Medium-high entropy multi-element metal oxide catalyst, preparation method and application

Abstract

The invention belongs to the technical field of synthesis gas preparation through catalytic reforming, and particularly relates to a medium-high entropy multi-element metal oxide catalyst, a preparation method and application. The invention provides a medium-high entropy multi-element metal oxide catalyst which has a magnesium aluminate spinel structure doped with transition metal elements, and the transition metal elements comprise at least one of nickel, cobalt, zinc and manganese. Compared with a traditional catalyst only loaded with nickel, the medium-high-entropy multi-element metal oxide catalyst provided by the invention has higher catalytic activity and stability. The invention also provides a preparation method of the catalyst, and the preparation method is simple and feasible, does not need to use an organic solvent, and is favorable for realizing large-scale preparation.

Description

Technical Field

[0001] The present invention belongs to the technical field of catalytic reforming synthesis gas, and in particular relates to a medium-high entropy multinary metal oxide catalyst, a preparation method and application thereof. Background Art

[0002] As a clean energy, natural gas is mainly used as fuel. It is mainly composed of methane, a small amount of ethane and propane, of which methane accounts for the largest proportion. Natural gas catalytic reforming is an important process for the industrial production of synthesis gas (mixed gas of CO and H2). Catalytic reforming to prepare synthesis gas mainly includes methane steam reforming (methane wet reforming), methane partial oxidation reforming, methane carbon dioxide reforming (methane dry reforming) and low-carbon alkane reforming technologies.

[0003] At present, the catalysts used in methane dry reforming technology are mostly nickel-based catalysts. However, traditional nickel-based catalysts are easily deactivated due to carbon deposition and sintering under long-term high-temperature conditions, resulting in a decrease in catalyst activity and stability, limiting their industrial application. Summary of the invention

[0004] In view of this, the present invention provides a medium-high entropy multi-metal oxide catalyst, which has higher catalytic activity and stability than traditional catalysts loaded with nickel only.

[0005] In order to solve the above technical problems, the present invention provides a medium-high entropy multinary metal oxide catalyst, which has a pure phase magnesium aluminum spinel structure doped with transition metal elements, and the transition metal elements include nickel, and at least one of cobalt, zinc and manganese.

[0006] The present invention creatively applies the medium-high entropy theory to the design of catalysts for alkane reforming reactions. By introducing specific types of metal elements into magnesium-aluminum spinel, a catalyst with a pure phase magnesium-aluminum spinel structure doped with transition metal elements is obtained. The stability of the catalyst is enhanced through the high entropy process, and the synergistic effect between multiple active sites is strengthened, so that the catalyst has excellent catalytic performance and thermal stability.

[0007] In combination with the first aspect, the medium-high entropy multi-metal oxide catalyst is of the general chemical formula (Mg x Ni y Co z Zn m Mn n )Al2O4; wherein 0.2≤x<1, 0<y≤0.4, 0≤z≤0.2, 0≤m≤0.2, 0≤n≤0.2 and x+y+z+m+n=1. x, y, z, m and n can be any values ​​within the above-defined range.

[0008] Preferably, the chemical formula of the medium-high entropy multi-metal oxide catalyst is (Mg 0.6 Ni 0.2 Co 0.2 )Al2O4.

[0009] Preferably, the chemical formula of the medium-high entropy multi-metal oxide catalyst is (Mg 0.4 Ni 0.2 Co 0.2 Zn 0.2 )Al2O4 or (Mg 0.4 Ni 0.2 Co 0.2 Mn 0.2 )Al2O4.

[0010] Preferably, the chemical formula of the medium-high entropy multi-metal oxide catalyst is (Mg 0.2 Ni 0.2 Co 0.2 Zn 0.2 Mn 0.2 )Al2O4.

[0011] The second aspect of the present invention provides a method for preparing the above-mentioned medium-high entropy multinary metal oxide catalyst, the steps comprising:

[0012] S1. Evenly mix a soluble aluminum salt, a soluble magnesium salt and a soluble salt of a doped transition metal element according to a preset molar ratio of each element to obtain a multi-metal mixed solution;

[0013] S2, adjusting the pH of the mixed solution to 9-10, separating the solid and the liquid after the metal ions are completely precipitated, washing the solid product to neutrality, and drying to obtain a multi-metal precursor;

[0014] S3, grinding the multi-metal precursor into powder, calcining, cooling and reducing to obtain a medium-high entropy multi-metal oxide catalyst.

