by the following Chemical Formula 1 contains strontium hydroxide. [Chemical formula 1] Sr 1-x A x Ti α B y O 3-δ In the above chemical formula 1, A is selected from Y, La and the lanthanide series elements; B is Ni, Co, Fe, Cr, Mo, Ru or Rh; x is a real number between 0 and 1, y is a real number greater than or equal to 0 and less than 0.3, δ is a real number between 0 and 1, α is a real number greater than 0.7 and less than or equal to 1, (x+y)>0.

[0023] In one embodiment of the present application, the support may be a metal support. In this case, the metal support may include one or more selected from NiFeCrAl, NiCrAl, Al, stainless steel, and inconel. The metal support may be a porous metal support such as a porous metal foam, or a metal support of a fixed shape. The support may also be an inorganic oxide support known in the art.

[0024] The porous metal support is a structure having various shapes, has a small heat capacity, and has excellent heat transfer ability, and can be formed into a desired shape for use. The shape and size of the porous metal support are not particularly limited, and the porosity of the porous metal support may be 10% to 99%, 50% to 96%, or 85% to 96%. The pore size of the porous metal support may be 400 μm to 1,500 μm or 450 μm to 1,400 μm. If the pore size of the porous metal support is less than 400 μm, it is difficult to coat the precursor solution. If the pore size exceeds 1,500 μm, the surface area available for catalyst coating is reduced, which may cause processing disadvantages, and is therefore undesirable. The porous metal support can be appropriately prepared by those skilled in the art using methods known in the art, taking into account the material, pore size, and porosity of the porous metal support.

[0025] The metal support of the above-mentioned certain form can be a tubular reactor itself, or a spring-like metal plate with an enlarged surface area can also be used.

[0026] A method for producing a methane reforming catalyst according to one embodiment of the present application includes the step of preparing a solution containing a precursor of the perovskite compound represented by Chemical Formula 1 above.

[0027] While a conventional powder catalyst is prepared by adding a basic component to a catalyst precursor solution to form a precipitate, a methane reforming catalyst according to an embodiment of the present application is a supported catalyst in which a catalyst component is coated on a support, and differs from conventional powder catalysts. Therefore, in one embodiment of the present application, a solution containing a precursor of the perovskite-based compound represented by Chemical Formula 1 above may be applied in the form of a sol or gel.

[0028] The precursor of the perovskite compound is a precursor of a metal constituting the perovskite compound, and the content thereof can be adjusted to control the metal molar ratio of the perovskite compound. In addition, there is no particular limitation on the precursor of the metal other than strontium hydroxide as the precursor of the metal.

[0029] In one embodiment of the present application, the strontium hydroxide may be Sr(OH)2·9H2O. Although strontium carbonate, strontium acetate, and the like may be used instead of the strontium hydroxide, the effect of increasing the pH is small, so it is more preferable to use the strontium hydroxide.

[0030] In one embodiment of the present application, the pH of the solution containing the precursor of the perovskite compound represented by the above chemical formula 1 may be 2.5 to 3.7, or 3.0 to 3.5.

[0031] A solution containing a precursor of the perovskite-based compound represented by Formula 1 can be prepared by the Pechini method. When an aqueous solution of the oxide or salt required for preparation is mixed with a hydroxycarboxylic acid, a chelate reaction occurs, forming a complex ring compound around the metal cation. A polyhydroxy compound is then added and heated at 150-250°C to polymerize the chelate. After removing excess water, a solid polymer resin, which can be considered a precursor of the catalyst component, is obtained. Previously, citric acid, ethylene glycol, strontium nitrate, nickel nitrate, titanium isopropoxide, etc. were used to prepare perovskite-based materials. The pH of the conventional coating solution prepared in this way was between 0.1 and 0.5, posing significant limitations in the process of preparing a catalyst for dry methane reforming. Because of its extremely high acidity, not only must the manufacturing equipment be made of special materials, but also, to prevent the side effect of leaching when using a metal support, it is necessary to coat it with an additional protective layer or limit the number of times the coating solution can be reused.

[0032] According to one embodiment of the present application, by using strontium hydroxide instead of conventional strontium nitrate, a coating solution with a pH of 2.5 to 3.7 can be produced. This not only overcomes the limitations of the equipment materials mentioned above, but also eliminates the need for an additional protective layer to enhance the catalytic effect, thereby suppressing side effects from the reuse of the coating solution.

