Process for the preparation of a zeolitic material having the afx framework structure and the prepared zeolitic material

Abstract

The invention relates to a process for the preparation of a zeolitic material having an AFX framework structure comprising X2O3 and YO2 via interzeolitic conversion, the process comprising (1) providing a mixture comprising a first zeolitic material having a non-AFX framework structure comprising X2O3 and YO2 and an organic structure directing agent selected from the group consisting of di-quaternary ammonium cation containing compounds, and (2) heating the mixture from (1) to form a second zeolitic material having an AFX framework structure comprising X2O3 and YO2, wherein X is a trivalent element and Y is a tetravalent element, and wherein when the first material zeolite has a CHA framework structure, the organic structure directing agent is not 1,4-bis(1,4-diazabicyclo[2.2.2]octane)butyl-dihydroxide. The invention further relates to a zeolitic material having an AFX framework structure obtainable or obtained by the process and the use thereof as catalytically active material.

Description

[0001] Cross-references to related applications

[0002] This application claims priority to the entire contents of International Application No. PCT / CN2020 / 114793, filed on September 11, 2020. Invention Field

[0003] This invention relates to a method for preparing zeolite materials with an AFX framework structure via interzeolite conversion in the presence of an organic structure directing agent. Furthermore, this invention relates to zeolite materials with an AFX framework structure that can be obtained by this method or obtained by this method, and their use as catalytically active materials.

[0004] background

[0005] AFX zeolite, known as a microporous zeolite, can be used as a catalyst in various processes, such as selective catalytic reduction (SCR) of NOx in combustion exhaust, hydrocarbon cracking and reforming, and methanol-to-olefins (MTO). In recent years, the synthesis of AFX zeolite has attracted increasing attention. AFX zeolite is typically prepared by precipitating zeolite crystals from a synthetic mixture containing both silica and alumina sources. Alternatively, AFX zeolite can be prepared via inter-zeolite conversion from zeolites with different framework types in the presence of a structure-directing agent (SDA), as reported in the following non-patent and patent literature.

[0006] Boruntea CR et al. described the synthesis of AFX zeolite from FAU or CHA zeolite via zeolite-to-zeolite conversion using 1,4-bis(1,4-diazabicyclo[2.2.2]octane)butyl dihydroxy as SDA in Microporous and Mesoporous Materials, 278 (2019), pp. 105-114.

[0007] US2018 / 093259A1 and US2016 / 0137518A1 describe the use of 1,3-bis(1-adamantyl)imidazolium Hydroxide or 2,6-N,N-diethyl-cis-2,6-dimethyl-piperidine The hydroxide, as SDA, was synthesized from zeolite Y to form AFX zeolite.

[0008] US2018 / 093897A1 describes the use of 1,3-bis(1-adamantyl)imidazolium A multi-SDA system consisting of hydroxide and at least one neutral amine was synthesized from zeolite Y to form AFX zeolite.

[0009] WO 2019 / 048940 A1 describes the synthesis of AFX zeolite from zeolite Y using hexamethonium hydroxide as SDA.

[0010] WO 2019 / 224085 A1 describes the use of 1,5-bis(methylpiperidine) )Pentane, 1,6-bis(methylpiperidine) Hexane or 1,7-bis(methylpiperidine) Heptane, as SDA, is synthesized from at least two FAU zeolites to form AFX zeolite.

[0011] JP 6655959 B2 describes the synthesis of AFX zeolite from zeolite Y using 1,4-diazabicyclo[2.2.2]octane-C4-dibromodiquaternary ammonium salt as SDA.

[0012] The methods for preparing AFX zeolites reported in the literature are limited to very specific starting zeolites and certain organic structure directing agents (OSDAs). More methods are needed for preparing zeolite materials with AFX framework structures, particularly methods that can provide zeolite materials with AFX framework structures that offer improved catalytic activity. Invention Overview

[0014] The purpose of this invention is to provide a new method for preparing zeolite materials with an AFX framework structure, particularly zeolite materials with an AFX framework structure that are more effective in selectively catalytically reducing NOx at high temperatures.

[0015] Surprisingly, it was found that this objective could be achieved by preparing zeolite materials with an AFX framework from zeolites with a non-AFU framework structure via inter-zeolite conversion in the presence of an organic structure directing agent.

[0016] Therefore, in one aspect, the present invention relates to a method for preparing a zeolite material having an AFX framework structure comprising X2O3 and YO2 via zeolite interconversion, the method comprising:

[0017] (1) Provides a mixture comprising a first zeolite material having a non-AFX framework structure containing X2O3 and YO2 and an organic structure-directing agent selected from diquaternary ammonium cationic compounds, and

[0018] (2) Heating the mixture from (1) to form a second zeolite material having an AFX framework structure containing X2O3 and YO2.

[0019] Where X is a trivalent element and Y is a tetravalent element, and where the organic structure directing agent is not 1,4-bis(1,4-diazabicyclo[2.2.2]octane)butyl dihydroxide when the first material zeolite has a CHA framework structure.

[0020] In another aspect, the present invention relates to a zeolite material having an AFX framework structure that can be obtained by the method according to the first aspect or obtained by the method according to the first aspect.

[0021] In another aspect, the present invention relates to the use of zeolite materials having an AFX framework structure as described herein as catalysts and / or as catalyst components, preferably as catalysts and / or catalyst components for the selective catalytic reduction (SCR) of nitrogen oxides (NOx).

[0022] In another aspect, the present invention relates to a catalytic article comprising a catalytic coating on a substrate, wherein the catalytic coating comprises a zeolite material having an AFX framework structure as described herein.

[0023] In another aspect, the present invention relates to an exhaust treatment system comprising an internal combustion engine and an exhaust duct in fluid communication with the internal combustion engine, wherein a catalyst as described herein is present in the exhaust duct. Brief description of the attached diagram

[0025] Figure 1a , 1b 1c and 1d are SEM patterns of AFX zeolite materials obtained in Examples 1.1, 2.1, 3.1 and 3.2, respectively, showing the spherical aggregate morphology of the zeolite.

