Porous molded body containing spinel

Abstract

The present invention relates to a novel molded article having a finely tuned porosity. In particular, the present invention relates to a compositional formula M 1 M 2 A novel molded body comprising a mixed metal oxide having 2O4, where M 1 is one or more divalent elements M 1 This includes M 2 is one or more trivalent elements M 2 The present invention relates to a molded body comprising a mixed metal oxide comprising a crystalline phase having a spinel structure, wherein the molded body has a total pore volume in the range of 0.10 to 0.90 ml / g. Furthermore, the present invention relates to a novel molded body, in particular a process for producing a novel molded body, and a molded body obtained or obtainable by such process. Furthermore, the present invention relates to the use of a molded body as a catalyst or catalyst support.

Description

[Technical Field]

[0001] The present invention relates to compositional formula M 1 M 2 Regarding a molded body containing a mixed metal oxide having 2O4, M 1 It contains one or more divalent elements, M 2 The material contains one or more trivalent elements, the mixed metal oxide contains a crystalline phase having a spinel structure, and the molded body has a total pore volume in the range of 0.10 to 0.90 ml / g. Furthermore, the present invention relates to a method for producing a novel molded body, a molded body obtained by the method, and the use of the novel molded body of the present invention. [Background technology]

[0002] Typically, a catalyst comprises a carrier material and a catalyst material supported thereon. The carrier material used is usually in the form of a molded body that may have a specific shape. Supporting can be carried out by known methods, particularly impregnation, more specifically by incipient wetness impregnation using, for example, a metal solution. The immersion behavior of the carrier material is crucial for achieving a uniform distribution of the catalyst material.

[0003] Uniformly impregnating a molded body with a metal solution can be difficult due to the non-uniform distribution of the metal solution within the molded body. Such non-uniform distribution can lead to an undesirable core-shell structure, where higher metal density is observed in the shell. This can result in stronger sintering of these metal centers when used in catalytic processes.

[0004] CA1189052 relates to a method for producing a catalyst or catalyst support having both a high surface area and a large pore diameter. In particular, this method includes a step of mixing a metal oxide with water and an acid to form a dilute metal gel consisting of a loose three-dimensional network of oxides in which a large amount of water is uniformly dispersed throughout.

[0005] US4558031 discloses a method for producing a catalyst or catalyst support having both a high surface area and a large pore diameter, relating to a highly porous catalyst. This method particularly includes a step of mixing alumina with water and nitric acid to form an alumina gel consisting of a loose three-dimensional network, wherein the acid is present in an amount of at least 250 parts of 70% HNO3 per 100 parts of alumina.

[0006] EP0210681A1 relates to a catalyst suitable for reduction and oxidation reactions, wherein the catalyst is a combination of magnesium-aluminate spinel and copper, cobalt, a copper or cobalt compound, or a mixture thereof, and the spinel support optionally contains an oxide of a secondary divalent metal.

[0007] WO94 / 16798A1 relates to a process for catalytically decomposing pure or mixed gaseous nitrous oxide at 200–900°C and a pressure of 0.1–20 bar. This process uses a catalyst prepared by calcining CuAl2O4 in combination with tin, lead, or a major or minor group element of Group II of the periodic table (oxide, salt, or elemental form) at 300–1300°C and a pressure of 0.1–200 bar.

[0008] GB1377191A relates to a catalyst containing metallic cobalt, cobalt oxide, or both, supported on a mixed oxide material that mainly has a spinel structure and substantially does not contain cobalt oxide or unbonded oxides capable of forming spinels. Specifically, it contains less than 5% by weight of divalent or tetravalent oxides capable of forming such spinels, or less than 1% by weight of trivalent oxides capable of forming such spinels.

[0009] Therefore, there was a need to provide a molded article having finely tuned porosity, preferably a molded article with increased porosity. Furthermore, an object of the present invention is to provide a method for producing a molded article having finely tuned porosity, preferably a method for producing a molded article with increased porosity, and more preferably a method for producing a molded article that enables a uniform distribution of metal ions. [Prior art documents] [Patent Documents]

[0010] [Patent Document 1] CA1189052 [Patent Document 2] US4558031 [Patent Document 3] EP0210681A1 [Patent Document 4] WO94 / 16798A1 [Patent Document 5] GB1377191A [Overview of the project] [Problems that the invention aims to solve]

[0011] The object of the present invention is to provide a novel molded article containing a mixed metal oxide having a spinel structure and having finely tuned porosity. In particular, the object of the present invention is to provide a novel molded article with increased porosity that enables uniform impregnation with a metal solution. Furthermore, the object of the present invention is to provide a novel method for manufacturing a molded article, comprising a pre-sintering step, an acid treatment step, and a final sintering step. [Modes for carrying out the invention]

[0012] Surprisingly, it was found that a process including acid treatment after firing the molded body significantly improved the distribution of the metal solution throughout the molded body. In particular, it was found that the porosity of the molded body, especially the total pore volume, could be adjusted and fine-tuned through appropriate treatment, and could be increased. Therefore, it was found that acid treatment of a pre-fired molded body significantly improved its immersion properties. This treatment makes it possible to impregnate molded bodies, especially those with complex shapes. In particular, it allows for uniform impregnation even in molded bodies with a low surface area-to-volume ratio.

[0013] This effect is shown in Fig. 3. The molded bodies of two samples were impregnated with a metal solution, fired, and then cut in half. The sample of the molded body shown in Fig. 3A was not treated according to the present invention, whereas the sample of the molded body shown in Fig. 3B was treated according to the present invention before impregnation. As can be seen from Figs. 3A and 3B, the sample of the molded body that was not treated with the aqueous solution containing an acid according to the present invention was not uniformly impregnated, as indicated by different colorings. In contrast, the uniform coloring of the sample of the molded body shown in Fig. 3B indicates uniform impregnation.

[0014] Therefore, the present invention relates to a molded body containing a mixed metal oxide having a composition formula M 1 M 2 2O4, where M 1 includes one or more divalent elements M 1 and M 2 includes one or more trivalent elements M(2). The mixed metal oxide includes a crystal phase having a spinel structure, the crystal phase having the spinel structure is preferably determined according to Reference Example 1.2, the molded body has a total pore volume in the range of 0.10 to 0.90 ml / g, and the total pore volume is preferably determined according to Reference Example 1.4.

