Solid shaped body and use of solid shaped body
By designing a cylindrical solid molded body with a specific geometric structure, the problem of single optimization of catalyst performance in the prior art is solved, the balance of multiple performance indicators is achieved, and the efficiency of hydrocarbon reforming into synthesis gas is improved.
Patent Information
- Application Number
- CN202180059036.5
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Priority Date
- 2020-07-29
- Filing Date
- 2021-07-23
- Publication Date
- 2025-08-08
- Estimated Expiration
- 2041-07-23
AI Technical Summary
When performing performance optimization, existing catalyst solid molded bodies usually focus only on a single performance indicator, such as pressure drop or surface area, and ignore other performance indicators, resulting in the inability to achieve a balance between multiple performance indicators during hydrocarbon reforming.
A cylindrical solid molded body is designed with a specific geometric structure, including cross-sectional areas in the form of rholoid, including grooves and openings, optimizing mechanical strength, pressure drop, filler bed density, bed mass diffusion coefficient, heat transfer and mass transfer properties.
The balance between catalyst performance indicators is achieved, and the overall efficiency and stability of the catalyst is improved, especially during the process of hydrocarbon reforming into synthesis gas, and the generation efficiency of hydrogen and carbon monoxide is improved.
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Figure CN116133750B_ABST
Abstract
Description
[0001] The present invention relates to a solid shaped body having a cylindrical form, the cylindrical form comprising a first base region, a second base region, and a side region, wherein the solid shaped body comprises a first number of grooves in the side region, each extending from the first base region to the second base region, and a second number of openings, each extending from the first base region to the second base region. The present invention further relates to the use of the solid shaped body as a catalyst.
[0002] The performance of solid shaped bodies, especially when used as catalysts, depends largely on their shape and, therefore, their geometry. Mechanical strength, pressure drop, packed bed density, and bed mass diffusion coefficient are examples of performance indicators. Other important parameters are the weight, specific surface area, and heat and mass transfer properties of the individual solid shaped bodies.
[0003] Solid shaped bodies are used, for example, for the reforming of hydrocarbons to give synthesis gas, in which case catalysts based on Ni- or Co-containing oxides can be used.
[0004] WO 2013 / 118078 A1 relates to a catalyst comprising hexaaluminates for hydrocarbon reforming and a reforming process. The catalyst is prepared as blocks, sheets or strands.
[0005] EP 2 323 762 B1 describes shaped hydrogenous catalyst bodies having an equal number of pores and grooves.
[0006] DE 27 19 543 A1 discloses ceramic bodies for bonding catalysts, wherein a cylindrical body with a circular outer circumference is exemplified.
[0007] DE 39 35 073 A1 discloses a process for the catalytic dehydrogenation of hydrocarbons, using a catalyst body in the form of a gear with rectangular cocks.
[0008] WO 2007 / 051602 A1 relates to a shaped catalyst body for preparing maleic anhydride, which proposes a shaped catalyst body in the form of a prism having two triangular faces.
[0009] WO 2020 / 120078 A1 relates to a catalytic system comprising a tubular reactor and at least one catalyst particle located within the tubular reactor. The relationship between the form of the catalyst particle and the form of the tubular reactor is considered to improve heat transfer conditions.
[0010] US 4,441,990 is directed to cross-sectional shapes such as rectangular and triangular tubes for forming catalyst extrudates useful in hydrocarbon processing operations.
[0011] DE 31 41 942 A1 relates to shaped catalyst bodies in the form of cylinders having a specific circumference, wherein the convexities are wider than the concavities.
[0012] WO 2010 / 029324 A1 relates to a catalyst unit comprising a cylindrical body exhibiting five holes arranged in a pentagonal pattern and five riffles.
[0013] WO 2006 / 114320 A1 describes a cylindrical catalyst element, wherein embossing is provided on the peripheral surface of the catalyst element.
[0014] Typically, the geometry of a solid shaped catalyst body is optimized for only one performance characteristic, such as pressure drop or surface area, while other performance characteristics are ignored. One object of the present invention is to provide a solid shaped body that achieves an improvement in at least one performance characteristic while exhibiting good performance in the remaining performance characteristics. Therefore, the solid shaped body should provide a targeted compromise between various performance characteristics, including pressure drop, surface area, mechanical strength, weight of a single shaped body, packed bed density, specific surface area of the packed bed, heat transfer properties, and mass transfer properties.
[0015] This object is achieved by a solid shaped body having a cylindrical form, the cylindrical form having a first base region, a second base region and a side region, wherein the solid shaped body comprises a first number of grooves with at least one groove radius in the side region, each extending from the first base region to the second base region, and a second number of openings, each extending from the first base region to the second base region, wherein the solid shaped body has a cross-sectional area in the form of a rholoid.
[0016] The term rholoid is understood to mean, when viewed in two dimensions, the intersecting planes formed by three superimposed circles. A rholoid comprises three sides, particularly three curved sides, and three corners. Preferably, the lengths of each of the three sides differ from the arithmetic mean of the lengths of the three sides by less than 30%, more preferably by less than 10%, and most preferably by less than 5%, based on the arithmetic mean. In particular, the centers of the superimposed circles are equidistant from the adjacent centers, thereby forming an isosceles triangle. When viewed in three dimensions, the rholoid body is formed by the intersection of three cylinders corresponding to the three superimposed circles.
[0017] The rholoid forms the basic shape of the cylindrical cross-sectional area of the solid shaped body, wherein the first base area and the second base area are preferably arranged parallel to each other, especially in the case of a flat base area, and / or as mirror images, especially in the case of a curved or arched base area. The first base area and the second base area are preferably connected by a side area. The side area contains a first number of grooves, so that the rholoid perimeter of the cross-sectional area of the shaped body is interrupted by grooves, which can also be called grooves or embossings.
[0018] The solid shaped body further comprises a second number of openings, also referred to as pores, extending through the solid shaped body from the first base region to the second base region. The first number comprises grooves, and the second number comprises openings. In contrast to the openings, which are completely surrounded by the shaped body in a cross-sectional view, the grooves are located only at the outer periphery of the solid shaped body and are recessed portions of the shaped body's periphery.
[0019] Preferably, the longitudinal axes, more preferably the central axes, of the solid shaped body, the recess and / or the opening are arranged parallel to one another. The term "parallel" is understood to mean that the longitudinal axes, more preferably the central axes, of the solid shaped body, the recess and / or the opening each enclose an angle of less than 20°, preferably less than 10°, more preferably less than 5°, and most preferably less than 2°.
[0020] Preferably, the shaped body comprises 2 to 8, more preferably 3 to 7, in particular 3, openings.
