MXPA99011266A

MXPA99011266A - Shaped body and method for the production thereof

Info

Publication number: MXPA99011266A
Application number: MXPA/A/1999/011266A
Authority: MX
Inventors: Rieber Norbert; Muller Ulrich; Heinrich Grosch Georg; Harder Wolfgang; Walch Andreas
Original assignee: Basf Ag 67063 Ludwigshafen De
Priority date: 1997-06-06
Filing date: 1999-12-06
Publication date: 2000-05-01

Abstract

The invention relates to a shaped body, containing at least one porous oxidic material which can be obtained according to a method comprising the following steps:(I) adding a mixture containing a porous oxidic material or a mixture of two or more materials of the same type with a mixture containing at least one alcohol and water and (II) kneading, deforming, drying and calcinating the mixture added in step (I). The invention further relates to a method for the production of said body.

Description

MOLDED ARTICLE AND ITS PRODUCTION The present invention relates to a molded article that "contains at least one porous oxide material, one processed for its production, and its use for the reaction of organic compounds, particularly for the epoxidation of organic compounds having the minus one CC double bond The molded product described here has a high abrasion resistance and excellent mechanical properties Abrasion resistant molded products comprising catalytically active materials are used in many chemical processes, particularly in processes employing a fixed bed Therefore, there is a lot of information on this subject There is significantly less information on the use of catalysts based on porous, porous materials, for example zeolites, and especially in relation to the molding of such materials For the production of solids, a binder, an organic compound for improving the viscosity A liquid and a liquid for converting the material into a paste are generally added to the catalytically active material, ie the porous oxide material and the mixture is compacted in a mixing or kneading apparatus or in an extruder. The resulting plastic material is then molded, particularly using an extrusion press or extruder, and the resulting molded articles are dried and calcined.

Numerous inorganic compounds are used as binders.

