Zeolite synthesis in a reactor with controlled velocity profile

Abstract

The present invention relates to a process for preparing a zeolitic material, as well as to the catalyst itself obtainable or obtained according to said process. The present invention also relates to the use of said zeolitic material, in particular as a catalyst.

Description

Technical Field

[0001] The present invention relates to a process for preparing a zeolitic material, as well as to the catalyst itself obtainable or obtained according to said process. The present invention also relates to the use of said zeolitic material, in particular as a catalyst.

[0002] introduction

[0003] The synthesis of zeolitic materials by simple starting compounds involves a complex self-organizing process, which usually requires special conditions, such as elevated temperature and / or pressure, wherein these reactions usually require heating of raw materials under autogenous pressure to obtain zeolitic materials after a long reaction time of several days to several weeks. Accordingly, due to common harsh reaction conditions and long reaction time, batch synthesis has long been the method selected for the synthesis of zeolitic materials. But batch reaction brings many restrictions, particularly about the level of achievable space-time yield.

[0004] Efforts have therefore been made to find improved batch reaction procedures and alternative methods that offer advantages over the classical batch synthesis procedures for the synthesis of zeolitic materials. One method that has been investigated in this regard involves the use of a continuous stirred tank reactor, wherein fluid reagents are continuously introduced at the top of the tank reactor and an effluent containing the solid reaction product is continuously withdrawn from the bottom of the tank reactor. Although such a method eliminates the need to empty the reaction vessel between batch runs under discontinuous conditions, the reaction time required for crystallization is still very long.

[0005] In view of this, reactor geometries capable of rapidly synthesizing zeolite materials have been conceived. Thus, US 2016 / 0115039 A1 relates to a method for continuously producing zeolites in a tubular reactor exhibiting a low volume / lateral surface area ratio. Similarly, Liu et al. disclosed in Angew.Chem.Int.Ed.2015,54,5683-5687 the continuous synthesis of high-silicon zeolite SSZ-13 using extremely short reaction times. On the other hand, Ju, J. et al. in Chemical Engineering Journal 2006,116,115-121 and Vandermeersch, T. et al. in Microporous and Mesoporous Materials 2016,226,133-139 respectively disclosed the rapid synthesis of micron-sized NaA zeolite in a continuous flow reactor setting. Liu, Z. et al. in Chemistry of Materials 2014,26,2327-2331 relate to crystalline microporous aluminophosphate AlPO 4-5 ultrafast continuous flow synthesis. Slangen et al. "Continuous Synthesis of Zeolites using a Tubular Reactor", 12 th International Zeolites Conference, Materials Research Society 1999 relates to the continuous synthesis of NaA zeolite, NaY zeolite and silicalite-1 in a tubular reactor of 6 mm outer diameter (~3 mm inner diameter) and variable length. Bebon, C. et al., Microporous and Mesoporous Materials 2002, 53, 13-20, relate to a method for synthesizing zeolites using a guide tube contained in an autoclave, wherein the reaction mixture is conveyed through the guide tube by means of an Archimedean screw disposed in the guide tube along its axis.

[0006] For reactions that do not require high pressure, microwave-assisted procedures have been studied, such as Bonaccorsi, L. et al. in Microporous and Mesoporous Materials 2008, 112, 481-493, which relates to the continuous synthesis of zeolite LTA. Similarly, US 2001 / 0054549A1 relates to a continuous method and apparatus for preparing inorganic materials using microwaves.

[0007] Although significant progress has been made in reaction efficiency due to the use of continuous stirred tanks and multistage reactors, progress in reducing reaction times has been limited to reactor geometries used at the laboratory scale level. In addition, efforts to reduce reaction times have been very limited in terms of economically viable operating durations due to reactor clogging and, in particular, due to the significant changes in the rheology of the reaction mixture that occur during the zeolite synthesis process. More specifically, after heating in a tubular reactor with laminar flow, the synthesis gel generally exhibits high shear rates in the region near the walls, while the center exhibits almost no shear rate due to the slow heat transfer rate toward the center and, in particular, due to the insulating effect of the synthesis gel in the region near the walls. As a result, the synthesis gel exhibits a large temperature gradient from the wall region to the center, and a large residence distribution time is observed. In view of the severe inhomogeneous processing of the synthesis gel caused by this situation, it is necessary to use very long reactors to obtain satisfactory crystallinity.

[0008] Thus, despite the progress that has been made in the continuous synthesis of zeolitic materials, there remains a need for methods that avoid the problems of poor heat transfer and the attendant non-uniform reaction conditions experienced by the synthesis gel in the reactor.

[0009] Details

[0010] It is therefore an object of the present invention to provide an improved process for the preparation of zeolitic materials which enables uniform shear rates and temperature gradients of the synthesis gel in the reactor, particularly at an industrial scale. Thus, it has been surprisingly found that, depending on whether the reaction mixture exhibits shear-thinning or shear-thickening rheology during crystallization, by using a flow regimen with a specific velocity profile in the reactor, it is possible to obtain improved uniformity in terms of temperature and shear rate gradients of the synthesis gel in the flow direction. In particular, it has been quite unexpectedly found that, by generating a velocity profile of the reaction mixture in the reactor which is substantially opposite to the velocity profile generated by laminar flow of the same reaction mixture through a tubular reactor, an improved uniformity of the crystallization rate of the mixture in the reactor and of the transport rate of the mixture in the reactor is obtained, so as to avoid the significant disadvantages of uneven crystallization and mass transfer which occur in the conventional synthesis of zeolitic materials, particularly in continuous synthesis processes.

[0011] Therefore, the present invention relates to a method for preparing a method comprising YO 2 and optionally contains X 2 O 3 A method for preparing a zeolite material having a framework structure, wherein Y is a tetravalent element and X is a trivalent element, the method comprising

[0012] (i) Preparation of YO 2 Source, optional X 2 O 3 a mixture of a source and a liquid solvent system;

[0013] (ii) supplying the mixture prepared in (i) as a reaction mixture into a reactor;

[0014] (iii) heating the reaction mixture in the reactor to obtain a mixture containing YO 2 and optionally contains X 2 O 3 a reaction mixture of a zeolite material having a framework structure; and

[0015] (iv) collecting the reaction mixture obtained in (iii) containing the zeolitic material as an effluent from the reactor;

[0016] wherein in (iii) shear is applied to the reaction mixture to establish a flow of the reaction mixture relative to the outer wall of the reactor in contact with the reaction mixture, and

[0017] Wherein in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (I):

[0018] v(r)≤((v(r1 )-v min )·(r / r 1 ))+v min (I)

[0019] and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (II):

[0020] v(r)≥((v(r 1 )-v min )·(r / r 1 ))+v min (II)

[0021] wherein r defines the length of a straight line on the cross-sectional area of ​​the reactor space perpendicular to the flow direction of the reaction mixture in the reactor, wherein the straight line extends from a first point on the inner surface of the reactor wall in contact with the mixture to a second point, wherein at the first point r 0 is set to 0 and v exhibits its minimum value (v min =v(r 0 )), at the second point r is defined as r max And v shows its maximum value (v max =v(r max )), where r 1 =r max / x, x=5, preferably x=4, more preferably x=3, more preferably x=2.5, more preferably x=2, more preferably x=1.8, more preferably x=1.6, more preferably x=1.5, more preferably x=1.4, more preferably x=1.3, more preferably x=1.2, more preferably x=1.1, more preferably x≥1, wherein more preferably r=r max .

[0022] The straight line r is preferably perpendicular to the inner surface of the reactor wall which is in contact with the reaction mixture.

[0023] Preferably, in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (III):

[0024] v”(r)≥0 (III)

[0025] and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (IV):

[0026] v”(r)≤0 (IV).

[0027] In case the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the velocity profile v(r) of the reaction mixture in the flow direction preferably satisfies the condition according to (V):

[0028] v(r)<((v(r 1 )-v min )·(r / r 1 ))+v min (V)

[0029] Where 0 <r<r max , and wherein in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (VI):

[0030] v(r)>((v(r 1 )-v min )·(r / r 1 ))+v min (VI)

[0031] Where 0 <r<r max .

[0032] Preferably, in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (VII):

[0033] v”(r)>0 (VII)

[0034] Where 0 <r<r max , and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (VIII):

[0035] v”(r)<0 (VIII)

[0036] Where 0 <r<r max .

[0037] Furthermore and in addition, the present invention also relates to the preparation of a 2 and optionally contains X 2 O 3 A method for preparing a zeolite material having a framework structure, wherein Y is a tetravalent element and X is a trivalent element, the method comprising

[0038] (i) Preparation of YO 2 Source, optional X 2 O 3 a mixture of a source and a liquid solvent system;

[0039] (ii) supplying the mixture prepared in (i) as a reaction mixture into a reactor;

[0040] (iii) heating the reaction mixture in the reactor to obtain a mixture containing YO 2 and optionally contains X 2 O 3 a reaction mixture of a zeolite material having a framework structure; and

[0041] (iv) collecting the reaction mixture obtained in (iii) containing the zeolitic material as an effluent from the reactor;

[0042] The reactor is a Taylor-Couette reactor comprising coaxially aligned inner and outer cylinders.

[0043] In (iii), preferably the flow regime in at least one portion P of the reactor volume is laminar, wherein said portion P is preferably an uninterrupted portion of the reactor volume. Preferably, in (iii), the Reynolds number (Re) in at least said portion P of the reactor volume accommodating the reaction mixture is 2,500 or less, more preferably 2,000 or less, more preferably 1,500 or less, more preferably 1,000 or less, more preferably 500 or less, more preferably 300 or less, more preferably 200 or less, more preferably 100 or less, more preferably 80 or less, more preferably 60 or less, more preferably 40 or less, more preferably 20 or less, more preferably 10 or less, more preferably 5 or less, more preferably 3 or less, more preferably 1 or less. The term Reynolds number (Re) as used herein means Re=u ax ·d gap / n; where u ax is the axial velocity of the liquid used, n is the dynamic viscosity and d gap is the gap width in a reactor, preferably between rotating drums in a reactor; axial is thereby in the sense of being aligned with the axis of rotation of the drums in the reactor, preferably a Taylor-Couette reactor.