[0021] The solid shaped body preferably comprises more grooves than openings. More preferably, the difference between the first number of grooves and the second number of openings is at least 2, most preferably 3. In a particularly preferred embodiment, the ratio between the first number of grooves and the second number of openings is 2. Preferably, the at least one groove has a radius in the range of 0.8 mm to 5.0 mm, more preferably 1.4 mm to 5.0 mm.
[0022] Preferably, at least one opening has a second radius, more preferably all openings have a second radius, and the ratio between the radius of the at least one groove and the second radius of the at least one opening is preferably in the range of 0.2 to 5.0. Preferably, the ratio between the radius of the at least one groove and the diameter of the solid shaped body is in the range of 0.05 to 0.50, more preferably 0.10 to 0.30.
[0023] Preferably, the first number of grooves comprises a third number of first grooves having a third radius and a fourth number of second grooves having a fourth radius, wherein the third radius is less than the fourth radius. More preferably, the first number is the sum of the third number and the fourth number. Most preferably, the third number of first grooves is equal to the fourth number of second grooves. In a preferred embodiment, the solid molded body comprises 6 grooves, which comprise 3 first grooves and 3 second grooves, and further preferably, the solid molded body comprises 3 openings. In particular, each of the first grooves has the third radius, and / or each of the second grooves has the fourth radius. The first grooves and the second grooves are preferably arranged in an alternating manner.
[0024] The ratio between the third radius of the first groove and the second radius of the at least one opening is preferably in the range of 0.2 to 3.0, more preferably 0.5 to 1.5. Most preferably, the third radius of the first groove is equal to the second radius of the at least one opening. The ratio between the fourth radius of the second groove and the second radius of the at least one opening is preferably in the range of 0.3 to 5.0, more preferably 1.5 to 3.0, and most preferably 1.8 to 2.5.
[0025] It is further preferred that the ratio of the third radius of the first groove to the diameter of the solid shaped body is in the range of 0.05 to 0.45, more preferably 0.05 to 0.15, and / or the ratio of the fourth radius of the second groove to the diameter of the solid shaped body is in the range of 0.075 to 0.50, more preferably 0.20 to 0.30. The ratio between the third radius and the fourth radius is preferably in the range of 0.3 to 0.6.
[0026] Preferably, the third radius is in the range of 0.8 mm to 5.0 mm, more preferably 1.4 mm to 2.5 mm, and / or the fourth radius is in the range of 1.2 mm to 5.0 mm, more preferably 3.2 mm to 5.0 mm.
[0027] Further, each opening includes a first center. The center is understood to be a geometric center. The first center of one of the openings may be located on the central axis of the solid formed body. Preferably, at least one first center of the opening, more preferably all first centers of all openings are arranged in the solid formed body with a first distance from the central axis of the solid formed body. The ratio between the first distance from the central axis of the solid formed body to at least one first center of the opening, particularly to all first centers of all openings and the diameter of the solid formed body is preferably in the range of 0.00 to 0.40, more preferably in the range of 0.15 to 0.25. From the central axis of the solid formed body to the at least one first center, particularly to all first centers of all openings, the first distance is preferably in the range of 2.4mm to 9.0mm, more preferably in the range of 2.5mm to 4.0mm. Most preferably, the first distances of all openings are equal.
[0028] Thus, the second number of openings may include a central opening extending along the central axis of the solid shaped body, and at least one peripheral opening, wherein the second number of openings is preferably the sum of the number of peripheral openings and the number of central openings. The periphery of the at least one peripheral opening is still completely contained within and surrounded by the solid shaped body.
[0029] Each opening preferably has a circular cross-section.More preferably, the openings are arranged equidistant from adjacent peripheral openings and equidistant from a central axis of the solid shaped body - with reference to a first center of the opening.
[0030] Preferably, the ratio between the second radius of the at least one opening and the diameter of the solid shaped body is in the range of 0.01 to 0.50, more preferably 0.05 to 0.20. More preferably, the second radius is in the range of 0.1 mm to 5.0 mm, even more preferably 1.4 to 2.5 mm. In particular, the second radius of all openings is equal.
[0031] Preferably, the third number of first grooves and the fourth number of second grooves are equal to the second number of openings. More preferably, each opening is arranged between two second grooves. Accordingly, the opening and the second groove are preferably arranged in separate segments of the cross section of the solid molded body. An opening and a first groove are preferably arranged in the same segment of the cross section of the solid molded body. The segment in which the opening and the first groove are arranged can also be referred to as a leaf. Preferably, a leaf is arranged between two second grooves, and a second groove is arranged between two leaves. Accordingly, the second grooves and the leaves are preferably arranged in an alternating manner on the periphery of the solid molded body and therefore on the side areas. In addition, each leaf preferably includes a first groove.
[0032] The first grooves are preferably arranged equidistantly with respect to adjacent grooves and with respect to the central axis of the solid shaped body, and / or the second grooves are preferably arranged equidistantly with respect to adjacent grooves and with respect to the central axis of the solid shaped body.
[0033] Each of the first grooves has a second center of its imaginary, preferably circular, cross-sectional area, and each of the second grooves has a third center of its imaginary, preferably circular, cross-sectional area. The second center and the third center may each be located outside the solid body. Preferably, at least one second center of the first groove, at least one first center of the opening, and a point on the central axis of the solid body form a line.
[0034] The ratio of the second distance from the central axis of the solid shaped body to the second center of the at least one first recess to the diameter of the solid shaped body is preferably in the range of 0.3 to 0.8, more preferably in the range of 0.4 to 0.6, for example 0.5. The second distance between the second center of the at least one first recess and the central axis of the solid shaped body is preferably in the range of 4 mm to 15 mm, more preferably in the range of 7 mm to 12 mm.
[0035] The ratio of the third distance from the central axis of the solid shaped body to the third center of the at least one second groove to the diameter of the solid shaped body is preferably in the range of 0.3 to 0.8, more preferably in the range of 0.4 to 0.6, for example 0.5. The third distance between the third center of the at least one second groove and the central axis of the solid shaped body is preferably in the range of 4 mm to 15 mm, more preferably in the range of 7 mm to 12 mm.
[0036] Preferably, the second distances of all first grooves are equal, and / or the third distances of all second grooves are equal. More preferably, the second distance is equal to the third distance.
[0037] Preferably, the ratio between the diameter of the solid shaped body and the height of the solid shaped body is in the range of 0.5 to 4.0, more preferably 1.5 to 2.5. The diameter of a solid shaped body having a cross-sectional area in the form of a rholoid is preferably the diameter of an embracing circle containing the three corners of the rholoid. Furthermore, the height of the solid shaped body is preferably understood to be the maximum distance between the first base area and the second base area measured perpendicular to the base area.