For example, according to US Pat. No. 5,430,000, titanium dioxide or titanium dioxide hydrate is used as binder. Examples of additional binders of the prior art are: Hydrated alumina or other aluminum-containing binders (WO 94/29408); Mixtures of silicon and aluminum compounds WO (94/13584); Silicon compounds (EP-A 0 592 050); Clay minerals (JP-A 03 037 156); Alcoxysilanes (EP-B 0 102 544). The organic substances which improve the viscosity employed are generally hydrophilic polymers, cellulose or polyacrylates. The applicant himself, in DE-A 196 23 611.8 further describes an oxidation catalyst having a structure of zeolite and molded by compacting processes, and its use in the preparation of epoxides from olefins and hydrogen epoxide and, in DE-A 196 23 609.6, an oxidation catalyst based on titanium or vanadium silicalites having the structure of zeolite and which has also been molded by forming processes by compaction and containing 0.01 to 30% of one or more noble metals as defined there. In all the publications according to the prior art mentioned above, water is used in the preparation of the molded products described therein, as a liquid for converting the material into paste (pulping agent). However, the molded articles described above and based on a porous oxide material, for example, zeolite and on particular titanium silicalites, have several disadvantages. Thus, many of the molded articles described in the aforementioned literature have insufficient mechanical strength for use as a catalyst in a fixed bed. This is particularly when side reactions of certain binders are undesirable and for this reason whole classes of binders which can provide sufficient strength to such a molded product can not be used, for example, due to other adverse properties. For example, aluminum-containing binders can not be used in the preparation of titanium silicalite which is used as a catalyst for the epoxidation, for example, of propylene with hydrogen peroxide, since the acidity induced by the aluminum-containing binder results in a higher degree of ring dissociation and formation of by-products. In addition, titanium-containing binders can cause high decomposition rates of the hydrogen peroxide employed if these titanium-containing binders result in detectable titanium dioxide contents in the molded product. It is also undesirable to employ binder containing more than 100 ppm of alkali metals or alkaline earth metals. Through the use of such binders, the catalytic activity, for example, of titanium silicalite can be negatively affected since the catalytically active Ti centers are deactivated by the alkali metal ions or alkaline earth metal ions. Accordingly, it is an object of the present invention to provide a molded article containing at least one porous oxide material and having sufficient mechanical stability to be used as a catalyst in a fixed bed. When used for catalytic reactions, losses of activity or selectivity due to side reactions of the aggregate binder should be avoided in comparison with prior art catalysts. A process for its production is also provided. We have surprisingly found that this object is achieved and, a molded article containing at least one porous oxide material and having virtually no loss of activity or selectivity, or no loss whatsoever, when used as a catalyst, can obtained if a mixture containing at least one alcohol and water is used as a paste-forming agent for its production. Further improved molded articles of the type discussed herein are obtained if a metallic acid ester or a mixture of two or more of these is employed as the binder in addition to the above-defined paste-forming agent. Accordingly, the present invention relates to a molded article containing at least one porous oxide material and obtainable through a process comprising the following steps: (I) addition of a mixture containing at least one alcohol and water to a mixture containing a porous oxide material or a mixture of two or more of them and (II) kneading, molding, drying and calcination of the mixture according to step (I) after the addition, and (III) a process for the production of a molded article containing at least one porous oxide material, comprising the following steps: (I) adding a mixture containing at least one alcohol and water to a mixture containing a porous oxide material or a mixture of two or more of them and (II) knead, mold, dry and. calcining the mixture according to step (I) after addition. The novel preparation of the molded articles described above starting from a porous oxide material in powder comprises the formation of. a plastic material containing at least one porous oxide material, a binder, a mixture containing at least one alcohol and water, if one or more organic substances that increase the viscosity and additional additives of the prior art are required. The plastic material obtained by the complete mixing, particularly kneading, of the aforementioned components is preferably molded through pressing and extrusion or extrusion and the resulting molded article is then dried and finally calcined. There are no particular restrictions as regards the porous oxide materials that can be used for the production of the novel molded article, to the extent that it is possible to prepare a molded article according to what is described here starting from these materials. The porous oxide material is preferably a zeolite, particularly a zeolite containing titanium, zirconium, chromium, niobium, iron or vanadium, particularly a titanium silicalite. Zeolites are known to be crystalline aluminosilicates having ordered channel and cage structures that have micropores. The term micropores as used in the present invention corresponds to the definition Puré Appl.

Chem. 45 (1976), page 71 et seq., Particularly page 79, and refers to pores having a diameter of less than 2 nm. The network of such zeolites is composed of tetrahedra of SI04 and A10, linked through common oxygen bridges.