[0044] Preferably, the Taylor number (Ta), more preferably the tangential Taylor number in at least the portion P of the reactor volume accommodating the reaction mixture in (iii) satisfies the condition according to (III):

[0045] Ta≤(1.52·Re)+n (III)

[0046] wherein n≤102, preferably ≤100, more preferably ≤98, more preferably ≤95, more preferably ≤90, more preferably ≤80, more preferably ≤60, more preferably ≤40, more preferably ≤20, more preferably ≤10, more preferably ≤5, more preferably ≤1. The term Taylor number (Ta) as used herein refers to Ta=r i ·u i ·d gap / n, where n is the dynamic viscosity, ri is the radius of the inner cylinder, and u i is the rotation speed of the inner cylinder, d gap is the gap width in the reactor, preferably the gap width between the rotating drums in the reactor; wherein the reactor is preferably a Taylor-Couette reactor. The tangential Taylor number used herein refers to the Taylor number (Ta) further defined for the tangential flow relative to the reactor, preferably the rotating drum wall of the Taylor-Couette reactor.

[0047] Preferably, the uninterrupted portion P of the reactor volume preferably constitutes 5 to 100%, more preferably 10 to 95%, more preferably 20 to 90%, more preferably 30 to 85%, more preferably 40 to 80%, more preferably 50 to 75%, more preferably 60 to 70% of the total volume of the reactor containing the reaction mixture.

[0048] Preferably, the reaction mixture exhibits a shear-thinning rheology (pseudoplastic rheology) or wherein the reaction mixture exhibits a shear-thinning rheology (dilatant rheology), wherein the reaction mixture preferably exhibits a shear-thinning rheology (pseudoplastic rheology).

[0049] Regarding step (iii), the mixture is heated to a temperature of preferably 100 to 300°C, more preferably 120 to 280°C, more preferably 140 to 260°C, more preferably 160 to 250°C, more preferably 180 to 240°C, more preferably 190 to 230°C, more preferably 200 to 220°C.

[0050] Regarding the reactor, the volume of the reactor accommodating the reaction mixture is preferably 5 cm3 to 1 m3, more preferably 10 cm3 to 1 m3, more preferably 20 cm3 to 0.5 m3, more preferably 30 cm3 to 0.1 m3, more preferably 50 cm3 to 0.05 m3, more preferably 80 cm3 to 0.01 m3, more preferably 100 to 5,000 cm3, more preferably 120 to 3,000 cm3. 3 , more preferably 150 to 1,000 cm 3 , more preferably 200 to 700 cm 3 , more preferably 230 to 500 cm 3 , more preferably 250 to 300 cm 3Preferably, the inner surface of the reactor wall in contact with the mixture is made of a metal material, wherein the metal material comprises one or more metals selected from Ta, Cr, Fe, Ni, Cu, Al, Mo and combinations and / or alloys thereof, more preferably selected from Ta, Cr, Fe, Ni, Mo and combinations and / or alloys thereof, preferably selected from Cr, Fe, Ni, Mo and combinations and / or alloys thereof, wherein the metal material preferably comprises a nickel alloy, a nickel-molybdenum alloy, more preferably a nickel-molybdenum-chromium alloy. Preferably, the inner surface of the reactor wall in contact with the mixture is lined with an organic polymer material, wherein the organic polymer material more preferably comprises one or more polymers selected from fluorinated polyolefins and mixtures of two or more thereof, preferably selected from (C2-C3) polyolefins and mixtures of two or more thereof, preferably selected from fluorinated polyethylene and mixtures of two or more thereof, wherein the polymer material more preferably comprises poly(tetrafluoroethylene), wherein the reactor inner wall is more preferably lined with poly(tetrafluoroethylene).

[0051] As for step (iii), the reaction mixture is preferably heated under autogenous pressure in (iii), wherein the pressure is preferably in the range of 0.1 to 9 MPa, more preferably in the range of 0.5 to 7 MPa, more preferably in the range of 0.8 to 5 MPa, more preferably in the range of 1.3 to 3 MPa, more preferably in the range of 1.4 to 2 MPa, more preferably in the range of 1.5 to 1.7 MPa.

[0052] The reactor preferably consists of a single stage. Preferably, no material is added to the reaction mixture and / or no material is removed from the reaction mixture during its passage through the reactor in (iii), wherein no material is added, wherein more preferably no material is added and no material is removed from the reaction mixture during its passage through the reactor in (iii).

[0053] Preferably, prior to (ii), the mixture prepared in (i) is aged at a temperature of 40 to 120°C, more preferably 50 to 110°C, more preferably 60 to 105°C, more preferably 70 to 100°C, more preferably 75 to 95°C, more preferably 80 to 90°C. Preferably, in (i) and prior to (ii), the mixture prepared in (i) is not heated to a temperature of 40°C or higher, more preferably 35°C or higher, more preferably 30°C or higher, wherein more preferably in (i) and prior to (ii), the mixture prepared in (i) is not subjected to a heating step. Preferably, prior to (ii), the mixture prepared in (i) is aged for a duration of 1 to 72 h, more preferably 6 to 62 h, more preferably 12 to 56 h, more preferably 24 to 50 h, more preferably 36 to 44 h, more preferably 38 to 42 h.

[0054] The mixture prepared in (i) is preferably fed directly to the reactor in (ii), wherein the mixture prepared in (i) is preheated to a temperature of preferably 100 to 300°C, more preferably 100 to 280°C, more preferably 140 to 260°C, more preferably 160 to 250°C, more preferably 180 to 240°C, more preferably 190 to 230°C, more preferably 200 to 220°C while being fed to the reactor in (ii).

[0055] With regard to the collection of the reacted mixture in (iv), this preferably comprises quenching the reacted mixture effluent leaving the reactor in (iii) with a liquid comprising one or more solvents and / or by expansion of the reacted mixture effluent. Preferably, the liquid used for quenching comprises one or more solvents selected from polar protic solvents and mixtures thereof, more preferably selected from n-butanol, isopropanol, propanol, ethanol, methanol, water and mixtures thereof, more preferably selected from ethanol, methanol, water and mixtures thereof, wherein the liquid more preferably comprises water, and wherein more preferably water is used as liquid, preferably deionized water.

[0056] In the present invention, the method preferably further comprises

[0057] (v) isolating the zeolitic material obtained in (iii) or (iv);

[0058] and / or, preferably and,

[0059] (vi) washing the zeolitic material obtained in (iii), (iv) or (v);

[0060] and / or, preferably and,

[0061] (vii) drying the zeolitic material obtained in (iii), (iv), (v) or (vi);

[0062] and / or, preferably and,

[0063] (viii) calcining the zeolitic material obtained in (iii), (iv), (v), (vi) or (vii).

[0064] If step (v) is carried out, the zeolitic material is preferably separated from the reaction mixture obtained from (iii) or (iv) in (v) by filtration, centrifugation and / or decantation, more preferably by microfiltration and / or ultrafiltration, wherein microfiltration and / or ultrafiltration is more preferably achieved by membrane filtration. The supernatant obtained from the separation of the zeolitic material in (v) is preferably recycled to (i) and / or (ii), more preferably to (i).

[0065] If step (vii) is carried out, the zeolitic material is dried in (vii) preferably by means of microwave irradiation and / or flash drying of the zeolitic material obtained in (iii), (iv), (v) or (vi).

[0066] If steps (vii) and (viii) are carried out, the drying in (vii) and the calcining in (viii) are preferably achieved by one or more steps of calcining the zeolitic material obtained in (iii), (iv), (v) or (vi).

[0067] If step (v) is carried out, the separation of the zeolitic material in (v) preferably comprises a step of spray drying the zeolitic material obtained in (iii) or (iv), and / or wherein the drying of the zeolitic material in (vii) comprises a step of spray drying the zeolitic material obtained in (iii), (iv), (v) or (vi).

[0068] If step (vii) is carried out, the drying in (vii) is preferably carried out at a temperature of 50 to 220°C, more preferably 70 to 180°C, more preferably 80 to 150°C, more preferably 90 to 130°C, more preferably 100 to 125°C, more preferably 110 to 120°C.

[0069] If step (viii) is performed, the calcination in (viii) is preferably carried out at a temperature of 300 to 800°C, more preferably 350 to 750°C, more preferably 400 to 725°C, more preferably 450 to 700°C, more preferably 500 to 675°C, more preferably 550 to 650°C.

[0070] Generally, it is possible to include seed crystals in the method according to the present invention. Preferably, the mixture prepared in (i) further comprises seed crystals, wherein the amount of seed crystals in the mixture prepared in (i) is preferably based on 100 wt % of YO contained in the mixture prepared in (i). 2 The calculated Y is 0.1 to 20 wt %, more preferably 0.3 to 10 wt %, more preferably 0.5 to 5 wt %, more preferably 1 to 3 wt %, still more preferably based on 100 wt % contained in the mixture prepared in (i) as YO 2The calculated Y is 1.5 to 2.5 wt%. Preferably, the seed crystals include one or more selected from AEI, AFX, ANA, BEA, BEC, CAN, CHA, CDO, EMT, ERI, EUO, FAU, FER, GME, HEU, ITH, ITW, KFI, LEV, MEI, MEL, MFI, MOR, MTN, MWW, OFF, RRO, RTH, SAV, SFW, SZR and TON (including a mixture of two or more thereof), more preferably selected from CAN, AEI, EMT, SAV, SZR, KFI, ERI, OFF, RTH, GME, AFX, SFW, BEA, CHA, FAU, FER, HEU, LEV, MEI, MEL, MFI, MOR and MWW (including a mixture of two or more thereof). structure), more preferably selected from the group consisting of AEI, AFX, BEA, CHA, ERI, FAU, FER, GME, LEV, MEL, MFI, MOR and MWW (including a mixed structure of two or more thereof), more preferably selected from the group consisting of AEI, AFX, BEA, CHA, ERI, FER, GME, MEL, MFI, MOR and MWW (including a mixed structure of two or more thereof), more preferably selected from the group consisting of AEI, BEA, CHA, ERI, MFI and MWW (including a mixed structure of two or more thereof), more preferably selected from the group consisting of zeolites having a framework structure of AEI, BEA, CHA, MFI and MWW (including a mixed structure of two or more thereof), wherein the seed more preferably comprises one or more zeolites having a CHA and / or AEI framework structure.

