The method of preparation of the catalyst carrier

 

(57) Abstract:

The preparation of a carrier (the predecessor) of a catalyst containing highly porous layer of non-porous or malabaristas basis, comprises applying to the non-porous base material followed by drying and oxidation treatment. As the applied substance use powdered components, which together with non-porous base is placed in the mold, permeable for the introduction and removal of gaseous components. The overall composition of the composite coating is described by the formula AlxAaBbCcDdFfOywhere A, B, C, D, F - elements 3, 4, 5, 6 periods and rare-earth 4f elements of the Periodic table. Prepared with carriers for catalysts effective in operation. 33 C.p. f-crystals, 1 table.

The invention relates to the field of technical chemistry, and in particular to methods of cooking media (systems-precursors for catalysts that can be used in almost any heterogeneous catalytic processes in the chemical industry and in the energy sector, such as catalytic oxidation (full and partial), hydrogenation (including the Fischer-Tropsch synthesis), the conversion of coal is eactor need regular device catalyst layer, placed in the reactor. Such a device can be achieved by the use of catalysts in the form of honeycomb structures, tubes, rods, plates, foams, etc., [and.with. USSR N 695697, class B 01 J 37/02, BI N 41, 1979; U.S. patent N 4783436, class B 01 J 21/04, 1988; and.with. USSR N 1754205, class B 01 J 37/02, B N 30, 1992; Japan patent N 4-354544, class B 01 J 35/06, 1992]. In addition, the use as a carrier for catalysts of metals having high mechanical strength, heat conductivity and reduces the entrainment of catalyst from the reactor and reduce the risk of local overheating, as well as to produce catalysts in the form of the above-mentioned complex shapes and designs.

The most common problem for all structural materials (metals, ceramics, glass, etc. are used as the basis for catalyst complex forms, is their low specific surface area, which significantly reduces the activity of such catalysts. To increase the specific surface area of catalysts on structural materials used as base catalysts, pre-applied high-porous layer (usually of oxide ceramics). This layer, on the one hand, provides high dispersion applied to the next stage acti; U.S. patent N 4783436, class B 01 J 21/04, 1988; a.c. USSR N 1754205, class B 01 J 37/02, B N 30, 1992; Japan patent N 4-354544, class B 01 J 35/06, 1992].

One of the main characteristics of high-porous layer on the porous or malabarista basis, is its thickness. The thickness of most of the known highly porous coatings does not exceed 100 μm [U.S. patent N 4771029, class B 01 J 24/04, 1988]. In some cases refers to the thickness of the oxide layer on the basis of non-porous 0.2-0.5 mm [A. with. USSR N 1754205, class B 01 J 37/02, B N 30, 1992]. The small thickness of the coating causes a very low absorption capacity (or capacity unit geometric surface structural basis. This leads to the fact that the number of active component is introduced into the catalyst as a whole, is small. Therefore, in order to increase the specific activity of such catalysts predominantly use the active component-based highly active, but expensive platinum group metals. However, for many highly selective processes replacement of one element by another is impossible because of the strong influence of the composition of the active component on the activity and selectivity of the catalyst. In addition, interaction with the media can strongly modify the properties of the active component when wet catalyst to catalytic poisons, the influence of the reaction medium and, in General, reduces the time of operation ("life") catalyst [U.S. patent N 4771029, class B 01 J 24/04, 1988].

Another important characteristic of the media based on non-porous or monopolistic structural materials is the amount of high-porous layer per unit geometric surface of the substrate or its density. Given the number of patents concentrations of elements in high-porosity layer, referred to the unit weight of the catalyst, in General, [U.S. patent N 4410454, class B 01 J 23/10, 1983] , it is not always explicitly characterize the properties of these catalysts or carriers. Indeed, if the active component or highly porous layer deposited on one side of the plate or tube, the catalyst activity in General, when changing the thickness of the plate or tube will be determined by the density of the highly porous layer, attributed to the geometric surface of the base, not its concentration per unit weight. The density of high-porous layer is determined by its thickness, chemical composition and porous structure. Known catalysts containing cobalt oxide on the metallic titanium in an amount of not more than 710-4g/cm2[A. C. the USSR N910180, class B 01 J 23/74, BI N 9, 1982], SUP>2[US patent N 4046712, class B 01 J 23/56, 1977]. However, in these catalysts is missing a highly porous layer, which reduces their specific activity.