[0015] M 1 is preferably selected from Group 2, Group 10, Group 11, and Group 12 of the periodic table of the elements, and M 1 is more preferably selected from the group consisting of Mg, Ni, Cu, Zn, Mn, Co, and mixtures of two or more thereof, even more preferably selected from the group consisting of Mg, Ni, Cu, Zn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Mg, Zn, Cu, and mixtures thereof, and even more preferably selected from the group consisting of Mg, Zn, and mixtures thereof. Here, M 1 is more preferably Mg. <​​​​​is more preferably selected from the group consisting of Al, Cr, Fe, V, Mn, Co, and mixtures of two or more thereof, even more preferably selected from the group consisting of Al, Cr, Fe, V, Mn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Al, Cr, V, Mn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Al, Cr, and mixtures of two or more thereof, where M 2 It is more preferably Al.

[0017] The molded body is M 1 It is preferable that the mixture contains 10% by weight or less, more preferably 5% by weight or less, more preferably 1.0% by weight or less, more preferably 0.1% by weight or less, and more preferably 0.01% by weight or less of O, which preferably contains one or more divalent elements M according to Reference Example 1.2. 1 Based on the total weight, M in the molded body 1 It is calculated as O. Here, M in the molded body 1 One or more divalent elements M in the molded body, calculated as O. 1 The total weight is preferably determined according to Reference Example 1.6.

[0018] The crystallinity of the mixed metal oxide is preferably 50-100%, more preferably 60-100%, more preferably 70-95%, and more preferably 80-90%, and this crystallinity is determined according to Reference Example 1.2.

[0019] When the mixed metal oxide has 50-100% crystallinity, it is preferable that 50-100%, more preferably 70-100%, and more preferably 95-100% of the crystalline phase, determined by XRD, preferably according to Reference Example 1.2, have a spinel structure.

[0020] The molded article preferably exhibits an X-ray diffraction pattern that includes at least the following reflections:

[0021] [Table 1]

[0022] Here, 100% corresponds to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and more preferably includes at least the following reflections:

[0023] [Table 2]

[0024] Here, 100% corresponds to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and more preferably includes at least the following reflections:

[0025] [Table 3]

[0026] Here, 100% represents the intensity of the maximum peak in the X-ray powder diffraction pattern, and this X-ray diffraction pattern is preferably determined according to Reference Example 1.2. Here, M 1 is more Mg, and M 2 Al is more preferable.

[0027] The average pore size of the molded article is preferably in the range of 0.001 to 0.1 μm, more preferably in the range of 0.005 to 0.05 μm, even more preferably in the range of 0.02 to 0.04 μm, more preferably in the range of 0.027 to 0.035 μm, and more preferably in the range of 0.028 to 0.034 μm. Here, the pore size distribution is preferably measured according to Reference Example 1.5.

[0028] The molded article preferably has a water adsorption amount in the range of 10 to 80% by weight, more preferably in the range of 30 to 60% by weight, even more preferably in the range of 40 to 50% by weight, and more preferably in the range of 43 to 47% by weight, and the water adsorption amount is preferably measured according to Reference Example 1.1.

[0029] The molded body has a BET specific surface area of ​​20.0 to 150.0 m². 2 It is preferably in the range of / g, and more preferably 30.0 to 90.0 m 2 The range is / g, more preferably 40.0 to 65.0 m 2 Range of / g, more preferably 47.0 to 49.0 m 2 The BET specific surface area is preferably in the range of / g, and is preferably measured according to Reference Example 1.3.

[0030] The total pore volume of the molded article is preferably in the range of 0.18 to 0.75 ml / g, more preferably in the range of 0.25 to 0.60 ml / g, and even more preferably in the range of 0.33 to 0.53 ml / g. More preferably in the range of 0.37 to 0.49 ml / g, and even more preferably in the range of 0.40 to 0.46 ml / g. Here, the total pore volume is preferably determined according to Reference Example 1.4.

[0031] Furthermore, the molded body is made of one or more metals M 3 It is preferable that it contains M 3 The element is selected from the group consisting of Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag, Mo, Sn, and mixtures of two or more of these, and more preferably selected from the group consisting of Fe, Ru, and mixtures of two or more of these. One or more metals M 3 It is more preferable that the material is supported on a mixed metal oxide.

[0032] The molded body further contains one or more metal M 3 Includes M 3 If is selected from the group consisting of Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag, Mo, Sn and mixtures of two or more of them, the molded body contains one or more divalent elements M 1 (M 1 (calculated as O) and one or more trivalent elements M 2 (M 2Based on the total weight (calculated as 2O3), one or more metals M should be calculated as elements, making up 20% by weight or less, more preferably 10% by weight or less, and more preferably 5% by weight or less. 3 Preferably, the molded article contains one or more divalent elements M 1 (M 1 (calculated as O) and one or more trivalent elements M 2 (M 2 The total weight (calculated as 2O3) is preferably determined according to Reference Example 1.6.

[0033] Furthermore, the molded body contains one or more metal M 3 If M further includes 3 It is selected from the group consisting of Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag, Mo, Sn and mixtures of two or more of these, and one or more metal M 3 It is preferable that the material is uniformly dispersed throughout the molded body.

[0034] 85-100% by weight, more preferably 90-100% by weight, more preferably 95-100% by weight, more preferably 98-100% by weight, more preferably 99-100% by weight, more preferably 99.9-100% by weight of the molded body, 1 M 2 , O, H, and any one or more metals M 3 It is preferable that it be composed of the following.

[0035] 85-100% by weight, more preferably 90-100% by weight, more preferably 95-100% by weight, more preferably 98-100% by weight, more preferably 99-100% by weight, more preferably 99.9-100% by weight of the molded body is a mixed metal oxide and any one or more metal M 3 It is preferable that it be composed of the following.

[0036] The molded article is preferably an extruded article, a tablet, or a granule.

[0037] When the molded body is an extruded body, a tablet, or granules, the extruded body or tablet has a cross-section, which is preferably circular, hexagonal, rectangular, square, triangular, elliptical, star-shaped, or cloverleaf-shaped; more preferably circular, hexagonal, rectangular, square, triangular, elliptical, star-shaped with 3, 4, 5, 6, 7, or 8 points, trilobe, quadrilobe, or hexalobe; and even more preferably circular, hexagonal, rectangular, square, triangular, elliptical, star-shaped with 3 or 4 points, trilobe, quadrilobe, or hexalobe.