[0071] Typically, the method according to the present invention may include an organic template. Preferably, the mixture prepared in (i) further comprises one or more organic templates. The one or more organic templates are preferably selected from tetraalkylammonium compounds, 1N-alkyl-3-quinuclidine or N,N,N-trialkyl-exo-aminonorbornane and mixtures of two or more thereof, more preferably selected from 1-adamantyltri(C 1 -C 3 ) alkyl-ammonium compounds, N,N,N-tri(C 1 -C 2 )alkyl-(C 5 -C 6 ) cycloalkylammonium compounds, N,N,N-trimethyl-N-benzylammonium compounds and mixtures of two or more thereof, more preferably selected from 1-adamantyltri(C 1 -C 2 ) alkyl-ammonium compounds, N,N,N-tri(C 1 -C 2 )alkyl-cyclopentyl ammonium compounds, N,N,N-tri(C 1 -C2 ) Alkyl-cyclohexylammonium compounds and mixtures of two or more thereof, more preferably selected from 1-adamantyltriethyl-ammonium compounds, 1-adamantyldiethyl-methylalkylammonium compounds, 1-adamantylethyl-dimethylammonium compounds, 1-adamantyltrimethylammonium compounds, N,N,N-triethyl-cyclohexylammonium compounds, N,N-diethyl-N-methyl-cyclohexylammonium compounds, N,N-dimethyl-N-ethyl-cyclohexylammonium compounds, N,N,N-trimethyl-cyclohexylammonium compounds and mixtures of two or more thereof, wherein said one or more organic templates more preferably comprise one or more 1-adamantyltrimethylammonium compounds and / or one or more N,N,N-trimethyl-cyclohexylammonium compounds, wherein said one or more organic templates more preferably comprise one or more N,N,N-trimethyl-cyclohexylammonium compounds. Preferably, the tetraalkylammonium compounds are independently salts, more preferably selected from halides, preferably chlorides and / or bromides, more preferably one or more salts selected from chlorides, hydroxides, sulfates, nitrates, phosphates, acetates and mixtures of two or more thereof, more preferably one or more salts selected from chlorides, hydroxides, sulfates and mixtures of two or more thereof, wherein said one or more tetraalkylammonium compounds are more preferably tetraalkylammonium hydroxides and / or chlorides, even more preferably tetraalkylammonium hydroxides.

[0072] Alternatively, said one or more organic templates are preferably selected from tetraalkyl compounds, more preferably selected from tetra(C 1 -C 6 )alkyl compounds, more preferably selected from tetra(C 1 -C 5 )alkyl compounds, more preferably selected from tetra(C 1 -C 4 )alkyl compounds, more preferably selected from tetra(C 2 -C 3 )alkyl compounds, more preferably selected from tetramethyl compounds, ethyltrimethyl compounds, diethyldimethyl compounds, methyltriethyl compounds, tetraethyl compounds and mixtures of two or more thereof, wherein said one or more organic templates are more preferably selected from tetraethyl compounds.

[0073] Preferably, the mixture prepared in (i) and heated in (iii) does not contain one or more organic templates.

[0074] In the present invention, Y can be any tetravalent element. Y is preferably selected from Si, Sn, Ti, Zr, Ge and a combination of two or more thereof, and Y is more preferably Si. Generally, according to (i), any suitable YO can be used. 2 Preferably, YO 2 The source comprises one or more compounds selected from the group consisting of fumed silica, silica hydrosol, reactive amorphous solid silica, silica gel, silicic acid, water glass, hydrated sodium metasilicate, sesquisilicates, disilicates, colloidal silica, silicates, and mixtures of two or more thereof, more preferably selected from the group consisting of fumed silica, silica hydrosol, reactive amorphous solid silica, silica gel, silicic acid, colloidal silica, silicates, and mixtures of two or more thereof, more preferably selected from the group consisting of fumed silica, silica hydrosol, reactive amorphous solid silica, silica gel, silicic acid, colloidal silica, silicates, and mixtures of two or more thereof, wherein YO 2 Even more preferably, the source comprises fumed silica and / or colloidal silica, preferably colloidal silica.

[0075] In the present invention, X can be any trivalent element. X is preferably selected from Al, B, In, Ga and a combination of two or more thereof, and X is more preferably Al. Generally, according to (i), any suitable X can be used. 2 O 3 Preferably, X 2 O 3 The source comprises alumina, aluminates, aluminum salts and mixtures of two or more thereof, more preferably alumina, aluminum salts and mixtures of two or more thereof, more preferably alumina, tri(C 1 -C 5 )Aluminum alcoholate, AlO(OH), Al(OH) 3 , aluminum halides, preferably aluminum fluoride and / or aluminum chloride and / or aluminum bromide, more preferably aluminum fluoride and / or aluminum chloride, aluminum sulfate, aluminum phosphate, aluminum fluorosilicate, containing [Al 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ Salts of, alkali metal aluminates and mixtures of two or more thereof, more preferably selected from tri(C 2 -C 4 )Aluminum alcoholate, AlO(OH), Al(OH) 3 , aluminum chloride, aluminum sulfate, aluminum phosphate, containing [Al 13 O 4 (OH) 24 (H 2 O) 12 ] 7+Salts of, sodium aluminate, potassium aluminate and mixtures of two or more thereof, more preferably selected from tri(C 2 -C 3 )Aluminum alcoholate, AlO(OH), Al(OH) 3 , aluminum chloride, aluminum sulfate, containing [Al 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ salts, sodium aluminate and mixtures of two or more thereof, more preferably selected from aluminum tripropoxide, AlO(OH), aluminum sulfate, 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ salts thereof, sodium aluminate and mixtures of two or more thereof, more preferably selected from aluminum tripropoxide, AlO(OH), Al(OH) 3 , aluminum sulfate, sodium aluminate and a mixture of two or more thereof.

[0076] Preferably, the mixture prepared in (i) further comprises at least one OH - source, wherein the at least one OH - The source preferably comprises a metal hydroxide, more preferably a hydroxide of an alkali metal M, more preferably sodium hydroxide and / or potassium hydroxide, more preferably sodium hydroxide.

[0077] Including YO 2 Source, optional X 2 O 3 The mixture prepared in (i) of the source and the liquid solvent system, YO of the mixture prepared in (i) 2 :X 2 O 3 The molar ratio is not subject to any specific restrictions. Preferably, YO of the mixture prepared in (i) 2 :X 2 O 3 The molar ratio is 1 to 1,000, more preferably 2 to 500, more preferably 4 to 200, more preferably 5 to 150, more preferably 20 to 100, more preferably 30 to 80, more preferably 40 to 60, and still more preferably 45 to 55.

[0078] Preferably, the liquid solvent system in the mixture prepared in (i) comprises one or more solvents, wherein the liquid solvent system preferably comprises one or more solvents selected from polar protic solvents and mixtures thereof, more preferably selected from n-butanol, isopropanol, propanol, ethanol, methanol, water and mixtures thereof, more preferably selected from ethanol, methanol, water and mixtures thereof, wherein the liquid solvent system more preferably comprises water, and wherein water is more preferably used as the liquid solvent system, preferably deionized water. Preferably, in (i), the liquid solvent system comprises water, wherein the H of the mixture prepared in (i) is 2 O:YO 2 The molar ratio is preferably 1 to 400, more preferably 1 to 300, more preferably 2 to 200, more preferably 2 to 150, more preferably 2 to 100, more preferably 3 to 50, more preferably 4 to 30, more preferably 4.5 to 20, more preferably 5 to 15, more preferably 5.5 to 12, still more preferably 6 to 10.

[0079] As for step (iii), the zeolitic material obtained in (iii) preferably has a zeolite selected from the group consisting of AEI, AFX, ANA, BEA, BEC, CAN, CHA, CDO, EMT, ERI, EUO, FAU, FER, GME, HEU, ITH, ITW, KFI, LEV, MEI, MEL, MFI, MOR, MTN, MWW, OFF, RRO, RTH, SAV, SFW, SZR and TON (including mixed structures of two or more thereof), more preferably selected from the group consisting of CAN, AEI, EMT, SAV, SZR, KFI, ERI, OFF, RTH, GME, AFX, SFW, BEA, CHA, FAU, The zeolite material obtained in (iii) is preferably selected from the framework structure of FER, HEU, LEV, MEI, MEL, MFI, MOR and MWW (including mixed structures of two or more thereof), more preferably selected from the framework structure of BEA, CHA, FAU, FER, GME, LEV, MFI, MOR and MWW (including mixed structures of two or more thereof), more preferably selected from the framework structure of BEA, CHA, GME, MFI, MOR and MWW (including mixed structures of two or more thereof), more preferably selected from the framework structure of BEA, CHA, MFI and MWW (including mixed structures of two or more thereof), wherein the zeolite material obtained in (iii) more preferably has a CHA and / or BEA framework structure, preferably a CHA framework structure.

[0080] Preferably, the mixture prepared in (i) and heated in (iii) consists of a single liquid phase optionally containing a solid phase. Preferably, the mixture heated in the reactor in (iii) is mechanically agitated, wherein more preferably the mechanical agitation is achieved by a moving part contained in the reactor.

[0081] Generally, it is possible to use any reactor according to the method of the present invention. The term "reactor" as used herein refers to any reactor that allows the reaction mixture to flow with a velocity distribution according to the present invention, while allowing the reaction mixture to react and thereby obtain a reaction mixture. Preferably, the reactor is a tubular reactor, and the reactor is more preferably a Taylor-Couette reactor comprising an inner cylinder and an outer cylinder aligned coaxially, wherein the Taylor-Couette reactor preferably has a rotor-stator arrangement, with the outer cylinder being a stator. Preferably, two coaxial cylinders are rotated at a speed of 5 to 5,000rpm relative to each other, more preferably 10 to 3,000rpm, more preferably 30 to 2,500rpm, more preferably 50 to 2,000rpm, more preferably 100 to 1,500rpm, more preferably 150 to 1,200rpm, more preferably 200 to 1,000rpm, more preferably 250 to 800rpm, more preferably 300 to 700rpm, more preferably 350 to 650rpm, more preferably 400 to 600rpm, more preferably 450 to 550rpm. Preferably, the gap between the two coaxial cylinders is in the range of 0.3 to 50 cm, more preferably 0.4 to 30 cm, more preferably 0.5 to 25 cm, more preferably 0.6 to 20 cm, more preferably 0.6 to 15 cm, more preferably 0.7 to 10 cm, more preferably 0.7 to 5 cm, more preferably 0.8 to 3 cm, more preferably 0.8 to 2 cm, more preferably 0.9 to 1.5 cm, more preferably 0.9 to 1.2 cm, more preferably 1.0 to 1.1 cm. Preferably, the diameter of the inner cylinder is in the range of 0.5 to 100 cm, more preferably 1 to 50 cm, more preferably 1.5 to 30 cm, more preferably 2 to 20 cm, more preferably 2.5 to 15 cm, more preferably 3 to 10 cm, more preferably 3.5 to 8 cm, more preferably 4 to 7 cm, more preferably 4.5 to 6 cm, more preferably 5 to 5.5 cm. The length of the two coaxial cylinders is preferably in the range of 5 to 500 cm, more preferably 8 to 300 cm, more preferably 10 to 200 cm, more preferably 12 to 150 cm, more preferably 15 to 100 cm, more preferably 18 to 80 cm, more preferably 20 to 50 cm, more preferably 23 to 35 cm, more preferably 25 to 30 cm. Preferably, the inner cylinder and / or the outer cylinder, more preferably the outer cylinder, is heated to a temperature of 120 to 310° C., preferably 140 to 290° C., more preferably 160 to 270° C., more preferably 180 to 260° C., more preferably 200 to 250° C., more preferably 210 to 240° C., more preferably 220 to 230° C.

