TECHNICAL FIELD

The present invention relates to a process for the preparation of a metal-exchanged zeolitic ma terial comprising S1O2 and X2O3, wherein X is a trivalent element, in its framework structure. Further, the present invention relates to metal-exchanged zeolitic materials obtained and/or ob tainable according to the inventive process as disclosed herein. Yet further, the present inven tion relates to the use of metal-exchanged zeolitic materials as disclosed herein.

INTRODUCTION

The preparation of zeolitic materials usually involves two steps, a gelation- and crystallization- step. However, current needs of the chemical industry, in particular as regards high selective catalysts, require controlled design of the zeolite properties like surface properties or atomic dispersion of the active sites. This is quite challenging with the current manufacturing concepts. The synthesis of zeolites usually involves the formation of different metastable intermediates which may be fully or in part amorphous and/or crystalline. These metastable intermediates are very difficult to generate on purpose and handle. Therefore, novel and flexible strategies are needed for the preparation of zeolites.

In general, the formation of crystalline materials via amorphous intermediates is not new. These processes are widely known and described as non-classical crystallization routes. These routes have been deeply studied in the last decades thanks to the advances done in the field of mate rial analytics. Most of the non-classical routes have been identified and studied in bio mineralization processes. Further, it has been tried to transfer the gained knowledge to the for mation of novel functional materials.

Thus, a bottom-up synthesis approach as exemplified in bio-mineralization processes of syn thetic materials has become one of the most versatile tools of nanochemistry in the last dec ades.

For example, the synthesis of nanocrystalline ZnO nanoparticles possessing a new non equilibrium shape has been presented in WO 201 1/095589 A1 . It has been shown that the reac tion of special metal alkoxide precursors at the interface of a water-in-oil emulsion facilitated the synthesis of fairly monodisperse prismatic ZnO nanocrystallites with an adjustable aspect ratio in gram amounts. Moreover, said crystallization method has been also used for the formation of ZnO nanoparticles having different shape, composition, assembly behavior and crystal quality. K. Iwakai et al. disclose in Microporous and Mesoporous Materials 2001 , vol. 141 , p. 167-174 the preparation of nano-crystalline zeolite via hydrothermal synthesis in water/surfactant/organic solvent using fumed silica as the Si source.

Y. Shen et al. disclose in Bulletin Material Science 201 1 , vol. 34, p. 755-758 the nonionic emul sion-mediated synthesis of zeolite beta.

P. Sharma et al. disclose in Journal of Colloid and Interface Science 2014, vol. 422, p. 45-53 the emulsion-based droplet hydrothermal synthesis method for the production of uniform sized zeolite nanocrystals.

J. Zhu et al. disclose in Reaction Chemistry and Engineering 2018, vol. 3, p. 844-848 an ultra fast, stable-flow synthesis of zeolites with an emulsion method. The emulsion-based, continu ous flow synthesis of three important zeolites - ERI, BE A, and CHA - was achieved.

R. Limin et al. disclose in Chemical Communications a study on a designed copper-amine com plex as an efficient template for one-pot synthesis of Cu-SSZ-13 zeolite with excellent activity for selective catalytic reduction of NOx by NH ₃ . In particular, use of a copper complex of tetra ethylenepentamine is disclosed as structure directing agent.

X. Lijuan et al. also disclose a one-pot synthesis of a Cu-SSZ-13 and use of the same organo template as R. Limin et al. The study of X. Lijuan et al. relates to the performance of a Cu-SSZ- 13 catalyst prepared by a one-pot synthesis for the selective catalytic reduction of NOx with

NHs.

R. Martinez-Franco et al. disclose a one-pot preparation of Cu-SSZ-13 materials using a combi nation of copper tetraethylenepentamine (Cu-TEPA) and N,N,N-trimethyladamantammonium as organotemplates. Further, their studies are related to the catalytic application of the prepared Cu-SSZ-13 materials in the SCR of NOx.

Z. Ling et al. disclose a review on recent advances in the preparation of zeolites for the selec tive catalytic reduction of NOx in Diesel engines. A one-pot synthesis for SSZ-13 zeolites using copper tetraethylenepentamine is inter alia disclosed.

EP 2297036 B1 discloses a process for the direct synthesis of Cu containing zeolites having CHA structure, the process comprising preparing an aqueous solution containing at least one source for X ₂ O ₃ and at least one source for YO ₂ , at least one structure directing agent, and at least one Cu source. According to the examples, either a combination of trimethyl-1 - adamantylammonium and tetramethylammonium or of trimethyl-1 -adamantylammonium and trimethyl benzylammonium can be used as organotemplate.

DETAILED DESCRIPTION In view of the prior art, the present invention targets at the development of a novel route for syn thesizing zeolitic materials at mild conditions and controlled kinetics. In particular, it may be seen as an object of the present invention to provide an improved process for the preparation of a metal-exchanged zeolitic material. Thus, the present invention targets at the provision of a cost competitive method for producing zeolitic materials.

To this aim, a water-in-oil emulsion approach for the formation of zeolitic materials was estab lished.

Surprisingly, this approach allows for a controlled formation of precursor species, said species usually being amorphous, and their subsequently controlled crystallization. Further, it has been found that, on the one hand, several process steps can be avoided in order to save resources, such as separate ion exchange-, calcination- and/or spray drying-steps and on the other hand, the formation of zeolites can be done with better space time yield values than in prior art pro cesses. Furthermore, it has been surprisingly been found that the proposed emulsion system was demonstrated as feasible for the synthesis of well-defined zeolitic materials in the range of greater than 20 nm to several micrometers. Moreover, the addition of different Cu-sources can yield the formation of Cu-CHA materials according to the present inventive process and the de gree of Cu-insertion can be adjusted by variation of the Cu-source. Thus, it has surprisingly been found that comparatively higher amounts of copper can be introduced in a zeolitic material when compared to known preparation methods according to the prior art.

Therefore, the present invention relates to a process for the preparation of a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure, wherein X is a trivalent element, said process comprising

(1 ) preparing a first mixture comprising one or more nonpolar organic solvents, one or more polar pro tic solvents, one or more organotemplates as structure directing agents, one or more bases, and optionally one or more emulsifiers;

(2) emulsifying the mixture prepared in (1 );

(3) adding one or more sources of S1O2 to the emulsified mixture obtained in (2);

(4) preparing a second mixture comprising one or more nonpolar organic solvents;

(5) adding one or more sources of a metal M to the second mixture obtained in (4);

(6) adding the mixture obtained in (5) to the mixture obtained in (3);

(7) heating the mixture obtained in (6) for crystallizing a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure, wherein the metal M is contained as coun ter-ions at the ion exchange sites of the framework structure, and wherein the first mixture pre pared in (1 ) and/or the second mixture prepared in (4) further comprises one or more sources of X2O3.

In particular, the present invention relates to a process for the preparation of a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure, wherein X is a trivalent element, said process comprising (1 ) preparing a first mixture comprising one or more nonpolar organic solvents, one or more polar pro tic solvents, one or more organotemplates as structure directing agents, one or more bases, and one or more emulsifiers;

(2) emulsifying the mixture prepared in (1 );

(3) adding one or more sources of SiC>2 to the emulsified mixture obtained in (2);

(4) preparing a second mixture comprising one or more nonpolar organic solvents and one or more sources of X2O3;

(5) adding one or more sources of a metal M to the second mixture obtained in (4);

(6) adding the mixture obtained in (5) to the mixture obtained in (3);

(7) heating the mixture obtained in (6) for crystallizing a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure, wherein the metal M is contained as coun ter-ions at the ion exchange sites of the framework structure.

Further, the present invention relates to a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure, wherein X is a trivalent element, wherein said metal- exchanged zeolitic material is obtained and/or obtainable according to the process of any one of the embodiments disclosed herein.

Yet further, the present invention relates to a use of a metal-exchanged zeolitic material accord ing to any one of the embodiments disclosed herein as a molecular sieve, as an adsorbent, for ion-exchange, as a catalyst or a precursor thereof, and/or as a catalyst support or a precursor thereof.

As regards the inventive process, it is preferred that the preparation of the second mixture in (4) is conducted under an inert atmosphere, more preferably in an inert atmosphere comprising N2, He, Ar, Ne, or mixtures of two or more thereof, more preferably in an inert atmosphere compris ing N2 and/or Ar, wherein more preferably the second mixture in (4) is conducted under an at mosphere consisting of N2 and/or Ar, preferably of Ar.

Further, it is preferred that the addition of the one or more sources of a metal M to the second mixture in (5) is conducted under an inert atmosphere, more preferably in an inert atmosphere comprising N2, He, Ar, Ne, or mixtures of two or more thereof, more preferably in an inert at mosphere comprising N2 and/or Ar, wherein more preferably the addition of the one or more sources of a metal M to the second mixture in (5) is conducted under an atmosphere consisting of N2 and/or Ar, preferably of Ar.

It is particularly preferred that the preparation of the second mixture in (4) is conducted under the same inert atmosphere as the addition of the one or more sources of a metal M to the sec ond mixture in (5).

As regards the one or more nonpolar organic solvents in (1 ), it is preferred that the one or more nonpolar organic solvents in (1) are selected from the group consisting of (Cs-Cio)alkanes, (C5- Cio)alkenes, (Cs-Cio)aromatic organic compounds, (C ₄ -C ₈ )alkylethers, (Ci-C3)alkylhalides, or mixtures of two or more thereof, preferably from the group consisting of (C6-Cio)alkanes, {CQ- Cio)alkenes, (C ₆ -Cio)aromatic organic compounds, (C ₄ -C ₆ )alkylethers, (Ci-C ₂ )alkylhalides, or mixtures of two or more thereof, more preferably from the group consisting of (C ₆ -Ce)alkanes, (C ₆ -Ce)alkenes, (C ₆ -C ₈ )aromatic organic compounds, or mixtures of two or more thereof, where in more preferably the one or more nonpolar organic solvents in (1 ) are selected from the group consisting of hexane, heptane, octane, cylcohexane, cycloheptane, cyclooctane, benzene, tolu ene, ethylbenzene, mesitylene, durene, xylene, and mixtures of two or more thereof, more pref erably of cylcohexane, benzene, toluene, ethylbenzene, mesitylene, durene, xylene, and mix tures of two or more thereof, wherein more preferably the one or more nonpolar organic sol vents in (1 ) comprise toluene and/or xylene, preferably xylene, more preferably o-xylene, wherein more preferably the one or more nonpolar organic solvents in (1 ) consist of toluene and/or xylene, preferably of xylene, more preferably of o-xylene.

As regards the one or more nonpolar organic solvents in (4), it is preferred that the one or more nonpolar organic solvents in (4) are selected from the group consisting of (Cs-Cio)alkanes, (Cs- Cio)alkenes, (Cs-Cio)aromatic organic compounds, (C4-Ce)alkylethers, (Ci-C3)alkylhalides, or mixtures of two or more thereof, preferably from the group consisting of (C ₆ -Cio)alkanes, {C _& - Cio)alkenes, (C ₆ -Cio)aromatic organic compounds, (C4-C6)alkylethers, (Ci-C2)alkylhalides, or mixtures of two or more thereof, more preferably from the group consisting of (C ₆ -Cs)alkanes, (C ₆ -Cs)alkenes, (C ₆ -C ₈ )aromatic organic compounds, or mixtures of two or more thereof, where in more preferably the one or more nonpolar organic solvents in (4) are selected from the group consisting of hexane, heptane, octane, cylcohexane, cycloheptane, cyclooctane, benzene, tolu ene, ethylbenzene, mesitylene, durene, xylene, and mixtures of two or more thereof, more pref erably of cylcohexane, benzene, toluene, ethylbenzene, mesitylene, durene, xylene, and mix tures of two or more thereof, wherein more preferably the one or more nonpolar organic sol vents in (4) comprise toluene and/or xylene, preferably xylene, more preferably o-xylene, wherein more preferably the one or more nonpolar organic solvents in (4) consist of toluene and/or xylene, preferably of xylene, more preferably of o-xylene.

It is particularly preferred that the one or more nonpolar organic solvents in (1 ) are the same as the one or more nonpolar organic solvents in (4).

As regards the amount of the one or more nonpolar organic solvents in the mixture obtained in (6) and heated in (7), no particular restriction applies. It is preferred that the amount of the one or more nonpolar organic solvents in the mixture obtained in (6) and heated in (7) ranges from 10 to 95 weight- % based on 100 weight- % of the total amount of the one or more nonpolar or ganic solvents, the one or more polar protic solvents, and the one or more emulsifiers, prefera bly from 30 to 85 weight-%, more preferably from 50 to 80 weight-%, more preferably from 60 to 75 weight-%, more preferably from 65 to 72 weight-%, and more preferably from 67 to 69 weight-%.

Further, it is preferred that the one or more polar protic solvents are selected from the group consisting of n-hexanol, n-pentanol, n-butanol, isopropanol, propanol, ethanol, methanol, water, and mixtures thereof, more preferably from the group consisting of ethanol, methanol, water, and mixtures thereof. It is particularly preferred that the one or more polar pro tic solvents com prise water, and more preferably that water is used as the one or more polar protic solvents, preferably deionized water.

As regards the amount of the one or more polar protic solvents in the mixture obtained in (6) and heated in (7), no particular restriction applies. It is preferred that the amount of the one or more polar protic solvents in the mixture obtained in (6) and heated in (7) ranges from 5 to 90 weight- % based on 100 weight- % of the total amount of the one or more nonpolar organic sol vents, the one or more polar protic solvents, and the one or more emulsifiers, more preferably from 10 to 70 weight-%, more preferably from 15 to 50 weight-%, more preferably from 20 to 40 weight-%, more preferably from 26 to 34 weight-%, more preferably from 25 to 35 weight-%, more preferably from 27 to 33 weight-%, and more preferably from 29 to 31 weight-%.

It is preferred that the mixture obtained in (6) and heated in (7) comprises water as the one or more polar protic solvents, wherein the H2O : S1O2 molar ratio of the mixture ranges from 1 to 200, preferably from 3 to 100, more preferably from 5 to 50, more preferably from 7 to 30, more preferably from 9 to 25, more preferably from 10 to 20, more preferably from 1 1 to 16, more preferably from 12 to 14, and more preferably from 12.5 to 13.5.