[0038] Preferably, the diameter of the solid shaped body is in the range of 8 mm to 25 mm, more preferably 10 mm to 22 mm, most preferably 14 mm to 20 mm. The height of the solid shaped body is preferably in the range of 4.0 mm to 12.5 mm, more preferably 7.0 mm to 12.0 mm.
[0039] The first base area and / or the second base area of the solid molded body are preferably arched. More preferably, the first base area and the second base area are arched. In particular, the ratio between the arch height and the diameter of the solid molded body relative to the first base area and / or the second base area is in the range of 0.01 to 0.40, more preferably in the range of 0.05 to 0.10. The arch height is preferably in the range of 0.2mm to 4.0mm, more preferably in the range of 0.8mm to 2.0mm. The arch is understood to be the top and bottom of the solid molded body, respectively, wherein its surface is curved in two directions. Accordingly, the arch and therefore the arch height end where the side area is curved only in one direction (which is with reference to the radial direction of the solid molded body).
[0040] The present invention further relates to the use of solid shaped bodies as catalysts, preferably for the reforming of one or more hydrocarbons, preferably in the presence of carbon dioxide, into synthesis gas comprising hydrogen and carbon monoxide, wherein the hydrocarbon is preferably selected from methane, ethane, propane and butane, wherein the hydrocarbon is more preferably methane.
[0041] More preferably, the solid shaped bodies are used in a process for reforming one or more hydrocarbons, preferably methane, into synthesis gas comprising hydrogen and carbon monoxide, the process comprising
[0042] (a) providing a reactor comprising a reaction zone containing the solid shaped body;
[0043] (b) passing a reactant gas stream to the reaction zone obtained from (a), wherein the reactant gas stream passed to the reaction zone comprises the one or more hydrocarbons, carbon dioxide, and water; subjecting the reactant gas stream to reforming conditions in the reaction zone; and withdrawing a product stream from the reaction zone, the product stream comprising hydrogen and carbon monoxide.
[0044] The solid shaped body preferably comprises a mixed oxide. More preferably, the mixed oxide comprises cobalt, or the mixed oxide comprises nickel. Further preferably, the mixed oxide comprises oxygen, aluminum, cobalt, and at least one rare earth metal, such as lanthanum, or the mixed oxide comprises oxygen, aluminum, nickel, and at least one alkaline earth metal, such as magnesium. In particular, the at least one rare earth metal is lanthanum. In particular, the at least one alkaline earth metal is magnesium.
[0045] Preferably, 50% to 100% by weight, more preferably 60% to 100% by weight, even more preferably 70% to 100% by weight, further preferably 80% to 100% by weight, in particular 90% to 100% by weight, particularly preferably 95% to 100% by weight, and most preferably 99% to 100% by weight of the solid shaped body consists of mixed oxides and optionally at least one suitable binder. 99% to 100% by weight, even more preferably 99.5% to 100% by weight, and most preferably 99.9% to 100% by weight of the solid shaped body may also consist of mixed oxides.
[0046] When the mixed oxide contains nickel, the mixed oxide preferably comprises at least a nickel-magnesium mixed oxide and a magnesium spinel, and optionally hydrated aluminum oxide. The nickel-magnesium mixed oxide preferably has an average crystallite size of ≤100 nm, more preferably ≤70 nm, and even more preferably ≤50 nm. The magnesium spinel phase preferably has an average crystallite size of ≤100 nm, more preferably ≤70 nm, and even more preferably ≤50 nm. The proportion of nickel in the mixed oxide is preferably approximately 30 mol%, more preferably in the range of 6 mol% to 30 mol%, the proportion of magnesium is preferably in the range of 8 mol% to 38 mol%, more preferably in the range of 23 mol% to 35 mol%, and the proportion of aluminum is preferably in the range of 50 mol% to 70 mol%. The intensity of the diffraction reflection of the mixed oxide at 43.09°2θ is preferably less than or equal to the intensity of the diffraction reflection at 44.82°2θ, and the intensity of the diffraction reflection at 43.08°2θ is more preferably less than the intensity of the reflection at 44.72°2θ.
[0047] Solid shaped bodies can be produced, for example, as described in EP 3 574 994 A1, in particular when the solid shaped body comprises a nickel-containing mixed oxide.
[0048] In case the mixed oxide comprises cobalt, the weight ratio of cobalt to aluminum in the mixed oxide, calculated as element, is preferably at least 0.17:1.
[0049] There are no particular restrictions on the content of cobalt, lanthanum, and aluminum in the mixed oxide contained in the solid shaped body. Preferably, 6% to 9% by weight, more preferably 6.5% to 8.5% by weight, and most preferably 7% to 8% by weight of the mixed oxide, calculated as an element, consists of cobalt. Furthermore, preferably, 15% to 20% by weight, more preferably 16% to 19% by weight, most preferably 17% to 18% by weight, and in particular 17.5% to 17.8% by weight of the mixed oxide, calculated as an element, consists of lanthanum. Furthermore, preferably, 33% to 40% by weight, more preferably 34% to 38% by weight, most preferably 35% to 37% by weight, and in particular 35.5% to 36.5% by weight of the mixed oxide, calculated as an element, consists of aluminum.
[0050] The cobalt-containing mixed oxide may comprise an amorphous phase, one or more crystalline phases, or an amorphous phase and one or more crystalline phases. Preferably, the mixed oxide comprises one or more crystalline phases, more preferably at least two crystalline phases, and most preferably at least three crystalline phases. Preferably, 80% to 100% by weight of the mixed oxide is in crystalline form, more preferably 90% to 100% by weight, and most preferably 92% to 100% by weight.
[0051] Furthermore, it is preferred that the mixed oxide comprises LaCoAl 11 O 19 The mixed oxide contains one or more of the crystalline phases of LaCoAl and LaAl(Co)O3. 11 O 19 In the case of the crystalline phase and the crystalline phase of LaAl(Co)O3, the LaCoAl 11 O 19 The weight ratio relative to LaAl(Co)O3 is in the range of 5:1 to 30:1, more preferably in the range of 10:1 to 25:1, most preferably in the range of 12:1 to 22:1, in particular in the range of 13:1 to 20:1, for example in the range of 13:1 to 15:1. It is particularly preferred that the mixed oxide contains a further crystalline phase La(OH)3. Furthermore, it is particularly preferred that the mixed oxide contains a further crystalline phase LaAlO3.
[0052] Furthermore, it is preferred that the mixed oxide contains another crystalline phase CoAl2O4. 11 O 19 In the case of the crystalline phase and the crystalline phase CoAl2O4, it is preferred that the LaCoAl 11 O 19 The weight ratio relative to CoAl2O4 is in the range of 8:1 to 35:1, more preferably in the range of 10:1 to 30:1, further preferably in the range of 12:1 to 30:1, in particular in the range of 15:1 to 27:1, most preferably in the range of 17:1 to 25:1, for example in the range of 20:1 to 22:1.