[0082] Generally, the method of the present invention can be carried out in continuous mode or batch mode. Preferably, the feeding of the mixture in (ii) and the collection of the reacted mixture in (iv) are carried out in continuous mode and / or in batch mode, more preferably in continuous mode. Preferably, the method is carried out in continuous mode and / or in batch mode, more preferably in continuous mode. The feeding of the mixture in (ii) and the collection of the reacted mixture in (iv) are preferably carried out in continuous mode, with a liquid hourly space velocity in the range of 0.3 to 250 h -1 , more preferably 0.5 to 150 h -1 , more preferably 1 to 100 h -1 , more preferably 2 to 70 h -1 , more preferably 5 to 50 h -1 , more preferably 8 to 30 h -1 , more preferably 10 to 20 h -1 , more preferably 12 to 14 h -1 . Preferably, the mixture is continuously fed into the reactor in (ii) for a duration of at least 1 hour to 10 years, more preferably 6 hours to 8 years, more preferably 12 hours to 7 years, more preferably 1 day to 6 years, more preferably 7 days to 5 years, more preferably 15 days to 4 years, more preferably 1 month to 3.5 years, more preferably 2 months to 3 years, more preferably 4 months to 2.5 years, more preferably 6 months to 2 years, more preferably 8 months to 18 months, more preferably 10 to 14 months.

[0083] The present invention also relates to a zeolite material having a framework structure comprising YO 2 and optionally comprising X 2 O 3 obtainable and / or obtained according to the above method, wherein Y is a tetravalent element and X is a trivalent element.

[0084] Depending on the intended use of the zeolitic material, the material preferably obtained from (iv) can be used as such. In addition, it is conceivable that this zeolitic material is subjected to one or more further post-treatment steps. For example, the zeolitic material more preferably obtained in powder form can be suitably processed into a molded product or a shaped body by any suitable method, including but not limited to extrusion, tableting, spraying, etc. Preferably, the shaped body can have a rectangular, triangular, hexagonal, square, elliptical or circular cross-section, and / or preferably in the form of a star, a thin sheet, a sphere, a cylinder, a strip or a hollow cylinder. When preparing the shaped body, one or more adhesives that can be selected according to the intended use of the shaped body can be used. Possible adhesive materials include but are not limited to, graphite, silicon dioxide, titanium dioxide, zirconium oxide, aluminum oxide and two or more mixed oxides of silicon, titanium and zirconium. The weight ratio of the zeolitic material to the adhesive is generally not subject to any specific restrictions, and can be, for example, in the range of 10:1 to 1:10. According to a further example, whereby the zeolitic material is used as a catalyst or catalyst component, for example for treating exhaust streams, such as engine exhaust streams, the zeolitic material may be used as a component of a washcoat to be applied to a suitable substrate, such as a wall flow filter or the like.

[0085] With YO 2 and optionally contains X 2 O 3 The zeolite material of the present invention having a framework structure in which Y is a tetravalent element and X is a trivalent element can be used for any conceivable purpose, including but not limited to molecular sieves, as adsorbents, for ion exchange, as catalysts and / or as catalyst supports, preferably as catalysts and / or as catalyst supports, or for the preparation of one or more intermediates thereof.

[0086] The present invention is further illustrated by the following set of embodiments and the combination of embodiments resulting from dependencies and back-references as shown. In particular, it is pointed out that in each case where a series of embodiments is mentioned, for example in a term such as "the method of any one of embodiments 1 to 4", it is intended to explicitly disclose each embodiment in this series to the skilled person, i.e. the wording of this term should be understood by the skilled person as synonymous with "the method of any one of embodiments 1, 2, 3 and 4".

[0087] 1. A preparation having a 2 and optionally contains X 2 O 3 A method for preparing a zeolite material having a framework structure, wherein Y is a tetravalent element and X is a trivalent element, the method comprising

[0088] (i) Preparation of YO 2 Source, optional X 2 O 3 a mixture of a source and a liquid solvent system;

[0089] (ii) supplying the mixture prepared in (i) as a reaction mixture into a reactor;

[0090] (iii) heating the reaction mixture in the reactor to obtain a mixture containing YO 2 and optionally contains X 2 O 3 a reaction mixture of a zeolite material having a framework structure; and

[0091] (iv) collecting the reaction mixture obtained in (iii) containing the zeolitic material as an effluent from the reactor;

[0092] wherein in (iii) shear is applied to the reaction mixture to establish a flow of the reaction mixture relative to the outer wall of the reactor in contact with the reaction mixture, and

[0093] Wherein in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (I):

[0094] v(r)≤((v(r 1 )-v min )·(r / r 1 ))+v min (I)

[0095] and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (II):

[0096] v(r)≥((v(r 1 )-v min )·(r / r 1 ))+v min (II)

[0097] wherein r defines the length of a straight line on the cross-sectional area of ​​the reactor space perpendicular to the flow direction of the reaction mixture in the reactor, wherein the straight line extends from a first point on the inner surface of the reactor wall in contact with the mixture to a second point, wherein at the first point r 0 is set to 0 and v exhibits its minimum value (v min =v(r 0 )), at the second point r is defined as r max And v shows its maximum value (v max =v(r max )), where r 1 =r max / x, x=5, preferably x=4, more preferably x=3, more preferably x=2.5, more preferably x=2, more preferably x=1.8, more preferably x=1.6, more preferably x=1.5, more preferably x=1.4, more preferably x=1.3, more preferably x=1.2, more preferably x=1.1, more preferably x≥1, wherein more preferably r=r max .

[0098] 2. The process of embodiment 1, wherein the straight line r is perpendicular to the inner surface of the reactor wall in contact with the reaction mixture.

[0099] 3. The process of embodiment 1 or 2, wherein in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (III):

[0100] v”(r)≥0 (III)

[0101] and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (IV):

[0102] v”(r)≤0 (IV).

[0103] 4. The process according to any one of embodiments 1 to 3, wherein, in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the velocity profile v(r) of the reaction mixture in the flow direction satisfies the condition according to (V):

[0104] v(r)<((v(r 1 )-v min )·(r / r 1 ))+v min (V)

[0105] Where 0 <r<r max , and wherein in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (VI):

[0106] v(r)>((v(r 1 )-v min )·(r / r 1 ))+v min (VI)

[0107] Where 0 <r<r max .

[0108] 5. The process of embodiment 4, wherein in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (VII):

[0109] v”(r)>0 (VII)

[0110] Where 0 <r<r max , and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (VIII):

[0111] v”(r)<0 (VIII)

[0112] Where 0 <r<r max .

[0113] 6. The process according to any of embodiments 1 to 5, wherein the mixture heated in the reactor in (iii) is mechanically agitated, wherein the mechanical agitation is preferably achieved by moving parts contained in the reactor.

[0114] 7. The process according to any one of embodiments 1 to 6, wherein the reactor is a Taylor-Couette reactor comprising an inner cylinder and an outer cylinder aligned coaxially, wherein the Taylor-Couette reactor preferably has a rotor-stator arrangement with the outer cylinder being the stator.

[0115] 8. The method of embodiment 7, wherein the two coaxial cylinders rotate at a speed of 5 to 5,000 rpm, preferably 10 to 3,000 rpm, more preferably 30 to 2,500 rpm, more preferably 50 to 2,000 rpm, more preferably 100 to 1,500 rpm, more preferably 150 to 1,200 rpm, more preferably 200 to 1,000 rpm, more preferably 250 to 800 rpm, more preferably 300 to 700 rpm, more preferably 350 to 650 rpm, more preferably 400 to 600 rpm, more preferably 450 to 550 rpm relative to each other.

[0116] 9. The method of embodiment 7 or 8, wherein the gap between the two coaxial cylinders is in the range of 0.3 to 50 cm, preferably 0.4 to 30 cm, more preferably 0.5 to 25 cm, more preferably 0.6 to 20 cm, more preferably 0.6 to 15 cm, more preferably 0.7 to 10 cm, more preferably 0.7 to 5 cm, more preferably 0.8 to 3 cm, more preferably 0.8 to 2 cm, more preferably 0.9 to 1.5 cm, more preferably 0.9 to 1.2 cm, more preferably 1.0 to 1.1 cm.

[0117] 10. The method according to any one of embodiments 7 to 9, wherein the diameter of the inner cylinder is in the range of 0.5 to 100 cm, preferably 1 to 50 cm, more preferably 1.5 to 30 cm, more preferably 2 to 20 cm, more preferably 2.5 to 15 cm, more preferably 3 to 10 cm, more preferably 3.5 to 8 cm, more preferably 4 to 7 cm, more preferably 4.5 to 6 cm, more preferably 5 to 5.5 cm.

[0118] 11. The method according to any one of embodiments 7 to 10, wherein the length of the two coaxial cylinders is in the range of 5 to 500 cm, preferably 8 to 300 cm, more preferably 10 to 200 cm, more preferably 12 to 150 cm, more preferably 15 to 100 cm, more preferably 18 to 80 cm, more preferably 20 to 50 cm, more preferably 23 to 35 cm, more preferably 25 to 30 cm.