It is particularly preferred that in the case where the amount of the one or more polar protic sol vents in the mixture obtained in (6) and heated in (7) ranges from 5 to 90 weight-% based on 100 weight-% of the total amount of the one or more nonpolar organic solvents, the one or more polar protic solvents, and the one or more emulsifiers, more preferably from 10 to 70 weight-%, more preferably from 15 to 50 weight-%, more preferably from 20 to 40 weight-%, more prefer ably from 25 to 35 weight-%, more preferably from 27 to 33 weight-%, and more preferably from 29 to 31 weight-%, the mixture obtained in (6) and heated in (7) comprises water as the one or more polar protic solvents, wherein the H2O : S1O2 molar ratio of the mixture ranges from 1 to 200, preferably from 3 to 100, more preferably from 5 to 50, more preferably from 7 to 30, more preferably from 9 to 25, more preferably from 10 to 20, more preferably from 1 1 to 16, more preferably from 12 to 14, and more preferably from 12.5 to 13.5.

According to a first alternative as regards the one or more organotem plates in (1 ), it is preferred that the one or more organotem plates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , R ³ , and R ⁴ independently from one another stand for alkyl, wherein preferably R ¹ , R ² , and R ³ independently from one another stand for al kyl, and wherein R ⁴ stands for adamantyl.

Further, it is preferred that the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more 1 -adamantyltri(Ci-C ₃ )alkylammonium compounds, more preferably one or more 1 -adamantyltri(Ci-C ₂ )alkylammonium compounds, more preferably one or more compounds selected from the group consisting of 1 -adamantyltriethylammonium com pounds, 1 -adamantyldiethyl-methylalkylammonium compounds, 1 -adamantylethyl-dimethyl- ammonium compounds, 1 -adamantyltrimethylammonium compounds, and mixtures of two or more thereof. It is particularly preferred that the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more 1 -adamantyltrimethylammonium compounds, wherein more preferably the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ - containing compounds consist of one or more 1 -adamantyltrimethylammonium compounds.

It is preferred that the one or more organotemplates in (1 ) comprise one or more

tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , and R ³ inde pendently from one another stand for alkyl, and wherein R ⁴ stands for cycloalkyl, preferably for optionally heterocyclic 5- to 8-membered cycloalkyl, preferably for 5- to 7-membered cycloalkyl, more preferably for 5- or 6-membered cycloalkyl, wherein even more preferably R ⁴ stands for optionally heterocyclic 6-membered cycloalkyl, and more preferably for cyclohexyl.

In the case where the one or more organotemplates in (1 ) comprise one or more

tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , and R ³ inde pendently from one another stand for alkyl, and wherein R ⁴ stands for cycloalkyl, it is preferred that the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more /V,/V,/V-tri(Ci-C ₄ )alkyl-(C ₅ -C ₇ )cycloalkylammonium compounds, preferably one or more /V,/V,/V-tri(Ci-C3)alkyl-(C5-C6)cycloalkylammonium compounds, more preferably one or more /V,/V,/V-tri(Ci-C2)alkyl-(C5-C6)cycloalkylammonium compounds, more preferably one or more /V,/V,/V-tri(Ci-C ₂ )alkyl-cyclopentylammonium and/or one or more /V,/V,/V-tri(Ci-C2)alkyl- cyclohexylammonium compounds, more preferably one or more compounds selected from N,N,N- triethyl-cyclohexylammonium, /V,/V-diethyl-/V-methyl-cyclohexylammonium, /V,/V-dimethyl- /V-ethyl-cyclohexylammonium, N,N,N- trimethyl-cyclohexylammonium compounds, and mixtures of two or more thereof, wherein more preferably the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more /V,/V,/V-trimethyl- cyclohexylammonium compounds, and wherein more preferably the one or more

tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds consist of one or more N,N,N- trimethyl-cyclohexylammonium compounds.

In the case where the one or more organotemplates in (1 ) comprise one or more

tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , and R ³ inde pendently from one another stand for alkyl, and wherein R ⁴ stands for adamantly, it is preferred that R ¹ , R ² , and R ³ independently from one another stand for optionally branched (Ci-Ce)alkyl, preferably (Ci-Cs)alkyl, more preferably (Ci-C ₄ )alkyl, and more preferably for optionally branched (Ci-C3)alkyl, wherein more preferably R ¹ , R ² , and R ³ independently from one another stand for methyl or ethyl, wherein more preferably R ¹ , R ² , and R ³ stand for methyl.

According to a second alternative as regards the one or more organotemplates in (1 ), it is pre ferred that the one or more organotemplates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , R ³ and R ⁴ independently from one another stand for alkyl, more preferably for optionally branched (Ci-Ce)alkyl, more preferably (Ci-Cs)alkyl, more preferably (C2-C4)alkyl, and more preferably for optionally branched (C2- C3)alkyl, wherein more preferably R ¹ , R ² , R ³ , and R ⁴ independently from one another stand for ethyl or propyl, wherein more preferably R ¹ , R ² , R ³ , and R ⁴ stand for propyl, preferably for n- p ropy I.

Further in the case where the one or more organotemplates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , and R ³ inde pendently from one another stand for alkyl, and wherein R ⁴ preferably stands for adamantyl, it is preferred that the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds independently of one another are salts, more preferably one or more salts selected from the group consisting of halides, preferably chloride and/or bromide, more preferably chloride, hy droxide, sulfate, nitrate, phosphate, acetate, and mixtures of two or more thereof, more prefera bly from the group consisting of chloride, hydroxide, sulfate, and mixtures of two or more there of, wherein more preferably the one or more organotemplate compounds are hydroxides and/or chlorides, and even more preferably hydroxides.

Further in the case where the one or more organotemplates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds, wherein R ¹ , R ² , and R ³ inde pendently from one another stand for alkyl, and wherein R ⁴ stands for adamantly, it is preferred that the mixture obtained in (6) and heated in (7) displays a molar ratio of the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds to the one or more sources of SiC>2 calculated as SiC>2 in the range of from 0.01 to 2.0, more preferably from 0.05 to 1.0, more preferably from 0.06 to to 0.6, more preferably from 0.07 to 0.55, more preferably from 0.08 to 0.5, more preferably from 0.1 to 0.3, more preferably from 0.12 to 0.25, more preferably from 0.15 to 0.22, more preferably from 0.16 to 0.2, more preferably from 0.17 to 0.19, and even more preferably from 0.175 to 0.18.

It is preferred that the S1O2 : X2O3 molar ratio of the mixture obtained in (6) and heated in (7) is in the range of from 1 to 500, more preferably from 2 to 200, more preferably from 5 to 150, more preferably from 10 to 100, more preferably from 15 to 50, more preferably from 19 to 45, more preferably from 20 to 40, more preferably from 24 to 35, more preferably from 25 to 33, and more preferably from 27 to 29.

It is preferred that the one or more emulsifiers are selected from the group consisting of ionic and nonionic surfactants, including mixtures thereof, more preferably from the group consisting of nonionic surfactants.

In the case where the one or more emulsifiers are selected from the group consisting of ionic and nonionic surfactants, including mixtures thereof, it is preferred that the ionic surfactants comprise one or more anionic surfactants, more preferably one or more anionic surfactants se lected from the group consisting of salts of (C ₆ -Cie)sulfate, (C ₆ -Cie)ethersulfate, {C _& - Cie)sulfonate, (C ₆ -Ci ₈ )sulfosuccinate (C ₆ -Cis)phosphate, (C ₆ -Ci ₈ )carboxylate, and mixtures of two or more thereof, more preferably from the group consisting of salts of (C ₈ -Ci ₆ )sulfate, (Cs- Ci ₆ )ethersulfate, (C ₈ -Ci ₆ )sulfonate, (C ₈ -Ci ₆ )sulfosuccinate, (C ₈ -Ci ₆ )phosphate, (Cs- Ci ₆ )carboxylate, and mixtures of two or more thereof, more preferably from the group consisting of salts of (Cio-Ci4)sulfate, (Cio-Ci4)ethersulfate, (Cio-Ci4)sulfonate, (C8-Ci4)sulfosuccinate, (Cio-Ci4)phosphate, (Cio-Ci4)carboxylate, and mixtures of two or more thereof, more preferably from the group consisting of salts of laurylsulfate, laurylsulfonate, di octyl sulfosuccinate, lau- rylphosphate, laurate, and mixtures of two or more thereof, wherein the counterion is preferably selected from the group consisting of H ⁺ , alkali metals, alkaline earth metals, ammonium, and combinations of two or more thereof, more preferably from the group consisting of H ⁺ , Li ⁺ , Na ⁺ , K ⁺ , ammonium, and combinations of two or more thereof, more preferably from the group con sisting of Na ⁺ , K ⁺ , ammonium, and combinations of two or more thereof, wherein even more preferably the counterion is Na ⁺ and/or ammonium, preferably Na ⁺ .

Further in the case where the one or more emulsifiers are selected from the group consisting of ionic and nonionic surfactants, including mixtures thereof, it is preferred that the ionic surfac tants comprise one or more cationic surfactants, preferably one or more cationic surfactants selected from the group consisting of primary, secondary, tertiary, and quaternary ammonium compounds, including mixtures of two or more thereof, wherein more preferably the cationic surfactants comprise one or more quaternary ammonium compounds, preferably selected from the group consisting of salts of (C ₈ -Ci ₈ )trimethylammonium, (C ₈ -Ci ₈ )pyridinium, benzalkonium, benzethonium, dimethyldioctadecylammonium, cetrimonium, dioctadecyldimethylammonium, and mixtures of two or more thereof, more preferably from the group consisting of salts of cetyltrimethylammonium, dodecyltrimethylammonium, cetylpyridinium, benzalkonium, ben zethonium, dimethyldioctadecylammonium, cetrimonium, dioctadecyldimethylammonium, wherein the counterion is preferably selected from the group consisting of halides, carbonates, hydroxide, nitrate, phosphate, sulfate, and combinations of two or more thereof, more preferably from the group consisting of chloride, fluoride, bromide, hydrogen carbonate, hydroxide, nitrate, sulfate, and combinations of two or more thereof, wherein more preferably the counterion is chloride and/or nitrate, preferably chloride.

Further in the case where the one or more emulsifiers are selected from the group consisting of ionic and nonionic surfactants, including mixtures thereof, it is preferred that the ionic surfac tants comprise one or more zwitterionic surfactants, more preferably one or more betaines, wherein more preferably the ionic surfactants comprise cocamidopropylbetaine or alkyldime- thylaminoxide.

Further in the case where the one or more emulsifiers are selected from the group consisting of ionic and nonionic surfactants, including mixtures thereof, it is preferred that the nonionic surfac tants are selected from the group consisting of (C ₈ -C ₂₂ )alcohols, (C ₆ -C ₂ o)alcohol ethoxylates with 1 to 8 ethylene oxide units, (C6-C2o)alkyl polyglycosides, polyoxyethylene glycol alkyl ethers, polyoxypropylene glycol alkyl ethers, glucoside alkyl ethers, polyoxyethylene glycol al- kylphenol ethers, glycerol alkyl esters, sorbitan alkyl esters, polyoxyethylene glycol sorbitan alkyl esters, cocamide monoethanolamine, cocamide diethanolamine, dodecyldimethylamine oxide, block copolymers of polyethylene glycol and polypropylene glycol, polyethoxylated tallow amine, and mixtures of two or more thereof, wherein more preferably the one or more nonionic surfactants are selected from the group con sisting of (Ci ₄ -C ₂ o)alcohols, (C ₈ -Ci ₈ )alcohol ethoxylates with 2 to 6 ethylene oxide units, (Ce- Cie)alkyl polyglycosides, octaethylene glycol monododecyl ether and/or pentaethylene glycol monododecyl ether, polyoxypropylene glycol alkyl ethers, decyl glucoside, lauryl glucoside, myristil glucoside, octyl glucoside, polyoxyethylene glycol octylphenol ethers, preferably triton X- 100, nonoxynol-9, glyceryl laurate, polyglycerol polyricinoleate, sorbitan monolaurate, sorbitan monopalmitate, sorbitan monostearate, sorbitan monooleate, polyoxyethylene sorbitan monolaurate, polyoxyethylene sorbitan monopalmitate, polyoxyethylene sorbitan monostearate, polyoxyethylene sorbitan monooleate, polyoxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, cocamide monoethanolamine, cocamide diethanolamine, dodecyldimethylamine oxide, block copolymers of polyethylene glycol and polypropylene glycol, polyethoxylated tallow amine, and mixtures of two or more thereof,

wherein more preferably the one or more nonionic surfactants are selected from the group con sisting of (Ci ₆ -Ci ₈ )alcohols, (Ci6-Cis)alcohol ethoxylates with 2 to 6 ethylene oxide units, (Ce- Ci4)alkyl polyglycosides, preferably cetyl alcohol, stearyl alcohol, oleyl alcohol, and mixtures of two or more thereof, octaethylene glycol monododecyl ether and/or pentaethylene glycol mono dodecyl ether, polyoxypropylene glycol alkyl ethers, decyl glucoside, lauryl glucoside, myristil glucoside, octyl glucoside, polyoxyethylene glycol octylphenol ethers, nonoxynol-9, glyceryl laurate, polyglycerol polyricinoleate, sorbitan monolaurate, sorbitan monopalmitate, sorbitan monostearate, sorbitan oleate, polyoxyethylene (20) sorbitan monolaurate, polyoxyethylene (20) sorbitan monopalmitate, polyoxyethylene (20) sorbitan monostearate, polyoxyethylene (20) sor bitan monooleate, polyoxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, cocamide monoethanolamine, cocamide diethanolamine, dodecyldimethylamine oxide, block copolymers of polyethylene glycol and polypropylene glycol, polyethoxylated tallow amine, Stearyl-EC> ₂ , pol- yglyceryl-2-dipolyhydroxystearate, polyglyceryl-distearate, C13/15 - PEG ₃ , C13 - PEG ₂ , glyceryl monooleate, C16/18 - PEG ₂ , oleyl - PEG ₂ , PEG ₂₀ - sorbitan monooleate, functionalized poly isobutene, C16/18 - PEGg, and mixtures of two or more thereof,

more preferably from the group consisting of polyg lyceryl-2-d i polyhyd roxystearate, diglyceryl- distearate, triglyceryl-distearate, C13/15 - PEG ₃ , C13 - PEG ₂ , glyceryl monooleate, sorbitan monooleate, polyglycerol-3-polyricinoleate, C16/18 - PEG ₂ , oleyl - PEG ₂ , PEG ₂₀ - sorbitan monooleate, functionalized polyisobutene, C16/18 - PEGg, polyoxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, and mixtures of two or more thereof,

more preferably from the group consisting of polyg lyceryl-2-d i polyhyd roxystearate, diglyceryl- distearate, triglyceryl-distearate, polyoxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, and mixtures of two or more thereof,

wherein it is even more preferred that the nonionic surfactant comprises polyoxyethylene (10) oleyl ether and/or polyoxyethylene (20) oleyl ether.