[0053] Preferably, the solid shaped body is a calcined solid shaped body. More preferably, the solid shaped body is a calcined solid shaped body, wherein in the first alternative, calcination has been carried out in a gas atmosphere having a temperature of 350°C to 450°C, preferably 390°C to 410°C. Furthermore, preferably, the gas atmosphere contains oxygen, more preferably one or more of oxygen, air, or lean air. Preferably, calcination is carried out for 2 to 10 hours.
[0054] In the second alternative, it is more preferred that the solid shaped body is a calcined solid shaped body, wherein the calcination has been carried out in a gas atmosphere having a temperature of 1100° C. to 1400° C., more preferably 1175° C. to 1225° C., wherein the gas atmosphere preferably contains oxygen, more preferably one or more of oxygen, air or dilute air. Preferably, the calcination is carried out for 2 hours to 10 hours.
[0055] Solid shaped bodies can be produced, for example, by a process comprising:
[0056] (i) preparing a mixture comprising a lanthanum salt, a cobalt salt, an oxidic aluminum compound, and an acid, wherein one or more of the lanthanum salt and the cobalt salt, preferably both, are not nitrates;
[0057] (ii) preparing a solid shaped body from the mixture obtained in (i), comprising
[0058] (ii.1) subjecting the mixture obtained in (i) to a shaping process to obtain a first solid shaped body;
[0059] (ii.2) drying the first solid shaped body obtained from (ii.1), preferably in a gas atmosphere;
[0060] (ii.3) calcining the first solid shaped body obtained from (ii.1) or (ii.2), preferably from (ii.2), in a gas atmosphere having a temperature of 350° C. to 470° C.;
[0061] (iii) subjecting the calcined first solid shaped body obtained from (ii) to a reshaping process to obtain a second solid shaped body having a geometry different from that of the first solid shaped body;
[0062] (iv) calcining the solid shaped body obtained from (ii) or (iii), preferably from (iii), in a gas atmosphere having a temperature of 1100° C. to 1400° C. to obtain a solid shaped body comprising a mixed oxide.
[0063] Preferably, preparing the mixture according to (i) comprises kneading the mixture.
[0064] Furthermore, it is preferred that, when the reshaping process in (iii) is carried out, the shaping process subjected to the mixture obtained from (i) according to (ii.1) comprises extrusion, more preferably consists of extrusion.
[0065] Regarding the drying according to (ii.2), according to a first alternative, it is preferred that the first solid shaped body is dried in a gas atmosphere, which preferably has a temperature of 50°C to 150°C, more preferably 80°C to 110°C, wherein the gas atmosphere preferably contains oxygen, more preferably one or more of oxygen, air or dilute air, wherein the drying according to (ii.2) is preferably carried out for 5 hours to 25 hours.
[0066] Regarding the drying according to (ii.2), according to the second alternative, it is preferred that the first solid shaped body is dried in a gas atmosphere, which preferably has a temperature of 80°C to 150°C, more preferably 90°C to 140°C, wherein the gas atmosphere preferably contains oxygen, more preferably one or more of oxygen, air or dilute air, wherein the drying according to (ii.2) is preferably carried out for 0.2 hours to 2 hours, wherein the drying is preferably carried out using a belt dryer.
[0067] Regarding the calcination according to (ii.3), according to a first alternative, it is preferred that the first solid shaped body be calcined in a gas atmosphere having a temperature of 350°C to 450°C, more preferably 390°C to 410°C. Furthermore, it is preferred that the gas atmosphere contain oxygen, more preferably one or more of oxygen, air, or dilute air. Furthermore, the calcination according to (ii.3) is preferably carried out for 2 to 10 hours.
[0068] Regarding the calcination according to (ii.3), according to a second alternative, it is preferred that the first solid shaped body is calcined according to (ii.3) in a rotary kiln in a gas atmosphere having a temperature of 350° C. to 450° C., more preferably 390° C. to 410° C. Furthermore, it is preferred that the gas atmosphere contains oxygen, more preferably one or more of oxygen, air, or dilute air. In the case where the first solid shaped body is calcined according to (ii.3) as disclosed herein, the calcination preferably comprises separating carbon dioxide from the gas stream, more preferably using a carbon dioxide scrubber.
[0069] Regarding the reshaping according to (iii), it is preferred that the reshaping according to (iii) comprises crushing the calcined solid shaped body obtained from (ii) and subjecting the resulting crushed material to a reshaping process to obtain a second solid shaped body, wherein the crushing is more preferably performed by milling.
[0070] In the case where the reshaping comprises crushing the calcined solid shaped body obtained in (ii) and subjecting the obtained crushed material to a reshaping process to obtain a second solid shaped body, it is particularly preferred that, after crushing the calcined solid shaped body obtained in (ii) and before subjecting the obtained crushed material to a reshaping process according to (iii), the method further comprises preparing a mixture comprising the crushed material and one or more binders, more preferably one or more of graphite, polysaccharides, sugar alcohols and synthetic polymers, even more preferably one or more of graphite, sugar alcohols, synthetic polymers, cellulose, modified cellulose and starch, most preferably graphite, sugar alcohols, synthetic polymers, microcrystalline cellulose, cellulose ethers, more preferably graphite, sorbitol, mannitol, polyethylene glycol (PEG), polyvinylpyrrolidone (PVP), hydroxypropyl cellulose (HPC) and hydroxypropyl methylcellulose (HPMC). In this respect, it is preferred according to a first alternative that in the mixture, the weight ratio of the one or more binders relative to the crushed material is preferably in the range of 1:10 to 1:20, more preferably in the range of 1:12 to 1:18, and even more preferably in the range of 1:13 to 1:17. According to a second alternative, it is preferred that in the mixture, the weight of the one or more binders, calculated relative to the total weight of the mixture, is in the range of 0.5% to 10% by weight, more preferably in the range of 2% to 9% by weight, even more preferably in the range of 4% to 8% by weight, and most preferably in the range of 5% to 7% by weight.
[0071] Furthermore, in the case where the reshaping comprises crushing the calcined solid shaped body obtained in (ii) and subjecting the resulting crushed material to a reshaping process to obtain a second solid shaped body, it is preferred that, after crushing the calcined solid shaped body obtained in (ii) and before the reshaping process according to (iii), the method further comprises separating the particles of the crushed material into two or more fractions according to their size. Preferably, the reshaping process is applied to those fractions of particles having the smallest size, preferably to the fraction of particles having the smallest size. Preferably, the particles having the smallest size have a maximum diameter of 2.0 mm, more preferably a maximum diameter of 1.5 mm, and even more preferably a maximum diameter of 1.0 mm. Fractions having smaller maximum sizes, such as 0.75 mm or 0.5 mm, are generally conceivable.