[0033] In the past, the process of coating a metal support surface with a catalytic component could result in the loss of catalytic activity due to undesired components caused by leaching and washing. In particular, the widely known Pechni method for preparing a sol solution has been carried out in a strongly acidic (pH < 0.3) atmosphere using nitrates as catalyst component precursors. However, the use of nitrates as catalyst component precursors results in the formation of a sol solution with a very low pH, which can leach out the metal components of the metal support during the catalytic component coating process and also introduce components that are unfavorable to catalytic activity, resulting in a decrease in catalytic activity. Furthermore, when using nitrates as catalyst component precursors, the pH can be increased somewhat by adding an alcohol component, but this significantly increases process costs, making it undesirable for commercial production.

[0034] That is, in order to solve the above-mentioned problems, in one embodiment of the present application, strontium hydroxide is used instead of conventional nitrates, thereby increasing the pH, which has the advantage of broadening the range of choices for reactor materials when producing a large amount of sol solution.

[0035] In one embodiment of the present application, (α+y) in Chemical Formula 1 may be 1. Also, in one embodiment of the present application, (α+y) in Chemical Formula 1 may be a real number greater than 0.90 and less than 1. In Chemical Formula 1, B, such as Ni, replaces a portion of Ti, and in the theoretical stoichiometric ratio, (α+y) is 1. However, if the Ti content is slightly less than the theoretical stoichiometric ratio during the preparation of the perovskite-based compound represented by Chemical Formula 1, the substitution of Ti in Chemical Formula 1 with B, such as Ni, can be more easily achieved.

[0036] In one embodiment of the present application, the above Chemical Formula 1 can be represented by the following Chemical Formula 2 or 3, but is not limited thereto. [Chemical formula 2] SrTi α By O 3-δ [Chemical formula 3] Sr 1-x Y x Ti α B y O 3-δ In the above chemical formulas 2 and 3, B is Ni or Rh; x is a real number greater than 0 and less than 1, y is a real number greater than 0 and less than 0.3, δ is a real number greater than 0 and less than 1, α is a real number greater than 0.7 and less than or equal to 1.

[0037] In one embodiment of the present application, the method of coating the solution onto the carrier may be a method known in the art, such as, but not limited to, dip coating, wash coating, etc.

[0038] In one embodiment of the present application, the heat treatment process may include drying and calcination steps. The drying may be performed at a temperature of 50°C to 150°C for 1 hour to 48 hours, or at a temperature of 60°C to 100°C for 5 hours to 36 hours, but is not limited thereto. The calcination may be performed in an air atmosphere at a temperature of 350°C to 1,100°C for 1 hour to 10 hours, or at a temperature of 500°C to 1,000°C for 1.5 hours to 8 hours, but is not limited thereto. If the calcination step is performed at a temperature lower than 350°C, the perovskite phase may not be properly formed, and if it exceeds 1,100°C, the durability of the metal support may be reduced, which is undesirable.

[0039] In one embodiment of the present application, the method may further include a step of measuring the weight of the coating layer supported on the support after the heat treatment step. In addition, by measuring the weight of the coating layer supported on the support, the step of coating the above-mentioned solution and then performing the heat treatment step may be repeated 2 to 10 times until a desired amount of catalyst is supported on the support.

[0040] Another embodiment of the present application provides a methane reforming catalyst produced by the above-mentioned method for producing a methane reforming catalyst.

[0041] A catalyst for methane reforming according to one embodiment of the present application includes a support; and a coating layer provided on the support and including the perovskite compound represented by Chemical Formula 1 above.

[0042] In one embodiment of the present application, the content of the coating layer containing the perovskite-based compound represented by Chemical Formula 1 may be 3 wt% to 40 wt%, 6 wt% to 35 wt%, or 7 wt% to 30 wt%, based on the total weight of the methane reforming catalyst. If the content of the coating layer containing the perovskite-based compound represented by Chemical Formula 1 is less than 3 wt%, based on the total weight of the methane reforming catalyst, the reactivity may be reduced due to the relatively small number of active sites on the catalyst surface, which is undesirable. Furthermore, if the content of the coating layer containing the perovskite-based compound represented by Chemical Formula 1 exceeds 40 wt%, the coating layer contains a relatively large amount of catalyst components compared to the support, making it difficult to maintain the pore structure and to easily bond the catalyst components to the support, which may reduce the practical benefits of the methane reforming reaction.

[0043] In one embodiment of the present application, the methane reforming catalyst may be applied to a steam reforming process, a carbon dioxide reforming process, a catalytic partial oxidation process, an autothermal reforming process, a tri-reforming process, or a mixed reforming process, and the methane reforming process is not particularly limited.

[0044] The methane reforming catalyst according to one embodiment of the present application is prepared by using strontium hydroxide as a precursor of the perovskite compound represented by Chemical Formula 1 above, thereby suppressing the dissolution of components that may cause side reactions or coke from the metal support due to low pH.