As regards the amount of the amount of the one or more emulsifiers in the mixture obtained in (6) and heated in (7), no particular restriction applies. It is preferred that the amount of the one or more emulsifiers in the mixture obtained in (6) and heated in (7) is in the range of from 0.1 to 10 weight- % based on 100 weight- % of the total amount of the one or more nonpolar organic solvents, the one or more polar protic solvents, and the one or more emulsifiers, more prefera- bly from 0.3 to 5 weight-%, more preferably from 0.5 to 3 weight-%, and more preferably from 1 to 2 weight-%.

Further, it is preferred that the one or more bases comprise one or more metal hydroxides and/or one or more metal hydroxide precursors, more preferably one or more metal hydroxides, more preferably one or more metal hydroxides selected from the group consisting of potassium hydroxide, sodium hydroxide, magnesium hydroxide, calcium hydroxide, iron hydroxide, alumi num hydroxide, and copper hydroxide, wherein more preferably the one or more bases com prise sodium hydroxide.

It is preferred that emulsification in (2) is achieved by agitation, more preferably by stirring and/or sonication, and more preferably by stirring.

Further, it is preferred that emulsification in (2) is achieved by use of a homogenizer, more pref erably with a rotor-stator homogenizer, with an ultrasonic homogenizer, with a high pressure homogenizer, by microfluidic systems, or by membrane emulsification, more preferably with a high pressure homogenizer or with a rotor-stator homogenizer, and more preferably with a rotor- stator homogenizer.

In the case where emulsification in (2) is achieved by use of a homogenizer, it is particularly preferred that stirring is performed at a speed in the range of from 500 to 35,000, more prefera bly from 1 ,000 to 32,000, more preferably from 3,000 to 30,000, more preferably from 5,000 to 28,000, more preferably from 7,000 to 26,000, more preferably from 9,000 to 22,000, more preferably from 1 1 ,000 to 20,000, more preferably from 13,000 to 18,000, and more preferably from 15,000 to 16,000.

Further, it is preferred that emulsification in (2) is conducted for a period in the range of from 0.1 to 10 min, more preferably from 0.2 to 6 min, more preferably from 0.4 to 4 min, more preferably from 0.6 to 3 min, more preferably from 0.8 to 2.5 min, more preferably from 1 to 2 min, more preferably from 1.2 to 1.8 min, and more preferably from 1.4 to 1.6 min.

As regards the trivalent element X, it is preferred that X is selected from the group consisting of Al, B, In, Ga, and combinations of two or more thereof. It is particularly preferred that X is Al.

Further, it is preferred that the one or more sources of X2O3 comprises one or more compounds selected from the group consisting of aluminum salts and aluminum alkoxides, more preferably from the group consisting of aluminates of an alkali metal, aluminum hydroxides, aluminum alkoxides, and mixtures of two or more thereof, wherein more preferably the one or more sources of X2O3 comprises one or more aluminum alkoxides AI(OR)3, wherein R stands for op tionally branched (Ci-Ce)alkyl, preferably (Ci-Cs)alkyl, more preferably (Ci-C ₄ )alkyl, and more preferably for optionally branched (Ci-C3)alkyl, wherein more preferably R stands for methyl, ethyl, n-propyl, isopropyl, or mixtures of two or more thereof, more preferably for ethyl, n-propyl, isopropyl, or mixtures of two or more thereof, more preferably for n-propyl and/or isopropyl, and more preferably for isopropyl.

In the case where the one or more sources of X2O3 comprises one or more compounds selected from the group consisting of aluminum salts and aluminum alkoxides, preferably from the group consisting of aluminates of an alkali metal, it is particularly preferred that the alkali metal is se lected from the group consisting of Li, Na, K, Rb, and Cs, wherein more preferably the alkali metal is Na and/or K, and wherein even more preferably the alkali metal is Na.

As regards the metal M, it is preferred that the metal M is selected from the group consisting of Mg, Ti, Cu, Co, Cr, Ni, Fe, Mo, Mn, Ru, Rh, Pd, Ag, Os, Ir, Pt, Au, and mixtures of two or more thereof, more preferably from the group consisting of Ti, Cu, Fe, Rh, Pd, Pt, and mixtures of two or more thereof, wherein more preferably the metal M comprises Cu and/or Fe, preferably Cu, wherein more preferably the metal M is Cu and/or Fe, preferably Cu.

As regards the one or more sources of a metal M, it is preferred that the one or more sources of a metal M is selected from the group consisting of metal salts, metal alkoxides, metal carbox yl ates, and mixtures of two or more thereof, wherein more preferably the one or more sources of a metal M comprises one or more metal alkoxides and/or metal carboxyl ates, wherein more preferably one or more metal alkoxides are employed as the one or more sources of a metal M.

In the case where the one or more sources of a metal M is selected from the group consisting of metal salts, metal alkoxides, metal carboxylates, and mixtures of two or more thereof, it is pre ferred that the one or more metal salts are selected from the group consisting of halides, hy droxides, sulfates, nitrates, phosphates, acetates, octadecanoate, 2-(2-methoxy- ethoxy)ethanolate, and mixtures of two or more thereof, more preferably from the group consist ing of chlorides, bromides, sulfates, nitrates, acetates, octadecanoate, 2-(2-methoxy- ethoxy)ethanolate, and mixtures of two or more thereof, more preferably from the group consist ing of bromides, nitrates, octadecanoate, 2-(2-methoxyethoxy)ethanolate, and mixtures of two or more thereof, wherein more preferably the one or metal salts comprise nitrates, octadecano ate and/or 2-(2-methoxyethoxy)ethanolate, preferably 2-(2-methoxyethoxy)ethanolate, and wherein more preferably the one or metal salts are nitrates, octadecanoate and/or 2-(2- m eth oxyeth oxy) etha no I ate , preferably 2-(2-methoxyethoxy)ethanolate.

Further in the case where the one or more sources of a metal M is selected from the group con sisting of metal salts, metal alkoxides, metal carboxylates, and mixtures of two or more thereof, it is preferred that the one or more metal alkoxides comprise a trivalent metal ion and a divalent metal ion, wherein the trivalent metal ion is selected from the group consisting of Al, Ga, In, Fe, Co, Mn, Cr, La, Pr, Ce, Nd, Sm, Gd, Dy, Ho, Er, Yb, Lu, Sc, Y, and combinations of two or more thereof, and the divalent metal ion is selected from the group consisting of Mg, Ca, Sr, Ba, Zn, Cd, Cu, Ni, Co, Mn, Be, Zr, and combinations of two or more thereof, wherein preferably the trivalent metal ion is selected from the group consisting of Al, Ga, In, Fe, Co, Mn, Cr, La, Pr, Ce, Y, and combinations of two or more thereof, and the divalent metal ion is selected from the group consisting of Zn, Cu, Ni, Co, Mn, and combinations of two or more thereof, wherein more preferably the trivalent metal ion is selected from the group consisting of Al, Ga,

Y, and combinations of two or more thereof, and the divalent metal ion is selected from the group consisting of Cu, Ni, Co, and combinations of two or more thereof,

wherein more preferably the one or more metal alkoxides comprises Cu and Al as metal ions, wherein more preferably the metal ions in the one or more alkoxides are Cu and Al.

Further in the case where the one or more sources of a metal M is selected from the group con sisting of metal salts, metal alkoxides, metal carboxylates, and mixtures of two or more thereof, it is preferred that the alkoxides are selected from the group consisting of (Ci-Cio)alkoxides, more preferably of (C3-Cs)alkoxides, more preferably of (Cs-C ₇ )alkoxides, where more prefera bly the alkoxides are C6-alkoxides, preferably alkoxides of hexanol, and more preferably alkox ides of n-hexanol.

Further in the case where the one or more sources of a metal M is selected from the group con sisting of metal salts, metal alkoxides, metal carboxylates, and mixtures of two or more thereof, it is preferred that the carboxylates are selected from the group consisting of (C ₁₀ -C ₂₅ ) carbox ylates, more preferably of (C ₁₆ -C ₂₀ ) carboxylates, more preferably of (C ₁₇ -C ₁₉ ) carboxylates, wherein more preferably the carboxylates are octadecanoate.

Further in the case where the one or more sources of a metal M is selected from the group con sisting of metal salts, metal alkoxides, and mixtures of two or more thereof, it is particularly pre ferred that the one or more metal alkoxides comprise CuAh(OR) ₆ , wherein R is hexyl, preferably n-hexyl.

As regards the one or more sources of S1O ₂ , it is preferred that the one or more sources of S1O ₂ comprises one or more compounds selected from the group consisting of silicas, silicates, and mixtures thereof, more preferably from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, silicic acid, water glass, sodium metasilicate hydrate, sesquisilicate, disilicate, colloidal silica, pyrogenic silica, silicic acid esters, tetraalkoxysilanes, and mixtures of two or more thereof,

more preferably from the group consisting of fumed silica, silica hydrosols, silica gel, silicic acid, water glass, colloidal silica, pyrogenic silica, silicic acid esters, tetraalkoxysilanes, and mixtures of two or more thereof,

more preferably from the group consisting of silica hydrosols, silicic acid, water glass, colloidal silica, silicic acid esters, tetraalkoxysilanes, and mixtures of two or more thereof,

more preferably from the group consisting of water glass, colloidal silica, silicic acid esters, tetraalkoxysilanes, and mixtures of two or more thereof

more preferably from the group consisting of water glass, colloidal silica, and mixtures thereof, wherein more preferably the one or more sources of S1O ₂ is selected from the group consisting of water glass, colloidal silica, and mixtures thereof. It is particularly preferred that colloidal silica is employed as the one or more sources of S1O ₂ . As regards (1), (3), (4), (5), (6), and (7), it is preferred that independently from one another, (1), (3), (4), (5), (6), and (7) are performed under agitation of the mixture, more preferably under stirring and/or sonication of the mixture, and more preferably under stirring of the mixture.

As regards heating in (7), no particular restriction applies especially as regards the temperature at which the mixture obtained in (6) is heated. It is preferred that heating in (7) is conducted at a temperature in the range of from 80 to 260°C, more preferably from 100 to 240°C, more prefer ably from 120 to 220°C, more preferably from 140 to 200°C, more preferably from 160 to 180°C, and more preferably from 165 to 175°C.

Further, no particular restriction applies as to the period in which heating in (7) is conducted. It is preferred that heating in (7) is conducted for a period in the range of from 0.5 to 120 h, pref erably from 1 to 1 14 h, more preferably from 3 to 108 h, more preferably from 6 to 102 h, more preferably from 12 to 96 h, more preferably from 18 to 84 h, more preferably from 24 to 72 h, more preferably from 30 to 66 h, more preferably from 36 to 60 h, more preferably from 42 to 54 h, more preferably from 45 to 51 h, and more preferably from 47 to 49 h.

It is particularly preferred that heating in (7) is conducted under autogenous pressure.

As regards further process steps, no particular restriction applies such that the inventive pro cess may comprise further process steps. It is preferred that the process further comprises

(8) isolating the metal-exchange zeolitic material obtained in (7);

and/or, preferably and

(9) washing the metal-exchange zeolitic material obtained in (7) or (8);

and/or, preferably and

(10) drying the metal-exchange zeolitic material obtained in (7), (8), or (9);

and/or, preferably and

(1 1) calcining the metal-exchange zeolitic material obtained in (7), (8), (9) or (10).

In the case where the inventive process further comprises isolation in (8), it is preferred that isolation in (8) is achieved by filtration and/or centrifugation, preferably by filtration.

In the case where the inventive process further comprises washing in (9), it is preferred that washing in (9) is conducted with a solvent system comprising one or more solvents, wherein preferably the one or more solvents are selected from the group consisting of polar protic sol vents, polar aprotic solvents, and mixtures thereof, more preferably from the group consisting of n-butanol, isopropanol, propanol, ethanol, methanol, water, acetone, and mixtures thereof, more preferably from the group consisting of ethanol, methanol, water, acetone, and mixtures thereof, wherein more preferably the solvent system comprises water or acetone, and wherein more preferably water is used as the solvent system, preferably deionized water.

In the case where the inventive process further comprises drying in (10), it is preferred that dry ing in (10) is conducted at a temperature in the range of from 20 to 160°C, more preferably from 30 to 140°C, more preferably from 40 to 120°C, more preferably from 50 to 110°C, more prefer ably from 60 to 100°C, more preferably from 70 to 90°C, and more preferably from 75 to 85°C.

In the case where the inventive process further comprises calcining in (1 1 ), it is preferred that calcining in (11 ) is conducted at a temperature in the range of from 300 to 750°C, more prefera bly from 325 to 650°C, more preferably from 350 to 600°C, more preferably from 375 to 575 °C, more preferably from 375 to 550°C, more preferably from 400 to 500°C, and more preferably from 425 to 475°C.

Further, it is preferred that the mixture obtained in (6) and heated in (7) further comprises seed crystals, wherein the seed crystals preferably comprise one or more zeolitic materials, more preferably one or more zeolitic materials having the framework structure type of the zeolitic ma terial obtained in (7), wherein more preferably the one or more zeolitic materials comprise SSZ- 13 and/or chabazite, preferably SSZ-13.

In the case where the mixture obtained in (6) and heated in (7) further comprises seed crystals, it is preferred that the amount of seed crystals in the mixture is in the range of from 0.1 to 20 weight- % based on 100 weight- % of the one or more sources of SiC>2, calculated as S1O2, and the one or more sources of X2O3, calculated as X2O3, contained in the mixture obtained in (6), more preferably from 0.3 to 15 weight-%, more preferably from 0.5 to 10 weight-%, more pref erably from 1 to 8 weight-%, more preferably from 3 to 7 weight-%, more preferably from 4 to 6 weight-%, and more preferably from 4.5 to 5.5 weight-%.

As regards the addition of the seed crystals to the mixture during the inventive process, no par ticular restrictions apply such that in principle the seed crystals may be added at any point in the process up to and including step (6). Thus, the seed crystals may be added in any one of steps (1 ), (3), (4), (5), or (6), or in two or more of said steps, wherein it is preferred according to the present invention that the seed crystals are added as a further component during the prepara tion of the first mixture in (1 ).

Further, it is preferred that (7) is conducted in a batch mode and/or in a continuous mode.