[0119] 12. The method according to any one of embodiments 7 to 11, wherein the inner cylinder and / or the outer cylinder, preferably the outer cylinder, is heated to a temperature of 120 to 310°C, preferably 140 to 290°C, more preferably 160 to 270°C, more preferably 180 to 260°C, more preferably 200 to 250°C, more preferably 210 to 240°C, more preferably 220 to 230°C.

[0120] 13. A preparation comprising YO 2 and optionally contains X 2 O 3 A method for preparing a zeolite material having a framework structure, wherein Y is a tetravalent element and X is a trivalent element, the method comprising

[0121] (i) Preparation of YO 2 Source, optional X 2 O 3 a mixture of a source and a liquid solvent system;

[0122] (ii) supplying the mixture prepared in (i) as a reaction mixture into a reactor;

[0123] (iii) heating the reaction mixture in the reactor to obtain a mixture containing YO 2 and optionally contains X 2 O 3 a reaction mixture of a zeolite material having a framework structure; and

[0124] (iv) collecting the reaction mixture obtained in (iii) containing the zeolitic material as an effluent from the reactor;

[0125] The reactor is a Taylor-Couette reactor comprising coaxially aligned inner and outer cylinders.

[0126] 14. The method of embodiment 13, wherein the Taylor-Couette reactor has a rotor-stator configuration with the outer cylinder being the stator.

[0127] 15. The method of embodiment 13 or 14, wherein the two coaxial cylinders rotate at a speed of 5 to 5,000 rpm, preferably 10 to 3,000 rpm, more preferably 30 to 2,500 rpm, more preferably 50 to 2,000 rpm, more preferably 100 to 1,500 rpm, more preferably 150 to 1,200 rpm, more preferably 200 to 1,000 rpm, more preferably 250 to 800 rpm, more preferably 300 to 700 rpm, more preferably 350 to 650 rpm, more preferably 400 to 600 rpm, more preferably 450 to 550 rpm relative to each other.

[0128] 16. The method according to any one of embodiments 13 to 15, wherein the gap between the two coaxial cylinders is in the range of 0.3 to 50 cm, preferably 0.4 to 30 cm, more preferably 0.5 to 25 cm, more preferably 0.6 to 20 cm, more preferably 0.6 to 15 cm, more preferably 0.7 to 10 cm, more preferably 0.7 to 5 cm, more preferably 0.8 to 3 cm, more preferably 0.8 to 2 cm, more preferably 0.9 to 1.5 cm, more preferably 0.9 to 1.2 cm, more preferably 1.0 to 1.1 cm.

[0129] 17. The method according to any one of embodiments 13-16, wherein the diameter of the inner cylinder is in the range of 0.5 to 100 cm, preferably 1 to 50 cm, more preferably 1.5 to 30 cm, more preferably 2 to 20 cm, more preferably 2.5 to 15 cm, more preferably 3 to 10 cm, more preferably 3.5 to 8 cm, more preferably 4 to 7 cm, more preferably 4.5 to 6 cm, more preferably 5 to 5.5 cm.

[0130] 18. The method according to any one of embodiments 13 to 17, wherein the length of the two coaxial cylinders is in the range of 5 to 500 cm, preferably 8 to 300 cm, more preferably 10 to 200 cm, more preferably 12 to 150 cm, more preferably 15 to 100 cm, more preferably 18 to 80 cm, more preferably 20 to 50 cm, more preferably 23 to 35 cm, more preferably 25 to 30 cm.

[0131] 19. The method according to any one of embodiments 13 to 18, wherein the inner cylinder and / or the outer cylinder, preferably the outer cylinder, is heated to a temperature of 120 to 310°C, preferably 140 to 290°C, more preferably 160 to 270°C, more preferably 180 to 260°C, more preferably 200 to 250°C, more preferably 210 to 240°C, more preferably 220 to 230°C.

[0132] 20. The process according to any of embodiments 1 to 19, wherein in (iii) the flow regime in at least one portion P of the reactor volume is laminar, wherein the portion P is preferably an uninterrupted portion of the reactor volume.

[0133] 21. The process of any of embodiments 1 to 20, wherein in (iii) the Reynolds number (Re) in at least the portion P of the reactor volume accommodating the reaction mixture is 2,500 or less, preferably 2,000 or less, more preferably 1,500 or less, more preferably 1,000 or less, more preferably 500 or less, more preferably 300 or less, more preferably 200 or less, more preferably 100 or less, more preferably 80 or less, more preferably 60 or less, more preferably 40 or less, more preferably 20 or less, more preferably 10 or less, more preferably 5 or less, more preferably 3 or less, more preferably 1 or less.

[0134] 22. The process of embodiment 21, wherein in (iii) the Taylor number (Ta), preferably the tangential Taylor number, in at least the portion P of the reactor volume accommodating the reaction mixture satisfies the condition according to (III):

[0135] Ta≤(1.52·Re)+n (III)

[0136] wherein n≤102, preferably ≤100, more preferably ≤98, more preferably ≤95, more preferably ≤90, more preferably ≤80, more preferably ≤60, more preferably ≤40, more preferably ≤20, more preferably ≤10, more preferably ≤5, more preferably ≤1.

[0137] 23. The method of any of embodiments 20-22, wherein the uninterrupted portion P of the reactor volume preferably constitutes 5 to 100% of the total volume of the reactor accommodating the reaction mixture, preferably 10 to 95%, more preferably 20 to 90%, more preferably 30 to 85%, more preferably 40 to 80%, more preferably 50 to 75%, more preferably 60 to 70% of the total volume of the reactor accommodating the reaction mixture.

[0138] 24. The process according to any one of embodiments 1 to 23, wherein the reaction mixture exhibits a shear thinning rheology (pseudoplastic rheology) or wherein the reaction mixture exhibits a shear thickening rheology (dilatant rheology), wherein the reaction mixture preferably exhibits a shear thinning rheology (pseudoplastic rheology).

[0139] 25. The process according to any one of embodiments 1 to 24, wherein the reaction mixture is heated to a temperature of 100 to 300°C, preferably 120 to 280°C, more preferably 140 to 260°C, more preferably 160 to 250°C, more preferably 180 to 240°C, more preferably 190 to 230°C, more preferably 200 to 220°C.

[0140] 26. The method according to any one of embodiments 1-25, wherein the volume of the reactor containing the reaction mixture is from 5 cm 3 to 1 m 3 , more preferably from 10 cm 3 to 1 m 3 , more preferably from 20 cm 3 to 0.5 m 3 , more preferably from 30 cm 3 to 0.1 m 3 , more preferably from 50 cm 3 to 0.05 m 3 , more preferably from 80 cm 3 to 0.01 m 3 , more preferably from 100 to 5,000 cm 3 , more preferably from 120 to 3,000 cm 3 , more preferably from 150 to 1,000 cm 3 , more preferably from 200 to 700 cm 3 , more preferably from 230 to 500 cm 3 , more preferably from 250 to 300 cm 3 in the range.

[0141] 27. The method according to any one of embodiments 1-26, wherein the inner surface of the reactor wall in contact with the mixture is made of a metallic material, wherein the metallic material comprises one or more metals selected from Ta, Cr, Fe, Ni, Cu, Al, Mo and combinations and / or alloys of two or more thereof, preferably one or more metals selected from Ta, Cr, Fe, Ni, Mo and combinations and / or alloys of two or more thereof, preferably one or more metals selected from Cr, Fe, Ni, Mo and combinations and / or alloys of two or more thereof, wherein the metallic material preferably comprises a nickel alloy, a nickel-molybdenum alloy, more preferably a nickel-molybdenum-chromium alloy.

[0142] 28. The method according to any one of embodiments 1-27, wherein the inner surface of the reactor wall in contact with the mixture is lined with an organic polymer material, wherein the organic polymer material preferably comprises one or more polymers selected from fluorinated polyolefins and mixtures of two or more thereof, preferably one or more polymers selected from (C2-C3) polyolefins and mixtures of two or more thereof, preferably one or more polymers selected from fluorinated polyethylene and mixtures of two or more thereof, wherein the polymer material more preferably comprises poly(tetrafluoroethylene), and wherein the inner wall of the reactor is more preferably lined with poly(tetrafluoroethylene).

[0143] 29. The process according to any one of embodiments 1 to 28, wherein the reaction mixture is heated under autogenous pressure in (iii), wherein the pressure is preferably in the range of 0.1 to 9 MPa, more preferably in the range of 0.5 to 7 MPa, more preferably in the range of 0.8 to 5 MPa, more preferably in the range of 1.3 to 3 MPa, more preferably in the range of 1.4 to 2 MPa, more preferably in the range of 1.5 to 1.7 MPa.

[0144] 30. The process according to any of embodiments 1 to 29, wherein the reactor consists of a single stage.

[0145] 31. The process of any one of embodiments 1 to 30, wherein no substances are added to the reaction mixture and / or no substances are removed from the reaction mixture during its passage through the reactor in (iii), wherein preferably no substances are added, wherein more preferably no substances are added and no substances are removed from the reaction mixture during its passage through the reactor in (iii).

[0146] 32. The method of any one of embodiments 1 to 31, wherein prior to (ii), the mixture prepared in (i) is aged at a temperature of 40 to 120°C, preferably 50 to 110°C, more preferably 60 to 105°C, more preferably 70 to 100°C, more preferably 75 to 95°C, more preferably 80 to 90°C.

[0147] 33. The method of any one of embodiments 1 to 32, wherein in (i) and before (ii), the mixture prepared in (i) is not heated to a temperature of 40°C or higher, preferably 35°C or higher, more preferably 30°C or higher, wherein more preferably in (i) and before (ii), the mixture prepared in (i) is not subjected to a heating step.

[0148] 34. The method of any one of embodiments 1-33, wherein prior to (ii), the mixture prepared in (i) is aged for a duration of 1 to 72 h, preferably 6 to 62 h, more preferably 12 to 56 h, more preferably 24 to 50 h, more preferably 36 to 44 h, more preferably 38 to 42 h.

[0149] 35. The process of any one of embodiments 1 to 34, wherein the mixture prepared in (i) is fed directly to the reactor in (ii), wherein while being fed to the reactor in (ii), the mixture prepared in (i) is preheated to a temperature of preferably 100 to 300°C, more preferably 100 to 280°C, more preferably 140 to 260°C, more preferably 160 to 250°C, more preferably 180 to 240°C, more preferably 190 to 230°C, more preferably 200 to 220°C.