The above-mentioned disadvantages of media systems-predecessors) because of the inadequacy of the methods of their preparation. One of the main ways to obtain a highly porous coating on the porous base is impregnated porous framework in the suspension containing highly porous substance or its precursor, followed by drying and calcination. So, [and.with. USSR N 695697 class. B 01 J 37/02, BI N 41, 1979] used a suspension containing aluminum compounds and nitric acid. [US patent N 4771029, class B 01 J 24/04, 1988] describes a suspension containing fine powder milled in the wet state of the aluminum oxide, the promoter and the noble metal, which is non-porous monolith is immersed, followed by drying and calcination. The disadvantage of this method of cooking is too low concentration of the applied substances in suspension, since the greater the concentration of the slurry becomes too viscous. In the result, the thickness of the highly porous layer, as noted above, is insufficient.

To obtain thick you the basis. Thus, in [patent RF N 2062402, CL F 23 D 14/18, 1994] catalytic coating in the form of a reinforced material (metal mesh or parametrov), containing as an active ingredient the oxides of cobalt, copper, chromium, iron, metals of group VIII, as well as aluminum oxide, attached to the outer side of the metal tube (basics) using alloys based on Ti, Ti-Al, Ni-Al, Ni-Cr, Ti-Si. The disadvantage of this method of cooking is its large consumption compared with other ways of making highly porous coatings on non-porous basis.

In [international patent WO 092/13637, class B 01 J 35/06, 1992], we have chosen as a prototype, patented method of preparation of the carrier (the predecessor) of a catalyst containing a stable, highly porous layer is less porous or non-porous base, which includes a spray on non-porous base solutions of ORGANOMETALLIC compounds In, Si, Zr, Ti, CE, Sc, or Y, or the other, removing the solvent by drying, and the transformation of the ORGANOMETALLIC compound in an oxidizing medium. As an example malabaristas basis specified-Al2O3. There are also carbon, glass, metals. As a highly porous layer patented oxides, Anisimova connection liquid-phase system. In the result, the maximum thickness of the highly porous layer marked in the examples is 1 μm. The small thickness of the highly porous layer, which determines its low absorption capacity (capacity per unit geometric surface of the porous base. This reduces the number of active component that can be introduced in a highly porous layer, so as an active component of such catalysts are mainly used platinum metals.

The invention solves the problem of creating efficient in operation and manufacture of carriers for catalysts. The problem is solved by using as the applied powdery substance components that are placed together with non-porous base in the mold, permeable for the introduction and removal of gaseous components, with subsequent processing of the mold in an oxidizing and/or humid environments, and removing the resulting product from the mold, resulting in a highly porous, thick, samozakravatayasa coating on non-porous or malabaristas basis with thick highly porous layer of 0.6-20 mm and a density of 0.1-10 g/cm2.

As a non-porous or malabaristas basics in the present invention so on my in the form of tubes, plates, rods, foam and other complex geometric shapes with a specific surface area not exceeding 20 m2/g, similar to [U.S. patent N 4046712, class B 01 J 23/56, 1977] . As a highly porous layer applied to structural materials, in the present invention can be used porous oxide or metal oxide composites with uniform or nonuniform distribution of components by layer, single-phase or multiphase composition, with different combination of individual and mixed non-volatile compounds on the basis of the elements 3, 4, 5, 6 periods and rare-earth 4f elements of the Periodic table. As the main binder in the present invention are compounds based on aluminum, so in all variants of the porous composite layer includes aluminum. Thus, the overall composition of the composite is described by the formula AlxAaBbCcDdFtOy; where A, B, C, D, F - elements 3, 4, 5, 6 periods and rare-earth 4f elements of the Periodic table, respectively. Thus the composite includes an aluminum or aluminum and at least one of the components denoted by the letters A, B, C, D, F.