[0026] Figure 2 The XRD patterns of the AFX zeolite materials prepared as described in Examples 1.1, 2.1, 3.1 and 3.2 are shown.

[0027] Figure 3 The XRD patterns of zeolite materials prepared from ZSM-5 zeolite with different Na / SiO2 molar ratios according to Examples 1.1 to 1.6 are shown, where the peaks indicated by the arrows belong to the unconverted ZSM-5 framework in samples 1.3 and 1.6, respectively.

[0028] Figure 4 The XRD patterns of zeolite materials prepared from SSZ-13 zeolite with different Na / SiO2 molar ratios according to Examples 2.1 to 2.4 are shown, where the peaks indicated by the arrows belong to minor impurities in samples 2.2 and 2.4, respectively.

[0029] Figure 5The XRD patterns of zeolite materials prepared from SSZ-13 zeolite with different Na / SiO2 molar ratios according to Examples 2.5 to 2.8 are shown, where the peaks indicated by the arrows belong to minor impurities in samples 2.5 and 2.8, respectively. Invention Details

[0031] The invention will now be described in detail. It should be understood that the invention can be embodied in many different ways and should not be construed as being limited to the embodiments described herein.

[0032] In this document, the singular forms “a,” “an,” and “the” include plural references unless the context clearly specifies otherwise. The terms “comprising,” etc., are used interchangeably with “containing,” etc., and should be interpreted in a non-restrictive, open-ended manner. That is, for example, other components or elements may exist. The terms “consisting of,” “substantially consisting of,” or synonyms may be included within “comprising” or its synonyms.

[0033] The terms “AFX”, “FAU”, “MFI” and “CHA” used in this article refer to the AFX, FAU, MFI and CHA skeleton types recognized by the International Zeolite Association (IZA) Structural Committee, respectively.

[0034] The term “interzeolite conversion” as used herein has the same meaning as commonly understood by those skilled in the art of zeolite synthesis, and is often used interchangeably with “zeolite-to-zeolite conversion” and “interzeolite transformation”.

[0035] The term "zeolite material having an AFX framework structure" as used herein is intended to include any form of zeolite having said framework, including, for example, synthetic forms, NH4 forms, H forms, and metal-supported H forms. The term "having an AFX framework structure" means a framework that is at least 90% phase-pure AFX, i.e., at least 90% of the zeolite framework is of the AFX type.

[0036] In the context of this invention, X can be any trivalent element. Preferably, X is selected from the group consisting of Al, B, In, and Ga, and any combination thereof, with Al being more preferred. In the context of this invention, Y can be any tetravalent element. Preferably, Y is selected from the group consisting of Si, Sn, Ti, Zr, Ge, and any combination thereof, with Si being more preferred.

[0037] For step (1), there are no particular restrictions on the first zeolite material having a non-FAU framework; however, it is preferred to be a zeolite with a CHA framework structure, more preferably SSZ-13 zeolite, or preferably a zeolite with an MFI framework structure, more preferably ZSM-5 zeolite. The first zeolite having a non-FAU framework can be in the corresponding NH4, H, or M form, where M represents an alkali metal or alkaline earth metal.

[0038] In one particular embodiment, an aluminosilicate zeolite having a non-FAU framework can be used as the first zeolite having a non-FAU framework structure in step (1). Preferably, the aluminosilicate zeolite structure does not include phosphorus or other substituted metals in the framework, and does not include aluminophosphate materials such as SAPO, ALPO, and MeAPO.

[0039] It should be understood that the first zeolite material with a non-FAU framework included in the mixture provided in step (1) can function as a source of both X2O3 and YO2. In some embodiments, there is no additional source of X2O3 or YO2 in the mixture provided in step (1). In some other embodiments, the mixture provided in step (1) may optionally include an additional source of YO2. A suitable additional source of YO2 can be any known material that can be used to provide a tetravalent framework element during zeolite synthesis. In a particular embodiment, where Y is Si, a suitable source of YO2 may be selected from the group consisting of: fumed silica, precipitated silica, silica hydrosol, silica gel, colloidal silica, silicic acid, silanoxyides, alkali metal silicates such as sodium silicate and potassium silicate, sodium metasilicate hydrate, sesquisilicates, disilicates, silicates, other zeolites with a non-FAU framework, dealuminite zeolites, and any combination thereof.

[0040] Preferably, the mixture provided in step (1) has a YO2:X2O3 molar ratio of YO2 source calculated as YO2 to X2O3 source calculated as X2O3 in the range of 5 to 60, preferably 15 to 40, more preferably 20 to 35, and even more preferably 26 to 32.

[0041] The organic structure-directing agent can be any compound containing a diquaternary ammonium cation (Q), without particular limitation. Preferably, the organic structure-directing agent is selected from compounds containing a diquaternary ammonium cation of formula (I):

[0042] (R1R2R3)N + (CH2) n N + (R4R5R6)(I)

[0043] in

[0044] R1, R2, R3, R4, R5, and R6 are independently selected from C1-C1. 10 Alkyl group, and n is an integer from 3 to 10, or

[0045] in

[0046] One of R1, R2, and R3 is selected from C1-C 10 Alkyl groups and two others linked together to form C4-C6 alkylene groups.

[0047] One of R4, R5, and R6 is selected from C1-C 10 Alkyl groups and two others linked together to form C4-C6 alkylene groups, and

[0048] n is an integer from 3 to 10.

[0049] In a preferred embodiment, the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I), wherein R1, R2, R3, R4, R5 and R6 are independently selected from C1-C6 alkyl groups, and n is an integer from 4 to 7.

[0050] In a more preferred embodiment, the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I), wherein R1, R2, R3, R4, R5 and R6 are the same and selected from C1-C6 alkyl groups, and n is 5, 6 or 7.

[0051] In the most preferred embodiment, the organic structure directing agent is selected from the diquaternary ammonium cationic compound of formula (I), wherein R1, R2, R3, R4, R5 and R6 are each methyl, ethyl or propyl, preferably ethyl, and n is 5, 6 or 7.

[0052] In one particular embodiment, the organic structure directing agent is N,N,N,N',N',N'-hexaethyl-1,5-pentanediammonium (Et6-diquat-5), i.e., a diquaternary ammonium cationic compound of formula (I), wherein R1, R2, R3, R4, R5 and R6 are each ethyl and n is 5.