[0150] 36. The method of any of embodiments 1 to 35, wherein the collecting of the reaction mixture in (iv) comprises quenching the reaction mixture effluent leaving the reactor in (iii) with a liquid comprising one or more solvents and / or by expansion of the reaction mixture effluent.

[0151] 37. The method of embodiment 36, wherein the liquid used for quenching comprises one or more solvents selected from polar protic solvents and mixtures thereof, preferably selected from n-butanol, isopropanol, propanol, ethanol, methanol, water and mixtures thereof, more preferably selected from ethanol, methanol, water and mixtures thereof, wherein the liquid more preferably comprises water, and wherein water is more preferably used as the liquid, preferably deionized water.

[0152] 38. The method according to any one of embodiments 1 to 37, wherein the method further comprises

[0153] (v) isolating the zeolitic material obtained in (iii) or (iv);

[0154] and / or,

[0155] (vi) preferably washing the zeolitic material obtained in (iii), (iv) or (v);

[0156] and / or,

[0157] (vii) preferably drying the zeolitic material obtained in (iii), (iv), (v) or (vi);

[0158] and / or,

[0159] (viii) Preferably the zeolitic material obtained in (iii), (iv), (v), (vi) or (vii) is calcined.

[0160] 39. The process according to embodiment 38, wherein in (v) the zeolitic material is separated from the reaction mixture obtained from (iii) or (iv) by means of filtration, centrifugation and / or decantation, preferably by means of microfiltration and / or ultrafiltration, wherein the microfiltration and / or ultrafiltration is more preferably achieved by membrane filtration.

[0161] 40. The process according to embodiment 39, wherein the supernatant obtained from the separation of the zeolitic material in (v) is recycled to (i) and / or (ii), preferably to (i).

[0162] 41. The process according to any of embodiments 38 to 40, wherein in (vii) the zeolitic material is dried by means of microwave irradiation and / or flash drying of the zeolitic material obtained in (iii), (iv), (v) or (vi).

[0163] 42. The process according to any of embodiments 38 to 41, wherein the drying in (vii) and the calcining in (viii) are achieved by one or more steps of calcining the zeolitic material obtained in (iii), (iv), (v) or (vi).

[0164] 43. The process of embodiment 38, wherein the separation of the zeolitic material in (v) comprises a step of spray drying the zeolitic material obtained in (iii) or (iv),

[0165] and / or

[0166] wherein the drying of the zeolitic material in (vii) comprises the step of spray drying the zeolitic material obtained in (iii), (iv), (v) or (vi).

[0167] 44. The process according to any one of embodiments 38 to 43, wherein the drying in (vii) is carried out at a temperature of 50 to 220°C, preferably 70 to 180°C, more preferably 80 to 150°C, more preferably 90 to 130°C, more preferably 100 to 125°C, more preferably 110 to 120°C.

[0168] 45. The process according to any one of embodiments 38 to 44, wherein the calcination in (viii) is carried out at a temperature of 300 to 800°C, preferably 350 to 750°C, more preferably 400 to 725°C, more preferably 450 to 700°C, more preferably 500 to 675°C, more preferably 550 to 650°C.

[0169] 46. ​​The method according to any one of embodiments 1 to 45, wherein the mixture prepared in (i) further comprises seed crystals, wherein the amount of seed crystals in the mixture prepared in (i) is preferably based on 100 wt % of YO contained in the mixture prepared in (i). 2 The calculated Y is 0.1 to 20 wt %, preferably 0.3 to 10 wt %, more preferably 0.5 to 5 wt %, more preferably 1 to 3 wt %, still more preferably based on 100 wt % contained in the mixture prepared in (i) as YO 2 The calculated Y is 1.5 to 2.5 wt%.

[0170] 47. The method of embodiment 46, wherein the seed comprises one or more structures selected from the group consisting of AEI, AFX, ANA, BEA, BEC, CAN, CHA, CDO, EMT, ERI, EUO, FAU, FER, GME, HEU, ITH, ITW, KFI, LEV, MEI, MEL, MFI, MOR, MTN, MWW, OFF, RRO, RTH, SAV, SFW, SZR and TON (including mixed structures of two or more thereof), preferably selected from the group consisting of CAN, AEI, EMT, SAV, SZR, KFI, ERI, OFF, RTH, GME, AFX, SFW, BEA, CHA, FAU, FER, HEU, LEV, MEI, MEL, MFI, MOR and MWW (including two or more thereof). more preferably selected from the group consisting of AEI, AFX, BEA, CHA, ERI, FAU, FER, GME, LEV, MEL, MFI, MOR and MWW (including a mixed structure of two or more thereof), more preferably selected from the group consisting of AEI, AFX, BEA, CHA, ERI, FER, GME, MEL, MFI, MOR and MWW (including a mixed structure of two or more thereof), more preferably selected from the group consisting of AEI, BEA, CHA, ERI, MFI and MWW (including a mixed structure of two or more thereof), more preferably selected from the group consisting of zeolites having a framework structure of AEI, BEA, CHA, MFI and MWW (including a mixed structure of two or more thereof), wherein the seed crystals more preferably comprise one or more zeolites having a CHA and / or AEI framework structure.

[0171] 48. The method of any one of embodiments 1 to 47, wherein the mixture prepared in (i) further comprises one or more organic templates.

[0172] 49. The method of embodiment 48, wherein the one or more organic templates are selected from tetraalkylammonium compounds, 1N-alkyl-3-quinuclidine alcohols or N,N,N-trialkyl-exo-aminonorbornanes and mixtures of two or more thereof, preferably selected from 1-adamantyltri(C 1 -C 3 ) alkyl-ammonium compounds, N,N,N-tri(C 1 -C 2 )alkyl-(C 5 -C 6 ) cycloalkylammonium compounds, N,N,N-trimethyl-N-benzylammonium compounds and mixtures of two or more thereof, more preferably selected from 1-adamantyltri(C 1 -C 2 ) alkyl-ammonium compounds, N,N,N-tri(C 1 -C 2)alkyl-cyclopentyl ammonium compounds, N,N,N-tri(C 1 -C 2 )alkyl-cyclohexylammonium compounds and mixtures of two or more thereof, more preferably selected from 1-adamantyltriethylammonium compounds, 1-adamantyldiethyl-methylalkylammonium compounds, 1-adamantylethyl-dimethylammonium compounds, 1-adamantyltrimethylammonium compounds, N,N,N-triethyl-cyclohexylammonium compounds, N,N-diethyl-N-methyl-cyclohexylammonium compounds, N,N-dimethyl-N-ethyl-cyclohexylammonium compounds, N,N,N-trimethyl-cyclohexylammonium compounds and mixtures of two or more thereof, wherein the one or more organic templates more preferably comprise one or more 1-adamantyltrimethylammonium compounds and / or one or more N,N,N-trimethyl-cyclohexylammonium compounds, wherein the one or more organic templates more preferably comprise one or more N,N,N-trimethyl-cyclohexylammonium compounds.

[0173] 50. The method of embodiment 48, wherein the one or more organic templates are selected from tetraalkyl Compounds, more preferably selected from tetra(C 1 -C 6 )alkyl Compounds, more preferably selected from tetra(C 1 -C 5 )alkyl Compounds, more preferably selected from tetra(C 1 -C 4 )alkyl Compounds, more preferably selected from tetra(C 2 -C 3 )alkyl Compounds, more preferably selected from tetramethyl Compound, ethyltrimethyl Compound, diethyl dimethyl Compound, methyl triethyl Compound, tetraethyl Compounds and mixtures of two or more thereof, wherein the one or more organic templates are more preferably selected from tetraethyl Compound.

[0174] 51. The method of embodiment 49 or 50, wherein the one or more organic templates are independently a salt, preferably selected from halides, preferably chlorides and / or bromides, more preferably chlorides, hydroxides, sulfates, nitrates, phosphates, acetates and mixtures of two or more thereof, more preferably one or more salts selected from chlorides, hydroxides, sulfates and mixtures of two or more thereof, wherein the one or more tetraalkylammonium compounds are more preferably tetraalkylammonium hydroxides and / or chlorides, even more preferably tetraalkylammonium hydroxides.

[0175] 52. The method of any one of embodiments 1 to 47, wherein the mixture prepared in (i) and heated in (iii) does not contain one or more organic templates.

[0176] 53. The method of any one of embodiments 1 to 52, wherein Y is selected from Si, Sn, Ti, Zr, Ge, and a combination of two or more thereof, and Y is preferably Si.

[0177] 54. The method according to any one of embodiments 1 to 53, wherein YO 2 The source comprises one or more compounds selected from the group consisting of fumed silica, silica hydrosol, reactive amorphous solid silica, silica gel, silicic acid, water glass, hydrated sodium metasilicate, sesquisilicates, disilicates, colloidal silica, silicates, and mixtures of two or more thereof, preferably selected from the group consisting of fumed silica, silica hydrosol, reactive amorphous solid silica, silica gel, silicic acid, colloidal silica, silicates, and mixtures of two or more thereof, more preferably selected from the group consisting of fumed silica, silica hydrosol, reactive amorphous solid silica, silica gel, colloidal silica, and mixtures of two or more thereof, wherein YO 2 Even more preferably, the source comprises fumed silica and / or colloidal silica, preferably colloidal silica.

[0178] 55. The method of any one of embodiments 1 to 54, wherein X is selected from the group consisting of Al, B, In, Ga, and combinations of two or more thereof, and X is preferably Al.