[0045] In addition, the amount of hydroxycarboxylic acid and polyhydroxy compound used in the conventional methane reforming catalyst manufacturing process can be minimized, and the generation of popcorn-like particles when the perovskite-based compound represented by Chemical Formula 1 is coated on the metal support can be prevented. This minimizes the loss of active components of the catalyst, and the perovskite-based compound represented by Chemical Formula 1 can be uniformly coated on the surface of the metal support to manufacture the catalyst.

[0046] Therefore, when the methane reforming catalyst according to an embodiment of the present application is applied to a methane reforming reaction, it can exhibit high activity even at a high space velocity, and can be stably operated for a long period of time of 1,000 hours or more without causing carbon deposition or sintering. [Example]

[0047] Hereinafter, the present application will be described in detail with reference to examples in order to specifically explain the present application. However, the examples of the present application can be modified in various different forms, and the scope of the present application should not be construed as being limited to the examples detailed below. The examples of the present application are provided to more completely explain the present application to those skilled in the art.

[0048] <Example> Example 1 The perovskite coating solution was prepared using the Pechini method. Strontium hydroxide (Sr(OH)2·9H2O) and nickel nitrate (Ni(NO3)2) were dissolved in distilled water at 80°C along with malic acid. Glycerin was then added, followed by titanium isopropoxide (Ti(OCH(CH3)2)4), and the temperature was maintained until a clear solution was obtained. The nickel content was 3 mol% relative to the titanium content. The pH of the coating solution was 3.5.

[0049] The perovskite-based coating solution was dip-coated (to form a coating layer) on a porous metal support (NiCrAl, average pore size: 1,200 μm), dried at 150°C for 5 hours, and then heat-treated at 900°C in an air atmosphere for 5 hours. The dip-coating of the perovskite-based solution, drying, and heat-treatment were repeated several times to finally form a coating layer (SrTi 0.97 Ni 0.03 O 3-δ , 0<δ<1) was prepared. Based on the total weight of the methane reforming catalyst, the perovskite-based compound (SrTi 0.97 Ni 0.03 O 3-δ , 0<δ<1) was 10.8 wt%.

[0050] The content of the perovskite-based compound represented by Chemical Formula 1 can be calculated using the following Equation 1. [Formula 1] Content (wt%) of the perovskite compound represented by Chemical Formula 1 = (total weight of catalyst - weight of porous metal support) / (total weight of catalyst) × 100

[0051] <Example 2> The same procedure as in Example 1 was carried out except that yttrium nitrate (Y(NO3)2) was added at 8 mol% relative to strontium, and a coating layer (Sr 0.92 Y 0.08 Ti 0.97 Ni 0.03 O 3-δ , 0<δ<1) were prepared. The coating solution had a pH of 3.0, and the perovskite-based compound (Sr 0.92 Y 0.08 Ti 0.97 Ni 0.03 O 3-δ , 0<δ<1) was 14.1% by weight.

[0052] <Comparative Example 1> Strontium nitrate (Sr(NO3)·3H2O) and nickel nitrate (Ni(NO3)2) were dissolved in distilled water at 80°C along with citric acid. Titanium isopropoxide (Ti(OCH(CH3)2)4) was dissolved in ethylene glycol at 60°C, then mixed with the distilled water solution and the temperature was maintained until a clear solution was obtained. Nickel was contained at 3 mol% relative to titanium. The pH of the coating solution was 0.30.

[0053] The perovskite-based coating solution was dip-coated (coating layer formation) onto a porous metal support (NiCrAl, average pore size: 1,200 μm), dried at 150°C for 5 hours, and then heat-treated at 900°C in an air atmosphere for 5 hours. The dip-coating of the perovskite-based solution, drying, and heat-treatment were repeated several times to finally form a coating layer (SrTi 0.97 Ni 0.03 O 3-δ, 0<δ<1) was prepared. Based on the total weight of the methane reforming catalyst, the perovskite-based compound (SrTi 0.97 Ni 0.03 O 3-δ , 0<δ<1) was 15.1% by weight.

[0054] <Comparative Example 2> The same procedure as in Comparative Example 1 was carried out except that yttrium nitrate (Y(NO3)2) was added at 8 mol% relative to strontium, and a coating layer (Sr 0.92 Y 0.08 Ti 0.97 Ni 0.03 O 3-δ , 0<δ<1) were prepared.

[0055] At this time, the pH of the coating solution was 0.30, and the amount of the perovskite-based compound (Sr 0.92 Y 0.08 Ti 0.97 Ni 0.03 O 3-δ , 0<δ<1) was 15% by weight.

[0056] <Experimental Example 1> Evaluation of dry reforming reaction of methane A fixed-bed reactor was installed to carry out the dry reforming of methane. A quartz tube reactor (internal diameter = 1 / 2 inch, length = 50 cm) was used and packed with approximately 2.2 g of each catalyst from the Examples and Comparative Examples. First, a reduction process was carried out at 800°C under 10% H2 / N2 conditions for 2 hours, followed by a catalytic reaction for 28 hours.