[0053] The diquaternary ammonium cation compound can be in the form of a salt, wherein the anion is selected from the group consisting of: halide ions, such as fluoride, chloride, and bromide ions; hydroxide ions, sulfate ions, nitrate ions, carboxyl ions, such as acetate ions, and any combination thereof; preferably selected from the group consisting of: chloride ions, bromide ions, hydroxide ions, sulfate ions, and any combination thereof. More preferably, the diquaternary ammonium cation compound is a hydroxide, chloride, or bromide, particularly a hydroxide of a diquaternary ammonium cation of formula (I) as described above.

[0054] Preferably, the mixture provided in step (1) has a diquaternary ammonium cation (Q) to a Q:YO2 molar ratio of YO2 source calculated as YO2 in the range of 0.01 to 1, preferably 0.02 to 0.5, more preferably 0.02 to 0.2, and even more preferably 0.05 to 0.15.

[0055] In some embodiments, the mixture provided in step (1) further comprises at least one solvent, preferably water, more preferably deionized water. Preferably, the mixture provided in step (1) has a molar ratio of water to YO2 source calculated as YO2 in the range of 3 to 60, preferably 10 to 35, more preferably 15 to 30, H2O:YO2.

[0056] In some embodiments, the mixture provided in step (1) further comprises at least one alkali metal and / or alkaline earth metal (AM) cation, preferably from a source of alkali metal cation. The alkali metal is preferably selected from the group consisting of Li, Na, K, Cs, and any combination thereof, more preferably Na and / or K, and most preferably Na. The alkaline earth metal is preferably selected from the group consisting of Mg, Ca, Sr, and Ba. The source of the alkali metal or alkaline earth metal (AM) cation is typically a salt of an alkali metal or alkaline earth metal having any anion that is harmless to interconversion in zeolites. Examples of available anions may include halide ions such as fluoride, chloride, and bromide ions; hydroxide, sulfate, nitrate, carboxylates such as acetate, and any combination thereof; preferably chloride, bromide, hydroxide, sulfate, and any combination thereof, more preferably hydroxide.

[0057] The mixture provided in step (1) has at least one alkali metal and / or alkaline earth metal in the range of 0.01 to 1.0, preferably 0.1 to 0.8, with an AM:YO2 molar ratio of YO2 source calculated as YO2.

[0058] In some preferred embodiments, the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2, ranging from 0.01 to 1.0, preferably 0.1 to 0.8, more preferably 0.3 to 0.8, even more preferably 0.4 to 0.7, and especially 0.5 to 0.65. More preferably, for embodiments in which the first zeolite material is a zeolite having an MFI framework structure, particularly ZSM-5, the AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 is in the range of 0.51 to 0.65; and for embodiments in which the first zeolite material is a zeolite having a CHA framework structure, the AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 is in the range of 0.56 to 0.64.

[0059] In some embodiments, the mixture provided in step (1) further comprises at least one OH group. - Source, including OH - The source is a metal hydroxide, such as an alkali metal hydroxide, or ammonium hydroxide. Preferably, OH - The anions originate from alkali metal and / or alkaline earth metal cations and / or organic structure directing agents.

[0060] The mixture provided in step (1) has an OH content in the range of 0.01 to 2, more preferably 0.05 to 1.2, more preferably 0.3 to 1.0, more preferably 0.4 to 0.9, more preferably 0.6 to 0.9. - OH from YO2 source calculated as YO2 - The molar ratio of YO2.

[0061] In some embodiments, the mixture provided in step (1) may further contain a certain amount of zeolite seed crystals having an AFX framework structure. These seed crystals may be commercially available or prepared by the method according to the invention or any other method known in the art.

[0062] Regarding step (2), the mixture is preferably heated at a temperature within the range of 80 to 250°C, more preferably 90 to 230°C, more preferably 100 to 200°C, more preferably 110 to 190°C, more preferably 120 to 180°C, more preferably 130 to 170°C, and most preferably 135 to 155°C. Heating can be carried out over a period of 0.25 to 12 days, more preferably 0.5 to 10 days, more preferably 1 to 7 days, more preferably 2 to 6 days, and more preferably 2.5 to 5 days. Preferably, heating is carried out under autogenous pressure, more particularly in a pressure-sealed vessel, and more preferably in an autoclave. Furthermore, heating is preferably carried out with stirring.

[0063] In one particular embodiment, the heating in step (2) is carried out at a temperature in the range of 130 to 170°C, more preferably 135 to 155°C, under autogenous pressure in a pressure-sealed container, more preferably in an autoclave, for a period of 1 to 7 days, preferably 2 to 6 days, more preferably 2.5 to 5 days.

[0064] The second zeolite material with an AFX framework structure formed in step (2) can typically undergo post-processing procedures, including separation, for example, by filtration, optional washing, and drying. Therefore, step (2) in the method according to the invention optionally further includes a post-processing procedure.

[0065] In some embodiments, the second zeolite material with an AFX framework structure from step (2) can undergo a calcination process. Therefore, the method according to the invention further includes:

[0066] (3) Calcining the second zeolite material with an AFX skeleton structure.

[0067] In some embodiments, the second zeolite material having an AFX framework structure can undergo an ion exchange process, causing one or more ionic non-framework elements contained in the zeolite material to be exchanged for H. + and / or NH4 + Therefore, the method according to the present invention further includes:

[0068] (4) Replace one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) with H. + and / or NH4 + NH4 is preferred + .

[0069] In step (4), H is usually exchanged. + and / or NH4 + The zeolite material can undergo post-processing procedures, including separation, for example, by filtration, optionally washing and drying, and / or calcination. Therefore, step (4) in the method according to the invention optionally further includes post-processing and / or calcination procedures.

[0070] In some embodiments, the zeolite material having an AFX framework structure can withstand the loading of promoter metal cations on and / or within the zeolite material. Therefore, the method according to the invention further comprises:

[0071] (5) Loading promoter metal cations onto the zeolite material obtained in step (3) or (4) and / or onto the zeolite material obtained in step (3) or (4), preferably by ion exchange or impregnation, more preferably by initial wet impregnation.