[0038] The molded body is a tablet having a cross-section, and the cross-section is preferably four-leaf shaped.

[0039] If the molded body is a tablet having a cross-section, and the cross-section is four-leaf clover-shaped, the tablet preferably has a thickness, which is in the range of 2.0 to 13.0 mm, more preferably in the range of 5.0 to 10.0 mm, and even more preferably in the range of 6.5 to 9.0 mm.

[0040] Furthermore, if the molded body is a tablet having a cross-section, it is preferable that the tablet has a diameter D in the range of 5 to 20 mm, more preferably in the range of 7 to 17 mm, and even more preferably in the range of 9 to 15 mm.

[0041] The molded body is a tablet having a cross-section, and the cross-section is preferably hexa-shaped.

[0042] If the molded body is a tablet having a cross-section, and the cross-section is hexa-lobed, the thickness of the tablet is in the range of 2.0 to 15.0 mm, more preferably in the range of 5.0 to 12.0 mm, and even more preferably in the range of 8.0 to 9.0 mm.

[0043] Furthermore, in the case of a tablet in which the molded body has a hexagonal cross-sectional shape, the diameter D of the tablet is preferably in the range of 5 to 25 mm, more preferably in the range of 12 to 19 mm, and even more preferably in the range of 14 to 17 mm.

[0044] Furthermore, the present invention relates to a method for manufacturing a molded article, preferably a method for manufacturing a molded article according to any of the specific preferred embodiments disclosed herein, the method including: (i)M 1 O and M 2 A process of providing one or more sources of 2O3, M 1 represents one or more divalent elements, M 2 This is a process that represents one or more trivalent elements; (ii) A process of molding one or more raw materials obtained in process (i); (iii) A step of firing the molded body obtained in step (ii) in a gas atmosphere; (iv) A step of treating the molded body obtained in step (iii) with acid; (v) A step of firing the molded body obtained in step (iv) in a gas atmosphere.

[0045] M 1 It is preferable that the element is selected from Group 2, Group 10, Group 11, and Group 12 of the periodic table, where M 1 is more preferably selected from the group consisting of Mg, Ni, Cu, Zn, Mn, Co, and mixtures of two or more thereof, even more preferably selected from the group consisting of Mg, Ni, Cu, Zn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Mg, Zn, Cu, and mixtures thereof, even more preferably selected from the group consisting of Mg, Zn, and mixtures thereof, even more preferably M 1 It is Mg.

[0046] M 2 It is preferable that the element is selected from Group 5, Group 6, Group 7, Group 8 and Group 13 of the periodic table, where M 2is more preferably selected from Al, Cr, Fe, V, Mn, Co, and mixtures of two or more thereof, even more preferably selected from Al, Cr, Fe, V, Mn, and mixtures of two or more thereof, even more preferably selected from Al, Cr, V, Mn, and mixtures of two or more thereof, even more preferably selected from Al, Cr, and mixtures of two or more thereof, and even more preferably M 2 It is Al.

[0047] M 1 O and M 2 One or more sources of 2O3 are preferably M 1 Oxides, M 1 Hydroxides, M 1 carbonate, M 1 bicarbonate, M 1 Hydroxy carbonate, M 2 Oxides, M 2 Hydroxides, M 2 carbonate, M 2 bicarbonate, M 2 Hydroxy carbonate, M 1 and M 2 Mixed metal oxides, M 1 and M 2 It is preferable, and more preferable, to contain, a mixed metal hydroxycarbonate and one or more compounds selected from the group consisting of two or more mixtures thereof.

[0048] M 1 O and M 2 One or more sources of 2O3 are preferably M 1 and M 2 Mixed metal oxides, M 1 and M 2 It is preferable, and more preferable, to contain, one or more compounds selected from the group consisting of mixed metal hydroxycarbonates and mixtures thereof.

[0049] M 1 O and M 2 One or more sources of 2O3 are M 1 and M 2The molar ratio is preferably in the range of 1:5 to 5:1.0, more preferably in the range of 1:2.5 to 2.5:1, still more preferably in the range of 1:2 to 2:1, and even more preferably in the range of 1:2.1 to 1:1.9.

[0050] M 1 O and M 2 One or more sources of M2O3 are M 1 O and M 2 M contained in one or more sources of M2O3 1 (Calculated as M2O) and M 1 Based on the total weight of (calculated as M2O3) and M 2 (M 2 22 to 34% by weight, more preferably 25 to 31% by weight, still more preferably 27 to 29% by weight of M 1 (M 1 (Calculated as M2O) is preferably included.

[0051] M 1 O and M 2 One or more sources of M2O3 are M 1 O and M 2 M contained in one or more sources of M2O3 1 (M 1 (Calculated as M2O) and M 2 (M 2 Based on the total weight of (calculated as M2O3) and M 2 (M 2 (Calculated as M2O3) is preferably included.

[0052] The shaping of the mixture in (ii) preferably includes tableting or extruding.

[0053] The firing in (iii) is preferably carried out at a temperature in the range of 300 to 1200 °C, more preferably in the range of 700 to 1100 °C, still more preferably in the range of 900 to 1000 °C.

[0054] (iii) The firing is preferably carried out for a range of 0.1 to 48 hours, more preferably 0.5 to 24 hours, and even more preferably 1 to 5 hours.

[0055] The gas atmosphere in (iii) preferably contains one or more oxygen and nitrogen, more preferably consists of them, and even more preferably is air.

[0056] The molded article obtained from (iii) preferably exhibits an X-ray diffraction pattern that includes at least the following reflections.

[0057] [Table 4]

[0058] Here, 100% corresponds to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and more preferably includes at least the following reflections.

[0059] [Table 5]

[0060] Here, 100% corresponds to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and more preferably includes at least the following reflections.

[0061] [Table 6]

[0062] Here, 100% corresponds to the intensity of the maximum peak in the X-ray powder diffraction pattern, and the X-ray diffraction pattern is preferably determined according to Reference Example 1.2, M 1 is more Mg, and M 2 Al is more preferable.