As samsaras the data, porous monoliths (in the form of granules, rings, etc.,) without any reinforcing components and without non-porous bases due to the high strength of the contact between the particles forming the composite. Under "non-volatile" refers to a solid connection, not vozgonaetsa in the process of synthesis or in the conditions of the catalytic reaction. Such compounds may include metals with body-centered, face-centered and other lattice types, as well as their alloys and oxides: as simple oxides with the structure of table salt, corundum, spinel, double oxides, rutile, anatase, and other structures, and mixed oxides with spinel structure, perovskite, zeolites, alumina, pyrochlore or solid solutions based on them and other possible structures. Under items 3-6 periods involve elements of both main and side groups of the Periodic table. Depending on the composition and method of preparation pore volume and size distribution can vary within wide limits.

The preparation of a carrier (the predecessor) of the catalyst includes the following stages:

a) preparing a mixture by mixing a powder of aluminum with other powdered, non-volatile, use the ve, permeable to gaseous components;

in the processing of the molding device in wet and/or an oxidizing atmosphere with the formation of thick, samosochranienija the surface of non-porous frameworks;

g) removing the resulting product from the molding device, its drying and calcination with the formation of highly porous coatings;

d) in some cases, part of the components of a highly porous layer can be introduced by impregnation of the product, followed by drying and calcination.

For use of the media (the predecessor) as the catalyst you need any additional application of any component or the activation of the carrier in the special conditions or the formation of the active component under the influence of the reaction medium directly in the reactor.

The invention is illustrated by the following examples.

Example 1. The aluminum powder is mixed with alumina powder, is poured into the molding device in which pre-placed tube made of metal, covered and placed in an autoclave. Autoclave molding device steamed, then remove it from autoclavability oxide layer composition AlO1,5with a density of 0.4 g/cm2, 2 mm thick, deposited on the outer side of the tube from largescale diameter 6 mm

Example 2. The preparation method of the carrier, similar to example 1, with a highly porous metal-oxide layer has a composition AlO0,04with a density of 0.1 g/cm20.6 mm thick, deposited on a copper tube with a diameter of 6 mm

Example 3. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,78Mg1,49Oywith a density of 0.2 g/cm2, 1 mm thick, deposited on a steel tube with a diameter of 2 mm.

Example 4. The preparation method of the carrier, similar to that described above, characterized in that the forming device handle in the air, while a highly porous metal oxide layer has a composition of Al3,52Si0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on a steel rod with a diameter of 2 mm.

Example 5. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,63Ca1,42Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on a ceramic tube diameter 6 mm

Example 6. Way prigot the ku, this highly porous metal oxide layer has a composition of Al3,62Ti0,02Oywith a density of 0.5 g/cm2, 2 mm thick, deposited on a ceramic rod with a diameter of 4 mm

Example 7. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Alof 0.53Zifor 0.3Yfor 0.3Oywith a density of 0.6 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 8. The preparation method of the carrier, similar to example 1, wherein the compound based on zirconium introduced by impregnation, with a highly porous metal oxide layer has a composition of Alto 3.73Zr0,02Oywith a density of 0.5 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 9. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,59W0,32Oywith a density of 3.5 g/cm210 mm thick, deposited on the tube from largescale diameter 8 mm

Example 10. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,57La0,01Oywith a density of 0.5 for drinking, preparing media, similar to example 1, with highly porous oxide layer has a composition of Al0,57Ce0,30Nd0,12Oywith a density of 0.6 g/cm22 mm thick, deposited on the tube from largescale diameter 8 mm

Example 12. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Alto 3.58Ce0,01Oywith a density of 0.5 g/cm22 mm thick, deposited on the tube from largescale diameter 6 mm