[0072] The promoter metal can be any metal known to be useful for improving the catalytic activity of zeolites in catalyst applications, including, for example, noble metals such as platinum group metals, Au and Ag, transition metals and alkaline earth metals. Preferably, the promoter metal is selected from the group consisting of Ca, Mg, Sr, Zr, Cr, Mo, Fe, Mn, V, Co, Ni, Cu, Zn, Ru, Rh, Pd, Ag, Os, Ir, Pt, Au and any combination thereof, more preferably from the group consisting of Ca, Mg, Sr, Cr, Mo, Fe, Mn, V, Co, Ni, Cu, Zn and any combination thereof, more preferably from the group consisting of Ca, Mn, Fe, Mn, Ni, Cu, Zn and any combination thereof, with Cu and / or Fe being the most preferred.

[0073] The accelerator metal can be loaded onto and / or into the zeolite material in an amount of 0.1 to 1.0 moles of aluminum per mole of the zeolite material, i.e., skeletal aluminum of the zeolite material having an AFX framework structure, preferably 0.15 to 0.8 moles, more preferably 0.2 to 0.75 moles.

[0074] Typically, the zeolite material loaded with the accelerator metal in step (5) can undergo post-treatment procedures, including separation, optionally washing and drying, and / or calcination. Therefore, step (5) in the method according to the invention optionally further includes post-treatment procedures and / or calcination procedures.

[0075] For the calcination carried out in step (3) and optionally in steps (4) and (5), the heating is carried out at a temperature in the range of 300 to 900°C, preferably 350 to 700°C, more preferably 400 to 650°C, and even more preferably 450 to 600°C. In particular, the calcination can be carried out in a gaseous atmosphere having a temperature in the above range, which can be air, oxygen, nitrogen, or a mixture of two or more of these. Preferably, the calcination is carried out for a period of 0.5 to 10 hours, preferably 3 to 7 hours, and even more preferably 4 to 6 hours.

[0076] The present invention further relates to zeolite materials having an AFX framework structure that can be obtained by the methods described above. It should be understood that zeolite materials having an AFX framework structure may be products that can be obtained by steps (3), (4), or (5) or directly obtained by steps (3), (4), or (5), depending on the actual steps performed in the methods described above.

[0077] The zeolite material with an AFX framework structure according to the present invention preferably has a YO2:X2O3 molar ratio in the range of 5 to 50, preferably 5 to 35, more preferably 5 to 20, and even more preferably 5 to 15, as determined in its calcined H form. The zeolite material with an AFX framework structure can exist in the form of spherical aggregated particles.

[0078] The zeolite material with an AFX framework structure according to the present invention can be used for any conceivable purpose, including but not limited to as a molecular sieve, as an adsorbent, for ion exchange, or as a catalyst and / or as a catalyst component, preferably as a catalyst for the selective catalytic reduction (SCR) of nitrogen oxides (NOx); for storing and / or adsorbing CO2; for oxidizing NH3, especially for oxidizing NH3 leaked in diesel systems; for decomposing N2O; 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.

[0079] In some embodiments, the zeolite material with an AFX framework structure according to the invention is used for selective catalytic reduction (SCR) of nitrogen oxides (NOx), more preferably for selective catalytic reduction (SCR) of NOx in exhaust gas from an internal combustion engine. Specifically, the zeolite material with an AFX framework structure according to the invention has an SCR efficiency at least 10%, preferably at least 20%, more preferably at least 30%, more preferably at least 40%, more preferably at least 50%, more preferably at least 60%, and more preferably at least 70% higher than that of a zeolite material prepared via inter-zeolite conversion from a zeolite with a FAU framework structure using the same organic structure directing agent. This is achieved by operating at 575°C with a gas hourly space velocity (GHSV) of 80,000 h⁻¹ in a gas stream containing 500 ppm NO, 500 ppm NH₃, 5% H₂O, 10% O₂, and the balance N₂. -1 NOx conversion determination under [condition / condition].

[0080] For SCR applications, the zeolite material with an AFX framework structure according to the present invention can be in the form of an extrusion or preferably as a carrier coating on a substrate. The term "carrier coating" has a common meaning in the art, referring to a thin, adherent coating of catalytic material or other material applied to a substrate. The term "substrate" generally refers to a monolithic material on which the catalytic coating is disposed, such as a monolithic honeycomb substrate, particularly a flow-through monolithic substrate and a wall-flow monolithic substrate. The zeolite material with an AFX framework structure according to the present invention can be processed into its application form by any known method without particular limitation.

[0081] Therefore, the present invention relates to a catalytic article comprising a catalytic coating on a substrate, wherein the catalytic coating comprises a zeolite material having an AFX framework structure according to the present invention.

[0082] In another embodiment, the present invention relates to an exhaust treatment system including an internal combustion engine and an exhaust duct in fluid communication with the internal combustion engine, wherein the catalyst as described above is present in the exhaust duct.

[0083] The present invention will be further illustrated by the following embodiments, which illustrate particularly advantageous implementations. While embodiments are provided to illustrate the invention, they are not intended to limit the invention.

[0084] Implementation Plan

[0085] The following embodiments are used to further illustrate the invention as disclosed herein and are not intended to be construed as limiting it.

[0086] Implementation Scheme 1. A method for preparing zeolite materials having an AFX framework structure comprising X2O3 and YO2 via zeolite interconversion, the method comprising:

[0087] (1) Provides a mixture comprising a first zeolite material having a non-AFX framework structure containing X2O3 and YO2 and an organic structure-directing agent selected from diquaternary ammonium cationic compounds, and

[0088] (2) Heating the mixture from (1) to form a second zeolite material having an AFX framework structure containing X2O3 and YO2.

[0089] Where X is a trivalent element and Y is a tetravalent element, and where the organic structure directing agent is not 1,4-bis(1,4-diazabicyclo[2.2.2]octane)butyl dihydroxide when the first material zeolite has a CHA framework structure.