[0063] The molded body obtained from (iii) is 40.0~60.0m 2 Range of / g, more preferably 47.0 to 53.0 m 2 The range is / g, more preferably 49.0 to 51.0 m 2 It is preferable to have a BET specific surface area in the range of / g, where the BET specific surface area is preferably determined according to Reference Example 1.3.

[0064] The molded article obtained from (iii) preferably has a total pore volume in the range of 0.20 to 0.55 ml / g, more preferably in the range of 0.30 to 0.42 ml / g, and even more preferably in the range of 0.33 to 0.39 ml / g, where the total pore volume is preferably determined according to Reference Example 1.4.

[0065] The process in (iv) preferably includes immersing the molded body in acid.

[0066] The process in (iv) is preferably carried out over a period of 20 to 100 minutes, more preferably 45 to 75 minutes, and even more preferably 55 to 65 minutes.

[0067] The process in (iv) is preferably carried out at a temperature in the range of 0 to 50°C, more preferably in the range of 10 to 40°C, and even more preferably in the range of 15 to 35°C.

[0068] (iv) The acid is preferably an aqueous acid.

[0069] If the acid in (iv) is an aqueous acid, it is preferable that the aqueous acid has a weight ratio of acid to water in the range of preferably 1:1 to 1:10, more preferably 1:3 to 1:5, and even more preferably 1:3.9 to 1:4.1.

[0070] Furthermore, if the acid in (iv) above is an aqueous acid, the acid concentration of the aqueous acid is preferably in the range of 2.5 to 4.5 mol / l, more preferably in the range of 3.2 to 3.7 mol / l, and even more preferably in the range of 3.3 to 3.6 mol / l.

[0071] The acid in (iv) preferably contains one or more inorganic acids and organic acids, more preferably consists of them, and more preferably is one or more of HNO3, HCl, H2SO4, H3PO4, formic acid, oxalic acid, and acetic acid, and even more preferably is HNO3.

[0072] The above method preferably further includes the following after (iv) and before (v): Wash the molded body obtained from (w)(iv) with deionized water.

[0073] The above method preferably further includes the following after (iv) and before (v), preferably after (w) and before (v): (d)(iv) or (w) is dried in a gas atmosphere.

[0074] If the method described above further includes drying as in (d), the drying is preferably carried out at a temperature in the range of 80 to 160°C, more preferably in the range of 100 to 140°C, and even more preferably in the range of 110 to 130°C.

[0075] Furthermore, if the method described above further includes drying of (d), the drying of (d) is preferably carried out over a period of time ranging from 0.5 to 16 hours, more preferably from 2 to 12 hours, and even more preferably from 3 to 8 hours.

[0076] Furthermore, if the method described above further includes drying in (d), the gas atmosphere in (d) preferably contains one or more oxygen and nitrogen, more preferably consists of them, and even more preferably is air.

[0077] The firing of (v) is preferably carried out at a temperature in the range of 400 to 1000°C, more preferably in the range of 600 to 950°C, and even more preferably in the range of 825 to 875°C.

[0078] The firing of (v) is preferably carried out for a range of 0.1 to 1.5 hours, more preferably 0.3 to 0.7 hours, and even more preferably 0.4 to 0.6 hours.

[0079] (v) The gas atmosphere preferably contains one or more oxygen and nitrogen, more preferably consists of them, and even more preferably is air.

[0080] The above method preferably further includes the following after (v):

[0081] (vi) One or more metals M are placed on the molded body obtained in (v). 3 To carry or bear.

[0082] Here, the loading is preferably carried out by impregnation, more preferably by wet impregnation, and even more preferably by incipient wet impregnation. 3 The material is selected from the group consisting of Fe, Ru, Os, Co, Rh, Ir, Pd, Pt, and mixtures of two or more of these, and more preferably from the group consisting of Fe, Ru, and mixtures of two or more of these.

[0083] Furthermore, the present invention preferably relates to a molded article according to any of the specific preferred embodiments disclosed herein, wherein the molded article may or may be obtained by a method according to any of the specific preferred embodiments disclosed herein.

[0084] Furthermore, the present invention relates to the use of a molded article, according to any of the specific preferred embodiments disclosed herein, as a catalyst or catalyst support.

[0085] The present invention is further described by the following set of embodiments and combinations of embodiments arising from the given dependencies and reference relationships. In particular, it should be noted that in each case where the scope of an embodiment is referred to, such as in the context of the term "any one of Embodiments 1 to 4," it is intended that all embodiments within that scope are expressly disclosed to those skilled in the art. That is, the wording of this term should be understood by those skilled in the art as synonymous with "any one of Embodiments 1, 2, 3, and 4." Furthermore, it should be explicitly noted that the following set of embodiments does not constitute a set of claims that would determine the scope of protection, but rather represents a well-structured description covering general and preferred aspects of the invention.

[0086] 1. Composition formula M 1 M 2 A molded body comprising a mixed metal oxide having 2O4, where M 1 is one or more divalent elements M 1 Includes M 2 is one or more trivalent elements M 2 A molded body comprising a mixed metal oxide comprising a crystalline phase having a spinel structure, wherein the crystalline phase having a spinel structure is preferably determined according to Reference Example 1.2, and the molded body having a total pore volume in the range of 0.10 to 0.90 ml / g, wherein the total pore volume is preferably determined according to Reference Example 1.4.

[0087] 2. M 1 It is selected from Groups 2, 10, 11, and 12 of the periodic table, M 1 It is preferably selected from the group consisting of Mg, Ni, Cu, Zn, Mn, Co, and mixtures of two or more thereof, more preferably selected from the group consisting of Mg, Ni, Cu, Zn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Mg, Zn, Cu, and mixtures thereof, and even more preferably selected from the group consisting of Mg, Zn, and mixtures thereof, M 1 The molded article of Embodiment 1, wherein is more preferably Mg.

[0088] 3. M 2 It is selected from Groups 5, 6, 7, 8 and 13 of the periodic table, M 2 It is preferably selected from the group consisting of Al, Cr, Fe, V, Mn, Co, and mixtures of two or more thereof, more preferably selected from the group consisting of Al, Cr, Fe, V, Mn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Al, Cr, V, Mn, and mixtures of two or more thereof, and even more preferably selected from the group consisting of Al, Cr, and mixtures of two or more thereof, M 2 The molded article of Embodiment 1 or 2, wherein is more preferably Al.

