Molecular sieve SSZ-120, its synthesis and uses

Abstract

An aluminogermanosilicate molecular sieve material with a small crystal size and high surface area, designated as SSZ-120, is provided. SSZ-120 can be synthesized using the 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1H-imidazolium] divalent cation as a structure guide. SSZ-120 can be used in organic compound conversion reactions and / or adsorption processes.

Description

Technology Field

[0001] Cross-reference regarding related applications

[0002] This application claims priority and interest of U.S. provisional application serial number 63 / 028,642 filed on May 22, 2020.

[0003] field

[0004] The present disclosure relates to an aluminogermanosilicate molecular sieve designated as SSZ-120, having a small crystal size and a large surface area, its synthesis, and its use in organic compound conversion reactions and adsorption processes. Background Technology

[0005] Molecular sieves are a commercially important class of materials characterized by distinct X-ray diffraction (XRD) patterns and a distinct crystal structure with a defined pore structure having a specific chemical composition. The crystal structure defines the cavities and voids that are characteristic of specific types of molecular sieves.

[0006] According to the present disclosure, an aluminogermanosilicate molecular sieve designated as SSZ-120, having a unique powder X-ray diffraction pattern, small crystal size, and large surface area, is used as a structure guide: 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] was synthesized using a divalent cation. means of solving the problem

[0007] In a first embodiment, an aluminogermanosilicate molecular sieve having a powder X-ray diffraction pattern including the peaks of the table below in a calcined form is provided:

[0008]

[0009] Calcined molecular sieves are at least 500 m 2 Total surface area of ​​ / g (determined by the t-plot method for nitrogen physicosorption) and / or at least 100 m 2It can have an external surface area of ​​ / g (determined by the t-plot method for nitrogen physical adsorption).

[0010] In a second embodiment, an aluminogermanosilicate molecular sieve having a powder X-ray diffraction pattern including the peaks of the table below is provided in a synthesized form:

[0011]

[0012] In the synthesized anhydrous form, the aluminogermanosilicate molecular sieve may have a chemical composition including the following molar relationships:

[0013]

[0014] Here, Q is 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] Contains divalent cations.

[0015] In a third embodiment, a method for synthesizing an aluminogermanosilicate molecular sieve is provided, the method comprising (1) (a) a FAU framework type zeolite; (b) a source of germanium; (c) 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H - A step of providing a reaction mixture containing a structure-inducing agent (Q) containing an imidazolium divalent cation; (d) a source of fluoride ions; and (e) water; and (2) applying the reaction mixture to crystallization conditions sufficient to form crystals of an aluminogermanosilicate molecular sieve.

[0016] In a fourth embodiment, a process for converting a feedstock containing an organic compound into a conversion product is provided, and the process comprises contacting the feedstock with a catalyst comprising an active form of the aluminogermanosilicate molecular sieve described herein under organic compound conversion conditions.

[0017] In a fifth embodiment, an organic nitrogen compound comprising a divalent cation having the following structure is provided:

[0018] Brief explanation of the drawing

[0019] Figure 1 shows the powder X-ray diffraction (XRD) pattern of the synthesized product of Example 2. Figures 2(a) to 2(d) show scanning electron microscope (SEM) images of the synthesized product of Example 2 at different magnifications. Figure 3 shows the powder XRD pattern of the calcined product of Example 3. Figure 4 is a graph illustrating the relationship between conversion or yield and temperature in the hydrogenation conversion of n-decane for Pd / SSZ-120 catalyst. Specific details for implementing the invention

[0020] definition

[0021] The term "framework type" refers to the literature[" Atlas of Zeolite Framework Types It has the meaning described in [Ch. Baerlocher and LB McCusker and DH Olsen (6th edition, Elsevier, 2007)].

[0022] The term "zeolite" refers to an aluminosilicate molecular sieve having a framework composed of alumina and silica (i.e., repeating AlO4 and SiO4 tetrahedral units).

[0023] The term "aluminogermanosilicate" refers to a molecular sieve having a framework composed of AlO4, GeO4, and SiO4 tetrahedral units. The aluminogermanosilicate may contain only the named oxides, in which case it is described as "pure aluminogermanosilicate," or it may contain other additional oxides.

[0024] The term "synthesized" is used herein to refer to a molecular sieve in the form after crystallization and before the removal of the structure-inducing agent.

[0025] The term "anhydrous" is used herein to refer to a molecular sieve that is substantially devoid of both physically adsorbed water and chemically adsorbed water.

[0026] The term "SiO2 / Al2O3 molar ratio" can be abbreviated as "SAR".