[0090] Implementation Scheme 2. The method according to Implementation Scheme 1, wherein X is selected from the group consisting of Al, B, In and Ga and any combination thereof, wherein preferably X is Al.

[0091] Implementation Scheme 3. According to the method of Implementation Scheme 1 or 2, wherein Y is selected from the group consisting of: Si, Sn, Ti, Zr, Ge and any combination thereof, wherein preferably Y is Si.

[0092] Implementation Scheme 4. The method according to any one of Implementation Schemes 1-3, wherein the first zeolite material is a zeolite having a CHA framework structure or a zeolite having an MFI framework structure.

[0093] Implementation Scheme 5. The method according to any one of the foregoing implementation schemes, wherein the first zeolite material is aluminosilicate zeolite, preferably SSZ-13 zeolite or ZSM-5 zeolite.

[0094] Implementation Scheme 6. The method according to any one of the foregoing implementation schemes, wherein the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I):

[0095] (R1R2R3)N + (CH2) n N + (R4R5R6)(I)

[0096] in

[0097] R1, R2, R3, R4, R5, and R6 are independently selected from C1-C1. 10 Alkyl group, and n is an integer from 3 to 10, or

[0098] in

[0099] One of R1, R2, and R3 is selected from C1-C 10 Alkyl groups and two others linked together to form C4-C6 alkylene groups.

[0100] One of R4, R5, and R6 is selected from C1-C 10 Alkyl groups and two others linked together to form C4-C6 alkylene groups, and

[0101] n is an integer from 3 to 10.

[0102] Implementation Scheme 7. The method according to any one of the preceding embodiments, wherein the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I), wherein R1, R2, R3, R4, R5 and R6 are independently selected from C1-C6 alkyl groups, and n is an integer from 4 to 7.

[0103] Implementation Scheme 8. The method according to any one of the preceding implementation schemes, wherein the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I), wherein R1, R2, R3, R4, R5 and R6 are the same and selected from C1-C6 alkyl groups, and n is 5, 6 or 7.

[0104] Implementation Scheme 9. The method according to any one of the preceding implementation schemes, wherein the organic structure directing agent is selected from a diquaternary ammonium cationic compound of formula (I), wherein R1, R2, R3, R4, R5 and R6 are each methyl, ethyl or propyl, preferably ethyl, and n is 5, 6 or 7.

[0105] Implementation Scheme 10. The method according to any one of the preceding implementation schemes, wherein the organic structure directing agent is N,N,N,N',N',N'-hexaethyl-1,5-pentanediamine.

[0106] Implementation Scheme 11. The method according to any one of the preceding embodiments, wherein the mixture in step (1) further comprises at least one alkali metal and / or alkaline earth metal cation source, preferably an alkali metal cation source, more preferably having a molar ratio of at least one alkali metal and / or alkaline earth metal to a YO2 source calculated as YO2 in the range of 0.01 to 1.0, preferably 0.1 to 0.8.

[0107] Implementation Scheme 12. The method according to Implementation Scheme 11, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 in the range of 0.01 to 1.0, preferably 0.1 to 0.8, more preferably 0.3 to 0.8, more preferably 0.4 to 0.7, especially 0.5 to 0.65.

[0108] Implementation Scheme 13. The method according to Implementation Scheme 12, wherein the first zeolite material is a zeolite having an MFI framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.51 to 0.65.

[0109] Implementation Scheme 14. The method according to Implementation Scheme 12, wherein the first zeolite material is a zeolite having a CHA framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.56 to 0.64.

[0110] Implementation Scheme 15. The method according to any one of the foregoing implementation schemes further includes (3) calcining a second zeolite material having an AFX framework structure.

[0111] Implementation Scheme 16. The method according to any one of the foregoing implementation schemes, further comprising (4) exchanging one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) for H + and / or NH4 + NH4 is preferred + .

[0112] Implementation Scheme 17. The method according to any one of the foregoing embodiments further includes (5) loading a co-catalyst metal cation onto the zeolite material obtained in step (3) or (4) and / or into the zeolite material obtained in step (3) or (4).

[0113] Implementation Scheme 18. A zeolite material having an AFX framework structure, which may be obtained by the method according to any one of the foregoing embodiments or by the method according to any one of the foregoing embodiments.

[0114] Implementation Scheme 19. The zeolite material with an AFX framework structure as described in Implementation Scheme 18 exists in the form of spherical aggregated particles.

[0115] Implementation Scheme 20. A zeolite material with an AFX framework structure according to Implementation Scheme 18 or 19, having an SCR efficiency at least 10%, preferably at least 20%, more preferably at least 30%, more preferably at least 40%, more preferably at least 50%, more preferably at least 60%, and more preferably at least 70% higher than that of a zeolite material prepared via inter-zeolite conversion from a zeolite with a FAU framework structure using the same organic structure directing agent. This is achieved by conducting an SCR at 575°C with a gas hourly space velocity (GHSV) of 80,000 h⁻¹ in a gas stream containing 500 ppm NO, 500 ppm NH₃, 5% H₂O, 10% O₂, and the balance N₂. -1 NOx conversion determination under [condition / condition].

[0116] Implementation Scheme 21. Use of the zeolite material having an AFX framework structure according to any one of the foregoing embodiments 18-20 as a catalyst and / or catalyst component, preferably as a catalyst and / or catalyst component for selective catalytic reduction (SCR) of nitrogen oxides (NOx).

[0117] Implementation Scheme 22. A catalyst article comprising a catalytic coating on a substrate, wherein the catalytic coating comprises a zeolite material having an AFX framework structure according to any one of the preceding embodiments 18-20.

[0118] Implementation Scheme 23. An exhaust treatment system comprising an internal combustion engine and an exhaust duct in fluid communication with the internal combustion engine, wherein the catalyst product according to Implementation Scheme 22 is present in the exhaust duct.

[0119] Implementation Scheme 24. A method for selective catalytic reduction of NO x Methods, including

[0120] (A) Provides NO x The gaseous material flow;

[0121] (B) Contact the gas stream with the zeolite material according to any one of embodiments 18-20 or with the catalyst according to embodiment 22. Example

[0122] Scanning electron microscopy (SEM) experiments were performed using a scanning electron microscope (Hitachi SU1510).