It is particularly preferred that the process is conducted in a batch mode and/or in a continuous mode.

As regards (7), it is preferred that (7) comprises

(i) continuously feeding the mixture obtained in (6) into a continuous flow reactor; and

(ii) heating the mixture obtained in (6) in the continuous flow reactor for crystallizing a metal- exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure.

In the case where (7) comprises (i) and (ii), it is preferred that heating in (ii) is conducted at a temperature in the range of from 100 to 300°C, more preferably of from 100 to 280°C, more preferably of from 150 to 270°C, more preferably of from 180 to 260°C, more preferably of from 200 to 250°C, more preferably of from 210 to 240°C, and more preferably of from 220 to 235°C.

Further in the case where (7) comprises (i) and (ii), it is preferred that in (i) the mixture is fed into the continuous flow reactor at a liquid hourly space velocity in the range of from 0.3 to 20 IT ¹ , more preferably of from 0.05 to 10 IT ¹ , more preferably from 0.1 to 5 IT ¹ , more preferably from 0.2 to 3 IT ¹ , more preferably from 0.4 to 2 IT ¹ , more preferably from 0.6 to 1.5 IT ¹ , more prefera bly from 0.8 to 1.2 IT ¹ , and more preferably from 0.9 to 1 IT ¹ .

Further in the case where (7) comprises (i) and (ii), it is preferred that the mixture obtained in (6) is continuously fed in (i) and heated in (ii) for at least 1 h, more preferably for a duration in the range of from 3 h to 360 d, more preferably from 6 h to 120 d, more preferably from 12 h to 90 d, more preferably from 18 h to 60 d, more preferably from 1 to 30 d, more preferably from 1 .5 to 25 d, more preferably from 2 to 20 d, more preferably from 2.5 to 15 d, more preferably from 3 to 12 d, more preferably from 3.5 to 8 d, and more preferably from 4 to 6 d.

Further in the case where (7) comprises (i) and (ii), it is preferred that the volume of the contin uous flow reactor is in the range of from 50 cm ³ to 75 m ³ , preferably of from 50 cm ³ to 3 m ³ , preferably from 55 cm ³ to 1 m ³ , more preferably from 60 cm ³ to 0.7 m ³ , more preferably from 65 cm ³ to 0.3 m ³ , more preferably from 70 cm ³ to 0.1 m ³ , more preferably from 75 to 70,000 cm ³ , more preferably from 80 to 50,000 cm ³ , more preferably from 85 to 30,000 cm ³ , more preferably from 90 to 10,000 cm ³ , more preferably from 95 to 7,000 cm ³ , more preferably from 100 to 5,000 cm ³ , more preferably from 105 to 3,000 cm ³ , more preferably from 1 10 to 1 ,000 cm ³ , more preferably from 1 15 to 700 cm ³ , more preferably from 120 to 500 cm ³ , more preferably from 125 to 350 cm ³ , more preferably from 130 to 250 cm ³ , more preferably from 135 to 200 cm ³ , more preferably from 140 to 180 cm ³ , and more preferably from 145 to 160 cm ³ .

Further in the case where (7) comprises (i) and (ii), it is preferred that the continuous flow reac tor is selected among a tubular reactor, a ring reactor, and a continuously oscillating reactor, more preferably among a plain tubular reactor, a tubular membrane reactor, a tubular reactor with Coanda effect, a ring reactor, a continuously oscillating baffled reactor, and combinations thereof, wherein more preferably the continuous flow reactor is a plain tubular reactor and/or a ring reactor, wherein more preferably the continuous flow reactor is a plain tubular reactor.

Further in the case where (7) comprises (i) and (ii), it is preferred that the continuous flow reac tor is a tubular reactor, and wherein at least a portion of the tubular reactor is of a regular cylin drical form having a constant inner diameter perpendicular to the direction of flow, wherein the inner diameter is preferably in the range of from 2 to 1200 mm, more preferably from 3 to 800 mm, more preferably from 3 to 500 mm, more preferably from 4 to 200 mm, more preferably from 4 to 100 mm, more preferably from 4.5 to 50 mm, more preferably from 4.5 to 30 mm, more preferably from 5 to 15 mm, more preferably from 5 to 10 mm, more preferably from 5.5 to 8 mm, and more preferably from 5.5 to 6.5 mm. Further in the case where (7) comprises (i) and (ii), it is preferred that the continuous flow reac tor has a length in the range of from 0.2 to 5,000 m, more preferably from 0.5 to 3,000 m, more preferably from 1 to 1 ,000 m more preferably from 3 to 500 m more preferably from 3.5 to 200 m, more preferably from 3.5 to 100 m, more preferably from 4 to 50 m, more preferably from 4 to 30 m, more preferably from 4.5 to 20 m, more preferably from 4.5 to 15 m, more preferably from 5 to 10 m, and more preferably from 5 to 7 m.

Further in the case where (7) comprises (i) and (ii), it is preferred that the wall of the continuous flow reactor is made of a metallic material, wherein the metallic material comprises one or more metals selected from the group consisting of Ta, Cr, Fe, Ni, Cu, Al, Mo, and combinations and/or alloys of two or more thereof, preferably from the group consisting of Ta, Cr, Fe, Ni, Mo, and combinations and/or alloys of two or more thereof, more preferably from the group consist ing of Cr, Fe, Ni, Mo, and combinations and/or alloys of two or more thereof wherein preferably the metallic material comprises a nickel alloy, a nickel-molybdenum alloy, and more preferably a nickel-molybdenum-chromium alloy.

Further in the case where (7) comprises (i) and (ii), it is preferred that the surface of the inner wall of the continuous flow reactor is lined with an organic polymer material, wherein the organic polymer material preferably comprises one or more polymers selected from the group consisting of fluorinated polyalkylenes and mixtures of two or more thereof, preferably from the group con sisting of (C2-C3)polyalkylenes and mixtures of two or more thereof, preferably from the group consisting of fluorinated polyethylenes and mixtures of two or more thereof, wherein more pref erably the polymer material comprises poly(tetrafluoroethylene), wherein more preferably the inner wall of the continuous flow reactor is lined with poly(tetrafluoroethylene).

Further in the case where (7) comprises (i) and (ii), it is preferred that the continuous flow reac tor is straight and/or comprises one or more curves with respect to the direction of flow, wherein more preferably the continuous flow reactor is straight and/or has a coiled form with respect to the direction of flow.

Further in the case where (7) comprises (i) and (ii), it is preferred that the walls of the continu ous flow reactor are subject to vibration during heating in (ii).

Further in the case where (7) comprises (i) and (ii), it is preferred that in (ii) the mixture is heated under autogenous pressure, wherein preferably the pressure is in the range of from 0.5 to 15 MPa, more preferably in the range of from 1 to 10 MPa, more preferably from 2 to 8 MPa, more preferably from 3 to 7 MPa, more preferably from 3.5 to 6.5 MPa, more preferably from 4 to 6 MPa, more preferably from 4.5 to 5.5 MPa, and more preferably from 4.8 to 5.2 MPa.

Further in the case where (7) comprises (i) and (ii), it is preferred that the continuous flow reac tor consists of a single stage. Further in the case where (7) comprises (i) and (ii), it is preferred that no matter is added to and/or removed from the mixture during its passage through the continuous flow reactor in (ii), wherein preferably no matter is added, wherein more preferably no matter is added and no mat ter is removed from the mixture during its passage through the continuous flow reactor in (ii).

Further in the case where (7) comprises (i) and (ii), it is preferred that prior to (i) the mixture ob tained in (6) is aged at a temperature in the range of from 40 to 120°C, more preferably from 50 to 1 10°C, more preferably from 60 to 105°C, more preferably from 70 to 100°C, more preferably from 75 to 95°C, and more preferably from 80 to 90°C.

Further in the case where (7) comprises (i) and (ii), it is preferred that prior to (i) the mixture ob tained in (6) is aged for a duration ranging from 1 to 72 h, more preferably from 6 to 60 h, more preferably from 12 to 54 h, more preferably from 14 to 42 h, more preferably from 16 to 36 h, more preferably from 18 to 32 h, and more preferably from 20 to 28 h.

Further in the case where (7) comprises (i) and (ii), it is preferred that (7) further comprises (iii) quenching the reaction product effluent continuously exiting the reactor in (ii) with a liquid comprising one or more solvents and/or via expansion of the reaction product effluent.

In the case where (7) further comprises (iii), it is preferred that in (iii) the liquid comprises one or more solvents selected from the group consisting of polar protic solvents and mixtures thereof, more preferably from the group consisting of n-hexanol, n-pentanol, n-butanol, isopropanol, propanol, ethanol, methanol, water, and mixtures thereof, more preferably from the group con sisting of ethanol, methanol, water, and mixtures thereof, wherein more preferably the liquid comprises water, and wherein more preferably water is used as the liquid, preferably deionized water.

Further, it is preferred that the mean particle size D50 by volume as determined according to ISO 13320:2009 of the zeolitic material obtained in (7) is of at least 0.5 pm, and is more prefer ably in the range of from 0.5 to 1.5 pm, more preferably in the range of from 0.6 to 1 .0 pm, and more preferably in the range of from 0.6 to 0.8 pm.

Further, the present invention relates to a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure, wherein X is a trivalent element, wherein said metal- exchanged zeolitic material is obtained and/or obtainable according to the process of any one of the embodiments disclosed herein.

As regards the framework structure of the metal-exchanged zeolitic material, no particular re striction applies. It is preferred that the metal-exchanged zeolitic material has a framework struc ture type selected from the group consisting of MFI, BE A, CHA, AEI, MWW, LEV, GME, FAU, FER, MEL, MOR, and intergrowth structures thereof, more preferably from the group consisting of MFI, BE A, CHA, AEI, MWW, and intergrowth structures thereof, more preferably from the group consisting of BE A, CHA, AEI, M FI, and intergrowth structures thereof, wherein more pref- erably the zeolitic material has a CHA and/or AEI and/or MFI type framework structure, prefera bly a CHA or MFI type framework structure.

According to a first alternative, it is preferred that the metal-exchanged zeolitic material is metal- exchanged SSZ-13 and/or chabazite, more preferably metal-exchanged SSZ-13.

According to a second alternative, it is preferred that the metal-exchanged zeolitic material is metal-exchanged Silicalite, ZSM-5, [Fe-Si-0]-M FI, [Ga-Si-0]-M FI, [As-Si-0]-M FI, AMS-1 B, AZ- 1 , Bor-C, Encilite, Boralite C, FZ-1 , LZ-105, Mutinaite, NU-4, NU-5, TS-1 , TSZ, TSZ-III, TZ-01 , USC-4, USI-108, ZBH, ZKQ-1 B, ZMQ-TB, MnS-1 , FeS-1 , or a mixture of two or more thereof, more preferably Silicalite, ZSM-5, AMS-1 B, AZ-1 , Encilite, FZ-1 , LZ-105, Mutinaite, N U-4, N U-5, TS-1 , TSZ, TSZ-III, TZ-01 , USC-4, USI-108, ZBH, ZKQ-1 B, ZMQ-TB, or a mixture of two or more thereof, wherein more preferably the metal-exchanged zeolitic material is metal- exchanged Silicalite and/or ZSM-5, wherein more preferably the metal-exchanged zeolitic mate rial is metal-exchanged ZSM-5.

Further, the present invention relates to a use of a metal-exchanged zeolitic material according to any one of the embodiments disclosed herein as a molecular sieve, as an adsorbent, for ion- exchange, as a catalyst or a precursor thereof, and/or as a catalyst support or a precursor thereof, preferably as a catalyst or a precursor thereof and/or as a catalyst support or a precur sor thereof, more preferably as a catalyst or a precursor thereof, more preferably as a catalyst for the selective catalytic reduction (SCR) of nitrogen oxides NO _x ; for the storage and/or adsorp tion of CO ₂ ; for the oxidation of NH ₃ , in particular for the oxidation of NH ₃ slip in diesel systems; for the decomposition of N ₂ O; as an additive in fluid catalytic cracking (FCC) processes; and/or as a catalyst in organic conversion reactions, preferably in the conversion of alcohols to olefins, and more preferably in methanol to olefin (MTO) catalysis; more preferably for the selective cat alytic reduction (SCR) of nitrogen oxides NO _x , and more preferably for the selective catalytic reduction (SCR) of nitrogen oxides NO _x in exhaust gas from a combustion engine, preferably from a diesel engine or from a lean burn gasoline engine.

The present invention is further illustrated by the following embodiments and combinations of embodiments as indicated by the respective dependencies and back-references. In particular, it is noted that in each instance where a range of embodiments is mentioned, for example in the context of a term such as "The process of any one of embodiments 1 to 4", every embodiment in this range is meant to be explicitly disclosed for the skilled person, i.e. the wording of this term is to be understood by the skilled person as being synonymous to "The process of any one of embodiments 1 , 2, 3, and 4". Further, it is explicitly noted that the following set of embodi ments is not the set of claims determining the extent of protection, but represents a suitably structured part of the description directed to general and preferred aspects of the present inven tion.