Example 13. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,59Nd0,02Fe1,17Oywith a density of 10 g/cm2, 20 mm thick, deposited on the tube from largescale diameter 4 mm

Example 14. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,55Si1,23Ti0,01Oydensity of 1.0 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 2 mm

Example 15. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,20Mg0,01Ti0,03Oywith a density of 0.4 g/cm2tol is a user, similar to example 1, with highly porous oxide layer has a composition of Al0,55Mg0,05Mo0,49Oywith a density of 9.0 g/cm2, 20 mm thick, deposited on the tube from largescale diameter 8 mm

Example 17. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al2,10Mg1,39Zr0,02Oywith a density of 0.2 g/cm2a thickness of 1 mm, printed on the tube from largescale diameter 6 mm

Example 18. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,33Na0,02Sr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 19. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,58Si0,03W0,30Oywith a density of 2.0 g/cm2, thickness of 5 mm is applied on the tube from largescale diameter 2 mm

Example 20. The preparation method of the carrier, similar to example 1, with a highly porous metal-oxide layer of the composition of Al2,24Mg1,46Re0,01Oydensity of 1.0 g/cm2the thickness of the body, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,54Si0,02Ba0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 22. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,67P0,01Ce0,38Oywith a density of 2.0 g/cm2, thickness of 5 mm is applied on the tube from largescale diameter 4 mm

Example 23. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,37Mg1,50Ce0,01Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 24. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,48Na0,02Pr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 25. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,56Fe1,16Mo0,01Oydensity of 1.0 g/cm2 media, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,10Ti0,01Zrof 0.48Oywith a density of 0.7 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 27. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,35Cu0,02Sn0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 28. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Alof 0.53Fe1,14Re0,01Oydensity of 1.0 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 29. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,37Ti0,01W0,32Oywith a density of 0.7 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 30. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,49Ca0,02Ba0,01Oywith a density of 0.4 g/cm0,54Mn0,01Ce0,36Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 2 mm

Example 32. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,24Ni0,94Pr0,01Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 33. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,51Ca0,01Ce0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 34. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,50Zr0,55Ce0,01Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 6 mm

Example 35. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,27Zr0,02Ce0,35Oywith a density of 1.6 g/cm23,59Sr0,01Pr0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 37. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,51Y0,56Ba0,01Oywith a density of 2.0 g/cm2, thickness of 5 mm is applied on the tube from largescale diameter 10 mm

Example 38. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,29Zr0,02W0,29Oywith a density of 0.7 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 39. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,53Sr0,01Ba0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 40. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,57CE0,35Pt0,003Oywith a density of 1.4 g/cm21,37Ce0,01W0,28Oywith a density of 1.6 g/cm24 mm thick, deposited on the tube from largescale diameter 2 mm

Example 42. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,45Ba0,02Pr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 43. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Alof 0.53Mg1,49Zn0,01Zr0,02Oywith a density of 0.1 g/cm20.6 mm thick, deposited on the tube from largescale diameter 8 mm

Example 44. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Alof 0.85Mg0,02Fe1,08Zr0,02Oywith a density of 5.0 g/cm210 mm thick, deposited on the tube from largescale diameter 6 mm

Example 45. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,30Si0,03V0,02Mo0,42="ptx2">

Example 46. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,42Mg0,01Cu0,01Sr0,03Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 47. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,57Mg1,54Ti0,03La0,02Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 48. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,86Si0,02Ca0,49Ti0,49La0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 49. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,03Si0,02Cu0,02W0,30Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 6 mm

Example 50. The preparation method of the carrier, similar to example 1, with vysokoporistogo 2 mm, applied on the tube from largescale diameter 4 mm

Example 51. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,54Na0,02Ni0,87Ce0,01Oywith a density of 0.6 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 52. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,89Si0,02Ti0,03Ce0,35Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 10 mm