[0123] X-ray powder diffraction (XRD) patterns were obtained using an X-ray diffractometer (X'pert 3 Powder, from Malvern Panalytical) (40 kV, 40 mA) with CuKα. Radiation measurement. Example 1: Preparation of AFX zeolite using ZSM-5 zeolite.

[0124] Example 1.1 (Sample 1.1, Na / SiO2 0.56)

[0125] 35.70 g of an 18.03 wt% aqueous solution of Et6-diquat-5 hydroxide was mixed with 59.24 g of DI water, and then 4.75 g of NaOH (99%, solid) was added under stirring to obtain a solution. 14.62 g of ZSM-5 zeolite powder (from China Catalyst Group Ltd. (CCG)) with a SiO2 / Al2O3 molar ratio (SAR) of 28 and 0.63 g of AFX powder (SAR 12.4) were added to this solution and stirred for 30 minutes. The resulting mixture was transferred to a 120 ml autoclave and rotary heated at 140 °C for 4 days. After cooling to room temperature and releasing the pressure, the product was filtered, washed with DI water, and dried at 120 °C. The synthesized product was calcined in air at 550 °C for 6 hours to obtain a SAR value of 10.7 and a BET surface area of ​​558 μm.2 / g of Na-form AFX zeolite. As observed from the SEM pattern shown in Figure 1, the Na-form AFX zeolite exists in the form of spherical aggregates.

[0126] XRD analysis showed that the synthesized product had the following properties: Figure 2 and 3 The AFX framework structure shown has an a-cell parameter of 13.667 Å, ​​a c-cell parameter of 19.648 Å, and a cell volume of 3179 Å. 3 .

[0127] Example 1.2 (Sample 1.2, Na / SiO2 0.52)

[0128] The method of Example 1.1 was repeated, except that 4.41 g of NaOH (99% solid) was used.

[0129] Example 1.3 (Sample 1.3, Na / SiO2 0.48)

[0130] Repeat the method of Example 1.1, except that 4.07 g of NaOH (99% solid) is used.

[0131] Example 1.4 (Sample 1.4, Na / SiO2 0.60)

[0132] Repeat the method of Example 1.1, except that 5.09 g of NaOH (99% solid) is used.

[0133] Example 1.5 (Sample 1.5, Na / SiO2 0.64)

[0134] Repeat the method of Example 1.1, except that 5.43 g of NaOH (99% solid) is used.

[0135] Example 1.6 (Sample 1.6, Na / SiO2 0.68)

[0136] Repeat the method of Example 1.1, except that 5.77 g of NaOH (99% solid) is used.

[0137] Example 2: Preparation of AFX zeolite using SSZ-13 zeolite

[0138] Example 2.1 (Sample 2.1, Na / SiO2 0.58)

[0139] 42.83 g of an 18.03 wt% aqueous solution of Et6-diquat-5 hydroxide was mixed with 39.69 g of DI water, and then 4.92 g of NaOH (99% solid) was added under stirring to obtain a solution. 14.19 g of SSZ-13 zeolite powder (from China Catalyst Group Ltd. (CCG)) with a SiO2 / Al2O3 molar ratio (SAR) of 30 was added to the solution and stirred for 30 minutes. The resulting mixture was transferred to a 120 ml autoclave and rotary heated at 150 °C for 3 days. After cooling to room temperature and releasing the pressure, the product was filtered, washed with DI water, and dried at 120 °C. The synthesized product was calcined in air at 550 °C for 6 hours to obtain a SAR value of 8.6 and a BET surface area of ​​554 μm. 2 / g of Na-form AFX zeolite. As observed from the SEM pattern shown in Figure 1, the Na-form AFX zeolite exists in the form of spherical aggregates.

[0140] XRD analysis showed that the synthesized product had the following properties: Figure 2 and 4 The AFX framework structure shown has an a-cell parameter of 13.672 Å, a c-cell parameter of 19.692 Å, and a cell volume of 3188 Å. 3 .

[0141] Example 2.2 (Sample 2.2, Na / SiO2 0.54)

[0142] Repeat the method of Example 2.1, except that 4.58 g of NaOH (99% solid) is used.

[0143] Example 2.3 (Sample 2.3, Na / SiO2 0.62)

[0144] Repeat the method of Example 2.1, except that 5.26 g of NaOH (99% solid) is used.

[0145] Example 2.4 (Sample 2.4, Na / SiO2 0.66)

[0146] Repeat the method of Example 2.1, except that 5.60 g of NaOH (99% solid) is used.

[0147] Example 2.5 (Sample 2.5, Na / SiO2 0.54)

[0148] The method of Example 2.1 was repeated, except that 4.58 g of NaOH (99% solid) was used and the heating temperature was 160 °C.

[0149] Example 2.6 (Sample 2.6, Na / SiO2 0.58)

[0150] The method of Example 2.1 was repeated, except that 4.92 g of NaOH (99% solid) was used and the heating temperature was 160 °C.

[0151] Example 2.7 (Sample 2.7, Na / SiO2 0.62)

[0152] The method of Example 2.1 was repeated, except that 5.26 g of NaOH (99% solid) was used and the heating temperature was 160 °C.

[0153] Example 2.8 (Sample 2.8, Na / SiO2 0.66)

[0154] The method of Example 2.1 was repeated, except that 5.60 g of NaOH (99% solid) was used and the heating temperature was 160 °C.

[0155] Example 3: Preparation of AFX zeolite using FAU zeolite

[0156] Example 3.1 (Sample 3.1, Na / SiO2 0.68)

[0157] 32.64 g of an 18.03 wt% aqueous solution of Et6-diquat-5 hydroxide was mixed with 74.93 g of DI water, and then 6.59 g of NaOH (99% solid) was added under stirring to obtain a solution. 16.16 g of FAU zeolite powder (HY, from Pacific Industrial Development Corporation (PIDC)) with a SiO2 / Al2O3 molar ratio (SAR) of 36 was added to the solution and stirred for 30 minutes. The resulting mixture was transferred to a 120 ml autoclave and rotary heated at 140 °C for 4 days. After cooling to room temperature and releasing the pressure, the product was filtered, washed with DI water, and dried at 120 °C. The synthesized product was calcined in air at 550 °C for 6 hours to obtain a SAR value of 10.4 and a BET surface area of ​​518 μm. 2 / g of Na-form AFX zeolite. As observed from the SEM pattern shown in Figure 1, the Na-form AFX zeolite exists in the form of spherical aggregates.