[0015] The present invention utilizes a coprecipitation method to prepare a medium-high entropy multinary metal oxide catalyst with higher catalytic activity and stability. The preparation method is simple and feasible, and no organic solvent is required during the preparation process, which is more conducive to industrial production.

[0016] In combination with the second aspect, the calcination is to grind the multi-metal precursor into powder, place it in a box furnace, heat it to 750-850° C. at a heating rate of 2-4° C. / min, and calcine it for 3-5 hours.

[0017] In combination with the second aspect, the temperature of the reduction reaction is 750-850° C., the gas used for reduction is a 10% hydrogen / argon mixed gas, and the gas flow rate is 40-50 mL / min.

[0018] The third aspect of the present invention provides an application of the above-mentioned medium-high entropy multinary metal oxide catalyst in an alkane reforming reaction.

[0019] Preferably, the alkane reforming reaction includes but is not limited to a methane wet reforming reaction, a methane dry reforming reaction, a methane partial oxidation reforming reaction and a low-carbon alkane reforming hydrogen production reaction. BRIEF DESCRIPTION OF THE DRAWINGS

[0020] Figure 1 The photos of the catalyst powders obtained from S2 to S5 and the metal oxide powders obtained from S1;

[0021] Figure 2 XRD patterns of the catalysts obtained from S2 to S5 and the metal oxides obtained from S1;

[0022] Figure 3 The SEM images of the catalysts obtained from S2 to S5 and the metal oxides obtained from S1, wherein (a), (b), (c), (d) and (e) are high-magnification SEM images corresponding to S1 to S5 from left to right, and (f), (g), (h), (i) and (j) are low-magnification SEM images corresponding to S1 to S5 from left to right;

[0023] Figure 4 The EDS graphs of the catalysts obtained from S4 and S5, wherein (a) is the EDS graph corresponding to S4, and (b) is the EDS graph corresponding to S5;

[0024] Figure 5 DRM test results of catalysts obtained from S2 to S5 and catalyst Ni / S1, wherein (a), (b), and (c) are comparison diagrams of CH4 conversion rate, CO2 conversion rate, and H2 / CO ratio of Ni / / S1 and S2, respectively; (d), (e), and (f) are comparison diagrams of CH4 conversion rate, CO2 conversion rate, and H2 / CO ratio of S2 to S5, respectively;

[0025] Figure 6 H2-TPR curves of catalysts S2~S5 and catalyst Ni / S1. DETAILED DESCRIPTION

[0026] In order to make the purpose, technical solution and advantages of the present invention more clearly understood, the present invention is further described in detail below in conjunction with specific embodiments. It should be understood that the specific embodiments described herein are only used to explain the present invention and are not used to limit the present invention.

[0027] In view of the fact that traditional nickel-based catalysts are easily deactivated due to sintering and carbon deposition during use, the present invention provides a medium-high entropy multi-metal oxide catalyst, which has higher catalytic activity and stability, and also has excellent sintering resistance and carbon deposition resistance.

[0028] The metal solutions used in the following examples and comparative examples are all prepared using corresponding water-soluble salts. 2+ The solution can be hydrolyzed by adding a small amount of concentrated hydrochloric acid.

[0029] Example 1

[0030] This embodiment provides a medium-high entropy multi-metal oxide catalyst (denoted as S3), whose chemical formula is (Mg 0.6 Ni 0.2 Co 0.2 )Al2O4, the preparation method is as follows:

[0031] According to the metal atomic molar ratio of Al:Mg:Ni:Co=10:3:1:1, 10mL of 1mol / L Al 3+ solution, 6mL of 0.5mol / L Mg 2+ solution, 10mL of 0.1mol / L Ni 2+ solution and 10mL of 0.1mol / L Co 2+ solution, and after mixing, a multi-metal mixed solution is obtained; under stirring, 1 mol / L sodium hydroxide solution and 0.25 mol / L sodium carbonate solution are used to control the pH of the obtained multi-metal solution within the range of 9 to 10, and after the complete precipitation of each metal ion, the solid-liquid separation is performed, and the solid product is washed until the pH of the washing liquid is 7. The washed solid product is dried at 80°C in a forced air drying oven for 12 hours to obtain a multi-metal precursor.