[0027] Synthesis of molecular bodies

[0028] The aluminogermanosilicate molecular sieve SSZ-120 can be synthesized as follows: (1) (a) a FAU framework type zeolite; (b) a source of germanium; (c) 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H - A step of providing a reaction mixture containing a structure-inducing agent (Q) containing an imidazolium] divalent cation; (d) a source of fluoride ions; and (e) water; and (2) applying the reaction mixture to crystallization conditions sufficient to form crystals of an aluminogermanosilicate molecular sieve.

[0029] The reaction mixture may have a composition in molar ratios within the ranges presented in Table 1:

[0030]

[0031] Here, Q is 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] Contains divalent cations.

[0032] In some embodiments, the reaction mixture may have a SiO2 / GeO2 molar ratio in the range of 4 to 12 (e.g., 6 to 10).

[0033] The FAU framework type zeolite may be an ammonium-type zeolite or a hydrogen-type zeolite (e.g., NH4-type zeolite Y, H-type zeolite Y). Examples of FAU framework type zeolites include zeolite Y (e.g., CBV720, CBV760, CBV780, HSZ-385HUA, and HSZ-390HUA). Preferably, the FAU framework type zeolite is zeolite Y. More preferably, zeolite Y has a SiO2 / Al2O3 molar ratio in the range of about 30 to about 500. The FAU framework type zeolite may comprise two or more zeolites. Typically, two or more zeolites are Y zeolites having different SiO2 / Al2O3 molar ratios. The FAU framework type zeolite may also be the sole source of silica and aluminum forming an aluminogermanosilicate molecular sieve.

[0034] Sources of germanium include germanium oxide and germanium alkoxide (e.g., germanium ethoxide).

[0035] Sources of fluoride ions include hydrogen fluoride, ammonium fluoride, and ammonium bifluoride.

[0036] SSZ-120 is represented by the following structure (1) as 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] can be synthesized using a structure-directing agent (Q) containing a divalent cation:

[0037]

[0038] Suitable sources of Q are hydroxides, chlorides, bromides, and / or other salts of diquaternary ammonium compounds.

[0039] The reaction mixture may contain a seed of a molecular sieve material, such as SSZ-120 from a previous synthesis, in an amount of 0.01 to 10,000 ppm by weight (e.g., 100 to 5,000 ppm by weight) of the reaction mixture. Seeding may be advantageous for improving the selectivity of SSZ-120 and / or shortening the crystallization process.

[0040] Note that the reaction mixture components may be supplied by more than one source. Additionally, two or more reaction components may be provided from a single source. The reaction mixture may be prepared in a batch or continuous manner.

[0041] Crystallization and Post-Synthesis Processing

[0042] Crystallization of the molecular sieve from the above reaction mixture may be carried out under static, tumbling, or stirring conditions in a suitable reactor vessel such as a polypropylene jar or a Teflon-lined or stainless steel autoclave, and the autoclave is placed in a convection oven maintained at a temperature of 100°C to 200°C for a time sufficient for crystallization to occur at the temperature used (e.g., 1 to 14 days). The hydrothermal crystallization process is generally carried out under autogenous pressure.

[0043] Once the desired molecular sieve crystals are formed, the solid product is separated from the reaction mixture by standard separation techniques such as filtration or centrifugation. The recovered crystals are washed with water and then dried for a few seconds to a few minutes (e.g., 5 seconds to 10 minutes for instant drying) or for a few hours (e.g., 4 to 24 hours for oven drying at 75°C to 150°C) to obtain synthesized SSZ-120 crystals having at least some of the structure-inducing agent within the pores. The drying step may be performed under atmospheric pressure or vacuum.

[0044] The synthesized molecular sieve may undergo heat treatment, ozone treatment, or other treatments to remove some or all of the structure-directing agents used in its synthesis. The removal of structure-directing agents may be carried out by heat treatment (i.e., calcination) in which the synthesized molecular sieve is heated in air or an inert gas at a temperature sufficient to remove some or all of the structure-directing agents. Pressures below atmospheric pressure may be used for heat treatment, but atmospheric pressure is preferred for convenience. Heat treatment may be carried out at a temperature of at least 370°C for at least 1 minute, generally for 20 hours or less (e.g., 1 to 12 hours). Heat treatment may be carried out at a temperature of up to 925°C. For example, heat treatment may be carried out in air at a temperature of 400°C to 600°C for approximately 1 to 8 hours. In particular, the heat-treated products in the form of metals, hydrogen, and ammonium are particularly useful for catalytic action in certain organic (e.g., hydrocarbon) conversion reactions.

[0045] Any additional framework metal cation within the molecular sieve can be replaced with hydrogen, ammonium, or any desired metal cation according to techniques well known in the art (e.g., by ion exchange).