[0089] 4. One or more divalent elements M contained in the molded body 1 (M 1 Based on the total weight (calculated as O), M is preferably determined according to Reference Example 1.2. 1 The molded body contains 10% by weight or less of O, preferably 5% by weight or less, more preferably 1.0% by weight or less, even more preferably 0.1% by weight or less, and even more preferably 0.01% by weight or less, and one or more divalent elements M in the molded body. 1 (M 1 The total weight (calculated as O) of any one of the molded bodies from Embodiments 1 to 3 is preferably determined according to Reference Example 1.6.

[0090] 5. One or more trivalent elements M contained in the molded body 2 (M 2 Based on the total weight (calculated as 2O3), preferably determined according to Reference Example 1.2, M 2 The molded article contains 10% by weight or less of 2O3, preferably 5% by weight or less, more preferably 1% by weight or less, even more preferably 0.1% by weight or less, and even more preferably 0.01% by weight or less, and one or more divalent elements M 2 (M 2 The total weight (calculated as 2O3) of any one of the molded bodies from Embodiments 1 to 4 is preferably determined according to Reference Example 1.6.

[0091] 6. A molded body according to any one of Embodiments 1 to 5, wherein the mixed metal oxide has a crystallinity of 50-100%, preferably 60-100%, more preferably 70-95%, and even more preferably 80-90%, where the crystallinity is determined according to Reference Example 1.2.

[0092] 7. A molded article of Embodiment 6, wherein 50-100%, preferably 70-100%, more preferably 95-100% of the crystalline phase, determined by XRD and preferably according to Reference Example 1.2, has a spinel structure.

[0093] 8. A molded body according to any one of Embodiments 1 to 7, exhibiting an X-ray diffraction pattern including at least the following reflections.

[0094] [Table 7]

[0095] Here, 100% corresponds to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Example 1.2 and preferably includes at least the following reflections.

[0096] [Table 8]

[0097] 100% relates to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and more preferably includes at least the following reflections.

[0098] [Table 9]

[0099] Here, 100% relates to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2, M 1 is more Mg, and M2 Al is more preferable.

[0100] 9. A molded body according to any one of Embodiments 1 to 8, having an average pore diameter in the range of 0.001 to 0.1 μm, preferably in the range of 0.005 to 0.05 μm, more preferably in the range of 0.02 to 0.04 μm, more preferably in the range of 0.027 to 0.035 μm, and even more preferably in the range of 0.028 to 0.034 μm, wherein the pore diameter distribution is preferably determined according to Reference Example 1.5.

[0101] 10. A molded body according to any one of Embodiments 1 to 9, having a water absorption rate in the range of 10 to 80% by weight, preferably in the range of 30 to 60% by weight, more preferably in the range of 40 to 50% by weight, and even more preferably in the range of 43 to 47% by weight, wherein the water absorption rate is preferably determined according to Reference Example 1.1.

[0102] 11. 20.0~150.0m 2 Range of / g, preferably 30.0 to 90.0 m 2 Range of / g, more preferably 40.0 to 65.0 m 2 The range is / g, more preferably 47.0 to 49.0 m 2 A molded body of any one of Embodiments 1 to 10 having a BET specific surface area in the range of / g, where the BET specific surface area is preferably determined according to Reference Example 1.3.

[0103] 12. A molded body of any one of Embodiments 1 to 11 having a total pore volume in the range of 0.18 to 0.75 ml / g, preferably in the range of 0.25 to 0.60 ml / g, more preferably in the range of 0.33 to 0.53 ml / g, even more preferably in the range of 0.37 to 0.49 ml / g, and more preferably in the range of 0.40 to 0.46 ml / g, where the total pore volume is preferably determined according to Reference Example 1.4.

[0104] 13. One or more additional metals M 3 This includes M 3The element is selected from the group consisting of Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag, Mo, Sn, and mixtures of two or more of these, preferably selected from the group consisting of Fe, Ru, and mixtures of two or more of these, and one or more metal M 3 A molded body according to any one of embodiments 1 to 12, more preferably supported on a mixed metal oxide.

[0105] 14. One or more divalent elements M contained in the molded body 1 (M 1 (calculated as O) and one or more trivalent elements M 2 (M 2 Based on the total weight (calculated as 2O3), one or more metals M are calculated as elements, making up 20% by weight or less, preferably 10% by weight or less, and more preferably 5% by weight or less. 3 The molded body contains one or more divalent elements M 1 (M 1 (calculated as O) and one or more trivalent elements M 2 (M 2 The total weight (calculated as 2O3) of the molded body of Embodiment 13 is preferably determined according to Reference Example 1.6.

[0106] 15. One or more metals M 3 A molded body of embodiment 13 or 14, wherein the substance is uniformly dispersed throughout the entire molded body.

[0107] 16. 85-100% by weight of the molded body, preferably 90-100% by weight, more preferably 95-100% by weight, even more preferably 98-100% by weight, more preferably 99-100% by weight, and even more preferably 99.9-100% by weight, M 1 M 2 , O, H, and any one or more metals M 3 A molded body comprising any one of embodiments 1 to 15.

[0108] 17. A molded body according to any one of Embodiments 1 to 16, wherein 85 to 100% by weight, preferably 90 to 100% by weight, more preferably 95 to 100% by weight, even more preferably 98 to 100% by weight, more preferably 99 to 100% by weight, and even more preferably 99.9 to 100% by weight of the molded body consists of a mixed metal oxide and any one or more metals M3.

[0109] 18. A molded body according to any one of Embodiments 1 to 17, which is an extruded body, a tablet, or granules.

[0110] 19. The extruded body or tablet having a cross-section that is circular, hexagonal, rectangular, quadratic, triangular, elliptical, star-shaped, or cloverleaf-shaped, preferably circular, hexagonal, rectangular, square, triangular, elliptical, star-shaped with 3, 4, 5, 6, 7, or 8 points, trefoil, tetrafoil, or hexafoil, more preferably circular, hexagonal, rectangular, square, triangular, elliptical, star-shaped with 3 or 4 points, trefoil, tetrafoil, or hexafoil, the molded body of Embodiment 18.

[0111] 20. A molded body according to any one of Embodiments 1 to 19, which is a tablet having a cross-section, the cross-section being four-leaf shaped.