[0032] The obtained precursor was ground into powder and placed in a box furnace, heated to 800°C at a heating rate of 3°C / min and calcined for 4 hours. It was then cooled to room temperature and reduced at 800°C for 1 hour using a 10% hydrogen / argon mixed gas at a flow rate of 50 mL / min to obtain a medium-high entropy multinary metal oxide catalyst.

[0033] Example 2

[0034] This embodiment provides a medium-high entropy multi-metal oxide catalyst (denoted as S4), whose chemical formula is (Mg 0.4 Ni 0.2 Co 0.2 Zn 0.2 )Al2O4, the preparation method is as follows:

[0035] According to the metal atomic molar ratio of Al:Mg:Ni:Co:Zn = 10:2:1:1:1, 10mL of 1mol / L Al 3+ solution, 4mL of 0.5mol / L Mg 2+solution, 10mL of 0.1mol / L Ni 2+ solution, 10mL of 0.1mol / L Co 2+ solution and 10mL of 0.1mol / L Zn 2+ The remaining steps are the same as those in Example 1 and will not be described in detail.

[0036] Example 3

[0037] This embodiment provides a medium-high entropy multi-metal oxide catalyst (denoted as S5), whose chemical formula is (Mg 0.2 Ni 0.2 Co 0.2 Zn 0.2 Mn 0.2 )Al2O4, the preparation method is as follows:

[0038] According to the metal atomic molar ratio of Al:Mg:Ni:Co:Zn:Mn=10:1:1:1:1:1, 10mL of 1mol / L Al 3+ solution, 2mL of 0.5mol / L Mg 2+ solution, 10mL of 0.1mol / L Ni 2+ solution, 10mL of 0.1mol / L Co 2+ solution, 10mL of 0.1mol / L Zn 2+ solution and 10mL of 0.1mol / L Mn 2+ The remaining steps are the same as those in Example 1 and will not be described in detail.

[0039] Comparative Example 1

[0040] This comparative example provides a catalyst Ni / MgAl2O4 (denoted as Ni / S1) with nickel loaded on the surface of MgAl2O4, and the preparation method is as follows:

[0041] The equal volume impregnation method was used to load 5 wt.% Ni on MgAl2O4, specifically: 2.48 g Ni(NO3)2·6H2O was weighed and dissolved in 10 mL deionized water, 100 μL of the solution was aspirated with a pipette and dropped into 1 g MgAl2O4, and then the mixture was ground and dried and transferred to a crucible, placed in a box furnace and heated to 450°C at a heating rate of 1°C / min and calcined for 4 h, and then cooled to obtain Ni / MgAl2O4.

[0042] Comparative Example 2

[0043] This comparative example provides a pure phase binary metal oxide (denoted as S1), whose chemical formula is MgAl2O4, and whose preparation method is as follows:

[0044] According to the metal atomic molar ratio of Al:Mg=10:5, 10mL of 1mol / L Al 3+ solution and 10mL of 0.5mol / L Mg 2+ The remaining steps are the same as those in Example 1 and will not be described in detail.

[0045] Comparative Example 3

[0046] This comparative example provides a pure phase ternary metal oxide (denoted as S2), whose chemical formula is (Mg 0.8 Ni 0.2 )Al2O4, the preparation method is as follows:

[0047] According to the metal atomic molar ratio of Al:Mg:Ni=10:4:1, 10mL of 1mol / L Al 3+ solution, 8mL of 0.5mol / L Mg 2+ solution and 10mL of 0.1mol / L Ni 2+ The remaining steps are the same as those in Example 1 and will not be described in detail.

[0048] Test Example 1

[0049] (I) Appearance observation

[0050] Figure 1 The oxide powders obtained from S1 to S5 show that, as the types of elements doped in the oxides increase, the color of the obtained oxides gradually becomes darker.