[0158] XRD analysis showed that the synthesized product had the following properties: Figure 2 The AFX framework structure shown has an a-cell parameter of 13.686 Å, a c-cell parameter of 19.686 Å, and a cell volume of 3193 Å. 3 .

[0159] Example 3.2 (Sample 3.2, Na / SiO2 0.76)

[0160] 21.42 g of an 18.03 wt% aqueous solution of Et6-diquat-5 hydroxide was mixed with 72.84 g of DI water, and then 6.45 g of NaOH (99% solid) was added under stirring to obtain a solution. 2.78 g of FAU zeolite powder (HY, from Shandong Duoyou) with a SiO2 / Al2O3 molar ratio (SAR) of 5.2 was added to this solution, followed by 27.24 g of colloidal silica (Ludox-AS-40), and the mixture was stirred for 30 minutes. The resulting mixture was transferred to a 150 ml autoclave and rotary heated at 140 °C for 4 days. After cooling to room temperature and releasing the pressure, the product was filtered, washed with DI water, and dried at 120 °C. The synthesized product was calcined in air at 550 °C for 6 hours to obtain a SAR value of 9.9 and a BET surface area of ​​566 μm. 2 / g of Na-form AFX zeolite. As observed from the SEM pattern shown in Figure 1, the Na-form AFX zeolite exists in the form of spherical aggregates.

[0161] XRD analysis showed that the synthesized product had the following properties: Figure 2 The AFX framework structure shown has an a-cell parameter of 13.696 Å, a c-cell parameter of 19.798 Å, and a cell volume of 3216 Å. 3 .

[0162] Example 4: Preparation of Fe-supported AFX zeolite

[0163] Example 4.1

[0164] The Na-form AFX zeolite powder from Example 1.1 was pulverized and added to a 10% by weight NH4Cl aqueous solution at a liquid-to-solid ratio of 10:1. The resulting slurry was heated to 80°C and held for 2 hours, then filtered, washed, and dried at 110°C. The ion exchange procedure was repeated once, and the dried product was calcined in air at 450°C in a furnace for 6 hours to obtain H-form AFX zeolite.

[0165] AFX zeolite powder in the H form was impregnated with an aqueous solution of ferric nitrate (III) by initial wet impregnation, dried and calcined in air at 450°C for 5 hours to obtain Fe-loaded AFX zeolite, wherein the Fe loading per mole of skeletal aluminum was 0.40 moles.

[0166] Example 4.2

[0167] The method of Example 4.1 was repeated, except that AFX zeolite powder in the form of Na from Example 3.2 was used as the starting material.

[0168] Example 5 Catalytic tests on aged catalysts

[0169] The test samples were prepared as follows: Fe-loaded AFX zeolite from Example 4 was slurried with an aqueous solution of Zr acetate, then dried in air at ambient temperature with stirring, and then calcined at 550°C to provide a product containing 5% by weight ZrO2 as a binder based on the product amount. The obtained product was pulverized, and then the 250-500 micrometer fraction was aged at 820°C in a 10% by volume steam / air stream for 16 hours.

[0170] Selective catalytic reduction (SCR) measurements were performed in a fixed-bed reactor under the following conditions: 120 mg of the corresponding test sample was loaded with corundum of the same sieve fraction as a diluent to achieve a bed volume of approximately 1 mL.

[0171] Gas feed: 500 ppm NO, 500 ppm NH3, 5% H2O, 10% O2 and balance N2, with a gas hourly space velocity (GHSV) of 80,000 h⁻¹. -1 ;

[0172] Temperature: RUN1 - 200, 400, 575℃ (First run for degreening)

[0173] RUN2-175, 200, 225, 250, 500, 550, 575℃

[0174] Table 1 summarizes the results of RUN2 at 250℃ and 575℃.

[0175] Table 1

[0176]

[0177] As shown in Table 1, the NOx conversion achieved using the zeolite catalyst prepared from ZSM-5 zeolite (non-FAU zeolite) at 575 °C is approximately twice that achieved using the zeolite catalyst prepared from FAU zeolite.

Claims

1. A method for preparing zeolite materials having an AFX framework structure comprising X2O3 and YO2 via zeolite interconversion, the method comprising: (1) A mixture comprising a first zeolite material having a non-AFX framework structure containing X2O3 and YO2 and an organic structure-directing agent selected from diquaternary ammonium cationic compounds, wherein the first zeolite material is a zeolite having a CHA framework structure or a zeolite having an MFI framework structure, and (2) Heating the mixture from (1) to form a second zeolite material having an AFX framework structure containing X2O3 and YO2, Where X is a trivalent element and Y is a tetravalent element, and where, when the first material zeolite has a CHA framework structure, the organic structure directing agent is not 1,4-bis(1,4-diazabicyclo[2.2.2]octane)butyl dihydroxy, and The organic structure directing agent is selected from the diquaternary ammonium cationic compound of formula (I): (R1R2R3)N + (CH2) n N + (R4R5R6) (I) in R1, R2, R3, R4, R5, and R6 are independently selected from C1-C6 alkyl groups, and n is an integer from 4 to 7.

2. The method of claim 1, wherein X is selected from the group consisting of Al, B, In and Ga, and any combination thereof.

3. The method according to claim 2, wherein X is Al.

4. The method of claim 1, wherein Y is selected from the group consisting of: Si, Sn, Ti, Zr, Ge and any combination thereof.

5. The method of claim 2, wherein Y is selected from the group consisting of: Si, Sn, Ti, Zr, Ge and any combination thereof.

6. The method of claim 3, wherein Y is selected from the group consisting of: Si, Sn, Ti, Zr, Ge and any combination thereof.