[0112] 21. The molded body of Embodiment 20, wherein the tablet has a thickness, which is in the range of 2.0 to 13.0 mm, preferably in the range of 5.0 to 10.0 mm, and more preferably in the range of 6.5 to 9.0 mm.

[0113] 22. A molded body of Embodiment 20 or 21, wherein the tablet has a diameter D in the range of 5 to 20 mm, preferably in the range of 7 to 17 mm, more preferably in the range of 9 to 15 mm.

[0114] 23. A molded body according to any one of embodiments 1 to 19, which is a tablet having a cross-section, the cross-section being hexa-lobed.

[0115] 24. The molded body of Embodiment 23, wherein the tablet has a thickness, which is in the range of 2.0 to 15.0 mm, preferably in the range of 5.0 to 12.0 mm, and more preferably in the range of 8.0 to 9.0 mm.

[0116] 25. A molded body of Embodiment 23 or 24, wherein the tablet has a diameter D in the range of 5 to 25 mm, preferably in the range of 12 to 19 mm, and more preferably in the range of 14 to 17 mm.

[0117] 26. A method for manufacturing a molded article, preferably a method for manufacturing a molded article according to any one of Embodiments 1 to 25, the method comprising: (i) M 1 O and M 2 A process of providing one or more sources of 2O3, M 1 represents one or more divalent elements, M 2 This is a process that represents one or more trivalent elements; (ii) A process of forming one or more supply sources obtained in process (i); (iii) A step of firing the molded body obtained in step (ii) in a gas atmosphere; (iv) A step of treating the molded body obtained in step (iii) with acid; (v) A step of firing the molded body obtained in step (iv) in a gas atmosphere.

[0118] 27. M 1 The elements are selected from groups 2, 10, 11, and 12 of the periodic table, where M 1 It is preferably selected from the group consisting of Mg, Ni, Cu, Zn, Mn, Co, and mixtures of two or more thereof, more preferably selected from the group consisting of Mg, Ni, Cu, Zn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Mg, Zn, Cu, and mixtures thereof, and even more preferably selected from the group consisting of Mg, Zn, and mixtures thereof, M 1 The method of Embodiment 26, wherein is more preferably Mg.

[0119] 28. M 2The elements are selected from groups 5, 6, 7, 8 and 13 of the periodic table, where M 2 It is preferably selected from the group consisting of Al, Cr, Fe, V, Mn, Co, and mixtures of two or more thereof, more preferably selected from the group consisting of Al, Cr, Fe, V, Mn, and mixtures of two or more thereof, even more preferably selected from the group consisting of Al, Cr, V, Mn, and mixtures of two or more thereof, and even more preferably selected from the group consisting of Al, Cr, and mixtures of two or more thereof, M 2 The method of embodiment 26 or 27, wherein is more preferably Al.

[0120] 29. M 1 and M 2 One or more sources of 2O3 are M 1 Oxides, M 1 Hydroxides, M 1 carbonate, M 1 bicarbonate, M 1 Hydroxy carbonate, M 2 Oxides, M 2 Hydroxides, M 2 carbonate, M 2 bicarbonate, M 2 Hydroxy carbonate, M 1 and M 2 Mixed metal oxides, M 1 and M 2 A process which preferably comprises, and more preferably consists of, one of the embodiments 26 to 28, one of the compounds selected from the group consisting of mixed metal hydroxycarbonates and mixtures thereof.

[0121] 30. M 1 O and M 2 One or more sources of 2O3 are M 1 and M 2 Mixed metal oxides, M 1 and M 2 A method from any one of embodiments 26 to 29, which preferably comprises, and more preferably consists of, one or more compounds selected from the group consisting of mixed metal hydroxycarbonates and mixtures thereof.

[0122] 31. M 1 O and M 2 One or more sources of 2O3 are M 1 and M 2 Any one of Embodiments 1 to 30, wherein the molar ratio of is preferably in the range of 1:5 to 5:1.0, more preferably in the range of 1:2.5 to 2.5:1, even more preferably in the range of 1:2 to 2:1, and more preferably in the range of 1:2.1 to 1:1.9.

[0123] 32. M 1 O and M 2 One or more sources of 2O3 are M 1 O and M 2 M contained in one or more sources of 2O3 1 (M 1 (calculated as O) and M 2 (M 2 Based on the total weight (calculated as 2O3), 22-34% by weight, preferably 25-31% by weight, more preferably 27-29% by weight of M 1 (M 1 Any one of the methods from Embodiments 1 to 31, including (calculated as O).

[0124] 33. M 1 O and M 2 One or more sources of 2O3 are M 1 O and M 2 M contained in one or more sources of 2O3 1 (M 1 (calculated as O) and M 2 (M 2 Based on the total weight (calculated as 2O3), 66-78% by weight, preferably 69-75% by weight, more preferably 71-73% by weight of M 2 (M 2 Any one of the methods from Embodiments 1 to 32, including (calculated as 2O3).

[0125] 34. The molding of the mixture of (ii) is carried out by any one of the methods of Embodiments 26 to 33, including tableting or extrusion.

[0126] 35. The firing of (iii) is carried out at a temperature in the range of 300 to 1200°C, preferably in the range of 700 to 1100°C, more preferably in the range of 900 to 1000°C, according to any one of the embodiments 26 to 34.

[0127] 36. The firing of (iii) is carried out in any one of the methods of Embodiments 26 to 35, in which case the firing is carried out for a range of 0.1 to 48 hours, preferably in the range of 0.5 to 24 hours, and more preferably in the range of 1 to 5 hours.

[0128] 37. Any one of Embodiments 26 to 36, wherein the gas atmosphere in (iii) preferably contains one or more oxygen and nitrogen, preferably consists of them, and preferably is air.

[0129] 38. Any one of embodiments 26 to 37, wherein the molded article obtained from (iii) exhibits an X-ray diffraction pattern including at least the following reflections.

[0130] [Table 10]

[0131] Here, 100% relates to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and preferably includes at least the following reflections.

[0132] [Table 11]

[0133] Here, 100% relates to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2 and more preferably includes at least the following reflections.

[0134] [Table 12]

[0135] Here, 100% relates to the intensity of the maximum peak in the X-ray powder diffraction pattern, which is preferably determined according to Reference Example 1.2, M 1 is more Mg, and M 2 Al is more preferable.