Example 53. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,32Mg1,48Ca0,02Ce0,01Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 54. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,44Na0,01K0,01Pr0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 55. The method of preparation UB>Pr0,01Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 56. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,74Si0,02Zrof 0.53Ce0,01Oywith a density of 1.4 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 2 mm

Example 57. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,30Mg0,04Sr0,02Ce0,36Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 58. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,53Mg0,01Sr0,02Pr0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 59. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Alof 0.53Mg0,02W0,38Ce0,01Oywith a density of 0.2 g/cm2a thickness of 1 mm, printed on the tube from largescale di the first metal oxide layer has a composition of Alof 0.85Si0,02La0,01Dy0,32Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 4 mm

Example 61. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,18Mg1,56Bi0,01Ce0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 62. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Alto 3.58Na0,01Ba0,02Pr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 63. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,54Mg1,43Y0,02Ba0,02Oywith a density of 0.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 8 mm

Example 64. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,83Si0,03Y0,02La0,37Oywith a density of 0.8 g/cm2thickness 4 mm caused the ERU 1, this highly porous metal oxide layer has a composition of Al1,30Si0,02Zr0,50La0,01Oywith a density of 0.7 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 66. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,53Na0,01Ba0,01Pr0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 67. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,55Cu1,12Zr0,02La0,01Oywith a density of 0.4 g/cm22 mm thick, deposited on the tube from largescale diameter 10 mm

Example 68. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,90Ti0,02Y0,02La0,36Oywith a density of 0.5 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 69. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,16Cr0,02Mo0,45W0,01">

Example 70. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Alof 3.46Cd0,01Sr0,01Ba0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 71. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,52Cu0,92Y0,01Ce0,01Oywith a density of 0.6 g/cm2thickness 1 mm, printed on the tube from largescale diameter 2 mm

Example 72. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,83Ti0,01Zr0,02Ce0,35Oywith a density of 0.8 g/cm2, 3 mm thick, deposited on the tube from largescale diameter 10 mm

Example 73. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,28Ti0,02Zr0,50Nd0,01Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 8 mm

Example 74. The preparation method of the carrier, similar to example 1, with a highly porous metal-the other 2 mm, applied on the tube from largescale diameter 6 mm

Example 75. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,58Ga0,03Ba0,01Ce0,36Oywith a density of 1.6 g/cm2, 3 mm thick, deposited on the tube from largescale diameter 4 mm

Example 76. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,80Tiof 0.85Ba0,02Ce0,01Oywith a density of 1.2 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 77. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,12V0,02W0,39Ce0,01Oydensity of 1.0 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 10 mm

Example 78. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,42Ca0,01Ba0,01Pr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 79. Method of cooking wear the Pr0,01Nd0,01Oywith a density of 4.0 g/cm210 mm thick, deposited on the tube from largescale diameter 4 mm

Example 80. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,83Zr0,50La0,01Ce0,02Oywith a density of 0.8 g/cm2, 8 mm thick, deposited on the tube from largescale diameter 2 mm

Example 81. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,23Sr0,01La0,02Ce0,37Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 10 mm

Example 82. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,53Sr0,02Ba0,01Pr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 83. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,59Na0,02Fe1,08Mo0,01W0,01Oywith a density of 5.0 g/cm210 mm thick, deposited on the tube this highly porous metal oxide layer has a composition of Al0,74Mg1,54Ca0,02Cs0,01Bi0,02Oywith a density of 0.2 g/cm2a thickness of 1 mm, printed on the tube from largescale diameter 4 mm

Example 85. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,86Mg0,01Ti0,01Zrof 0.48La0,01Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 2 mm

Example 86. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,25Si0,02K0,02Zr0,02La0,32Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 87. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,45Mg0,03Ca0,01Sr0,02Ba0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 88. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,62Mg1,46Ca0,02Sr0,01Pr0,01Oywith the 89. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,83Na0,03Fe1,11Pd0,001Ce0,02Oywith a density of 0.9 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 90. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,84Mg0,01Ti0,02Zr0,51Ce0,01Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 91. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,22P0,03Ti0,02Zr0,01Ce0,36Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 10 mm