7. The method of claim 6, wherein Y is Si.

8. The method according to claim 1, wherein the first zeolite material is aluminosilicate zeolite.

9. The method according to claim 2, wherein the first zeolite material is aluminosilicate zeolite.

10. The method according to claim 3, wherein the first zeolite material is aluminosilicate zeolite.

11. The method according to claim 4, wherein the first zeolite material is aluminosilicate zeolite.

12. The method according to claim 5, wherein the first zeolite material is aluminosilicate zeolite.

13. The method according to claim 6, wherein the first zeolite material is an aluminosilicate zeolite.

14. The method according to claim 7, wherein the first zeolite material is an aluminosilicate zeolite.

15. The method according to claim 14, wherein the first zeolite material is SSZ-13 zeolite or ZSM-5 zeolite.

16. The method according to any one of claims 1-14, wherein the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I), wherein R1, R2, R3, R4, R5 and R6 are the same and selected from C1-C6 alkyl groups, and n is 5, 6 or 7.

17. The method according to claim 15, wherein the organic structure directing agent is selected from diquaternary ammonium cationic compounds of formula (I), wherein R1, R2, R3, R4, R5 and R6 are the same and selected from C1-C6 alkyl groups, and n is 5, 6 or 7.

18. The method according to any one of claims 1-14, wherein the organic structure directing agent is selected from a diquaternary ammonium cationic compound of formula (I), wherein R1, R2, R3, R4, R5 and R6 are each methyl, ethyl or propyl, and n is 5, 6 or 7.

19. The method according to claim 17, wherein the organic structure directing agent is selected from a diquaternary ammonium cationic compound of formula (I), wherein R1, R2, R3, R4, R5 and R6 are each methyl, ethyl or propyl, and n is 5, 6 or 7.

20. The method according to claim 19, wherein the organic structure directing agent is selected from a diquaternary ammonium cationic compound of formula (I), wherein R1, R2, R3, R4, R5 and R6 are each ethyl, and n is 5, 6 or 7.

21. The method according to any one of claims 1-14, wherein the organic structure directing agent is N,N,N,N',N',N'-hexaethyl-1,5-pentanediamine.

22. The method according to claim 19 or 20, wherein the organic structure directing agent is N,N,N,N',N',N'-hexaethyl-1,5-pentanediamine.

23. The method according to any one of claims 1-14, wherein the mixture in step (1) further comprises at least one alkali metal and / or alkaline earth metal cation source.

24. The method of claim 22, wherein the mixture in step (1) further comprises at least one alkali metal and / or alkaline earth metal cation source.

25. The method according to claim 24, wherein the mixture in step (1) further has a molar ratio of at least one alkali metal and / or alkaline earth metal in the range of 0.01 to 1.0 to a YO2 source calculated as YO2.

26. The method according to claim 25, wherein the mixture in step (1) further has a molar ratio of at least one alkali metal and / or alkaline earth metal in the range of 0.1 to 0.8 to a YO2 source calculated as YO2.

27. The method of claim 23, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 in the range of 0.01 to 1.

0.

28. The method according to any one of claims 24-26, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated in YO2 in the range of 0.01 to 1.

0.

29. The method of claim 28, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 in the range of 0.1 to 0.

8.

30. The method of claim 29, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 in the range of 0.3 to 0.

8.

31. The method of claim 30, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 in the range of 0.4 to 0.

7.

32. The method of claim 31, wherein the mixture provided in step (1) comprises at least one alkali metal source and has an AM:YO2 molar ratio of at least one alkali metal to a YO2 source calculated as YO2 in the range of 0.5 to 0.

65.

33. The method of claim 27, wherein the first zeolite material is a zeolite having an MFI framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.51 to 0.

65.

34. The method of claim 28, wherein the first zeolite material is a zeolite having an MFI framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.51 to 0.

65.

35. The method according to any one of claims 29-32, wherein the first zeolite material is a zeolite having an MFI framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.51 to 0.

65.

36. The method of claim 27, wherein the first zeolite material is a zeolite having a CHA framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.56 to 0.

64.

37. The method of claim 28, wherein the first zeolite material is a zeolite having a CHA framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.56 to 0.

64.

38. The method according to any one of claims 29-32, wherein the first zeolite material is a zeolite having a CHA framework structure, and the molar ratio of at least one alkali metal to the source of YO2 calculated as YO2, AM:YO2, is in the range of 0.56 to 0.

64.

39. The method according to any one of claims 1-14, further comprising (3) calcining a second zeolite material having an AFX framework structure; and / or It further includes (4) exchanging one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) for H. + and / or NH4 + ; and / or It further includes (5) loading a co-catalyst metal cation onto the zeolite material obtained in step (3) or (4) and / or onto the zeolite material obtained in step (3) or (4).

40. The method according to claim 33 or 34, further comprising (3) calcining a second zeolite material having an AFX framework structure; and / or It further includes (4) exchanging one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) for H. + and / or NH4 + ; and / or It further includes (5) loading a co-catalyst metal cation onto the zeolite material obtained in step (3) or (4) and / or onto the zeolite material obtained in step (3) or (4).

41. The method of claim 35, further comprising (3) calcining a second zeolite material having an AFX framework structure; and / or It further includes (4) exchanging one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) for H. + and / or NH4 + ; and / or It further includes (5) loading a co-catalyst metal cation onto the zeolite material obtained in step (3) or (4) and / or onto the zeolite material obtained in step (3) or (4).

42. The method according to claim 36 or 37, further comprising (3) calcining a second zeolite material having an AFX framework structure; and / or It further includes (4) exchanging one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) for H. + and / or NH4 + ; and / or It further includes (5) loading a co-catalyst metal cation onto the zeolite material obtained in step (3) or (4) and / or onto the zeolite material obtained in step (3) or (4).

43. The method of claim 38, further comprising (3) calcining a second zeolite material having an AFX framework structure; and / or It further includes (4) exchanging one or more ionic non-framework elements contained in the zeolite material obtained in step (2) or (3) for H. + and / or NH4 + ; and / or It further includes (5) loading a co-catalyst metal cation onto the zeolite material obtained in step (3) or (4) and / or onto the zeolite material obtained in step (3) or (4).

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