1 . A process for the preparation of a metal-exchanged zeolitic material comprising S1O ₂ and X ₂ O ₃ in its framework structure, wherein X is a trivalent element, said process comprising (1 ) preparing a first mixture comprising one or more nonpolar organic solvents, one or more polar protic solvents, one or more organotemplates as structure directing agents, one or more bases, and optionally one or more emulsifiers;

(2) emulsifying the mixture prepared in (1);

(3) adding one or more sources of S1O2 to the emulsified mixture obtained in (2);

(4) preparing a second mixture comprising one or more nonpolar organic solvents;

(5) adding one or more sources of a metal M to the second mixture obtained in (4);

(6) adding the mixture obtained in (5) to the mixture obtained in (3);

(7) heating the mixture obtained in (6) for crystallizing a metal-exchanged zeolitic mate rial comprising S1O2 and X2O3 in its framework structure, wherein the metal M is contained as counter-ions at the ion exchange sites of the framework structure, and wherein the first mixture prepared in (1) and/or the second mixture prepared in (4) further comprises one or more sources of X2O3. The process of embodiment 1 , wherein the preparation of the second mixture in (4) and the addition of the one or more sources of a metal M to the second mixture in (5) are con ducted under an inert atmosphere, preferably in an inert atmosphere comprising N2, He, Ar, Ne, or mixtures of two or more thereof, preferably in an inert atmosphere comprising N2 and/or Ar, wherein more preferably the preparation of the second mixture in (4) and the addition of the one or more sources of a metal M to the second mixture in (5) are con ducted under an atmosphere consisting of N2 and/or Ar, preferably of Ar. The process of embodiment 1 or 2, wherein independently from one another, the one or more nonpolar organic solvents in (1 ) and (4) are selected from the group consisting of (C5-Cio)alkanes, (Cs-Cio)alkenes, (Cs-Cio)aromatic organic compounds, (C4- Ce)alkylethers, (Ci-C3)alkylhalides, or mixtures of two or more thereof, preferably from the group consisting of (C ₆ -Cio)alkanes, (C ₆ -Cio)alkenes, (C ₆ -Cio)aromatic organic com pounds, (C4-C6)alkylethers, (Ci-C2)alkylhalides, or mixtures of two or more thereof, prefer ably from the group consisting of (C ₆ -Ce)alkanes, (C ₆ -Ce)alkenes, (C ₆ -C ₈ )aromatic organic compounds, or mixtures of two or more thereof, wherein more preferably the one or more nonpolar organic solvents in (1 ) and (4) are selected from the group consisting of hexane, heptane, octane, cylcohexane, cycloheptane, cyclooctane, benzene, toluene, ethylben zene, mesitylene, durene, xylene, and mixtures of two or more thereof, more preferably of cylcohexane, benzene, toluene, ethylbenzene, mesitylene, durene, xylene, and mixtures of two or more thereof, wherein more preferably the one or more nonpolar organic sol vents in (1) and (4) comprise toluene and/or xylene, preferably xylene, more preferably o- xylene, wherein more preferably the one or more nonpolar organic solvents in (1) and (4) consist of toluene and/or xylene, preferably of xylene, more preferably of o-xylene. The process of any one of embodiments 1 to 3, wherein the amount of the one or more nonpolar organic solvents in the mixture obtained in (6) and heated in (7) ranges from 10 to 95 weight- % based on 100 weight- % of the total amount of the one or more nonpolar organic solvents, the one or more polar protic solvents, and the one or more emulsifiers, preferably from 30 to 85 weight-%, more preferably from 50 to 80 weight-%, more prefer ably from 60 to 75 weight-%, more preferably from 65 to 72 weight-%, and more prefera bly from 67 to 69 weight-%.

5. The process of any one of embodiments 1 to 4, wherein the one or more polar protic sol vents are selected from the group consisting of n-hexanol, n-pentanol, n-butanol, isopro panol, propanol, ethanol, methanol, water, and mixtures thereof,

preferably from the group consisting of ethanol, methanol, water, and mixtures thereof, wherein more preferably the one or more polar protic solvents comprise water, and where in more preferably water is used as the one or more polar protic solvents, preferably de ionized water.

6. The process of any one of embodiments 1 to 5, wherein the amount of the one or more polar protic solvents in the mixture obtained in (6) and heated in (7) ranges from 5 to 90 weight- % based on 100 weight- % of the total amount of the one or more nonpolar organic solvents, the one or more polar protic solvents, and the one or more emulsifiers, prefera bly from 10 to 70 weight-%, more preferably from 15 to 50 weight-%, more preferably from 20 to 40 weight-%, more preferably from 25 to 35 weight-%, more preferably from 26 to 34 weight-%, more preferably from 27 to 33 weight-%, and more preferably from 29 to 31 weight-%.

7. The process of embodiment 6, wherein the mixture obtained in (6) and heated in (7) com prises water as the one or more polar protic solvents, wherein the H2O : S1O2 molar ratio of the mixture ranges from 1 to 200, preferably from 3 to 100, more preferably from 5 to 50, more preferably from 7 to 30, more preferably from 9 to 25, more preferably from 10 to 20, more preferably from 1 1 to 16, more preferably from 12 to 14, and more preferably from 12.5 to 13.5.

8. The process of any one of embodiments 1 to 7, wherein the one or more organotemplates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing com pounds, wherein R ¹ , R ² , R ³ , and R ⁴ independently from one another stand for alkyl, wherein preferably R ¹ , R ² , and R ³ independently from one another stand for alkyl, and wherein R ⁴ stands for adamantyl.

9. The process of any one of embodiments 1 to 8, wherein the one or more tetraalkylammo nium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more 1 -adamantyltri(Ci- C ₃ )alkylammonium compounds, preferably one or more 1 -adamantyltri(Ci-C2)alkyl- ammonium compounds, more preferably one or more compounds selected from the group consisting of 1 -adamantyl triethylammonium compounds, 1 -adamantyldiethyl-methylalkyl- ammonium compounds, 1 -adamantylethyl-dimethylammonium compounds, 1 - adamantyltrimethylammonium compounds, and mixtures of two or more thereof, wherein more preferably the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ - containing compounds comprise one or more 1 -adamantyltrimethylammonium com pounds,

wherein more preferably the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ - containing compounds consist of one or more 1 -adamantyltrimethylammonium com pounds.

10. The process of any one of embodiments 1 to 7, wherein the one or more organotemplates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing com pounds, wherein R ¹ , R ² , and R ³ independently from one another stand for alkyl, and wherein R ⁴ stands for cycloalkyl, preferably for optionally heterocyclic 5- to 8-membered cycloalkyl, preferably for 5- to 7-membered cycloalkyl, more preferably for 5- or 6- membered cycloalkyl, wherein even more preferably R ⁴ stands for optionally heterocyclic 6-membered cycloalkyl, and more preferably for cyclohexyl.

1 1 . The process of embodiment 10, wherein the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more N,N,N- tri(Ci-C ₄ )alkyl-(C ₅ - C ₇ )cycloalkylammonium compounds, preferably one or more TV, TV, V-tri (C i -C3)al kyl-(Cs- C6)cycloalkylammonium compounds, more preferably one or more TV, TV, TV-tri(Ci-C2)alkyl- (C ₅ -C ₆ )cycloalkylammonium compounds, more preferably one or more TV, TV, TV-tri (C i - C ₂ )alkyl-cyclopentylammonium and/or one or more TV, TV, TV-tri(Ci-C2)alkyl- cyclohexylammonium compounds, more preferably one or more compounds selected from /V,/V,/V-triethyl-cyclohexylammonium, /V,/V-diethyl-/V-methyl-cyclohexylammonium, /V,/V-dimethyl-/V-ethyl-cyclohexylammonium, TV, TV, TV- trimethyl-cyclohexylammonium com pounds, and mixtures of two or more thereof, wherein more preferably the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds comprise one or more TV, TV, TV- trimethyl-cyclohexylammonium compounds, and wherein more preferably the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds consist of one or more TV, TV, TV- trimethyl-cyclohexylammonium compounds.

12. The process of any one of embodiments 8 to 1 1 , wherein R ¹ , R ² , and R ³ independently from one another stand for optionally branched (Ci-Ce)alkyl, preferably (Ci-Cs)alkyl, more preferably (Ci-C ₄ )alkyl, and more preferably for optionally branched (Ci-C3)alkyl, wherein more preferably R ¹ , R ² , and R ³ independently from one another stand for methyl or ethyl, wherein more preferably R ¹ , R ² , and R ³ stand for methyl.

13. The process of any one of embodiments 1 to 7, wherein the one or more organotemplates in (1 ) comprise one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing com pounds, wherein R ¹ , R ² , R ³ and R ⁴ independently from one another stand for alkyl, prefer ably for optionally branched (Ci-Ce)alkyl, preferably (Ci-Cs)alkyl, more preferably (C2- C4)alkyl, and more preferably for optionally branched (C2-C3)alkyl, wherein more prefera bly R ¹ , R ² , R ³ , and R ⁴ independently from one another stand for ethyl or propyl, wherein more preferably R ¹ , R ² , R ³ , and R ⁴ stand for propyl, preferably for n-propyl.

14. The process of any one of embodiments 8 to 13, wherein independently of one another the one or more tetraalkylammonium cation R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds are salts, preferably one or more salts selected from the group consisting of halides, preferably chloride and/or bromide, more preferably chloride, hydroxide, sulfate, nitrate, phosphate, acetate, and mixtures of two or more thereof, more preferably from the group consisting of chloride, hydroxide, sulfate, and mixtures of two or more thereof, wherein more preferably the one or more organotem plate compounds are hydroxides and/or chlorides, and even more preferably hydroxides.

15. The process of any one of embodiments 8 to 14, wherein the mixture obtained in (6) and heated in (7) displays a molar ratio of the one or more tetraalkylammonium cation

R ¹ R ² R ³ R ⁴ N ⁺ -containing compounds to the one or more sources of SiC>2 calculated as S1O2 in the range of from 0.01 to 2.0, preferably from 0.05 to 1.0, more preferably from 0.06 to to 0.6, more preferably from 0.07 to 0.55, more preferably from 0.08 to 0.5, more prefera bly from 0.1 to 0.3, more preferably from 0.12 to 0.25, more preferably from 0.14 to 0.23, more preferably from 0.15 to 0.22, more preferably from 0.16 to 0.2, more preferably from 0.17 to 0.19, and even more preferably from 0.175 to 0.18.

16. The process of any one of embodiments 1 to 15, wherein the S1O2 : X2O3 molar ratio of the mixture obtained in (6) and heated in (7) ranges from 1 to 500, preferably from 2 to 200, more preferably from 5 to 150, more preferably from 10 to 100, more preferably from 15 to 50, more preferably from 19 to 45, more preferably from 20 to 40, more preferably from 24 to 35, more preferably from 25 to 33, and more preferably from 27 to 29.

17. The process of any one of embodiments 1 to 16, wherein the one or more emulsifiers are selected from the group consisting of ionic and nonionic surfactants, including mixtures thereof, preferably from the group consisting of nonionic surfactants.

18. The process of embodiment 17, wherein the ionic surfactants comprise one or more ani onic surfactants, preferably one or more anionic surfactants selected from the group con sisting of salts of (C ₆ -Cis)sulfate, (C ₆ -Cie)ethersulfate, (C ₆ -Ci ₈ )sulfonate, {C _& - Ci ₈ )sulfosuccinate (C ₆ -Cis)phosphate, (C ₆ -Ci ₈ )carboxylate, and mixtures of two or more thereof, more preferably from the group consisting of salts of (C ₈ -Ci ₆ )sulfate, (Ce- Ci ₆ )ethersulfate, (C ₈ -Ci ₆ )sulfonate, (C ₈ -Ci ₆ )sulfosuccinate, (C ₈ -Ci ₆ )phosphate, (Ce- Ci ₆ )carboxylate, and mixtures of two or more thereof, more preferably from the group consisting of salts of (Cio-Ci4)sulfate, (Cio-Ci4)ethersulfate, (Cio-Ci4)sulfonate, (Ce- Ci4)sulfosuccinate, (Cio-Ci4)phosphate, (Cio-Ci4)carboxylate, and mixtures of two or more thereof, more preferably from the group consisting of salts of laurylsulfate, laurylsulfonate, di octyl sulfosuccinate, laurylphosphate, laurate, and mixtures of two or more thereof, wherein the counterion is preferably selected from the group consisting of H ⁺ , alkali met als, alkaline earth metals, ammonium, and combinations of two or more thereof, more preferably from the group consisting of H ⁺ , Li ⁺ , Na ⁺ , K ⁺ , ammonium, and combinations of two or more thereof, more preferably from the group consisting of Na ⁺ , K ⁺ , ammonium, and combinations of two or more thereof, wherein even more preferably the counterion is Na ⁺ and/or ammonium, preferably Na ⁺ . The process of embodiment 17 or 18, wherein the ionic surfactants comprise one or more cationic surfactants, preferably one or more cationic surfactants selected from the group consisting of primary, secondary, tertiary, and quaternary ammonium compounds, includ ing mixtures of two or more thereof, wherein more preferably the cationic surfactants comprise one or more quaternary ammonium compounds, preferably selected from the group consisting of salts of (C ₈ -Ci ₈ )trimethylammonium, (C ₈ -Ci ₈ )pyridinium, benzalkoni- um, benzethonium, dimethyldioctadecylammonium, cetrimonium, dioctadecyldime- thylammonium, and mixtures of two or more thereof, more preferably from the group con sisting of salts of cetyltrimethylammonium, dodecyltrimethylammonium, cetylpyridinium, benzalkonium, benzethonium, dimethyldioctadecylammonium, cetrimonium, dioctadecyl- dimethylammonium, wherein the counterion is preferably selected from the group consist ing of halides, carbonates, hydroxide, nitrate, phosphate, sulfate, and combinations of two or more thereof, more preferably from the group consisting of chloride, fluoride, bromide, hydrogen carbonate, hydroxide, nitrate, sulfate, and combinations of two or more thereof, wherein more preferably the counterion is chloride and/or nitrate, preferably chloride. The process of any one of embodiments 17 to 19, wherein the ionic surfactants comprise one or more zwitterionic surfactants, preferably one or more betaines, wherein more pref erably the ionic surfactants comprise cocamidopropyl betaine or alkyldimethylaminoxide. The process of any one of embodiments 17 to 20, wherein the nonionic surfactants are selected from the group consisting of (C8-C22)alcohols, (C6-C2o)alcohol ethoxylates with 1 to 8 ethylene oxide units, (C6-C2o)alkyl polyglycosides, polyoxyethylene glycol alkyl ethers, polyoxypropylene glycol alkyl ethers, glucoside alkyl ethers, polyoxyethylene glycol al- kylphenol ethers, glycerol alkyl esters, sorbitan alkyl esters, polyoxyethylene glycol sorbi- tan alkyl esters, cocamide monoethanolamine, cocamide diethanolamine, dodecyldime- thylamine oxide, block copolymers of polyethylene glycol and polypropylene glycol, poly- ethoxylated tallow amine, and mixtures of two or more thereof,

wherein more preferably the one or more nonionic surfactants are selected from the group consisting of (Ci4-C2o)alcohols, (C ₈ -Ci ₈ )alcohol ethoxylates with 2 to 6 ethylene oxide units, (Ce-Ci ₈ )alkyl polyglycosides, octaethylene glycol monododecyl ether and/or pen- taethylene glycol monododecyl ether, polyoxypropylene glycol alkyl ethers, decyl gluco side, lauryl glucoside, myristil glucoside, octyl glucoside, polyoxyethylene glycol octylphe- nol ethers, preferably triton X-100, nonoxynol-9, glyceryl laurate, polyglycerol polyricinole- ate, sorbitan monolaurate, sorbitan monopalmitate, sorbitan monostearate, sorbitan monooleate, polyoxyethylene sorbitan monolaurate, polyoxyethylene sorbitan monopalmi tate, polyoxyethylene sorbitan monostearate, polyoxyethylene sorbitan monooleate, poly oxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, cocamide monoethanola- mine, cocamide diethanolamine, dodecyldimethylamine oxide, block copolymers of poly ethylene glycol and polypropylene glycol, polyethoxylated tallow amine, and mixtures of two or more thereof,