A general presentation of the known structures is offered, for example, in the Atas of Zeolite Structure Types (Atlas of Types of Zeolite Structures), by W. M. Meier and D.H. Olson Elsevier, fourth edition, London, 1996. There are also zeolites that do not contain aluminum and in which one of the Si (IV) has been replaced by titanium as Ti (IV) in the silicate lattice. Titanium zeolites, in particular those with a crystal structure of the MFI type and possibilities for their preparation, are described, for example, in EP-A 0 311 983 or EP-A 0 405 978. Apart from silicone and of titanium, such materials may also contain additional elements, for example aluminum, zirconium, tin, iron, cobalt, nickel, gallium, boron or even small amounts of fluorine. In the zeolites. described, some or all of the titanium itself may be replaced by vanadium, zirconium, chromium, niobium or iron. The molar ratio between titanium and / or vanadium, zirconium, chromium, niobium, or iron and the sum of silicon and titanium and / or vanadium, zirconium, niobium or iron is generally from 0.01: 1 to 0.1: 1. Titanium zeolites having the structure of MFI are known to be identifiable by a certain pattern in terms of X-ray diffraction photographs and in addition by a structural vibration band in the infrared (IR) region at approximately 960 cm-1 and by consequently they differ from alkali metal titanates or crystalline and amorphous Ti02 phases. Usually, the established titanium, zirconium, chromium, niobium, iron and vanadium zeolites are prepared by the reaction of an aqueous mixture comprising a source of Si04, a source of titanium, zirconium, chromo niobium, iron or vanadium, for example, titanium dioxide, or a corresponding vanadium oxide, zirconium alcoholate, chromium oxide, niobium oxide or iron oxide, and an organic base containing nitrogen as quenched, for example, tetrapropylammonium hydroxide, if necessary also with addition of basic compounds, in a pressure resistant container at elevated temperature for several hours or several days, forming a crystalline product. This is filtered, washed, dried and subjected to combustion at elevated temperatures in order to remove the organic nitrogen base. In the powder obtained in this way, some or all of the titanium or zirconium, chromium, niobium, iron and / or vanadium is present within the zeolite structure in various quantities with 4.5 or 6-fold coordination. To improve the catalytic behav a repeated washing with a hydrogen peroxide solution containing sulfuric acid can be carried out subsequently, after which the zeolite powder of titanium or zirconium, chromium, niobium, iron or vanadium must be dried again and subjected to combustion; this can be followed by a treatment with alkali metal compounds in order to convert the zeolite from the H form to the cationic form. The powder of titanium zeolite, or zirconium, chromium, niobium, iron or vanadium prepared in this way is then processed to provide the molded article according to what is described below. Preferred zeolites are titanium, zirconium, chromium, niobium, or vanadium zeolites, especially those having a pentasyl zeolite structure particularly those types assigned by X-ray analysis to the structures BEA, MOR, TON, MTW, FER, MFI, MEL, CHA, ERI, RHO, GIS, BOG, NON, EMT, HEU, KFI, FAU, DDR, MTT, RUT, LTL, MAZ, GME, NES, OFF, SGT, EUO, MFS, MCM-22 or well to the mixed structure MFI / MEL. Zeolites of this type are described, for example, in the aforementioned publication of Meier and Olson. Zeolites containing titanium having the structure UDT-1, CIT-1, CIT-S, ZSM-48, MCM-48, ZSM-12, ferrierite, beta-zeolite or mordenite are also possible for the present invention. Such zeolites are described, for example, in US-A 5,430,000 and in WO 94/29408, the contents of which in this context are fully incorporated by reference in the present Application. There are also no particular restrictions as to the pore structure of the novel molded articles, ie, novel molded articles can have micropores, mesopores, macropores, micropores and mesopores, micropores and macropores, or micropores, mesopores, and macropores, the The definition of the terms mesopores and macropores also corresponds to the definitions stated in the aforementioned literature according to Puré Appl. Chem. And they refer to pores that have a diameter of >2 nm to about 50 nm and greater than about 50 nm, respectively. In addition, the novel molded article may be a material based on an oxide containing mesoporous silicon and a xerogel containing silicone. The mesoporous oxides containing silicone will also contain Ti, V, Zr, Sn, Cr, Nb or Fe, particularly Ti, V, Zr, Cr, Nb or a mixture of two or more of them, particularly preferred. Suitable binders are, in principle, all the compounds used to date for these purposes. Compounds, particularly oxides of silicon, aluminum, boron, phosphorus, zirconium and / or titanium are preferably used. A particularly interesting binder is silica, where Si02 can be introduced into the forming step as a silica sol or in the form of tetraalkoxysilanes. Magnesium and beryllium oxides, as well as clays, for example, montmorillonites, kaolins, bentonites, haloisites, diquitos, nacruses and anauxites, can