[0051] (ii) XRD test

[0052] XRD tests were performed on the medium-high entropy multi-metal oxide catalysts obtained in Examples 1 to 3 and the pure metal oxides obtained in Comparative Examples 2 to 3, respectively. The results are as follows: Figure 2 By comparing with the standard card, it was determined that the diffraction peaks of the medium-high entropy multi-metal oxide catalyst obtained in Examples 1 to 3 at 19.00°, 31.28°, 36.86°, 44.83°, 59.38° and 65.26° belong to Mg 8.00 Al 16.00 O 32.00 (PDF#96-900-3482), corresponding to spinel Mg 8.00 Al 16.00 O 32.00The (111), (022), (311), (040), (151) and (044) crystal planes. Figure 2 It can be seen that the diffraction peaks of the corresponding spectra of the medium-high entropy multi-metal oxide catalysts obtained in Examples 1 to 3 are sharp, symmetrical, and free of impurity peaks. The sample crystal structure is complete, indicating that it has good crystallinity and high purity. After magnifying and observing the (311) crystal plane, it is found that as the number of elements increases, the characteristic peaks shift, indicating that other metal ions (Ni 2+ / Co 2+ / Zn 2+ / Mn 2+ ) was successfully introduced and successfully replaced the corresponding Mg 2+ .

[0053] From the above XRD results, it can be seen that the present invention successfully synthesized a multinary metal oxide with a pure phase spinel structure; and according to the Bragg equation nλ=2dsinθ, it was found that the diffraction angle shifted to a smaller angle, indicating that the present invention successfully incorporated active metal elements with a larger ionic radius into the crystal lattice; comparing the XRD spectra of Examples 1 to 3 and Comparative Examples 2 to 3, it can be seen that with the increase in the types of metal elements incorporated, the entropy stability and material crystallinity of the obtained multinary oxide are gradually improved.

[0054] (III) SEM test

[0055] The medium-high entropy multi-metal oxide catalysts obtained in Examples 1 to 3 (S3 to S5 in sequence) and the pure phase metal oxides obtained in Comparative Examples 2 to 3 (S1 to S2 in sequence) were subjected to SEM tests, and the results are as follows: Figure 3 shown.

[0056] Depend on Figure 3 As can be seen from (b), (g), (c) and (h), S2 and S3 are irregular blocks; as can be seen from (a), (f), (d), (i), (e) and (j), S1, S4 and S5 are all agglomerated nanoparticles with large particle size and obvious clustering effect, and the introduction of transition metal elements has no obvious effect on the micromorphology and structure of the multi-metal oxides.

[0057] (IV) EDS test

[0058] In order to determine the specific elemental composition and the proportion of each element of the medium-high entropy multi-metal oxide catalyst obtained in the present invention, the medium-high entropy multi-metal oxide catalyst (S4 and S5) obtained in Examples 2 to 3 was subjected to EDS testing. The results are shown in Table 1, and the spectra are shown in Table 1. Figure 4 As shown in (a) and (b).

[0059] Depend on Figure 4(a) It can be seen that Al, Mg, Ni, Co, Zn and O elements exist in S4. Figure 4 (b) It can be seen that Al, Mg, Ni, Co, Zn, O and Mn elements exist in S5, and the above elements are evenly distributed in the sample.

[0060] And the test ratios of the elements in S4 and S5 are calculated according to the data in Table 1: the test ratios of the elements in S4 are Mg:Al:Ni:Co:Zn=0.8:0.8:0.7:0.4:10, and the theoretical ratios are 2:1:1:1:10; the test ratios of the elements in S5 are Mg:Al:Ni:Co:Zn:Mn=0.4:0.7:0.7:1:0.5:10, and the theoretical ratios are 1:1:1:1:1:10. It can be seen that the differences between the test ratios of the elements in S4 and S5 and the theoretical ratios are within the error range, that is, the test values ​​are consistent with the feed ratios, proving that the present invention successfully synthesizes a high-entropy multi-metal oxide catalyst in a pure phase with uniform distribution of the elements.

[0061] Table 1 Mass percentage and atomic percentage of each element in S4 and S5

[0062]

[0063]

[0064] (V) Specific surface area test

[0065] The specific surface area tests were performed on the medium-high entropy multinary metal oxide catalysts obtained in Examples 1 to 3 and the pure phase metal oxides obtained in Comparative Examples 2 to 3, respectively. The results are shown in Table 2.

[0066] Table 2 Calcination temperature and specific surface area of ​​catalysts prepared by S1-S5

[0067]

[0068] From Table 2, we can see that the specific surface area of ​​S1 is 93.90m 2 / g, the specific surface area of ​​S2 is 82.80m 2 / g, the specific surface area of ​​S3 is 95.72m 2 / g, the specific surface area of ​​S4 is 86.11m 2 / g, the specific surface area of ​​S5 is 124.08m 2 / g. This indicates that the co-precipitation method for preparing medium-high entropy multi-metal oxides can retain the high specific surface area advantage of the multi-metal oxide precursors, which is beneficial to the catalytic dry reforming of methane (DRM) reaction.