[0136] 39. A method of any one of embodiments 26 to 38, wherein the molded article obtained from (iii) has a water absorption rate in the range of 25 to 50% by weight, preferably in the range of 37 to 47% by weight, more preferably in the range of 40 to 44% by weight, the water absorption rate is preferably determined according to Reference Example 1.1.

[0137] 40. The molded body obtained in (iii) is 40.0~60.0m 2 Range of / g, preferably 47.0 to 53.0 m 2 Range of / g, more preferably 49.0 to 51.0 m 2 A method from any one of Embodiments 26 to 39, having a BET specific surface area in the range of / g, wherein the BET specific surface area is preferably determined according to Reference Example 1.3.

[0138] 41. Any one of Embodiments 26 to 40, wherein the molded article obtained in (iii) has a total pore volume in the range of 0.20 to 0.55 ml / g, preferably in the range of 0.30 to 0.42 ml / g, and more preferably in the range of 0.33 to 0.39 ml / g, the total pore volume being preferably determined according to Reference Example 1.4.

[0139] 42. Any one of embodiments 26 to 41, wherein the process of (iv) includes immersing the molded body in acid.

[0140] 43. Any one of Embodiments 26 to 42, wherein the process of (iv) is carried out over a period of 20 to 100 minutes, preferably 45 to 75 minutes, and more preferably 55 to 65 minutes.

[0141] 44. Any one of embodiments 26 to 43, wherein the process of (iv) is carried out at a temperature in the range of 0 to 50°C, preferably in the range of 10 to 40°C, more preferably in the range of 15 to 35°C.

[0142] 45. Any one of embodiments 26 to 44, wherein the acid in (iv) is an aqueous acid.

[0143] 46. ​​The method of Embodiment 45, wherein the aqueous acid has an acid-to-water weight ratio in the range of 1:1 to 1:10, preferably in the range of 1:3 to 1:5, and more preferably in the range of 1:3.9 to 1:4.1.

[0144] 47. The method of Embodiment 45 or 46, wherein the aqueous acid has an acid concentration in water in the range of 2.5 to 4.5 mol / l, preferably in the range of 3.2 to 3.7 mol / l, and more preferably in the range of 3.3 to 3.6 mol / l.

[0145] 48. The acid in (iv) preferably comprises one or more inorganic and organic acids, more preferably consisting of them, and more preferably being one or more of HNO3, HCl, H2SO4, H3PO4, formic acid, oxalic acid, and acetic acid, and even more preferably being HNO3, any one of the methods of Embodiments 26 to 47.

[0146] 49. Any one of the embodiments 26 to 48, further comprising the following, after (iv) and before (v): Wash the molded body obtained in (w)(iv) with deionized water.

[0147] 50. After (iv) and before (v), preferably after (w) and before (v), any one of the methods of Embodiments 26 to 49, further comprising: (d) Dry the molded body obtained from (iv) or (w) in a gas atmosphere.

[0148] 51. The drying of (d) is carried out at a temperature in the range of 80 to 160°C, preferably in the range of 100 to 140°C, more preferably in the range of 110 to 130°C, according to the method of Embodiment 50.

[0149] 52. The drying of (d) is carried out over a period of 0.5 to 16 hours, preferably 2 to 12 hours, and more preferably 3 to 8 hours, according to the method of Embodiment 50 or 51.

[0150] 53. The gas atmosphere in (d) preferably contains one or more oxygen and nitrogen, more preferably consists of them, and even more preferably is air, according to any one of Embodiments 50 to 52.

[0151] 54. The firing of (v) is carried out at a temperature in the range of 400 to 1000°C, preferably in the range of 600 to 950°C, and more preferably in the range of 825 to 875°C, according to any one of the methods of Embodiments 26 to 53.

[0152] 55. The firing of (v) is carried out over a period of 0.1 to 1.5 hours, preferably 0.3 to 0.7 hours, and more preferably 0.4 to 0.6 hours, in any one of the methods of Embodiments 26 to 54.

[0153] 56. The gas atmosphere in (v) is preferably composed of one or more oxygen and nitrogen, and more preferably air, according to any one of embodiments 26 to 55.

[0154] 57. Any one of the embodiments 26 to 56, further including the following after (v): (vi) One or more metal Ms. 3 To carry, Here, loading is preferably carried out by impregnation, more preferably by wet impregnation, and even more preferably by incipient wet impregnation, where M 3The element is selected from the group consisting of Fe, Ru, Os, Co, Rh, Ir, Pd, Pt, Cu, Ag, Mo, Sn, and mixtures of two or more of these, and is preferably selected from the group consisting of Fe, Ru, and mixtures of two or more of these.

[0155] 58. A molded article, preferably a molded article according to any one of Embodiments 1 to 57, wherein the molded article can be obtained or has been obtained by a method according to any one of Embodiments 26 to 57.

[0156] 59. Use of any one of the molded bodies from Embodiments 1 to 25 and 58 as a catalyst or catalyst support. [Examples]

[0157] The present invention is further illustrated by the following examples, comparative examples, and reference examples.

[0158] Reference example 1: Measurement method Reference Example 1.1: Measurement of Water Absorption Rate A dried molded body was placed in water so that it was completely submerged. The molded body was left in the water for 60 minutes. After that, the outer surface of the molded body was dried and its weight was measured. The water uptake (percentage by weight) was calculated according to Equation I.

[0159] Water absorption rate = (Weight of wet molded body - Weight of dry molded body) / Weight of dry molded body (I)

[0160] Reference Example 1.2: X-ray powder diffraction and determination of crystallinity Powder X-ray diffraction (PXRD) data were collected using a diffractometer (D8 Advance Series II, Bruker AXS GmbH) equipped with a LYNXEYE detector operated by a copper anode X-ray tube running at 40 kV and 40 mA. The geometry was Bragg-Brentano, and air scattering was reduced using an air scattering shield.

[0161] Crystallinity Calculation: The crystallinity of the sample was determined using the DIFFRAC.EVA software provided by Bruker AXS GmbH (Karlsruhe), following the method described on page 121 of the user manual. Default parameters were used for the calculation.