also be used as binders. However, a metal acid ester or a mixture of two or more of them is preferably added as a binder in step (I) of the novel product. Particular examples of these are orthosilicic esters, trialkoxysilanes, tetraalkoxytitanates, trialkoxyaluminates, tetraalkoxy zirconates and a mixture of two or more of them. However, tetraalkoxysilanes are preferably used as binders in the present invention. Specific examples of tetramethoxysilane, tetraethoxysilane, tetrapropoxysilane, and tetrabutylisilane, the tetraalkoxytitanium and tetraalkoxyzirconium analogs as well as trimethoxy, triethoxy-, tripropoxy- and tributoxyaluminium, tetramethoxysilane and tetraethoxysiline are especially preferred. The novel molded article preferably contains up to about 80, particularly preferably from about 1 to about 50% by weight and particularly from about 3 to about 30% by weight of the binder, in each case based on the total mass of the molded article, The content of binders is calculated from the amount of metal oxide formed. The metal acid ester used is preferably used in an amount such that the resulting metal oxide content in the molded article is from about 1 to about 80% by weight, preferably from about 2 to about 50% by weight, particularly from about 3 to about 30% by weight, based on the total mass of the molded article. As already evident from the foregoing, mixtures of two or more of the aforementioned binders can obviously also be used. It is essential for the present invention that a mixture containing at least one alcohol and water be used as a paste-forming agent in the production of the novel molded article. The alcohol content of this mixture is generally from about 1 to about 80% by weight, preferably from about 5 to about 70% by weight, particularly from about 10 to about 60% by weight, in each case based on the total weight of the mixture. The alcohol used corresponds preferably to the alcohol component of the metal acid ester preferably used as a binder, but it is also not critical to use another alcohol. There are no restrictions on the alcohols that can be used, provided they are miscible in water. Accordingly, both monoalcohols of 1 to 4 carbon atoms and polyhydric alcohols miscible with water can be used. Particularly, . methanol, ethanol, propanol, N-butanol, isobutanol, tert-butanol, and mixtures of two or more of them may be employed. The organic substance which increases the viscosity employed can be any substance of the prior art suitable for this purpose. Preferred substances are organic polymers, particularly hydrophilic, for example cellulose, starch, polyacrylates, polymethacrylates, polyvinyl alcohol, polyvinyl pyrrolidone, polyisobutene and polytetrahydrofuran. These substances primarily promote the formation of plastic material during the kneading, molding, and drying by creating bridges between the primary particles and also ensuring the mechanical stability of the molded article during molding and drying. These substances are removed from the molded product during calcination. Amines or amine-type compounds, for example tetraalkylammonium compounds or aminoalcohols, and carbonate-containing substances, such as for example calcium carbonate, can be used as additional additives. Such additional additives are described in EP-A 0 389 041, EP-A 0 200 260 and WO 95/19222, which are incorporated by reference in the context of the present Application. Instead of basic additives, acidic additives can also be used. These can effect, among other things, a faster reaction of the metal acid ester with the porous oxide material. Organic acid compounds that can be burned by calcination after the molding step are preferred compounds. Especially preferred are carboxylic acids. It is obviously also possible to incorporate mixtures of two or more of the aforementioned additives. The order of addition of the components of the material containing the porous oxide material is not a critical factor. It is possible to add the binder first, then the substance that increases the viscosity, and, if required, the additive, and finally the mixture containing at least one alcohol and water, or change the order in terms of the binder, organic substance that it increases the viscosity, and the additive. After the addition of the binder to the porous oxide powder to which the organic substance which increases the viscosity may have already been added, the material generally still in powder is homogenized for a period of 10 to 180 minutes in a kneader or in an extruder . In general terms, temperatures of about 10 ° C up to the boiling point of the pulping agent and atmospheric pressure or slightly superatmospheric pressure are employed. The remaining components are then added and the mixture obtained is kneaded until the formation of a plastic material capable of being molded in an extrusion press or in an extruder. In principle, kneading and molding can be achieved by employing all conventional kneading and molding apparatus or methods, many of which are presented in the prior art and are generally employed for the production, for example, of molded articles including catalysts. As indicated above, however, the preferred processes are processes in which