[0069] Test Example 2

[0070] (I) Thermal catalytic DRM activity test

[0071] At a total mass space velocity of 2.4 L / g cat The thermal catalytic DRM activity of the catalysts obtained in Examples 1 to 3, Comparative Example 1 and Comparative Example 3 was investigated under the condition of 1:1 / h. CH4 and CO2 were both introduced into the reactor at a flow rate of 20 mL / min, and 0.1 g of the above catalyst was passed through each of them. The reaction temperature was 800°C, and the products were quantified by gas chromatography, and plotted according to the results, as shown in FIG. Figure 5 shown.

[0072] Figure 5 (d) to (e) are the thermal catalytic DRM performance test results of the catalysts corresponding to S2 to S5 under the same reaction conditions. It can be seen that after the multi-component high-entropy design of the spinel structure multi-element oxide (i.e., the introduction of metal elements other than Ni at the A position in the S2 crystal structure), the conversion rates of CH4 and CO2 are greatly improved. The catalysts corresponding to S3 to S5 have a CH4 conversion rate of more than 85%, and a CO2 conversion rate of 92%. Moreover, the performance of the catalysts after reacting at 800°C for 10 hours is still relatively stable, and no deactivation occurs. The inventors speculate that the multi-component high-entropy design, i.e., the introduction of specific transition metal elements (Ni, Co, Zn, Mn) into the catalyst crystal structure, enhances the interaction between the transition metal inside the catalyst and the carrier, improves the catalyst structure stability, and thus makes the obtained catalyst have excellent sintering resistance and anti-carbon deposition performance. In addition, the improvement in CH4 conversion can be attributed to the synergistic effect of Ni-Co alloy; Zn as an additive can enhance the configuration entropy of multi-metal oxides, improve the metal-support interaction between NiO and the support, and increase the thermal stability and anti-carbon deposition performance of the catalyst; Mn as a promoter can enhance the reducibility of the catalyst, making NiO easier to reduce to more active metal Ni 0 morphology, thereby improving the catalytic activity; moreover, improving the redox ability of the catalyst can promote the necessary oxygen transfer in the CO2 activation process, and achieve effective activation of CO2 at low temperatures; in addition, the addition of Mn can promote the formation of the active intermediate -CH2OH at low temperatures, thereby significantly improving the low-temperature catalytic activity, that is, the introduction of Mn is conducive to improving the performance of the DRM catalyst. In summary, the medium-high entropy multi-metal oxide catalyst provided by the present invention can effectively improve the catalyst's own structural stability and the catalytic activity of DRM.

[0073] (II) H2-TPR test

[0074] The reducibility of the catalysts obtained in Examples 1 to 3, Comparative Example 1 and Comparative Example 3 was investigated by hydrogen temperature programmed reduction (H2-TPR) experiments. The H2-TPR curves are shown in FIG. Figure 6As shown in the figure, the presence of multiple reduction peaks indicates that the catalyst contains different metal oxidation states. Specifically, the reduction peak of Ni / S1 (Comparative Example 1) at 404°C belongs to the reduction of "free" NiO with weak interaction with the carrier to metallic Ni; the reduction peaks of S2, S3 and S4 at 524°C, 551°C and 430°C belong to the NiO with strong interaction with the carrier and high dispersion. x The reduction peak of S5 at 470℃ belongs to the reduction of high-valent Ni ions, Co ions, and Mn ions; the reduction peak of S2 at 614℃ belongs to the reduction of Ni ions, Co ions, and Mn ions; the reduction peak of S2 at 614℃ belongs to the reduction of Ni ions, Co ions, and Mn ions; the reduction peak of S3 at 614℃ belongs to the reduction of Ni ions, Co ions, and Mn ions; the reduction peak of S4 at 614℃ belongs to the reduction of Ni ions, Co ions, and Mn ions; the reduction peak of S5 ...2 at 614℃ belongs to the reduction of Ni ions, Co ions, and Mn ions; the reduction peak of x Mg 1-x The high-valent Ni ions in the Al2O4 spinel phase are reduced to low-valent Ni ions. The reduction peak at 746℃ belongs to Ni 2+ The reduction peaks of S3, S4, and S5 at 630°C, 638°C, and 682°C belong to the reduction of high-valent Ni and Co ions in the spinel phase to low-valent Ni and Co ions, and the reduction peaks at 772°C, 844°C, and 900°C belong to Ni 2+ and Co 2+ It can be seen that as the metal elements in the carrier increase, the reduction peaks of Ni ions, Co ions and Ni-Co alloys all shift to high temperatures, indicating that the introduction of metal elements into spinel-structured multi-metal oxides will enhance the interaction between metal carriers and improve structural stability, which is conducive to obtaining more uniformly dispersed and smaller active metal nanoparticles to enhance the DRM catalytic activity.