Example 92. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,52Na0,02K0,01Sr0,02Pr0,02Oywith a density of 0.4 g/cm22 mm thick, deposited on the tube from largescale diameter 8 mm

Example 93. The preparation method of the carrier, similar primarv>y
with a density of 0.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 6 mm

Example 94. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,82Na0,03Ca1,24W0,01Ce0,02Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 95. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Alof 0.85Si0,03Ti0,02La0,38Ce0,01Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 2 mm

Example 96. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,23Si0,01Cr0,02La0,02Ce0,35Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 10 mm

Example 97. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,47Mg0,02Ca0,01Ba0,01Pr0,02Oywith a density of 0.4 g/cm22 mm, NAS is hydrated to example 1, this highly porous oxide layer has a composition of Al0,64Mg1,48Sb0,02Bi0,01Sm0,01Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 99. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,79Si0,02Zr0,54Ba0,02Ce0,01Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 4 mm

Example 100. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,81Si0,04Mn0,02Laof 0.48Ce0,01Oywith a density of 0.4 g/cm2thickness 1 mm, printed on the tube from largescale diameter 2 mm

Example 101. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,21Na0,02Cr0,03W0,02Ce0,37Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 10 mm

Example 102. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has Cassany on the tube from largescale diameter 8 mm

Example 103. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,68Ca1,16Zr0,02W0,01Pr0,03Oywith a density of 0.2 g/cm2thickness 1 mm, printed on the tube from largescale diameter 6 mm

Example 104. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,78Ti0,01Y0,41Ba0,02Ce0,01Oywith a density of 2.0 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 4 mm

Example 105. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,86Ti0,02Mo0,02La0,37Ce0,02Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 106. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,25K0,03Sn0,01La0,01Ce0,38Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 10 mm

Example 107. The preparation method of the carrier, similar to the UB>Pr0,01Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 8 mm

Example 108. The preparation method of the carrier, similar to example 1, with highly porous oxide layer has a composition of Al0,57Mg1,46Ca0,02Sr0,01Ba0,01Pr0,01Oywith a density of 0.3 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

Example 109. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,69Si0,02Fe1,10Mo0,02W0,01Ce0,02Oywith a density of 5.0 g/cm210 mm thick, deposited on the tube from largescale diameter 4 mm

Example 110. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,79Si0,03Cr0,04Zr0,45Ba0,02Ce0,01Oywith a density of 0.8 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 2 mm

Example 111. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al0,83P0,02Cu0,01Zr0,02La0,39Ce0,01O Example 112. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al1,20Mg0,03Ca0,02Zr0,01La0,02Ce0,36Oywith a density of 1.6 g/cm2, 4 mm thick, deposited on the tube from largescale diameter 8 mm

Example 113. The preparation method of the carrier, similar to example 1, with a highly porous metal oxide layer has a composition of Al3,52Mg0,01Ca0,02Sr0,03Ba0,02Pr0,02Oywith a density of 0.4 g/cm2, 2 mm thick, deposited on the tube from largescale diameter 6 mm

All examples with data on specific surface area and high porosity layer in the form of the generalized formula AlxAaBbCcDdFfOypresented in the table. The analysis of cations in high-porosity layer was performed by atomic-absorption spectrophotometry and flame photometry; specific surface of a highly porous layer was determined by low-temperature adsorption of argon method BET. The stoichiometry of the porous layer was evaluated by atomic weights of the elements and rounded to 0.01, with the exception of the platinum group metals, the stoichiometry of which was rounded up to 0.001.

2), which varies from 9 to 100 m2/cm2. This value is significantly higher than similar values, which can be estimated from the data presented in the patent. For example, when the maximum specific surface film 250 m2/g and its maximum thickness is 80 μm [U.S. patent N 4771029 (1988), class B 01 J 24/04, 32/00], and also close to the value of the bulk density of the oxide film (see example 1 from table) specific surface of the film per unit geometric surface is 0.4 m2/cm2that is significantly lower than in the present invention.