wherein more preferably the one or more nonionic surfactants are selected from the group consisting of (Ci ₆ -Ci ₈ )alcohols, (Ci ₆ -Cis)alcohol ethoxylates with 2 to 6 ethylene oxide units, (Cs-Ci4)alkyl polyglycosides, preferably cetyl alcohol, stearyl alcohol, oleyl alcohol, and mixtures of two or more thereof, octaethylene glycol monododecyl ether and/or pen- taethylene glycol monododecyl ether, polyoxypropylene glycol alkyl ethers, decyl gluco- side, lauryl glucoside, myristil glucoside, octyl glucoside, polyoxyethylene glycol octylphe- nol ethers, nonoxynol-9, glyceryl laurate, polyglycerol polyricinoleate, sorbitan

monolaurate, sorbitan monopalmitate, sorbitan monostearate, sorbitan oleate, polyoxy ethylene (20) sorbitan monolaurate, polyoxyethylene (20) sorbitan monopalmitate, polyox yethylene (20) sorbitan monostearate, polyoxyethylene (20) sorbitan monooleate, polyox yethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, cocamide monoethanolamine, cocamide diethanolamine, dodecyldimethylamine oxide, block copolymers of polyethylene glycol and polypropylene glycol, polyethoxylated tallow amine, Stearyl-EC> ₂ , polyglyceryl- 2-dipolyhydroxystearate, polyglyceryl-distearate, C13/15 - PEG ₃ , C13 - PEG ₂ , glyceryl monooleate, C16/18 - PEG ₂ , oleyl - PEG ₂ , PEG ₂₀ - sorbitan monooleate, functionalized polyisobutene, C16/18 - PEGg, and mixtures of two or more thereof,

more preferably from the group consisting of polyglyceryl-2-dipolyhydroxystearate, diglyc- eryl-distearate, triglyceryl-distearate, C13/15 - PEG ₃ , C13 - PEG ₂ , glyceryl monooleate, sorbitan monooleate, polyglycerol-3-polyricinoleate, C16/18 - PEG ₂ , oleyl - PEG ₂ , PEG ₂₀ - sorbitan monooleate, functionalized polyisobutene, C16/18 - PEGg, polyoxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, and mixtures of two or more thereof, more preferably from the group consisting of polyg lyceryl-2-d i polyhyd roxystearate, diglyc- eryl-distearate, triglyceryl-distearate, polyoxyethylene (10) oleyl ether, polyoxyethylene (20) oleyl ether, and mixtures of two or more thereof,

wherein it is even more preferred that the nonionic surfactant comprises polyoxyethylene (10) oleyl ether and/or polyoxyethylene (20) oleyl ether.

22. The process of any one of embodiments 1 to 21 , wherein the amount of the one or more emulsifiers in the mixture obtained in (6) and heated in (7) ranges from 0.1 to 10 weight- % based on 100 weight- % of the total amount of the one or more nonpolar organic solvents, the one or more polar protic solvents, and the one or more emulsifiers, preferably from 0.3 to 5 weight-%, more preferably from 0.5 to 3 weight-%, and more preferably from 1 to 2 weight-%. The process of any one of embodiments 1 to 22, wherein the one or more bases comprise one or more metal hydroxides and/or one or more metal hydroxide precursors, preferably one or more metal hydroxides, more preferably one or more metal hydroxides selected from the group consisting of potassium hydroxide, sodium hydroxide, magnesium hydrox ide, calcium hydroxide, iron hydroxide, aluminum hydroxide, and copper hydroxide, wherein more preferably the one or more bases comprise sodium hydroxide. The process of any one of embodiments 1 to 23, wherein emulsification in (2) is achieved by agitation, preferably by stirring and/or sonication, and more preferably by stirring. The process of any one of embodiments 1 to 24, wherein emulsification in (2) is achieved by use of a homogenizer, preferably with a rotor-stator homogenizer, with an ultrasonic homogenizer, with a high pressure homogenizer, by microfluidic systems, or by mem brane emulsification, more preferably with a high pressure homogenizer or with a rotor- stator homogenizer, and more preferably with a rotor-stator homogenizer. The process of embodiment 25, wherein stirring is performed at a speed in the range of from 500 to 35,000, preferably from 1 ,000 to 32,000, more preferably from 3,000 to 30,000, more preferably from 5,000 to 28,000, more preferably from 7,000 to 26,000, more preferably from 9,000 to 22,000, more preferably from 11 ,000 to 20,000, more pref erably from 13,000 to 18,000, and more preferably from 15,000 to 16,000. The process of any one of embodiments 1 to 26, wherein emulsification in (2) is conduct ed for a period ranging from 0.1 to 10 min, preferably from 0.2 to 6 min, more preferably from 0.4 to 4 min, more preferably from 0.6 to 3 min, more preferably from 0.8 to 2.5 min, more preferably from 1 to 2 min, more preferably from 1.2 to 1.8 min, and more preferably from 1.4 to 1.6 min. The process of any one of embodiments 1 to 27, wherein X is selected from the group consisting of Al, B, In, Ga, and combinations of two or more thereof, X preferably being Al. The process of any one of embodiments 1 to 28, wherein the one or more sources of X2O3 comprises one or more compounds selected from the group consisting of aluminum salts and aluminum alkoxides, preferably from the group consisting of aluminates of an alkali metal, aluminum hydroxides, aluminum alkoxides, and mixtures of two or more thereof, wherein more preferably the one or more sources of X2O3 comprises one or more alumi num alkoxides AI(OR)3, wherein R stands for optionally branched (Ci-Ce)alkyl, preferably (Ci-Cs)alkyl, more preferably (Ci-C ₄ )alkyl, and more preferably for optionally branched (Ci-C3)alkyl, wherein more preferably R stands for methyl, ethyl, n-propyl, isopropyl, or mixtures of two or more thereof, more preferably for ethyl, n-propyl, isopropyl, or mixtures of two or more thereof, more preferably for n-propyl and/or isopropyl, and more preferably for isopropyl. The process of embodiment 29, wherein the alkali metal is selected from the group con sisting of Li, Na, K, Rb, and Cs, wherein preferably the alkali metal is Na and/or K, and wherein even more preferably the alkali metal is Na. The process of any one of embodiments 1 to 30, wherein the metal M is selected from the group consisting of Mg, Ti, Cu, Co, Cr, Ni, Fe, Mo, Mn, Ru, Rh, Pd, Ag, Os, Ir, Pt, Au, and mixtures of two or more thereof, preferably from the group consisting of Ti, Cu, Fe, Rh,

Pd, Pt, and mixtures of two or more thereof, wherein more preferably the metal M com prises Cu and/or Fe, preferably Cu, wherein more preferably the metal M is Cu and/or Fe, preferably Cu. The process of any one of embodiments 1 to 31 , wherein the one or more sources of a metal M is selected from the group consisting of metal salts, metal alkoxides, metal car- boxy I ates, and mixtures of two or more thereof, wherein preferably the one or more sources of a metal M comprises one or more metal alkoxides and/or metal carboxylates, wherein more preferably one or more metal alkoxides are employed as the one or more sources of a metal M. The process of embodiment 32, wherein the one or more metal salts are selected from the group consisting of halides, hydroxides, sulfates, nitrates, phosphates, acetates, octade- canoate, 2-(2-methoxyethoxy)ethanolate, and mixtures of two or more thereof, preferably from the group consisting of chlorides, bromides, sulfates, nitrates, acetates, octadecano- ate, 2-(2-methoxyethoxy)ethanolate, and mixtures of two or more thereof, more preferably from the group consisting of bromides, nitrates, octadecanoate, 2-(2-methoxyethoxy)- ethanolate, and mixtures of two or more thereof, wherein more preferably the one or metal salts comprise nitrates, octadecanoate, and/or 2-(2-methoxyethoxy)ethanolate, preferably 2-(2-methoxyethoxy)ethanolate, and wherein more preferably the one or metal salts are nitrates, octadecanoate and/or 2-(2-methoxyethoxy)ethanolate, preferably 2-(2- methoxyethoxy)ethanolate. The process of embodiment 32 or 33, wherein the one or more metal alkoxides comprise a trivalent metal ion and a divalent metal ion, wherein the tri valent metal ion is selected from the group consisting of Al, Ga, In, Fe, Co, Mn, Cr, La, Pr, Ce, Nd, Sm, Gd, Dy, Ho,

Er, Yb, Lu, Sc, Y, and combinations of two or more thereof, and the divalent metal ion is selected from the group consisting of Mg, Ca, Sr, Ba, Zn, Cd, Cu, Ni, Co, Mn, Be, Zr, and combinations of two or more thereof, wherein preferably the trivalent metal ion is selected from the group consisting of Al, Ga, In, Fe, Co, Mn, Cr, La, Pr, Ce, Y, and combinations of two or more thereof, and the divalent metal ion is selected from the group consisting of Zn, Cu, Ni, Co, Mn, and combinations of two or more thereof,

wherein more preferably the trivalent metal ion is selected from the group consisting of Al, Ga, Y, and combinations of two or more thereof, and the divalent metal ion is selected from the group consisting of Cu, Ni, Co, and combinations of two or more thereof, wherein more preferably the one or more metal alkoxides comprises Cu and Al as metal ions, wherein more preferably the metal ions in the one or more alkoxides are Cu and Al.

35. The process of any one of embodiments 32 to 34, wherein the alkoxides are selected from the group consisting of (Ci-Cio)alkoxides, preferably of (C3-C8)alkoxides, more preferably of (C5-C7)alkoxides, where more preferably the alkoxides are C ₆ -alkoxides, preferably alkoxides of hexanol, and more preferably alkoxides of n-hexanol.

36. The process of any one of embodiments 32 to 35, wherein the carboxylates are selected from the group consisting of (C10-C25) carboxylates, preferably of (C16-C20) carboxylates, more preferably of (C17-C19) carboxylates, wherein more preferably the carboxylates are octadecanoate.

37. The process of any one of embodiments 32 to 36, wherein the one or more metal alkox ides comprise CuA (OR) ₆ , wherein R is hexyl, preferably n-hexyl.

38. The process of any one of embodiments 1 to 37, wherein the one or more sources of S1O2 comprises one or more compounds selected from the group consisting of silicas, silicates, and mixtures thereof,

preferably from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, silicic acid, water glass, sodium metasilicate hydrate, sesquisilicate, disilicate, colloidal silica, pyrogenic silica, silicic acid esters, tetraalkoxysilanes, and mix tures of two or more thereof,

more preferably from the group consisting of fumed silica, silica hydrosols, silica gel, silicic acid, water glass, colloidal silica, pyrogenic silica, silicic acid esters, tetraalkoxysilanes, and mixtures of two or more thereof,

more preferably from the group consisting of silica hydrosols, silicic acid, water glass, col loidal silica, silicic acid esters, tetraalkoxysilanes, and mixtures of two or more thereof, more preferably from the group consisting of water glass, colloidal silica, silicic acid es ters, tetraalkoxysilanes, and mixtures of two or more thereof

more preferably from the group consisting of water glass, colloidal silica, and mixtures thereof,

wherein more preferably the one or more sources of S1O2 is selected from the group con sisting of water glass, colloidal silica, and mixtures thereof, wherein more preferably col loidal silica is employed as the one or more sources of S1O2. The process of any one of embodiments 1 to 38, wherein independently from one another,

(I ), (3), (4), (5), (6), and (7) are performed under agitation of the mixture, preferably under stirring and/or sonication of the mixture, and more preferably under stirring of the mixture. The process of any one of embodiments 1 to 39, wherein heating in (7) is conducted at a temperature in the range of from 80 to 260°C, preferably from 100 to 240°C, more prefer ably from 120 to 220°C, more preferably from 140 to 200°C, more preferably from 160 to 180°C, and more preferably from 165 to 175°C. The process of any one of embodiments 1 to 40, wherein heating in (7) is conducted for a period in the range of from 0.5 to 120 h, preferably from 1 to 114 h, more preferably from 3 to 108 h, more preferably from 6 to 102 h, more preferably from 12 to 96 h, more prefer ably from 18 to 84 h, more preferably from 24 to 72 h, more preferably from 30 to 66 h, more preferably from 36 to 60 h, more preferably from 42 to 54 h, more preferably from 45 to 51 h, and more preferably from 47 to 49 h. The process of any one of embodiments 1 to 41 , wherein heating in (7) is conducted un der autogenous pressure. The process of any one of embodiments 1 to 42, wherein the process further comprises

(8) isolating the metal-exchange zeolitic material obtained in (7);

and/or, preferably and

(9) washing the metal-exchange zeolitic material obtained in (7) or (8);

and/or, preferably and

(10) drying the metal-exchange zeolitic material obtained in (7), (8), or (9);

and/or, preferably and

(I I) calcining the metal-exchange zeolitic material obtained in (7), (8), (9) or (10). The process of embodiment 43, wherein isolation in (8) is achieved by filtration and/or centrifugation, preferably by filtration. The process of embodiment 43 or 44, wherein washing in (9) is conducted with a solvent system comprising one or more solvents, wherein preferably the one or more solvents are selected from the group consisting of polar protic solvents, polar aprotic solvents and mix tures thereof,

more preferably from the group consisting of n-butanol, isopropanol, propanol, ethanol, methanol, water, acetone, and mixtures thereof,

more preferably from the group consisting of ethanol, methanol, water, acetone, and mix tures thereof, wherein more preferably the solvent system comprises water or acetone, and wherein more preferably water is used as the solvent system, preferably deionized water.

46. The process of any one of embodiments 43 to 45, wherein drying in (10) is conducted at a temperature in the range of from 20 to 160°C, preferably from 30 to 140°C, more prefera bly from 40 to 120°C, more preferably from 50 to 110°C, more preferably from 60 to 100°C, more preferably from 70 to 90°C, and more preferably from 75 to 85°C.

47. The process of any one of embodiments 43 to 46, wherein calcining in (1 1) is conducted at a temperature in the range of from 300 to 750°C, preferably from 325 to 650°C, more preferably from 350 to 600°C, more preferably from 375 to 575 °C, more preferably from 375 to 550°C, more preferably from 400 to 500°C, and more preferably from 425 to 475°C.