molding is achieved by extrusion in conventional extruders, for example, to provide extruded products having a diameter, usually from about 1 to about 10 nm, particularly from about 2 to about 5 mm. Such extrusion apparatuses are described, for example, in Ullmann's Enzylopadie der Technischen Chemie (Ullman's Encyclopedia of Technical Chemistry), fourth edition, volume 2, page 295 et seq., 1972. In addition to the use of an extruder, it is also possible to use extrusion press for molding. After the end of the extrusion or extrusion pressing, the resulting molded articles are dried, generally at the temperature of 30 to 140 ° C (from about 1 to 20 hours at atmospheric pressure) and calcined at a temperature of about 400 to about 800 °. C (for approximately 3 to 10 hours at atmospheric pressure). The resulting molded products or extruded products can obviously be ground. They are preferably ground to provide granules or flakes having a particle diameter of 0.1 to 5 mm, particularly 0.5 to 2 mm. These granules or these flakes and also molded products produced by another method contain virtually no finer particles or fractions than those having a minimum particle diameter of approximately 0.1 mm. The molded articles according to the present invention contain a porous oxide material or produced by the novel process which have an improved mechanical stability while at the same time retaining the activity and selectivity in comparison with the molded articles of the corresponding prior art. The articles molded according to the present invention or produced according to the invention can be used for the catalytic conversion of organic molecules. Reactions of this type are, for example, oxidations, epoxidation of olefins, for example, the preparation of propylene oxide from propylene and H202, the hydroxylation of aromatics, such as for example hydroquinone from phenol and H202, the conversion of alkanes to alcohols, aldehydes and acids, isomerization reactions, for example, the conversion of epoxide to aldehydes, and further reactions described in the literature with such molded articles, particularly, zeolite catalysts, in accordance with what is described, for example, in W. Holderich, Zeolites : Catalysts for the Synthesis of Organic Compounds, (Zeolites: Catalysts for the Synthesis of Organic Compounds), Elsevier, Stud. Surfing. Sci. Catal., 49, Amsterdam (1989), pages 69 to 93 and, particularly, for possible oxidation reactions by B. Notari in Stud. Surfing. Sci. Catal., 37 (1987), 413 to 425. The zeolites discussed with details discussed above are especially suitable for the epoxidation of olefins, preferably those having from 2 to 8 carbon atoms, with special preference, ethylene, propylene. or butene, particularly propene, in order to offer the corresponding olefin oxides. Accordingly, the present invention relates to the use of the molded article described herein for the preparation of propylene oxide starting from propylene and hydrogen peroxide. The present invention in its most general embodiment refers to the use of a mixture containing at least one alcohol and water as a paste-forming agent, preferably in combination with a metal acid ester as a binder, for the preparation of mouldable mixtures which they contain at least one porous oxide material. EXAMPLES Example 1 910 g of tetraethyl orthosilicate were initially taken in a 4-neck 4-liter bottle and 15 g of tetraisopropyl orthotitanate were added from a dropping funnel over the course of 30 minutes with stirring (250 revolutions per minute). , stirrer blade). A clear, colorless mixture was formed. Then, 1600 g of a 20% by weight tetrapolyammonium hydroxide solution were added. (alkali metal content less than 10 ppm) and stirring continued for an additional hour. The alcohol mixture (approximately 900 g) formed from the hydrolysis was removed by distillation at a temperature of 90 to 100 ° C. The mixture was completed with 3 liters of water and the meanwhile slightly opaque sol was transferred to a stirred 5 liter stainless steel autoclave. The closed autoclave (anchor stirrer, 200 revolutions per minute) was brought to a reaction temperature of 175 ° C at a heating rate of 3 ° C / minute. The reaction ended after 92 hours. The cooled reaction mixture (white suspension) was centrifuged and the pellet was washed several times with water until neutral. The solid obtained was dried at a temperature of 110 ° C in the course of 24 hours (weight obtained: 298 g). The tempering remaining in the zeolite was then burned in air at a temperature of 550 ° C in 5 hours (loss by calcination: 14% by weight). In accordance with the wet chemical analysis, the pure white product had a Ti content of 1.5% by weight and a residual alkaline content of less than 100 ppm. The yield was 97%, based on Si02 used. The crystallites had a size of 0.05 to 0.25 μm and the product presented a typical band at approximately 960 cm-1 in IR. Example 2 120 g of a titanium silicalite powder, synthesized according to example 1, were mixed with 48 g of tetramethoxysilane for 2 hours in a kneader. Then 6 g of Walocel (methylcellulose) were added. For conversion into a paste, 77 ml of a water / methanol mixture containing 25% by weight of