[0072] In the case of separating one or more particle fractions without a minimum size, it is particularly preferred to crush the one or more fractions again to separate the particle fractions with the minimum size, preferably the particle fraction with the minimum size, for the reshaping process according to (iii). According to the above, it is preferred that the particles with the minimum size have a maximum diameter of 2.0 mm, more preferably a maximum diameter of 1.5 mm, and even more preferably a maximum diameter of 1.0 mm, whereby fractions with smaller maximum sizes, such as 0.75 mm or 0.5 mm, are also conceivable.
[0073] In case the reshaping comprises crushing the calcined solid shaped body obtained from (ii) and subjecting the obtained crushed material to a reshaping process to obtain a second solid shaped body, before the reshaping process according to (iii), the process further comprises separating the particles of the crushed material into two or more fractions according to their size, the process preferably further comprises recycling at least a part of the particles of said one or more fractions not having a minimum size to step (i) of the process, which comprises preparing a mixture according to (i), which comprises a lanthanum salt, a cobalt salt, an aluminum oxide compound, an acid, more preferably water, and at least said part of said fractions.
[0074] Furthermore, it is particularly preferred that 65% to 95% by weight, more preferably 75% to 95% by weight, even more preferably 85% to 95% by weight of the mixture prepared in (i) consists of the lanthanum salt, the cobalt salt, the aluminum oxide compound, the acid, more preferably water, and that 5% to 35% by weight, more preferably 5% to 25% by weight, even more preferably 5% to 15% by weight of the mixture consists of the fraction.
[0075] Particularly preferably, the particles of the one or more fractions not having minimum size are reagglomerated, preferably by compacting. More preferably, the gained reagglomerated particles are recycled to the reshaping according to (iii). As a first alternative, the gained reagglomerated particles are recycled to the reshaping according to (iii) alone as the first solid formed body obtained from the calcining of (ii). As a second alternative, the gained reagglomerated particles are recycled to the reshaping according to (iii) together with the first solid formed body obtained from the calcining of (ii).
[0076] Furthermore, it is preferred that the reforming process according to (iii) comprises tableting, more preferably consists of tableting.
[0077] With regard to the calcination of the solid shaped body obtained from (ii) or (iii) according to (iv), it is preferred that (iv) comprises drying the solid shaped body obtained from (ii) or (iii), more preferably from (iii), in a gas atmosphere having a temperature of 50° C. to 250° C., more preferably 80° C. to 100° C., before the calcination, wherein the gas atmosphere preferably comprises oxygen, more preferably one or more of oxygen, air or dilute air, wherein the drying is more preferably carried out for 5 hours to 22 hours.
[0078] Regarding the calcination of the second solid shaped body according to (iv), it is preferred that the second solid shaped body is calcined in a gas atmosphere having a temperature of 1125° C. to 1275° C., more preferably 1175° C. to 1225° C., wherein the gas atmosphere more preferably contains oxygen, more preferably one or more of oxygen, air or dilute air, wherein the calcination according to (iv) is more preferably carried out for 2 hours to 10 hours.
[0079] Furthermore, it is preferred that the method for producing a solid shaped body consists of steps (i), (ii), (iii), and (iv), wherein (iv) preferably comprises drying as described above. In this regard, it is preferred that (i) is more preferably carried out before (ii), wherein (ii) is more preferably carried out before (iii), wherein (iii) is more preferably carried out before (iv), wherein (ii) is more preferably carried out after (i), wherein (iii) is more preferably carried out after (ii), wherein (iv) is more preferably carried out after (iii). BRIEF DESCRIPTION OF THE DRAWINGS
[0081] The present invention will be described in more detail with reference to the accompanying drawings, in which:
[0082] Figure 1 showing a longitudinal section of a solid shaped body having a cylindrical form,
[0083] Figure 2 showing a cross section of a solid shaped body having a cross-sectional area in the form of a rholoid, Figure 3 showing a cross section of a solid shaped body having a cross-sectional area in the form of a rholoid and comprising openings and recesses,
[0084] Figures 4 to 6 Shows the test configuration for determining the side crushing strength,
[0085] Figure 7 and 8 shows a perspective view and a cross section, respectively, of a solid shaped body according to the state of the art,
[0086] Figure 9 A perspective view showing another solid shaped body according to the state of the art, and Figures 10 to 12Different embodiments of solid shaped bodies having a cross-sectional area in the form of a rholoid and comprising openings and recesses are shown.
[0087] Figure 1 A longitudinal section of a solid shaped body 1 having a cylindrical form is shown. The solid shaped body 1 comprises a first base region 3 and a second base region 5, which are connected by side regions 7. Figure 1 In the exemplary embodiment of FIG. 5 , the first base region 3 and the second base region 5 are domed with a dome height 35 . Furthermore, the solid shaped body 1 has a height 19 and a diameter 17 .
[0088] Figure 2 A cross section of a solid shaped body 1 is shown, having a cross-sectional area in the form of a rholoid 2. Rholoid 2 is geometrically formed by the intersection of three superimposed circles 4, each with a circle radius 6, and comprises three sides 8 and three corners 10. The three corners 10 lie on an enclosing circle 12 of diameter 17. Diameter 17 is understood to be the diameter 17 of the solid shaped body 1. Diameter 17 and circle diameter 6 have the same length.
[0089] Figure 3 A cross-section of a solid shaped body 1 is shown, having a cross-sectional area in the form of a rholoid 2 and comprising four openings 11 and six grooves 9, each groove having at least one groove radius 13. The four openings 11, each having a second radius 15, include a central opening 14. The central opening 14 is located on the central axis 30 of the solid shaped body 1. The grooves 9 are located on the side 7 of the solid shaped body 1. Furthermore, the grooves 9 and openings 11 extend from the first base region 3 to the second base region 5 of the solid shaped body 1. The first groove 21 has a third radius 25, which is smaller than the fourth radius 27 of the second groove 23.
[0090] Each second groove 23 is arranged between two first grooves 21, and vice versa. Two adjacent second grooves 23 are separated from each other by a leaf 37, which contains one of the first grooves 21 and one of the openings 11. Figure 3 The solid shaped body 1 comprises three lobes 37 .
[0091] A first distance 29 from the central axis 30 of the solid shaped body 1 to a first center 31 of the three openings 11 is expressed as the radius of the circle on which the first center 31 lies.