[0075] In summary, it can be concluded that as the number of metal elements in the catalyst increases, the interaction between metal supports increases. Therefore, the results of H2-TPR prove that the medium-high entropy multi-metal oxide catalyst provided by the present invention can enhance the strong interaction between metal supports, thereby promoting the DRM reaction.

[0076] What is described above is only a preferred specific implementation manner of the present invention, but the protection scope of the present invention is not limited thereto. Any technician familiar with the technical field can make equivalent replacements or changes according to the technical scheme and inventive concept of the present invention within the technical scope disclosed by the present invention, which should be covered by the protection scope of the present invention.

Claims

1. A medium-high entropy multinary metal oxide catalyst, characterized in that: The invention has a pure phase magnesium aluminum spinel structure doped with transition metal elements, wherein the transition metal elements include nickel and at least one of cobalt, zinc and manganese.

2. The medium-high entropy multinary metal oxide catalyst according to claim 1, characterized in that The medium-high entropy multi-metal oxide catalyst is represented by the chemical formula (Mg x Ni y Co z Zn m Mn n )Al2O4 represents; Among them, 0.2≤x<1, 0<y≤0.4, 0≤z≤0.2, 0≤m≤0.2, 0≤n≤0.2 and x+y+z+m+n=1.

3. The medium-high entropy multinary metal oxide catalyst according to claim 2, characterized in that: The chemical formula of the medium-high entropy multi-metal oxide catalyst is (Mg 0.6 Ni 0.2 Co 0.2 )Al2O4.

4. The medium-high entropy multinary metal oxide catalyst according to claim 2, characterized in that: The chemical formula of the medium-high entropy multi-metal oxide catalyst is (Mg 0.4 Ni 0.2 Co 0.2 Zn 0.2 )Al2O4 or (Mg 0.4 Ni 0.2 Co 0.2 Mn 0.2 )Al2O4.

5. The medium-high entropy multinary metal oxide catalyst according to claim 2, characterized in that: The chemical formula of the medium-high entropy multi-metal oxide catalyst is (Mg 0.2 Ni 0.2 Co 0.2 Zn 0.2 Mn 0.2 )Al2O4.

6. A method for preparing a medium-high entropy multinary metal oxide catalyst according to any one of claims 1 to 5, characterized in that the steps include: S1. Evenly mix a soluble aluminum salt, a soluble magnesium salt and a soluble salt of a doped transition metal element according to a preset molar ratio of each element to obtain a multi-metal mixed solution; S2, adjusting the pH of the mixed solution to 9-10, separating the solid and the liquid after the metal ions are completely precipitated, washing the solid product to neutrality, and drying to obtain a multi-metal precursor; S3, grinding the multi-metal precursor into powder, calcining, cooling and reducing to obtain a medium-high entropy multi-metal oxide catalyst.

7. The method for preparing a medium-high entropy multinary metal oxide catalyst according to claim 6, characterized in that: The calcination is to grind the multi-metal precursor into powder, place the powder in a box furnace, heat it to 750-850° C. at a heating rate of 2-4° C. / min, and calcine it for 3-5 hours.

8. The method for preparing a medium-high entropy multinary metal oxide catalyst according to claim 6, characterized in that: The temperature of the reduction reaction is 750-850° C., the gas used for reduction is a 10% hydrogen / argon mixed gas, and the gas flow rate is 40-50 mL / min.

9. Use of the medium-high entropy multinary metal oxide catalyst according to any one of claims 1 to 5 in an alkane reforming reaction.

10. The use according to claim 9, characterized in that The alkane reforming reaction includes a methane wet reforming reaction, a methane dry reforming reaction, a methane partial oxidation reforming reaction and a light alkane reforming reaction.

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