48. The process of any one of embodiments 1 to 47, wherein the mixture obtained in (6) and heated in (7) further comprises seed crystals, wherein the seed crystals preferably com prise one or more zeolitic materials, more preferably one or more zeolitic materials having the framework structure type of the zeolitic material obtained in (7), wherein more prefera bly the one or more zeolitic materials comprise SSZ-13 and/or chabazite, preferably SSZ- 13.

49. The process of embodiment 48, wherein the amount of seed crystals in the mixture ob tained in (6) and heated in (7) is in the range of from 0.1 to 20 weight- % based on 100 weight- % of the total amount of the one or more sources of SiC>2, calculated as S1O2, and the one or more sources of X2O3, calculated as X2O3, contained in the mixture obtained in (6), preferably from 0.3 to 15 weight-%, more preferably from 0.5 to 10 weight-%, more preferably from 1 to 8 weight-%, more preferably from 3 to 7 weight-%, more preferably from 4 to 6 weight-%, and more preferably from 4.5 to 5.5 weight-%.

50. The process of any one of embodiments 1 to 49, wherein (7) is conducted in a batch mode and/or in a continuous mode, wherein preferably the process is conducted in a batch mode and/or in a continuous mode.

51. The process of any one of embodiments 1 to 50, wherein (7) comprises

(i) continuously feeding the mixture obtained in (6) into a continuous flow reactor; and

(ii) heating the mixture obtained in (6) in the continuous flow reactor for crystallizing a metal-exchanged zeolitic material comprising S1O2 and X2O3 in its framework structure.

52. The process of embodiment 51 , wherein heating in (ii) is conducted at a temperature in the range of from 100 to 300 °C, preferably of from 100 to 280 °C, more preferably of from 150 to 270 °C, more preferably of from 180 to 260 °C, more preferably of from 200 to 250 °C, more preferably of from 210 to 240 °C, and more preferably of from 220 to 235 °C.

53. The process of embodiments 51 or 52, wherein in (i) the mixture is fed into the continuous flow reactor at a liquid hourly space velocity in the range of from 0.3 to 20 IT ¹ , preferably of from 0.05 to 10 IT ¹ , more preferably from 0.1 to 5 IT ¹ , more preferably from 0.2 to 3 IT ¹ , more preferably from 0.4 to 2 IT ¹ , more preferably from 0.6 to 1.5 IT ¹ , more preferably from 0.8 to 1.2 IT ¹ , and more preferably from 0.9 to 1 IT ¹ .

54. The process of any one of embodiments 51 to 53, wherein the mixture obtained in (6) is continuously fed in (i) and heated in (ii) for at least 1 h, preferably for a duration in the range of from 3 h to 360 d, more preferably from 6 h to 120 d, more preferably from 12 h to 90 d, more preferably from 18 h to 60 d, more preferably from 1 to 30 d, more prefera bly from 1.5 to 25 d, more preferably from 2 to 20 d, more preferably from 2.5 to 15 d, more preferably from 3 to 12 d, more preferably from 3.5 to 8 d, and more preferably from 4 to 6 d.

55. The process of any one of embodiments 51 to 54, wherein the volume of the continuous flow reactor is in the range of from 50 cm ³ to 75 m ³ , preferably of from 50 cm ³ to 3 m ³ , more preferably from 55 cm ³ to 1 m ³ , more preferably from 60 cm ³ to 0.7 m ³ , more prefer ably from 65 cm ³ to 0.3 m ³ , more preferably from 70 cm ³ to 0.1 m ³ , more preferably from 75 to 70,000 cm ³ , more preferably from 80 to 50,000 cm ³ , more preferably from 85 to 30,000 cm ³ , more preferably from 90 to 10,000 cm ³ , more preferably from 95 to 7,000 cm ³ , more preferably from 100 to 5,000 cm ³ , more preferably from 105 to 3,000 cm ³ , more preferably from 110 to 1 ,000 cm ³ , more preferably from 115 to 700 cm ³ , more preferably from 120 to 500 cm ³ , more preferably from 125 to 350 cm ³ , more preferably from 130 to 250 cm ³ , more preferably from 135 to 200 cm ³ , more preferably from 140 to 180 cm ³ , and more preferably from 145 to 160 cm ³ .

56. The process of any one of embodiments 51 to 55, wherein the continuous flow reactor is selected among a tubular reactor, a ring reactor, and a continuously oscillating reactor, preferably among a plain tubular reactor, a tubular membrane reactor, a tubular reactor with Coanda effect, a ring reactor, a continuously oscillating baffled reactor, and combina tions thereof, wherein more preferably the continuous flow reactor is a plain tubular reac tor and/or a ring reactor, wherein more preferably the continuous flow reactor is a plain tubular reactor.

57. The process of any one of embodiments 51 to 56, wherein the continuous flow reactor is a tubular reactor, and wherein at least a portion of the tubular reactor is of a regular cylindri cal form having a constant inner diameter perpendicular to the direction of flow, wherein the inner diameter is preferably in the range of from 2 to 1200 mm, more preferably from 3 to 800 mm, more preferably from 3 to 500 mm, more preferably from 4 to 200 mm, more preferably from 4 to 100 mm, more preferably from 4.5 to 50 mm, more preferably from 4.5 to 30 mm, more preferably from 5 to 15 mm, more preferably from 5 to 10 mm, more preferably from 5.5 to 8 mm, and more preferably from 5.5 to 6.5 mm.

58. The process of any one of embodiments 51 to 57, wherein the continuous flow reactor has a length in the range of from 0.2 to 5,000 m, preferably from 0.5 to 3,000 m, more prefer ably from 1 to 1 ,000 m more preferably from 3 to 500 m more preferably from 3.5 to 200 m, more preferably from 3.5 to 100 m, more preferably from 4 to 50 m, more preferably from 4 to 30 m, more preferably from 4.5 to 20 m, more preferably from 4.5 to 15 m, more preferably from 5 to 10 m, and more preferably from 5 to 7 m.

59. The process of any one of embodiments 51 to 58, wherein the wall of the continuous flow reactor is made of a metallic material, wherein the metallic material comprises one or more metals selected from the group consisting of Ta, Cr, Fe, Ni, Cu, Al, Mo, and combi nations and/or alloys of two or more thereof, preferably from the group consisting of Ta,

Cr, Fe, Ni, Mo, and combinations and/or alloys of two or more thereof, more preferably from the group consisting of Cr, Fe, Ni, Mo, and combinations and/or alloys of two or more thereof wherein preferably the metallic material comprises a nickel alloy, a nickel- molybdenum alloy, and more preferably a nickel-molybdenum-chromium alloy.

60. The process of any one of embodiments 51 to 59, wherein the surface of the inner wall of the continuous flow reactor is lined with an organic polymer material, wherein the organic polymer material preferably comprises one or more polymers selected from the group consisting of fluorinated polyalkylenes and mixtures of two or more thereof, more prefera bly from the group consisting of (C2-C3)polyalkylenes and mixtures of two or more there of, preferably from the group consisting of fluorinated polyethylenes and mixtures of two or more thereof, wherein more preferably the polymer material comprises

poly(tetrafluoroethylene), wherein more preferably the inner wall of the continuous flow reactor is lined with poly(tetrafluoroethylene).

61. The process of any one of embodiments 51 to 60, wherein the continuous flow reactor is straight and/or comprises one or more curves with respect to the direction of flow, wherein preferably the continuous flow reactor is straight and/or has a coiled form with respect to the direction of flow.

62. The process of any one of embodiments 51 to 61 , wherein the walls of the continuous flow reactor are subject to vibration during heating in (ii). The process of any one of embodiments 51 to 62, wherein in (ii) the mixture is heated under autogenous pressure, wherein preferably the pressure is in the range of from 0.5 to 15 MPa, more preferably in the range of from 1 to 10 MPa, more preferably from 2 to 8 MPa, more preferably from 3 to 7 MPa, more preferably from 3.5 to 6.5 MPa, more prefer ably from 4 to 6 MPa, more preferably from 4.5 to 5.5 MPa, and more preferably from 4.8 to 5.2 MPa. The process of any one of embodiments 51 to 63, wherein the continuous flow reactor consists of a single stage. The process of any one of embodiments 51 to 64, wherein no matter is added to and/or removed from the mixture during its passage through the continuous flow reactor in (ii), wherein preferably no matter is added, wherein more preferably no matter is added and no matter is removed from the mixture during its passage through the continuous flow re actor in (ii). The process of any one of embodiments 51 to 65, wherein prior to (i) the mixture obtained in (6) is aged at a temperature in the range of from 40 to 120 °C, preferably from 50 to 110 °C, more preferably from 60 to 105 °C, more preferably from 70 to 100 °C, more prefera bly from 75 to 95 °C, and more preferably from 80 to 90 °C. The process of any one of embodiments 51 to 66, wherein prior to (i) the mixture obtained in (6) is aged for a duration ranging from 1 to 72 h, preferably from 6 to 60 h, more prefer ably from 12 to 54 h, more preferably from 14 to 42 h, more preferably from 16 to 36 h, more preferably from 18 to 32 h, and more preferably from 20 to 28 h. The process of any one of embodiments 51 to 67, wherein (7) further comprises

(iii) quenching the reaction product effluent continuously exiting the reactor in (ii) with a liquid comprising one or more solvents and/or via expansion of the reaction product efflu ent. The process of embodiment 68, wherein in (iii) the liquid comprises one or more solvents selected from the group consisting of polar pro tic solvents and mixtures thereof, preferably from the group consisting of n-hexanol, n-pentanol, n-butanol, isopropanol, propanol, ethanol, methanol, water, and mixtures thereof,

more preferably from the group consisting of ethanol, methanol, water, and mixtures thereof,

wherein more preferably the liquid comprises water, and wherein more preferably water is used as the liquid, preferably deionized water. 70. The process of any one of embodiments 1 to 69, wherein the mean particle size D50 by volume as determined according to ISO 13320:2009 of the zeolitic material obtained in (7) is of at least 0.5 pm, and is preferably in the range of from 0.5 to 1.5 pm, more preferably in the range of from 0.6 to 1.0 pm, and more preferably in the range of from 0.6 to 0.8 pm.

71. A metal-exchanged zeolitic material comprising S1O ₂ and X ₂ O ₃ in its framework structure, wherein X is a trivalent element, wherein said metal-exchanged zeolitic material is ob tained and/or obtainable according to the process of any one of embodiments 1 to 70.

72. The metal-exchanged zeolitic material of embodiment 71 , wherein the metal-exchanged zeolitic material has a framework structure type selected from the group consisting of MFI, BEA, CHA, AEI, MWW, LEV, GME, FAU, FER, MEL, MOR, and intergrowth structures thereof, preferably from the group consisting of MFI, BEA, CHA, AEI, MWW, and inter growth structures thereof, more preferably from the group consisting of BEA, CHA, AEI, MFI, and intergrowth structures thereof, wherein more preferably the zeolitic material has a CHA and/or AEI and/or MFI type framework structure, preferably a CHA or MFI type framework structure.

73. The metal-exchanged zeolitic material of embodiment 71 or 72, wherein the metal- exchanged zeolitic material is metal-exchanged SSZ-13 and/or chabazite, preferably met al-exchanged SSZ-13.

74. The metal-exchanged zeolitic material of embodiment 71 or 72, wherein the metal- exchanged zeolitic material is metal-exchanged Silicalite, ZSM-5, [Fe-Si-0]-MFI, [Ga-Si- 0]-MFI, [As-Si-0]-MFI, AMS-1 B, AZ-1 , Bor-C, Encilite, Boralite C, FZ-1 , LZ-105, Mu- tinaite, NU-4, NU-5, TS-1 , TSZ, TSZ-III, TZ-01 , U SC-4, USI-108, ZBH, ZKQ-1 B, ZMQ-TB, MnS-1 , FeS-1 , or a mixture of two or more thereof, preferably Silicalite, ZSM-5, AMS-1 B, AZ-1 , Encilite, FZ-1 , LZ-105, Mutinaite, NU-4, NU-5, TS-1 , TSZ, TSZ-III, TZ-01 , U SC-4, USI-108, ZBH, ZKQ-1 B, ZMQ-TB, or a mixture of two or more thereof, wherein more pref erably the metal-exchanged zeolitic material is metal-exchanged Silicalite and/or ZSM-5, wherein more preferably the metal-exchanged zeolitic material is metal-exchanged ZSM- 5.

75. Use of a metal-exchanged zeolitic material according to any one of embodiments 71 to 74 as a molecular sieve, as an adsorbent, for ion-exchange, as a catalyst or a precursor thereof, and/or as a catalyst support or a precursor thereof, preferably as a catalyst or a precursor thereof and/or as a catalyst support or a precursor thereof, more preferably as a catalyst or a precursor thereof, more preferably as a catalyst for the selective catalytic re duction (SCR) of nitrogen oxides NO _x ; for the storage and/or adsorption of CO ₂ ; for the ox idation of NH ₃ , in particular for the oxidation of NH ₃ slip in diesel systems; for the decom position of N ₂ O; as an additive in fluid catalytic cracking (FCC) processes; and/or as a catalyst in organic conversion reactions, preferably in the conversion of alcohols to olefins, and more preferably in methanol to olefin (MTO) catalysis; more preferably for the selec tive catalytic reduction (SCR) of nitrogen oxides NO _x , and more preferably for the selec tive catalytic reduction (SCR) of nitrogen oxides NO _x in exhaust gas from a combustion engine, preferably from a diesel engine or from a lean burn gasoline engine.

DESCRIPTION OF THE FIGURES

Figures 1-3, and 5 respectively show the SEM images of a portion of a sample of the product obtained from Reference Example 2 and Examples 2, 3, and 5, respectively, at different magnifications, wherein the scale in the images are indicated by the leg end at the bottom right of the respective image.

Figure 4 displays a conceptual diagram of the location of the copper sources in the emul sion synthesis depending on its chemical nature.

EXPERIMENTAL SECTION

Reference Example 1 : Characterization via SEM and TEM

Crystal morphology and size were investigated using scanning electron microscopy (SEM) on a Philips XL30 SEM FEG microscope. High-resolution transmission electron microscopy

(HRTEM) data were collected with an FEI Tecnai G2 Spirit Twin TEM operating at 120 kV using a Gatan US1000 2k x 2k CCD camera.