[0092] Furthermore, in this exemplary embodiment, second distance 43 from central axis 30 of solid shaped body 1 to second center 33 of first recess 21 is equal to third distance 46 from central axis 30 of solid shaped body 1 to third center 45 of second recess 23 .
[0093] Second distance 43 is represented by the radius of a circle around second center 33 of first groove 21. Second center 33 is referenced to an imaginary circle whose arc forms first groove 21. Furthermore, third distance 46 is represented by the radius of a circle around third center 45 of second groove 23. Third center 45 is referenced to an imaginary circle whose arc forms second groove 23.
[0094] Figures 4 to 6 Three different test configurations are shown for determining the side crushing strength of a solid shaped body 1, wherein the solid shaped body 1 is in three different positions in a testing machine 47. Figure 4 , showing the determination of the side crushing strength A. Here, the sample solid molded body 1 is in a test position standing on the groove 9 , specifically the second groove 23 . Figure 5 The side crushing strength B is shown in the following figure: Figure 4 The configuration shown in is rotated 45° or 60°. In the case of an odd number of leaves, the side crush strength B is equivalent to the side crush strength A, because each leaf is opposite a groove. Figure 6 The side crushing strength C is measured and referenced to a position where the orientation of the opening 11 of the solid shaped body 1 is parallel to the direction of the force applied by the testing machine 47 to the sample solid shaped body 1 during the test.
[0095] Figure 7 shows a perspective view of a solid shaped body 1 according to the state of the art, Figure 7 Display according to Figure 7 The solid shaped body 1 comprises four grooves 9 and four openings 11 extending from the first base region 3 through the solid shaped body 1 .
[0096] Figure 9 A perspective view of another solid shaped body 1 according to the state of the art is shown, which also contains the same number of recesses 9 as openings 11 .
[0097] Figures 10 to 12 Various embodiments of solid shaped bodies 1 are shown, each having a cross-sectional area in the form of a rholoid 2. Each solid shaped body comprises three openings 11 and six recesses 9, three of which are first recesses 21 and three of which are second recesses 23. All openings 11 have a circular cross-section. The third radius 25 of the first recess 21 is smaller than the fourth radius 27 of the second recess 23. Furthermore, the openings 11 are arranged equidistant from adjacent openings 11, and the first recesses 21 and the second recesses 23 are arranged in an alternating manner in the side regions 7 of the solid shaped body 1.
[0098] Examples and Comparative Examples
[0099] The dimensions of the solid shaped bodies according to comparative examples 1.1, 1.2, 1.2.1 and 1.2.2 are summarized in Table 1. The reference numerals given refer to Figure 1 and 3 .
[0100] Table 1
[0101] Comparative Example No. Reference numerals unit 1.1 1.2 1.2.1 1.2.2 diameter 17 mm 13.00 16.50 14.03 12.87 high 19 mm 17.00 10.00 8.50 7.80 Vault height 35 mm 1.10 1.10 Groove radius 13 mm 1.50 2.05 Second distance 43 mm 6.50 8.25 First distance 29 mm 3.40 4.10 Second radius 15 mm 1.65 1.90
[0102] like Figures 10 to 12 The dimensions of the solid shaped bodies according to Examples 2.1 to 2.3 shown in Table 2 are summarized in each case.
[0103] Table 2
[0104] Reference numerals unit 2.1 2.2 2.2.1 2.2.2 2.3 diameter 17 mm 19.04 19.99 16.18 14.85 19.60 high 19 mm 9.14 9.84 7.77 7.13 11.42 Vault height 35 mm 1.68 1.13 1.13 Second radius 15 mm 1.90 2.14 2.14 The third radius 25 mm 1.90 2.14 2.14 Fourth radius 27 mm 4.74 4.74 4.23 First distance 29 mm 3.42 3.42 3.76 Second distance 43 mm 9.52 9.99 9.80 The third distance 46 mm 9.52 9.99 9.80
[0105] For all examples and comparative examples, the surface area, volume and relative weight of the respective solid shaped bodies were calculated and summarized in Table 3. The volume refers to the volume filled with material and is therefore the total outer volume of the solid shaped body minus the inner volume of the openings and recesses.
[0106] The geometric surface area and geometric volume of each solid shaped body are determined by CFD (Computational Fluid Dynamics) simulations based on a CAD (Computer Aided Design) model of the geometry of each solid shaped body.
[0107] Table 3
[0108] Nb. <![CDATA[Surface area (m 2 )]]> <![CDATA[Volume (m 3 )]]> Relative weight 1.1 <![CDATA[1.53·10 -3 ]]> <![CDATA[1.36·10 -6 ]]> 1.07 1.2 <![CDATA[1.19·10 -3 ]]> <![CDATA[1.26·10 -6 ]]> 1.00 1.2.1 <![CDATA[0.86·10 -3 ]]> <![CDATA[0.80·10 -6 ]]> 0.63 1.2.2 <![CDATA[0.72·10 -3 ]]> <![CDATA[0.62·10 -6 ]]> 0.49 2.1 <![CDATA[1.29·10 -3 ]]> <![CDATA[1.38·10 -6 ]]> 1.09 2.2 <![CDATA[0.98·10 -3 ]]> <![CDATA[0.96·10 -6 ]]> 0.76 2.2.1 <![CDATA[0.71·10 -3 ]]> <![CDATA[0.59·10 -6 ]]> 0.47 2.2.2 <![CDATA[0.60·10 -3 ]]> <![CDATA[0.46·10 -6 ]]> 0.36 2.3 <![CDATA[1.15·10 -3 ]]> <![CDATA[1.16·10 -6 ]]> 0.92
[0109] The resulting properties of the solid shaped bodies are summarized in Table 4, which represent calculated values.
[0110] The pressure drop for each solid body geometry is calculated by numerical flow simulation, which describes the flow in the spaces between the solid bodies of a bed of solid bodies. The program consists of three consecutive steps. First, a CAD model of each solid body is created. Assume that a tube with an inner diameter of a typical technical reactor of approximately 100 mm serves as the outer container containing the bed of solid bodies. Both the numerical container geometry and the numerical geometry of the solid bodies are entered into the simulation program, which can calculate the arrangement of the solid bodies filled into the container using Newton's equations of motion.
[0111] The pressure drop calculations were performed with air in a DN 100 pipe at ambient temperature and a surface velocity of 1 m / s. Literature values for air at a constant operating pressure of 1 bar and a temperature of 20° C. were used for the thermodynamic and transport properties of the gas.
[0112] To calculate the side crush strength (SCS), also referred to as crush strength, of each solid molded body, a side crush strength test using each CAD model of an aluminum oxide-based solid molded body was simulated using a numerical method such as finite element analysis.