methanol was then added. The material obtained was compacted for an additional 2 hours in a kneader and then molded in an extrusion press to provide molded articles of 2ml. The molded articles obtained were. dried at a temperature of 120 ° C for 16 hours and then calcined at a temperature of 500 ° C for 5 hours. The lateral compression force of the resulting molded articles was tested. The lateral compression force was 4.11 kg. 10 g of the molded articles obtained - in this way they were processed to provide flakes (particle size 1-2 mm) and used as catalyst A in the epoxidation of propylene with hydrogen peroxide. Comparative Example 1 120 g of titanium silicalite powder, synthesized according to example 1, were mixed with 48 g of tetramethoxysilane for two hours in a kneader. Then 6 g of Walocel (methylcellulose) were added. For its conversion into a paste, 80 ml of water was added. The material obtained was compacted for an additional 2 hours in the kneader and then molded in an extrusion press to provide 2 mm molded articles. The molded articles obtained were dried at 120 ° C for 16 hours and then calcined at 500 ° C for 5 hours. The lateral resistance to compression of the resulting articles was tested. The lateral resistance to compression was 3.59 kg. 10 g of the articles molded in this way were processed to provide flakes (particle size: 1-2 mm) and used as catalyst B in the epoxidation of propene with hydrogen peroxide. Example 3 120 g of titanium silicalite powder, synthesized according to Example 1, were dried and mixed with 6 g of Walocel (methyl cellulose) and this combination was mixed with 48 g of tetraethoxysiline for 30 minutes in a kneader. For its conversion into paste, 75 ml of a water / ethanol mixture containing 50% by weight of ethanol was then added. The material obtained was compacted for an additional hour in the kneader and then molded in an extrusion press to provide molded articles of 2 mm. The molded articles obtained were dried at a temperature of 120 ° C for 16 hours and then calcined at a temperature of 500 ° C for 5 hours. The lateral resistance to compression of the resulting molded articles was tested. The lateral resistance to compression was 3.08 kg. 10 g of the molded articles obtained in this way were processed to provide flakes (particle size: l-2 mm) and used as catalyst C in the epoxylation of propene with hydrogen peroxide. Comparison example 2 120 g of titanium silicalite powder were mixed, synthesized in accordance with Example 1, with 48 g of tetraethoxysilane for 2 hours in "a kneader." Then 6 g of Walocel (methyl cellulose) were added.To be converted into a paste, 79 ml of water were then added. obtained was compacted for an additional hour in the kneader and then molded in an extrusion press to provide molded articles of 2 mm The molded articles obtained were dried at a temperature of 120 ° C for 16 hours and then calcined at a temperature of 500 ° C for 5 hours The lateral resistance to compression of the resulting molded articles was tested The lateral resistance to compression was 1.92 kg 10 g of the molded articles obtained in this way were processed to provide flakes (particle size) : 1- 2 mm) and used as catalyst D in the epoxidation of propene with hydrogen peroxide Comparative example 3 120 g of powder were compacted titanium silicalite, synthesized according to example 1, with 6 g of Walocel (methyl cellulose), 30 g of silica sol (Ludox AS-40) and 85 ml of water to provide molded articles of 2 mm. The molded articles obtained were dried at a temperature of 120 ° C for 16 hours and then calcined at a temperature of 500 ° C for 5 hours. The lateral resistance to compression of the resulting molded articles was tested. The lateral resistance to compression was 0.89 kg. 10 g of the molded articles obtained in this way were processed to obtain flakes (particle size: 1-2 mm) and used as catalyst E in the epoxidation of propene with hydrogen peroxide. Examples 4 to 8 Catalysts A to E were installed in a steel autoclave with basket insert and gas removal stirrer in each case in an amount in grams such that the weight of the installed titanium silicalite was 0.5 g. The autoclave was filled with 100 g of methanol, closed and tested to determine the presence of leaks. It was then heated to a temperature of 40 ° C, and 11 g of liquid propene was added in the autoclave. Then, 9.0 g of an aqueous hydrogen peroxide solution (hydrogen peroxide content of the solution: 30% by weight) were pumped into the autoclave by means of an HPLC pump, and the residuals of hydrogen peroxide in the lines of feedings were then rinsed in the autoclave by means of 16 ml of methanol. The initial hydrogen peroxide content of the reaction solution was 2.5% by weight. After a reaction time of 2 hours, the autoclave was cooled and its pressure decreased. The discharge of liquid was investigated cerimétricamente to determine the peroxide of hydrogen. The analysis and determination of propylene oxide content were carried out by gas chromatography. Catalyst content of oxide content of peroxide Propylene (% in residual hydrogen (% Weight) by weight) A 1.42 0.99 B (comparison) 1.19 1.12 C 1.28 1.10 D (comparison) 1.15 1.20 E (comparison) 1.49 0.98