Reference Example 2: Determination of X-ray diffraction pattern and of crystallinity

Powder X-ray diffraction (PXRD) data was collected using a diffractometer (D8 Advance Series II, Bruker AXS GmbH) equipped with a LYNXEYE detector operated with a copper anode X-ray tube running at 40kV and 40mA. The geometry was Bragg-Brentano, and air scattering was reduced using an air scatter shield.

Computing crystallinity: The crystallinity of the samples was determined using the software DIF- F RAC. EVA provided by Bruker AXS GmbH, Karlsruhe. The method is described on page 121 of the user manual. The default parameters for the calculation were used.

Computing phase composition: The phase composition was computed against the raw data using the modelling software DIFFRAC.TOPAS provided by Bruker AXS GmbH, Karlsruhe. The crystal structures of the identified phases, instrumental parameters as well the crystallite size of the individual phases were used to simulate the diffraction pattern. This was fit against the data in addition to a function modelling the background intensities. Data collection: The samples were homogenized in a mortar and then pressed into a standard flat sample holder provided by Bruker AXS GmbH for Bragg-Brentano geometry data collection. The flat surface was achieved using a glass plate to compress and flatten the sample powder. The data was collected from the angular range 2 to 70 ° 2Theta with a step size of 0.02°

2Theta, while the variable divergence slit was set to an angle of 0.1 °. The crystalline content describes the intensity of the crystalline signal to the total scattered intensity. (User Manual for DIFFRAC.EVA, Bruker AXS GmbH, Karlsruhe.)

Reference Example 3: Synthesis of a zeolitic material having a CHA type framework structure

101.52 g water, 10.33 g sodium hydroxide, 192.72 g of an aqueous solution of adamantyl trime thyl ammonium hydroxide (20 weight- % in water), 657 g o-xylene, and 29.40 g emulsifier (Eu- mulgin® S2, BASF) were mixed within 3 min using a homogenizer (Polytron PT DA 30/4 EC, Draeger) under stirring with 11 ,250 rpm to obtain an emulsion. To this emulsion 32.40 g alumi num isopropoxide (AI(OiPr)3) were added and the resulting emulsion stirred for 1 h at 200 rpm in a beaker. Then, 388.03 g colloidal silica (Ludox AS-40) were added to the emulsion and the resulting emulsion stirred for 10 min. The resulting emulsion was then charged in a 2.5I auto clave. The emulsion was then heated under stirring with 200 rpm at a temperature of 170 °C. Said temperature was hold for 48 h. After that, a white suspension was obtained which was cooled down. For work-up, the suspension was filtrated and the separated solids washed with water until the washing water had a pH of 7. The solids were dried over night at 120 °C and subsequently calcined in air at 550 °C for 2 h, wherein the heating rate was set to 2 °C per min. The obtained solids had a crystallinity of 94 % and comprised a CHA phase, a ZSM-39 phase, and a Kenyaite phase, as determined according to Reference Example 2.

SEM images of the zeolitic material of Reference Example 3 are shown in Figure 1 , as deter mined according to Reference Example 1. In said SEM images it can be seen that the CHA crystals have a size of about 20-30 nm which aggregated. Moreover, residual by phases like ZSM-39 and Kenyaite phases have been detected. The particles of the crystalline by-phases have been much bigger than those from CHA.

Reference Example 4: Preparation of Copper aluminum hexanolate (CuA (OHex) ₈ )

Copper aluminum hexanolate (CuAh(OHex) ₈ ) which was used for the examples was prepared as disclosed in WO 2016/096990 A1.

Comparative Example 1 : One-pot synthesis of a Cu-CHA with lower amount of Cu source

Reference Example 3 was repeated, whereby 5.20 g copper aluminum hexanolate

(CuA (OHex) ₈ ) were added together with the colloidal silica. SEM images of the zeolitic material of Comparative Example 1 are shown in Figure 2, as de termined according to Reference Example 1. The obtained solids had a crystallinity of 90 %. As can be seen, the CHA crystals of Comparative Example 1 have a size of about 100 nm. How ever, the solids comprised a CHA phase, a ZSM-39 phase, and a ZSM-5 phase, as determined according to Reference Example 2.

Comparative Example 2: One-pot synthesis of a Cu-CHA with higher amount of Cu source

Reference Example 3 was repeated, whereby 23.4 g copper aluminum hexanolate

(CuAh(OHex) ₈ ) were added together with the colloidal silica.

SEM images of the zeolitic material of Comparative Example 2 are shown in Figure 3, as de termined according to Reference Example 1. The obtained solids had a crystallinity of 92 %. In said SEM pictures of the zeolitic material, no ZSM-5 and ZSM-39 phases have been detected but a Kenyaite phase was detected. Thus, the solids comprised a CHA phase, and a Kenyaite phase, as determined according to Reference Example 2.

Example 3: Preparation of a Cu-containing CHA zeolite

For a first mixture, 21.42 g of an aqueous solution of adamantyl trimethyl ammonium hydroxide (20 weight- % in water), 1.05 g of an aqueous solution of sodium hydroxide (50 weight- % in wa ter), 3.18 g of an aqueous solution of emulsifier (Eumulgin® S2, 3 weight- % in water, BASF) were mixed in a 225 ml Teflon insert for an autoclave (DAB-3 autoclave, Berghof) with 50 ml o- xylene. Said mixture was emulsified with 16000 rpm for 1-2 min until a milky white emulsion forms (Ultra-Turrax disperser, IKA). Then, a Teflon stirrer was used for further stirring. Under stirring, 21.67 g of colloidal silica (Ludox AS-40) was subsequently added to the emulsion to obtain the first mixture. The water content of the resulting first mixture was about 30 ml.

For a second mixture, 0.156 g aluminum isopropoxide (AI(OiPr)3) were dissolved in a crimp vial in 20 ml o-xylene under argon using ultra-sonification for approximately 20 min. Then, 17.61 g of copper aluminum hexanolate (CuAh(OHex) ₆ ) were added to the aluminum isopropoxide solu tion in o-xylene to obtain the second mixture.

Then, the second mixture was added to the first mixture. The resulting mixture having a water to o-xylene ratio of about 30 to 70 volume-% was stirred for 10 min in the Teflon insert. The mix ture was then subjected to hydrothermal treatment for 48 h at 170 °C under vigorous stirring.

For work-up, the solids were filtered of using a Buchner funnel equipped with a filter paper (white ribbon) and washed with 100-150 ml de-ionized water and approximately 50 ml acetone. The obtained solids were dried at 80 °C and subsequently calcined in air at 550 °C for 2 h (the heating rate was set to 2 °C per min). The relative content of silicon, aluminum and copper has been determined using TEM micros copy for Example 3, as determined according to Reference Example 1. The results are listed in table 1.

Table 1

Relative contents of silicon, aluminum, and copper according to TEM analysis for Example 3

According to the X-ray diffraction analysis the zeolitic material of Example 3 comprised only CHA as unique crystalline phase. The observed crystallinity in the XRD was 78 %. Further, it was found that the zeolitic material of Example 3 comprised a comparatively high content of aluminum and copper, indicating that the introduction of a metal source via the organic phase of the emulsion is very effective.

Example 4: Preparation of a Cu-containing CHA zeolite using a different Cu source

For Example 4, Example 3 was repeated whereby a different copper source has been used in a different amount. The source and amount thereof is listed in table 2. The ratio of water to o-xylene was approximately 30 to 70 volume-%.

Table 2

Copper source and amount thereof used for the preparation of Cu-containing CHA zeolite, wherein OMEE is a 2-(2-methoxyethoxy)ethanolate group

According to the X-ray diffraction analysis the zeolitic material of Example 4 comprised only CHA as unique crystalline phase. The observed crystallinity in the XRD was 71 %.

Figure 5 shows the SEM image of the zeolitic materials according to Example 4. It was found that the particles had sizes between 100 nm and up to greater than 5 pm. Surprisingly, particles with bigger sizes were obtained for Example 4 where the Cu source was placed“near” (see image for Cu(OMEE)2 as source) or in the water phase (see e. g. image for“Cu as chloride”) of the water/oil emulsion system. A conceptual drawing is given in figure 4 showing a general overview where the different species are located in the water/oil emulsion system.

Further, the relative content of silicon, aluminum and copper has been determined using TEM microscopy for Example 4, as determined according to Reference Example 1. The results are listed in table 3.

Table 3

Relative contents of silicon, aluminum, and copper according to TEM analysis for Example 4

It was found that the zeolitic material of Example 4 comprised a comparatively high content of aluminum and copper. Further, it was found that the amount of Cu and Al introduced in the zeo litic framework structure was lower in comparison to Example 3 synthesized using CuAl2(OHex)6 as precursor.

Comparative Examples 5-8: One-pot synthesis of Cu-CHA using different sources of copper

For each of Examples 5-8, Example 3 was repeated whereby each time a different copper source has been used in a different amount. Further, the copper source was added to the first mixture and not to the second mixture. The source and amount thereof are listed in table 4 be low for each example. The ratio of water to o-xylene was the same for all examples 5-8 being approximately 30 to 70 volume-%.

Table 4

Copper source and amount thereof used for the one-pot synthesis of Cu-CHA, wherein OMEE is a 2-(2-methoxyethoxy)ethanolate group

According to the X-ray diffraction analysis all of the zeolitic materials of Examples 5-8 com prised only CHA as unique crystalline phase. The observed crystallinity in the XRD was at least 78 %.

Figure 5 shows the SEM images of the zeolitic materials according to Examples 5-8 wherein the Cu source was varied. It was found that the particles had sizes between 100 nm and up to greater than 5 pm, depending on the used Cu source. Surprisingly, particles with bigger sizes were obtained for those examples where the Cu source was placed“near” (see image for CU(OM EE)2 as source) or in the water phase (see e. g. image for“Cu as chloride”) of the wa ter/oil emulsion system. A conceptual drawing is given in figure 4 showing a general overview where the different species are located in the water/oil emulsion system.

Further, the relative content of silicon, aluminum and copper has been determined using TEM microscopy for Examples 5 and 6, as determined according to Reference Example 1. The re sults are listed in table 5.

Table 5 Relative contents of silicon, aluminum, and copper according to TEM analysis for Examples 5 and 6

It was found that the zeolitic material with comparatively high contents of aluminum and copper was the material synthesized using CuAh(OHex) ₆ , indicating that the introduction of metal sources via the organic phase of the emulsion is the most effective as regards the inventive synthetic approach. The addition of copper salts in form of acetate or sulfate led to the introduc tion of less copper in the final particles, suggesting that the Cu incorporation using metal salts via the aqueous phase of the emulsion is comparatively less effective.

Further, it was found that the introduction of Cu is higher when Cu(OMEE)2 was used as copper source and the introduction of Al is lower than in the examples prepared using copper salts as Cu sources. The amount of Cu and Al introduced in the zeolitic framework structure in compari son to the example synthesized using CuAh(OHex) ₆ as precursor was lower.

Example 9: Preparation of a Cu-containing MFI zeolite

1.5 g copper(ll) stearate (Sigma Aldrich) were dissolved in 20 ml xylene and subjected to ultra- sonification. Separately, 0.8 g of sodium aluminate (NaAIC^; Alfa Aesar) were put in a Teflon insert for an autoclave (DAB-3 autoclave from Berghof GmbH). 2.5 ml of de-ionized water and 25 ml of an aqueous solution of tetrapropyl ammonium hydroxide (TPAOH; 40 weight- % in wa ter) were added thereto and the resulting mixture stirred for 5 minutes. Then, 50 ml xylene and 1.05 g of an aqueous solution of emulsifier (Eumulgin® S2, 3 weight- % in water, BASF) were added and the resulting mixture was emulsified for 2-3 minutes using an Ultraturrax. Subse quently, 14.3 g of a colloidal silica-containing aqueous suspension (Ludox-40; Sigma Aldrich) were added thereto. Then, the copper(ll) stearate-containing xylene solution was added thereto. A gel started to form, whereby phase separation occurred within 2 to 3 minutes. The mixture was further stirred for 5 minutes. The resulting reaction mixture was then subjected to hydro- thermal conditions at a temperature of 175 °C under stirring for 5 days. After that, the reaction mixture was cooled to room temperature, filtrated with a Buchner funnel (blue ribbon paper fil ter) and the thus obtained solids washed with 250 ml de-ionized water and subsequently with 50 ml acetone. The resulting washed solids were dried at 80 °C for 16 h.

According to the powder X-ray diffraction analysis according to Reference Example 2 the zeolit- ic material of Example 9 comprised only MFI as unique crystalline phase. The observed crystal linity in the XRD was at least 97 %. No copper oxide reflexes were observed in the powder X- ray diffraction pattern. The resulting product had a copper content of 2 weight-%. Example 10: Preparation of a Cu-containing CHA zeolite

In a crimp vial, 2.967 g copper(ll) stearate (Sigma Aldrich) were dissolved in 50 ml xylene and subjected to ultra-sonifi cation. Separately, a mixture of 0.926 g of aluminum hydroxide (AIOH3; gibbsite) and 20 ml xylene was provided in a Teflon insert for an autoclave (DAB-3 autoclave from Berghof GmbH). 21 .42 g of an aqueous solution of adamantyl trimethyl ammonium hydrox ide (AdaTAOH; 20 weight- % in water) and 1 .05 g of an aqueous solution of sodium hydroxide (NaOH ; 50 weight- % in water) were added thereto. The resulting mixture was mixed using an ultraturrax at 16000 rpm for 1 -2 min until a milky white emulsion started to form. A Teflon stirrer was used then for stirring. 21 .67 g of a colloidal silica-containing aqueous suspension (Ludox- 40; Sigma Aldrich) were added to the mixture. Subsequently, the copper(ll) stearate-containing xylene solution was added thereto. The resulting reaction mixture was then stirred for 10min in the Teflon insert. The autoclave was closed and sealed.

The reaction mixture was then subjected to hydrothermal conditions at a temperature of 170 °C under stirring for 96 h. After that, the reaction mixture was cooled to room temperature, filtrated with a Buchner funnel (blue ribbon paper filter) and the thus obtained solids washed with about 125 ml de-ionized water and subsequently with about 50 ml acetone. The resulting washed sol ids were dried at 80 °C for 16 h and then calcined in air at a temperature of 550 °C for 2 h, whereby a heating rate of 2 °C/min was applied.

According to the powder X-ray diffraction analysis according to Reference Example 2 the zeolit- ic material of Example 10 comprised only CHA as unique crystalline phase. The observed crys tallinity in the XRD was at least 80 %. No copper oxide reflexes were observed in the powder X- ray diffraction pattern. The resulting product had a copper content of 4 weight-%.

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- EP 2297036 B1