[0113] For the minimum SCS / particle volume, the lowest value of the crush strength determined is divided by the volume of the solid shaped body. The axial dispersion coefficient is calculated according to Levenspiel, The Chemical Reactor Omnibook, 4th edition, Chapter 64, 1993 using "Small Deviation from Plug Flow", where for an ideal plug flow reactor, D ax →0.
[0114] Table 4
[0115]
[0116] The results obtained from the model solid shaped bodies, as shown in Table 4, show that the Examples have enhanced axial dispersion coefficients compared to the Comparative Examples corresponding to the same geometric scale, while Examples 2.2.1 and 2.2.2 are scaled-down versions of Example 2.2 to represent different shrinkage levels. Furthermore, the pressure drop is reduced for Examples 2.1 and 2.3. The axial dispersion coefficient is improved compared to Comparative Examples 1.2, 1.2.1, and 1.2.2.
[0117] The resulting properties of the solid shaped bodies were further investigated using representative 3D-printed solid shaped bodies produced from CaSO 4 .
[0118] 3D printed solid molded bodies were manufactured using a Z Corporation Spectrum Z510 model 3D printer. Solid molded bodies with a constant composition, also referred to as sheets, were made from a mixture comprising gypsum (CaSO4) (using a commercial VisiJet PXL Core from 4Dconcepts) and a binder (using a commercial VisiJet PXL Binder from 4Dconcepts). During the 3D printing process, each solid molded body was not in contact with an adjacent solid molded body, and all molded bodies were oriented in a manner such that the openings of the solid molded body vertically penetrated the molded body. 3D printing was performed with a 3D printing layer thickness of 0.1 mm. Typically, approximately 200 layers were applied to complete a solid molded body, and approximately 100 solid molded bodies were 3D printed in one experiment. After completing the 3D printing process, the printed solid molded bodies were allowed to remain in the print chamber and build envelope for 1 hour, respectively. Thereafter, the solid molded bodies were removed one by one by hand and residual powder was removed.
[0119] The 3D-printed solid bodies were analyzed according to the following measurement methods. The measurement results are summarized in Table 5. For Comparative Example 1.2, three solid bodies of different sizes were studied. Each solid body was scaled down to different shrinkage levels.
[0120] The side crushing strength of the 3D-printed molded bodies was experimentally determined using a commercial materials testing machine of the type BZ2.5 / TS1S from Zwick, which is capable of testing mechanical properties according to DIN EN ISO 7500-1:2018-06. For each type of solid molded body, 10 individual solid molded bodies were studied. The analysis method used included a preload of 0.5 N and a preload speed of 10 mm / min. The analysis speed was 1.6 mm / min. Figures 4 to 6 The solid shaped body was tested as shown in , whereby three positions were investigated in order to determine the side crushing strength A, the side crushing strength B and the side crushing strength C.
[0121] The diameter and height of each solid shaped body were measured using calipers. The weight of the solid shaped body was determined using an analytical balance. Typically, 10 shaped bodies were analyzed and the average value was taken.
[0122] Table 5
[0123]
[0124] Analysis of the 3D printed samples showed that for Example 2.1, at least one of the three tested side crush strengths was improved, while Example 2.2 was characterized by a high minimum SCS / particle volume as shown in Table 4.
[0125] Reference numerals
[0126] 1: Solid molding
[0127] 2: Rholoid
[0128] 3: First base area
[0129] 4: Circle
[0130] 5: Second base area
[0131] 6: Circle radius
[0132] 7: Side area
[0133] 8: Edge
[0134] 9: Groove
[0135] 10: Horn
[0136] 11: Opening
[0137] 12: Enclosing circle
[0138] 13: Groove radius
[0139] 14: Center opening
[0140] 15: Second radius
[0141] 17: Diameter of solid body 1
[0142] 19: Height of solid body 1
[0143] 21: First groove
[0144] 23: Second groove
[0145] 25: The third radius of the first groove 21
[0146] 27: The fourth radius of the second groove 23
[0147] 29: First Distance
[0148] 30: Central axis of solid molded body 1
[0149] 31: First center of opening 11
[0150] 33: Second center of the first groove 21
[0151] 35: Vault height
[0152] 37: Leaf
[0153] 43: Second Distance
[0154] 45: The third center of the second groove 23
[0155] 46: The Third Distance
[0156] 47: Testing machine
Claims
1. A solid shaped body (1) having a cylindrical form with a first base region (3), a second base region (5) and side regions (7), wherein the solid shaped body (1) comprises a first number of grooves (9) having at least one groove radius (13) in the side regions (7), each extending from the first base region (3) to the second base region (5), and a second number of openings (11), each extending from the first base region (3) to the second base region (5), the rholoid perimeter of the cross section of the solid shaped body (1) being interrupted by the grooves (9); wherein the solid shaped body (1) has a cross-sectional area in the form of a rholoid (2); The term "rholoid" refers to an intersecting plane formed by three superimposed circles in a two-dimensional view, having three curved sides and three corners, with the centers of the superimposed circles being equidistant from the centers of the adjacent circles, thereby forming an isosceles triangle; The solid shaped body (1) has a diameter (17) which is the diameter of a circle encompassing the three corners of the rholoid. 2 . The solid shaped body ( 1 ) according to claim 1 , wherein the second number of openings ( 11 ) is in the range of 2 to 8.
3. The solid shaped body (1) according to claim 1, wherein the first number of grooves (9) is greater than the second number of openings (11).
4. The solid shaped body (1) according to claim 2, wherein the first number of recesses (9) is greater than the second number of openings (11).
5. The solid shaped body (1) according to claim 1, wherein the ratio between the first number of grooves (9) and the second number of openings (11) is 2.
6. The solid shaped body (1) according to claim 2, wherein the ratio between the first number of recesses (9) and the second number of openings (11) is 2.
7. The solid shaped body (1) according to claim 3, wherein the ratio between the first number of recesses (9) and the second number of openings (11) is 2.
8. The solid shaped body (1) according to claim 1, wherein the solid shaped body (1) comprises 6 grooves (9) and 3 openings (11).
9. The solid shaped body (1) according to claim 2, wherein the solid shaped body (1) comprises 6 grooves (9) and 3 openings (11).
10. The solid shaped body (1) according to claim 3, wherein the solid shaped body (1) comprises 6 grooves (9) and 3 openings (11).
11. The solid shaped body (1) according to claim 5, wherein the solid shaped body (1) comprises 6 grooves (9) and 3 openings (11).
12. The solid shaped body (1) according to claim 1, wherein the ratio between the diameter (17) of the solid shaped body (1) and the height (19) of the solid shaped body (1) is in the range of 0.5 to 4.
0.
13. The solid shaped body (1) according to claim 2, wherein the ratio between the diameter (17) of the solid shaped body (1) and the height (19) of the solid shaped body (1) is in the range of 0.5 to 4.