[0179] 56. The method according to any one of embodiments 1 to 55, wherein X 2 O 3 The source comprises alumina, aluminates, aluminum salts and mixtures of two or more thereof, preferably alumina, aluminum salts and mixtures of two or more thereof, more preferably alumina, tri(C 1 -C 5 )Aluminum alcoholate, AlO(OH), Al(OH) 3 , aluminum halides, preferably aluminum fluoride and / or aluminum chloride and / or aluminum bromide, more preferably aluminum fluoride and / or aluminum chloride, aluminum sulfate, aluminum phosphate, aluminum fluorosilicate, containing [Al13 O 4 (OH) 24 (H 2 O) 12 ] 7+ Salts of, alkali metal aluminates and mixtures of two or more thereof, more preferably selected from tri(C 2 -C 4 )Aluminum alcoholate, AlO(OH), Al(OH) 3 , aluminum chloride, aluminum sulfate, aluminum phosphate, containing [Al 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ Salts of, sodium aluminate, potassium aluminate and mixtures of two or more thereof, more preferably selected from tri(C 2 -C 3 )Aluminum alcoholate, AlO(OH), Al(OH) 3 , aluminum chloride, aluminum sulfate, containing [Al 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ salts, sodium aluminate and mixtures of two or more thereof, more preferably selected from aluminum tripropoxide, AlO(OH), aluminum sulfate, 13 O 4 (OH) 24 (H 2 O) 12 ] 7+ salts thereof, sodium aluminate and mixtures of two or more thereof, more preferably selected from aluminum tripropoxide, AlO(OH), Al(OH) 3 , aluminum sulfate, sodium aluminate and a mixture of two or more thereof.

[0180] 57. The method of any one of embodiments 1 to 56, wherein the mixture prepared in (i) further comprises at least one OH - source, wherein the at least one OH - The source preferably comprises a metal hydroxide, more preferably a hydroxide of an alkali metal M, more preferably sodium hydroxide and / or potassium hydroxide, more preferably sodium hydroxide.

[0181] 58. The method according to any one of embodiments 1 to 57, wherein the YO of the mixture prepared in (i) 2 :X 2 O 3The molar ratio is 1 to 1,000, preferably 2 to 500, more preferably 4 to 200, more preferably 5 to 150, more preferably 20 to 100, more preferably 30 to 80, more preferably 40 to 60, and still more preferably 45 to 55.

[0182] 59. The method according to any one of embodiments 1 to 58, wherein the liquid solvent system in the mixture prepared in (i) comprises one or more solvents, wherein the liquid solvent system preferably comprises one or more solvents selected from polar protic solvents and mixtures thereof, preferably selected from n-butanol, isopropanol, propanol, ethanol, methanol, water and mixtures thereof, more preferably selected from ethanol, methanol, water and mixtures thereof, wherein the liquid solvent system more preferably comprises water, and wherein water is more preferably used as the liquid solvent system, preferably deionized water.

[0183] 60. The method of any one of embodiments 1-59, wherein in (i) the liquid solvent system comprises water, wherein the H of the mixture prepared in (i) 2 O:YO 2 The molar ratio is preferably 1 to 400, more preferably 1 to 300, more preferably 2 to 200, more preferably 2 to 150, more preferably 2 to 100, more preferably 3 to 50, more preferably 4 to 30, more preferably 4.5 to 20, more preferably 5 to 15, more preferably 5.5 to 12, still more preferably 6 to 10.

[0184] 61. The process according to any one of embodiments 1 to 60, wherein the zeolitic material obtained in (iii) has a structure selected from the group consisting of AEI, AFX, ANA, BEA, BEC, CAN, CHA, CDO, EMT, ERI, EUO, FAU, FER, GME, HEU, ITH, ITW, KFI, LEV, MEI, MEL, MFI, MOR, MTN, MWW, OFF, RRO, RTH, SAV, SFW, SZR and TON (including mixed structures of two or more thereof), preferably selected from the group consisting of CAN, AEI, EMT, SAV, SZR, KFI, ERI, OFF, RTH, GME, AFX, SFW, BEA, CHA, FAU, FER, HEU, LEV, MEI, MEL, MFI, MOR and MWW (including mixed structures of two or more thereof), more preferably selected from BEA, CHA, FAU, FER, GME, LEV, MFI, MOR and MWW (including mixed structures of two or more thereof), more preferably selected from BEA, CHA, GME, MFI, MOR and MWW (including mixed structures of two or more thereof), more preferably selected from the framework structure of BEA, CHA, MFI and MWW (including mixed structures of two or more thereof), wherein the zeolite material obtained in (iii) more preferably has a CHA and / or BEA framework structure, preferably a CHA framework structure.

[0185] 62. The process according to any of embodiments 1 to 61, wherein the mixture prepared in (i) and heated in (iii) consists of a single liquid phase optionally containing a solid phase.

[0186] 63. The process according to any of embodiments 1 to 62, wherein the feeding of the mixture in (ii) and the collecting of the reacted mixture in (iv) are carried out in a continuous mode and / or in a batch mode, preferably in a continuous mode.

[0187] 64. The process according to any of embodiments 1 to 63, wherein the process is carried out in a continuous mode and / or in a batch mode, preferably in a continuous mode.

[0188] 65. The process of any one of embodiments 1 to 64, wherein the feeding of the mixture in (ii) and the collection of the reacted mixture in (iv) are carried out in a continuous mode at a liquid hourly space velocity of 0.3 to 250 h -1 , preferably 0.5 to 150h -1 , more preferably 1 to 100h -1 , more preferably 2 to 70h -1 , more preferably 5 to 50h -1 , more preferably 8 to 30h -1 , more preferably 10 to 20 hours -1 , more preferably 12 to 14 hours -1 within the range.

[0189] 66. The process according to any of embodiments 63 to 65, wherein in (ii) the mixture is continuously fed into the reactor for a duration of at least 1 hour to 10 years, preferably 6 hours to 8 years, more preferably 12 hours to 7 years, more preferably 1 day to 6 years, more preferably 7 days to 5 years, more preferably 15 days to 4 years, more preferably 1 month to 3.5 years, more preferably 2 months to 3 years, more preferably 4 months to 2.5 years, more preferably 6 months to 2 years, more preferably 8 months to 18 months, more preferably 10 to 14 months.

[0190] 67. Zeolitic material obtainable and / or obtained according to the process of any of embodiments 1 to 66.

[0191] 68. Use of the zeolitic material according to embodiment 67 as molecular sieve, as adsorbent, for ion exchange, as catalyst and / or as catalyst support, preferably as catalyst and / or as catalyst support.

[0192] Description of the drawings

[0193] Figure 1The general setup of a Taylor-Couette reactor is shown, with the inlet for the reaction mixture depicted at the upper right portion of the reactor and the outlet depicted at the lower left portion of the reactor. In the figure, arrows depict the incremental flow direction of the reaction mixture in the gap between the inner rotor of the reactor depicted as a hollow tube and the outer housing (stator) depicted as a transparent shell to show the reactor volume between the rotor and stator. The scale at the bottom of the figure shows the dimensions of the reactor used for the simulation in meters.

[0194] Figure 2 The rheology of the reaction mixture used for the simulations in the experimental part is shown, with the viscosity in Pa·s plotted along the abscissa and the viscosity in s plotted along the ordinate. -1 In this figure, the viscosity behavior is shown as a function of the shear rate.

[0195] Figure 3 The velocity contour of the reaction mixture in the simulated Taylor-Couette reactor for Example 1 is shown, wherein the scale in the figure indicates the velocity in m·s -1 The speed of the meter is 0 to 0.6177 m·s -1 The scale bar at the bottom of the figure shows the dimensions of the reactor used for the simulation in meters.

[0196] Figure 4 , 6 8 show velocity profiles of the reaction mixture in a simulated Taylor-Couette reactor for Examples 1, 2 and 3, respectively, wherein the scale in the figure indicates the temperature in degrees Kelvin (K), which is 300 to 500 K. The scale at the bottom of the figure shows the dimensions of the reactor used for the simulation in meters.

[0197] Figure 5 The velocity distribution diagram of the reaction mixture in the Taylor-Couette reactor used for the simulation of Example 2 is shown, wherein the scale in the diagram indicates the velocity in m·s -1 The speed of the meter is 0 to 0.7616 m·s -1 The scale bar at the bottom of the figure shows the dimensions of the reactor used for the simulation in meters.

[0198] Figure 7 The velocity distribution diagram of the reaction mixture in the Taylor-Couette reactor used for the simulation of Example 3 is shown, wherein the scale in the diagram indicates the velocity in m·s -1 The speed of the meter is 0 to 0.82965 m·s -1 The scale bar at the bottom of the figure shows the dimensions of the reactor used for the simulation in meters.

[0199] Fig. 9The viscosity measurement results obtained at different shear rates in Reference Example 1 are shown. In the figure, the temperature measurement points are shown with "■", the viscosity measurement points are shown with "●", wherein the temperature values ​​in ° C are plotted along the right abscissa, and the viscosity values ​​in Pa·s are plotted along the left abscissa. The duration of the viscosity measurement in minutes is plotted along the ordinate. In the legend, it is indicated that the viscosity measurement was performed at 250, 500 and 750 s. -1 The viscosity measurement points at different shear rates are shown in Table 1. -1 The shear rate measurement was interrupted after 119 min and at 750 s -1 The measurement at the shear rate was interrupted after 142 minutes. The dashed line in the figure indicates the viscosity level of the reaction mixture at the start of the measurement before heating.

[0200] Experimental Section

[0201] The simulation program used in the experiments described in this paper v17.0.0. The simulation is based on Figure 1 The Taylor-Couette reactor with an inner rotor and an outer stator is shown in FIG. Figure 1 The reaction mixture is introduced into the reactor at the upper right end of the reactor and allowed to flow concentrically around the rotor within the reactor volume and spiral down to the reactor outlet ( Figure 1 The parameters used for the simulation are as follows:

[0202] Cylinder Geometry:

[0203] Length = 25cm

[0204] D inner =5cm

[0205] D outer =6cm

[0206] Volume = 0.00027m 3 , area = 0.09m 2

[0207] Target reaction time:

[0208] Tau=5min(300s)

[0209] Feed = 0.6 g / s (36 ml / min)

[0210] temperature:

[0211] Wall 500K(227℃)

[0212] Feed 300K (27℃)

[0213] Pressure drop: 1550Pa

[0214] Material properties (non-Newtonian behavior):

[0215] Consistency index 1.1

[0216] Power law index 0.252

[0217] The viscosity properties of the reaction mixture used in the simulations are shown in Figure 2 middle.