[0162] Phase composition calculation: Phase composition was calculated for the raw data using the modeling software DIFFRAC.TOPAS provided by Bruker AXS GmbH (DIFFRAC.TOPAS version 6 user manual, 2017, Bruker AXS GmbH, Karlsruhe). Diffraction patterns were simulated using the crystal structure of the identified phases, instrument parameters, and crystallite sizes of the individual phases. This was fitted to the data, in addition to a function that models the background intensity.

[0163] Data Acquisition: Samples were homogenized in a mortar and pressed into a standard flat sample holder provided by Bruker AXS GmbH for Bragg-Brentano geometry data acquisition. A flat surface was obtained by using a glass plate to compress and flatten the sample powder. Data were collected from the angular range of 2 to 70°²Theta with a step size of 0.02°²Theta, while setting a variable divergence slit to an angle of 0.1°. Crystalline content represents the intensity of the crystalline signal relative to the total scattering intensity.

[0164] Reference Example 1.3: Measurement of BET specific surface area The BET specific surface area was determined by nitrogen physicoadsorption at 77 K according to the method disclosed in DIN 66131.

[0165] Reference Example 1.4: Measurement of Total Pore Volume The total pore volume was determined by mercury intrusion porosimetry in accordance with DIN 66133. For this purpose, a MicroActive AutoPore V 9600 was used.

[0166] Reference Example 1.5: Measurement of Pore Size Distribution The pore size distribution was determined by mercury intrusion porosimetry according to DIN 66133. A MicroActive AutoPore V 9600 was used for this purpose.

[0167] Reference example 1.6: Elemental analysis Elemental analysis was performed according to ICP-OES and DIN ISO 17025.

[0168] Pural Mg 30 (containing Mg (calculated as MgO) and Al (calculated as Al2O3) in a weight ratio of 30:70) quadrilobes were calcined in air at 950°C for 3 hours. The calcined quadrilobes were treated with nitric acid as follows. The calcined quadrilobes were placed in a glass beaker and then filled with an HNO3-containing aqueous solution (concentration 20% by weight, equivalent to 3.3 mol / l). All tablets were completely covered with the acidic solution described above. After 60 minutes, the acidic solution was removed and the resulting quadrilobes were washed with demineralized water. The quadrilobes were dried at 120°C for 4 hours (heating rate 5°C / min). After the drying process, a calcination process to remove residual nitrates was carried out at 850°C for 0.5 hours (heating rate 5°C / min). The properties of the molded bodies before and after acid treatment are shown in Table 1 below.

[0169] [Table 13] [Brief explanation of the drawing]

[0170] [Figure 1] The powder XRD of the molded body sample from Example 1 before acid treatment is shown. In addition to the MgAl2O4 spinel phase, the presence of the MgO periclase phase is also shown. [Figure 2] The powder XRD of the molded sample from Example 1 after acid treatment is shown. It shows that the MgAl2O4 spinel phase is present, but the MgO periclase phase is not. [Figure 3]Figure 3A shows a cross-section of an impregnated sample molded body that was not treated according to the present invention, and Figure 3B shows a cross-section of a sample molded body that was treated according to the present invention. [Figure 4] The pore size distribution of the molded article according to Example 1 of the present invention before and after HNO3 treatment is shown. The pore diameter is shown on the horizontal axis on a logarithmic scale in μm, and the relative differential intrusion volume is shown on the vertical axis.

Claims

1. Composition formula M １ M ２ ２ O ４ A molded article comprising a mixed metal oxide having M １ is one or more divalent elements M １ Includes M ２ is one or more trivalent elements M ２ A molded body comprising a mixed metal oxide having a crystalline phase having a spinel structure, wherein the molded body has a total pore volume in the range of 0.10 to 0.90 ml / g.

2. M １ The molded body according to claim 1, which is selected from Group 2, Group 10, Group 11, and Group 12 of the periodic table of the elements.

3. M ２ The molded article according to claim 1 or 2, wherein is selected from Group 5, Group 6, Group 7, Group 8 and Group 13 of the periodic table.

4. One or more divalent elements M are contained in the molded body. １ to M １ Based on the total weight calculated as O, M must be 1.0% by weight or less. １ A molded article according to claim 1 or 2, comprising O.

5. One or more trivalent elements M are contained in the molded body. ２ to M ２ ２ O ３ Based on the total weight calculated as follows, M is less than 1% by weight. ２ ２ O ３ A molded article according to claim 1 or 2, comprising:

6. A molded article according to claim 1 or 2, having an average pore diameter in the range of 0.001 to 0.1 μm.

7. A molded article according to claim 1 or 2, having a water absorption rate in the range of 10 to 80% by weight.

8. One or more metals M ３ This also includes 20.0 to 150.0 m ２ A molded article according to claim 1 or 2, having a BET specific surface area in the range of / g.

9. 85-100% by weight of the molded body is M １ M ２ , O, H, and any one or more metals M ３ A molded article according to claim 1 or 2, comprising the above.

10. The molded article according to claim 1 or 2, which is an extruded article, a tablet, or granules.

11. The molded article according to claim 10, wherein the extruded article or tablet has a cross-section, the cross-section being circular, hexagonal, rectangular, square, triangular, elliptical, star-shaped polygon, or cloverleaf-shaped.

12. (i) M １ O and M ２ ２ O ３ A process of providing one or more sources of M １ represents one or more divalent elements, M ２ A process that represents one or more trivalent elements; (ii) A step of forming one or more supply sources obtained in step (i); (iii) A step of firing the molded body obtained in step (ii) in a gas atmosphere; (iv) A step of treating the molded body obtained in step (iii) with acid; A method for producing a molded article, comprising the step of firing the molded article obtained in step (iv) in a gas atmosphere.

13. M １ O and M ２ ２ O ３ One or more sources of M １ Oxides, M １ Hydroxides, M １ carbonate, M １ bicarbonate, M １ Hydroxy carbonate, M ２ Oxides, M ２ Hydroxides, M ２ carbonate, M ２ bicarbonate, M ２ Hydroxy carbonate, M １ and M ２ Mixed metal oxides, M １ and M ２ The method according to claim 12, comprising one or more compounds selected from the group consisting of mixed metal hydroxycarbonates and mixtures thereof.

14. A molded article that can be obtained by the method of claim 12, or obtained by a molded article.

15. Use of the molded article according to claim 1 or 14 as a catalyst or catalyst support.

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