1. The method of preparation of the carrier (the predecessor) of a catalyst containing highly porous layer of non-porous or malabaristas basis, including the application of the non-porous base material followed by drying and oxidation treatment, characterized in that as the applied substance use powdered components, consisting of non-volatile compounds, which together with non-porous base placed together in a molding device, permeable to gaseous substances, with subsequent treatment in an oxidizing and/or humid environments moulder with powdered comparity layer is a thick, samozakravatayasa oxide or metal oxide composite consisting of compounds of aluminum and/or aluminum compounds with the addition of non-volatile compounds, selected from items 3, 4, 5, 6 periods and/or 4-f of the elements of the Periodic table, or various combinations of individual and mixed compounds all of the above elements with the following characteristics of the porous layer: layer thickness: from 0.6 to 20 mm; the density of the layer per unit geometric surface non-porous framework of 0.1 - 10 g/cm2.

2. The method according to p. 1, characterized in that the obtained product is further added components by impregnation in solution with subsequent drying and calcination.

3. The method according to PP.1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlOywhere 0 < y 1,5.

4. The method according to PP.1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaOywhere a is element 3 of the period; 0,58 x 3,52; 0 < a 1,49; y is determined by the degree of oxidation of aluminum, the valence of the cations, the size and.

5. The method according to PP.1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbOywhere In the item 4 of the period; 0,55 x 3,63; 0 < b 1,42; y operauser fact, the highly porous structure of the layer corresponds to the formula AlxCcOywhere is the element 5; 0,53 x to 3.73; 0 < c 0,50; y is determined by the degree of oxidation of aluminum, the valence of the cations, the size of S.

7. The method according to PP.1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxDdOywhere D is the element 6 period; 0,59 x 3.75; 0 < d 0,32; y is determined by the degree of oxidation of aluminum, the valence of the cations, the value of d.

8. The method according to PP.1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxFfOywhere F - 4f element; 0,57 in x 3.58; 0 < f 0,42; y is determined by the degree of oxidation of aluminum, the valence of the cations, the value of f.

9. The method according to PP.1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbOywhere a, b are elements of the 3rd and 4th periods, respectively; 0 x 3.20; 0 < a 1,23; 0 < b 1,17; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b.

10. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaCcOywhere As, With elements 3 and 5 periods, respectively; 0,55 x 3,33; 0 < a 1,39; 0 < c 0,49; y is determined by the degree oxide is AB a highly porous layer corresponds to the formula AlxAaDdOywhere a, D - elements 3 and 6 periods, respectively; 0,58 x 3.54; 0 < a 1,46; 0 < d 0,30; y is determined by the degree of oxidation of aluminum, the valence of the cations, the quantities a, d.

12. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaFfOywhere And F - elements 3 period 4 f elements, respectively; 0,57 x 3,48; 0 < a 1,50; 0 < f 0,38; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, f.

13. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbCcOywhere B, C are elements 4 and 5 periods, respectively; 0,56 x 3,36; 0 < b 1,16; 0 < c 0,48; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of b, c.

14. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbDdOywhere B, D are elements 4 and 6 periods, respectively; 0.54 x 3,49; 0 < b 1,14; 0 < d 0,32; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of b, d.

15. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbFfOywhere B, F elem is I, the valence of the cations, the values of b, f.

16. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxCcFfOywhere C, F - 5 elements of period 4 f elements, respectively; 0.50 x 3,59; 0 < c 0,55; 0 < f 0,35; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of c, f.

17. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxCcDdOywhere C, D are elements 5 and 6 period respectively; 0.51 x 3,53; 0 < c 0,56; 0 < d 0,29; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of c, d.

18. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxDdFfOywhere D, F - elements 6 period 4 f elements, respectively; 0,57 x 3,45; 0 < d 0,35; 0 < f 0,28; y is determined by the degree of oxidation of aluminum, the valence of the cations, the quantities d, f.

19. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbCcOywhere a, b, C elements 3, 4, 5 periods, respectively; 0,53 x 3,42; 0 < a 1,49; 0 < b 1,08; 0 < c 0,42; y is determined by the degree of oxidation of the aluminum, the valence to the resulted formula AlxAaBbDdOywhere a, b, D - items 3, 4, 6 periods, respectively; 0,57 x 3,36; 0 < a 1,54; 0 < b 1,98; 0 < d 0,30; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b, d.

21. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbFfOywhere a, b, F - elements 3, 4 periods and 4 f elements, respectively; 0.54 x 3,44; 0 < a 1,49; 0 < b 0,87; 0 < f 0,35; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b, f.

22. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaCcFfOywhere A, C, F - elements 3, 4 periods and 4 f elements, respectively; 0,63 x 3,53; 0 < a 1,51; 0 < c 0,53; 0 < f 0,36; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, c, f.

23. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaDdFfOywhere a, D, F - elements 3, 5 periods and 4 f elements, respectively; of 0.53 in x 3.58; 0 < a 1,56; 0 < d 0,38; 0 < f 0,32; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, d, f.

24. The method according to PP. 1 and 2, different C D - items 3, 4, 6 periods, respectively; 0.54 x 3,53; 0 < a 1,43; 0 < c 0,50; 0 < d 0,37; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, c, d.

25. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbCcDdOywhere B, C, D elements 4, 5, 6 periods, respectively; 0,62 x 3.46 in; 0 < b 1,12; 0 < c 0,45; 0 < d 0,36; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of b, c, d.

26. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbCcFfOywhere B, C, F - elements 4, 5 periods and 4 f elements, respectively; 0,52 x 3,51; 0 < b 0,92; 0 < c 0,50; 0 < f 0,35; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of b, c, f.

27. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbDdFfOywhere B, D, F - elements 4, 6 periods and 4 f elements, respectively; 0,58 x 3,42; 0 < b 0,85; 0 < d 0,39; 0 < f 0,36; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of b, d, f.

28. The method according to PP. 1 and 2, characterized in that the composition of the high porosity layer is responsible formulas,53; 0 < c 0,50; 0 < d 0,48; 0 < f 0,37; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of c, d, f.

29. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbCcDdOywhere A, B, C, D elements 3, 4, 5, 6 periods, respectively; 0,59 x 3,45; 0 < a 1,54; 0 < b 1,08; 0 < c 0,48; 0 < d 0,32; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b, c, d.

30. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbCcFfOywhere A, B, C, F - elements 3, 4, 5 periods and 4 f elements, respectively; 0,62 x 3,52; 0 < a 1,46; 0 < b 1,11; 0 < c 0,51; 0 < f 0,36; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b, c, f.

31. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbDdFfOywhere A, B, D, F - elements 3, 4, 6 periods and 4 f elements, respectively; 0,58 x 3,47; 0 < a 1.44MB; 0 < b 1,24; 0 < d 0,38; 0 < f 0,35; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b, d, f.

32. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer of the options, respectively; 0,64 x 3,51; 0 < a 1,48; 0 < c 1,54; 0 < d 0,48; 0 < f 0,35; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, c, d, f.

33. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxBbCcDdFfOywhere B, C, D, F - elements 4, 5, 6 periods and 4f elements, respectively; 0,58 x 3,55; 0 < b 1,16; 0 < c 0,54; 0 < d 0,48; 0 < f 0,38; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of b, c, d, f.

34. The method according to PP. 1 and 2, characterized in that the composition of the highly porous layer corresponds to the formula AlxAaBbCcDdFfOywhere A, B, C, D, F - elements 3, 4, 5, 6 periods and 4f elements, respectively; 0,57 x 3,52; 0 < a 1,46; 0 < b 1,10; 0 < c 0,45; 0 < d 0,39; 0 < f 0,36; y is determined by the degree of oxidation of aluminum, the valence of the cations, the values of a, b, c, d, f.

 

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