[0218] Example 1: Simulation with low Taylor number

[0219] The simulation was performed using the above reaction setup, where the shear rate of the Taylor-Couette reactor was set so that the Reynolds number (Re) of the reaction mixture was Re = 2.3 and the Taylor number (Ta) of the reaction mixture was Ta = 1. The velocity profile obtained from this simulation is shown in Figure 3 In the figure, the temperature distribution is shown in Figure 4 Therefore, Figure 3 The simulation results shown in show that, under the chosen conditions, the reaction mixture exhibits a substantially uniform velocity distribution along the entire length of the reactor volume, with a value of about 0.6 m·s -1 , indicating that the reaction mixture is in a laminar flow state along the entire length of the reactor. Figure 4 As can be seen from the temperature profile shown in , the reaction mixture exhibits a gradual increase in temperature from an upper inlet region showing a temperature value of approximately 350 K to a lower outlet region showing a value of approximately 460 K.

[0220] Example 2: Simulation with high Taylor number

[0221] A further simulation was performed using the above reaction setup, wherein the shear rate of the Taylor-Couette reactor was set so that the Reynolds number (Re) of the reaction mixture was Re = 2.6 and the Taylor number (Ta) of the reaction mixture was Ta = 111. The velocity profile obtained from this simulation is shown in Figure 5 In the figure, the temperature distribution is shown in Figure 6 Therefore, Figure 5 The simulation results shown in show that, under the chosen conditions, the reaction mixture exhibits an irregular velocity distribution along the length of the reactor volume, with velocities in the range of about 0.4 m·s -1 The value of about 0.7m·s -1 The velocity profile oscillates regularly between the values ​​of . Unlike the results obtained in Example 1, the velocity profile indicates at least intermittent (if not substantially) turbulent flow of the reaction mixture along the entire length of the reactor. In addition, Figure 6It can be seen from the temperature profile shown in that, unlike the results obtained in Example 1, essentially no temperature gradient is obtained under these simulation conditions, the temperature being approximately 500 K along the entire length of the reactor volume.

[0222] Example 3: Simulation of the transformation of the reaction mixture from an aqueous solution to a gel

[0223] Additional simulations were performed in which the rheology of the reaction mixture was varied to simulate the transition from the rheology of an aqueous solution to the rheology of a gel as typically encountered during crystallization of a zeolitic material from an aqueous solution or slurry containing precursor compounds. In particular, the rheology was simulated to exhibit a rheology typical of an aqueous solution in the first 1 / 3 of the reactor volume starting from the inlet end, and a rheology typical of a gel in the last 2 / 3 of the reactor volume down to the reactor outlet. For this purpose, no heating of the reaction mixture was applied in the first 1 / 3 of the reactor volume, and only to the last 2 / 3 down to the outlet. In addition, the feed of the reaction mixture was increased to 60 ml / min, and the rotation speed was increased to 100 ml / min.

[0224] Therefore, by Figure 7 The simulation results shown in show that, under the chosen conditions, the reaction mixture exhibits an irregular velocity distribution along the first 1 / 3 of the reactor volume, where the velocity is around 0.2 m·s -1 The value is about 0.8m·s -1 The velocity profile oscillates regularly between values ​​of , thus indicating at least intermittent, if not substantially, turbulent conditions. However, the velocity profile decreases to a constant value of about 0.45 m·s which is then observed over the remaining length of the reactor volume down to the outlet. -1 and again indicates the laminar flow conditions in this part of the reactor volume. Figure 8 As can be seen from the temperature profile shown in , the first 1 / 3 of the reactor length is not heated and therefore exhibits a temperature of 300 K, which is the temperature of the reaction mixture before entering the reactor. The reaction mixture is heated in the last 2 / 3 of the reactor length, the second 1 / 3 exhibits a gradual increase to a value of about 480 K, and then maintains said temperature in the last 1 / 3 of the reactor length down to the outlet. Thus, the reaction mixture in the last 2 / 3 of the reactor volume exhibits a velocity and temperature profile similar to the results obtained in Example 1.

[0225] Reference Example 1: Viscosity measurement of a reaction mixture for making chabazite

[0226] The reaction mixture for the synthesis of chabazite using N,N,N-trimethylcyclohexylammonium hydroxide was prepared as described in WO 2013 / 182974A1. The viscosity characteristics of the reaction mixture were then measured under reaction conditions, wherein the mixture was placed in a rotational viscometer (Anton Paar, Physica MCR301) using a pressurized cell with cylindrical geometry (DG35, 12 / PR). After a sample of the reaction mixture was placed in the measuring cell, it was pressurized with nitrogen to a pressure of 8 bar. The viscosity was then measured, wherein the sample was heated from room temperature to 170°C at a reaction rate of 2°C / min and then kept constant at this temperature. The reaction mixture was heated at 250s / min for 250s / min and then kept constant at 170°C for 250s / min for 250s / min. -1 , 500s -1 and 750s -1 Three samples were measured at a shear rate of 250 s -1 The shear rate measurement was interrupted after 119 min and at 750 s -1 The shear rate measurement was interrupted after 142 min and at 500 s -1 The shear rate measurement was interrupted after 300 minutes. The measurement results are shown in Fig. 9 Thus, it can be concluded from the results that the viscosity decreases gradually during the initial heating phase, wherein it suddenly increases significantly when the maximum temperature is reached, and then levels off until the end of the crystallization reaction, at which time a further significant increase in viscosity is observed.

[0227] Therefore, the viscosity measurement of the crystallization of the reaction mixture confirms the evolution of the rheology of the reaction mixture during the preparation of the zeolitic material as simulated in Example 3.

[0228] Prior art documents cited:

[0229] -US 2016 / 0115039A1

[0230] -Liu et al. in Angew. Chem. Int. Ed. 2015, 54, 5683-5687

[0231] -Ju, J. et al. in Chemical Engineering Journal 2006, 116, 115-121

[0232] -Vandermeersch, T. et al. in Microporous and Mesoporous Materials 2016, 226, 133-139

[0233] -Liu, Z. et al. in Chemistry of Materials 2014, 26, 2327-2331

[0234] - Slangen et al., "Continuous Synthesis of Zeolites using a Tubular Reactor", 12 th International Zeolites Conference, Materials Research Society 1999

[0235] - Bonaccorsi, L. et al. in Microporous and Mesoporous Materials 2008, 112, 481 - 493

[0236] - US 2001 / 0054549 A1

Claims

1. A preparation having a 2 and optionally contains X 2 O 3 A method for preparing a zeolite material having a framework structure, wherein Y is a tetravalent element and X is a trivalent element, the method comprising (i) Preparation of YO 2 Source, optional X 2 O 3 a mixture of a source and a liquid solvent system; (ii) supplying the mixture prepared in (i) as a reaction mixture into a reactor; (iii) heating the reaction mixture in the reactor to obtain a mixture containing YO 2 and optionally contains X 2 O 3 a reaction mixture of a zeolite material having a framework structure; and (iv) collecting the reaction mixture containing the zeolitic material obtained in (iii) as an effluent from the reactor; wherein the reactor is a Taylor-Couette reactor comprising coaxially aligned inner and outer cylinders; wherein in (iii) shear is applied to the reaction mixture to establish a flow of the reaction mixture relative to the outer wall of the reactor in contact with the reaction mixture, and Wherein in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (I): v(r)≤((v(r 1 )-v min )·(r / r 1 ))+v min (I) and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the velocity distribution v(r) of the reaction mixture in the flow direction satisfies the condition according to (II): v(r)≥((v(r 1 )-v min )·(r / r 1 ))+v min (II) wherein r defines the length of a straight line on the cross-sectional area of ​​the reactor space perpendicular to the flow direction of the reaction mixture in the reactor, wherein the straight line extends from a first point at the inner surface of the reactor wall in contact with the mixture to a second point, wherein at the first point r 0 is set to 0 and v exhibits its minimum value (v min =v(r 0 )), at the second point r is defined as r max And v shows its maximum value (v max =v(r max )), where r 1 =r max / x, x=5.

2. The process according to claim 1, wherein the Taylor-Couette reactor has a rotor-stator arrangement with the outer cylinder being the stator.

3. The process according to claim 1, wherein the straight line r is perpendicular to the inner surface of the reactor wall in contact with the reaction mixture.

4. The process according to claim 2, wherein the straight line r is perpendicular to the inner surface of the reactor wall in contact with the reaction mixture.

5. The process according to any one of claims 1 to 4, wherein in (iii) in the case where the reaction mixture exhibits shear-thinning rheology (pseudoplastic rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (III): v”(r)≥0(III) and wherein in (iii) in the case where the reaction mixture exhibits shear thickening rheology (dilatant rheology), the second derivative v" (r) of the velocity profile satisfies the condition according to (IV): v”(r)≤0(IV).

6. The process according to any one of claims 1 to 4, wherein in (iii) the flow regime in at least one portion P of the reactor volume is laminar, wherein said portion P is an uninterrupted portion of the reactor volume.

7. A process according to claim 5, wherein in (iii) the flow regime in at least one portion P of the reactor volume is laminar.

8. The process according to claim 6, wherein in (iii) the Reynolds number (Re) in at least the portion P of the reactor volume containing the reaction mixture is 2,500 or less.

9. The process according to claim 7, wherein in (iii) the Reynolds number (Re) in at least the portion P of the reactor volume containing the reaction mixture is 2,500 or less.

10. The process according to claim 8, wherein in (iii) the Taylor number (Ta) in at least the portion P of the reactor volume containing the reaction mixture satisfies the condition according to (III): Ta≤(1.52·Re)+n(III) Where n≤102.

11. The process according to claim 9, wherein in (iii) the Taylor number (Ta) in at least the portion P of the reactor volume containing the reaction mixture satisfies the condition according to (III): Ta≤(1.52·Re)+n(III) Where n≤102.

12. The process according to any one of claims 1 to 4, wherein the reaction mixture in the reactor is heated to a temperature of 100 to 300°C.

13. The process according to claim 11, wherein the reaction mixture in the reactor is heated to a temperature of 100 to 300°C.

14. The process according to any one of claims 1 to 4, wherein the volume of the reactor containing the reaction mixture is between 5 cm 3 Up to 1m 3 within the range.

15. The process according to claim 13, wherein the volume of the reactor containing the reaction mixture is 5 cm 3 Up to 1m 3 within the range.

16. The process according to any one of claims 1 to 4, wherein the reaction mixture is heated under autogenous pressure in (iii).

17. The process according to claim 15, wherein the reaction mixture is heated under autogenous pressure in (iii).

18. The process according to any one of claims 1 to 4, wherein the process is carried out in continuous mode and / or in batch mode.

19. The process according to claim 17, wherein the process is performed in continuous mode and / or in batch mode.

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