[0057] Gas composition: CH4:CO2:N2 = 1:1.1:0.1 Flow rate: GHSV (Gas Hour Space Velocity)=1,500hr -1 (CH4 standard) Reaction temperature: 850℃ Reaction pressure: 5 bar The composition of the produced gas was analyzed using gas chromatography (GC) to calculate the reaction conversion rate after 28 hours of reaction, which is shown in Table 1 below. Conversion rate (Xi, %) = [(Fi in - Fi out ) / Fi in × 100 (Fi = flow rate of i)

[0058] Also, based on the coke production amount in Comparative Example 1, the coke reduction rate was calculated by the following formula and is shown in Table 1 below. Coke reduction rate (%) = (Coke production amount in Comparative Example 1 - Coke production amount in the Example or Comparative Example) / (Coke production amount in Comparative Example 1) × 100

[0059] <GC analysis conditions> 1) GC model: Agilent 6890 2) Oven temp.: 40°C / 7 min - 90°C / 5 min - 180°C / 6 min 3) Detector: TCD, 250°C 4) Sample loop: 0.25 mL 5) Valve box Temp.: 150°C

[0060]

Table 1

[0061] From the results in Table 1 above, the fact that the coke reduction rate of Comparative Example 2 has a (-) value indicates that, compared with Comparative Example 1, the result of Comparative Example 2 shows that the coke production amount did not decrease but rather increased.

[0062] As described above, it can be confirmed that the methane reforming catalyst according to an embodiment of the present application, by being produced using strontium hydroxide, has a lower coke production amount compared to the methane reforming catalyst produced using strontium nitride as in the comparative examples. Accordingly, it can be confirmed that the side reactions caused by the coating layer containing the metal support and the perovskite-based compound are reduced in the methane reforming catalyst according to an embodiment of the present application.

[0063] Furthermore, the above results were obtained after the catalytic reaction was carried out for 28 hours. It is obvious to those skilled in the art that if the catalytic reaction is carried out for 1,000 hours or more, as is applied in an actual commercial process, the difference in the coke reduction rate between the above-mentioned Examples and Comparative Examples will become even greater.

[0064] Therefore, when the methane reforming catalyst according to an embodiment of the present application is applied to a methane reforming reaction, it can exhibit high activity even at a high space velocity, and can be stably operated for a long period of time of 1,000 hours or more without causing carbon deposition or sintering.

Claims

1. Preparing a solution containing a precursor of a perovskite compound represented by the following Chemical Formula 1: and coating the solution on a carrier and then carrying out a heat treatment process to prepare a catalyst. A method for producing a catalyst for methane reforming, wherein the precursor of the perovskite compound represented by the following chemical formula 1 contains strontium hydroxide: [Chemical formula 1] Sr １－ｘ A ｘ Three α B ｙ Oh ３－δ In the above Chemical Formula 1, A is selected from Y, La and the lanthanide series elements; B is Ni, Co, Fe, Cr, Mo, Ru, or Rh; x is a real number greater than or equal to 0 and less than 1, y is a real number greater than or equal to 0 and less than 0.3; δ is a real number greater than or equal to 0 and less than 1, α is a real number greater than 0.7 and less than or equal to 1, (x+y)>0 is satisfied.

2. The method for producing a methane reforming catalyst according to claim 1 , wherein the support is a metal support.

3. 3. The method for producing a methane reforming catalyst according to claim 2, wherein the metal support comprises at least one selected from the group consisting of NiFeCrAl, NiCrAl, Al, stainless steel, and inconel.

4. 2. The method for producing a methane reforming catalyst according to claim 1, wherein the solution containing the precursor of the perovskite compound represented by Chemical Formula 1 has a pH of 2.5 to 3.

7.

5. The strontium hydroxide is Sr(OH) ２ ・9H ２ 2. The method for producing a methane reforming catalyst according to claim 1, wherein the methane reforming catalyst is O.

6. 2. The method for producing a methane reforming catalyst according to claim 1, wherein the chemical formula 1 is represented by the following chemical formula 2 or 3: [Chemical formula 2] Srti α B ｙ Oh ３－δ [Chemical formula 3] Sr １－ｘ Y ｘ Ti α B ｙ O ３－δ In the above Chemical Formulas 2 and 3, B is Ni or Rh; x is a real number greater than 0 and less than 1, y is a real number greater than 0 and less than 0.3; δ is a real number greater than 0 and less than 1, α is a real number greater than 0.7 and equal to or less than 1.

7. A catalyst for methane reforming, produced by the method according to any one of claims 1 to 6.

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