0.
14. The solid shaped body (1) according to claim 3, wherein the ratio between the diameter (17) of the solid shaped body (1) and the height (19) of the solid shaped body (1) is in the range of 0.5 to 4.
0.
15. The solid shaped body (1) according to claim 5, wherein the ratio between the diameter (17) of the solid shaped body (1) and the height (19) of the solid shaped body (1) is in the range of 0.5 to 4.
0.
16. The solid shaped body (1) according to claim 8, wherein the ratio between the diameter (17) of the solid shaped body (1) and the height (19) of the solid shaped body (1) is in the range of 0.5 to 4.
0.
17. The solid shaped body (1) according to claim 12, wherein the ratio between the diameter (17) of the solid shaped body (1) and the height (19) of the solid shaped body (1) is in the range of 1.5 to 2.
5.
18. The solid shaped body (1) according to claim 1, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
19. The solid shaped body (1) according to claim 2, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
20. The solid shaped body (1) according to claim 3, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
21. The solid shaped body (1) according to claim 5, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
22. The solid shaped body (1) according to claim 8, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
23. The solid shaped body (1) according to claim 12, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
24. The solid shaped body (1) according to claim 17, wherein the at least one opening (11) has a second radius (15), and the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
20.
25. The solid shaped body (1) according to claim 18, wherein the ratio between the second radius (15) of the at least one opening (11) and the diameter (17) of the solid shaped body (1) is in the range of 0.05 to 0.
20.
26. A solid molded body (1) according to one of claims 1 to 25, wherein the first number of grooves (9) includes a third number of first grooves (21) having a third radius (25) and a fourth number of second grooves (23) having a fourth radius (27), wherein the third radius (25) is smaller than the fourth radius (27).
27. The solid shaped body (1) according to claim 26, wherein the ratio between the third radius (25) of the first recess (21) and the diameter (17) of the solid shaped body (1) is in the range of 0.05 to 0.45, and / or The ratio between the fourth radius (27) of the second groove (23) and the diameter (17) of the solid shaped body (1) is in the range of 0.075 to 0.
50.
28. The solid shaped body (1) according to claim 27, wherein the ratio between the third radius (25) of the first recess (21) and the diameter (17) of the solid shaped body (1) is in the range of 0.05 to 0.15, and / or The ratio between the fourth radius (27) of the second groove (23) and the diameter (17) of the solid shaped body (1) is in the range of 0.20 to 0.
30.
29. The solid shaped body (1) according to claim 26, wherein the third number of first grooves (21) is equal to the fourth number of second grooves (23).
30. The solid shaped body (1) according to claim 27, wherein the third number of first grooves (21) is equal to the fourth number of second grooves (23).
31. The solid shaped body (1) according to claim 28, wherein the third number of first grooves (21) is equal to the fourth number of second grooves (23).
32. The solid shaped body (1) according to claim 26, wherein each opening (11) is arranged between two second recesses (23).
33. The solid shaped body (1) according to claim 27, wherein each opening (11) is arranged between two second recesses (23).
34. The solid shaped body (1) according to claim 28, wherein each opening (11) is arranged between two second recesses (23).
35. The solid shaped body (1) according to claim 29, wherein each opening (11) is arranged between two second recesses (23).
36. A solid molded body (1) according to one of claims 1 to 25, wherein the ratio between the first distance (29) from the central axis (30) of the solid molded body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid molded body (1) is in the range of 0.00 to 0.
40.
37. A solid body (1) according to claim 26, wherein the ratio between the first distance (29) from the central axis (30) of the solid body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid body (1) is in the range of 0.00 to 0.
40.
38. A solid body (1) according to claim 27, wherein the ratio between the first distance (29) from the central axis (30) of the solid body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid body (1) is in the range of 0.00 to 0.
40.
39. A solid body (1) according to claim 28, wherein the ratio between the first distance (29) from the central axis (30) of the solid body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid body (1) is in the range of 0.00 to 0.
40.
40. A solid body (1) according to claim 29, wherein the ratio between the first distance (29) from the central axis (30) of the solid body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid body (1) is in the range of 0.00 to 0.
40.
41. A solid body (1) according to claim 32, wherein the ratio between the first distance (29) from the central axis (30) of the solid body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid body (1) is in the range of 0.00 to 0.
40.
42. A solid body (1) according to claim 36, wherein the ratio between the first distance (29) from the central axis (30) of the solid body (1) to at least one first center (31) of the opening (11) and the diameter (17) of the solid body (1) is in the range of 0.15 to 0.
25.
43. The solid shaped body (1) according to claim 1, wherein the first base region (3) and / or the second base region (5) is arched.
44. The solid shaped body (1) according to claim 26, wherein the first base region (3) and / or the second base region (5) is arched.
45. The solid shaped body (1) according to claim 27, wherein the first base region (3) and / or the second base region (5) is arched.
46. The solid shaped body (1) according to claim 28, wherein the first base region (3) and / or the second base region (5) is arched.
47. The solid shaped body (1) according to claim 29, wherein the first base region (3) and / or the second base region (5) is arched.
48. The solid shaped body (1) according to claim 32, wherein the first base region (3) and / or the second base region (5) is arched.
49. The solid shaped body (1) according to claim 36, wherein the first base region (3) and / or the second base region (5) is arched.
50. The solid shaped body (1) according to claim 42, wherein the first base region (3) and / or the second base region (5) is arched.
51. The solid shaped body (1) according to claim 43, wherein the ratio between the dome height (35) and the diameter (17) of the solid shaped body (1) is in the range of 0.01 to 0.
40.
52. The solid shaped body (1) according to claim 51, wherein the ratio between the dome height (35) and the diameter (17) of the solid shaped body (1) is in the range of 0.05 to 0.
10.
53. The solid shaped body (1) according to claim 1, wherein the solid shaped body (1) comprises a mixed oxide and The mixed oxide comprises oxygen, aluminum, cobalt and at least one rare earth metal, or the mixed oxide comprises oxygen, aluminum, nickel and at least one alkaline earth metal.
54. The solid shaped body (1) according to claim 53, wherein the rare earth metal is lanthanum and / or the alkaline earth metal is magnesium.
55. Use of the solid shaped body (1) according to any one of claims 1 to 54 as a catalyst.
56. Use according to claim 55 for reforming one or more hydrocarbons into synthesis gas comprising hydrogen and carbon monoxide.
57. The use according to claim 56, wherein the reforming is carried out in the presence of carbon dioxide.
58. Use according to claim 56 or 57, wherein the hydrocarbon is selected from methane, ethane, propane and butane.
59. Use according to claim 58, wherein the hydrocarbon is methane.
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