Claims

CLAIMS A molded article containing at least one zeolite and obtainable by a process comprising the following steps: (I) adding a mixture containing at least one alcohol and water to a mixture containing a zeolite or a mixture of two or several, and (II) kneading, molding, drying and calcination in accordance with step (I) after the addition.
A molded article according to claim 1, wherein the at least one zeolite is a zeolite of titanium, zirconium, chromium, niobium, iron, or vanadium, and particularly a titanium silicalite.
A process for the production of a molded article containing at least one zeolite, comprising the following steps: (I) adding a mixture containing at least one alcohol and water to a mixture containing a zeolite or a mixture of two or several, and (II) kneading, molding, drying, and calcining the mixture according to step (I) after the addition.
A process according to claim 3, wherein the at least one zeolite is a zeolite of titanium, zirconium, chromium, niobium, iron, or vanadium and particularly a titanium silicalite.
5. A process according to claim 3, or according to claim 4, wherein a metallic acid ester or a mixture of two or more of them is added further to the mixture in step (I).
6. A process according to claim 5, wherein the metal acid ester is selected from the group consisting of an orthosium ester, a tetraalkoxysilane, a tetraalkoxytitanate, a trialkoxyaluminate, a tetraalcoxyzirconate, and a mixture of two or more of them. •
7. A process according to any of claims 3 to 6, wherein the organic hydrophilic polymer or a mixture of two or more of them is added further to the mixture in step (I).
8. A process according to any of claims 5 to 7, wherein the alcohol in the mixture containing at least one alcohol and water corresponds to the alcohol in the metal acid ester.
9. A compliance process. with any of claims 3 to 8, wherein the mixture obtained in step (I) is molded by pressure and extrusion or extrusion.
10. A process according to any of claims 3 to 9, wherein the molded article containing a zeolite has micropores, mesopores, macropores, micropores and mesopores, micropores and macropores, or micropores, mesopores and macropores. . The use of the molded article according to claim 1, either according to claim 2, or the use of a molded article produced by a process according to claim as claimed in any of claims 3 to 10, or use of a mixture of two or more thereof for the epoxidation of organic compounds having at least one CC double bond for the hydroxylation of aromatic organic compounds, or for the conversion of alkanes to alcohols, ketones, aldehydes and acids. . The use of the molded article according to claim 1, or according to claim 2, or the use of a molded article produced by a process according to claim as claimed in any of claims 3 to 10 for the epoxidation of an olefin, preferably for the preparation of propylene oxide starting from propylene and hydrogen peroxide. . The use of a mixture containing at least one alcohol and water as a paste-forming agent, preferably in combination with a metallic acid ester as a binder, for the preparation of a mouldable mixture containing at least one zeolite.