[0046] Characterization of molecular sieves

[0047] In the synthesized anhydrous form, the molecular sieve SSZ-120 may have a chemical composition including the following molar relationships presented in Table 2:

[0048]

[0049] Here, Q is 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] Contains divalent cations.

[0050] In some embodiments, the molecular sieve may have a SiO2 / GeO2 molar ratio in the range of 4 to 12 (e.g., 6 to 10).

[0051] In its calcined form, molecular sieve SSZ-120 can have a chemical composition including the following molar relationships:

[0052] Al2O3: ( n )(SiO2+GeO2)

[0053] Here, n is ≥30 (e.g., 30 to 600, ≥60, 60 to 500, or 100 to 300).

[0054] The molecular sieve SSZ-120 has a powder X-ray diffraction pattern, which includes at least the peaks presented in Table 3 below in the synthesized form and at least the peaks presented in Table 4 in the calcined form.

[0055]

[0056]

[0057] The powder X-ray diffraction patterns presented herein were collected using standard techniques with copper K-alpha radiation. As understood by those skilled in the art, the determination of the parameter 2-theta is affected by both human and mechanical errors, which together may introduce an uncertainty of about ±0.3° for each reported 2-theta value. Of course, this uncertainty is also reflected in the reported values ​​of the d-interval calculated from the 2-theta value using Bragg's law. The relative intensity of the line I / Io represents the ratio of the peak intensity to the intensity of the strongest line against the background. Intensities are not corrected for Lorentz and polarization effects. Relative intensities are denoted by the symbols VS=very strong (>60 to 100), S=strong (>40 to 60), M=medium (>20 to 60), and W=weak (>0 to 20).

[0058] Minor changes in the powder X-ray diffraction pattern (e.g., experimental changes in peak ratios and peak positions) can occur due to changes in the atomic ratio of framework atoms resulting from changes in the lattice constant. Additionally, sufficiently small crystals can affect the shape and intensity of peaks, causing them to broaden. Calcination can also induce slight shifts in the powder X-ray diffraction pattern compared to the pre-calcined powder X-ray diffraction pattern. Despite these minor perturbations, the crystal lattice structure may remain unchanged even after calcination.

[0059] The synthesis described herein has a total surface area of ​​at least 500 m² of material 2 It can be / g and the external surface area is at least 100 m² 2 It is possible to produce molecular sieves having a small crystal size so that it can be / g. In some embodiments, the molecular sieves described herein are at least 600 m 2 / g, at least 625 m 2 / g, at least or at least 650 m 2 / g, e.g., 500 to 800 m 2 / g, 600 to 800 m 2 / g, or 650 to 800 m 2 It may include crystals having a total external surface area of ​​ / g. Additionally or alternatively, the molecular sieve described herein has at least 100 m 2 / g, at least 110 m 2 / g, at least 120 m 2 / g, at least 130 m 2 / g, or at least 140 m 2 / g, e.g., 100 to 300 m 2 / g, 120 to 300 m 2 / g, or 140 to 300 m 2It may include crystals having an external surface area of ​​ / g. All surface area values ​​given herein are determined from nitrogen physicosorption using the t-plot method. For details on this method, see the literature [BC Lippens and JH de Boer ( J. Catal It is described in . 1965, 4, 319-323).

[0060] Industrial applicability

[0061] Molecular sieve SSZ-120 (with some or all of the structure-directing agent removed) can be used as an adsorbent or catalyst to facilitate various organic compound conversion processes, including those of current commercial and industrial importance. Examples of chemical conversion processes effectively catalyzed by SSZ-120 alone or in combination with one or more other catalytically active materials, including other crystalline catalysts, include processes requiring catalysts with acid activity. Examples of organic conversion processes that can be catalyzed by SSZ-120 include aromatization, cracking, hydrogenation cracking, disproportionation, alkylation, oligomerization, and isomerization.

[0062] As with many catalysts, it may be desirable to incorporate SSZ-120 with other materials that resist the temperatures and other conditions used in organic conversion processes. Such materials include active and inert materials and synthetic or naturally occurring zeolites, as well as inorganic materials such as clay, silica, and / or metal oxides such as alumina. The latter may be in the form of gelatinous precipitates or gels, including naturally occurring materials or mixtures of silica and metal oxides. Using materials in combination with the active SSZ-120 (i.e., in combination with it or present during the synthesis of new materials) tends to alter the conversion and / or selectivity of the catalyst in specific organic conversion processes. Inert materials appropriately serve as diluents to control the conversion amount in a given process, allowing for the production of products in an economical and regular manner without the use of other means to control the reaction rate. These materials may be incorporated into naturally occurring clays (e.g., bentonite and kaolin) to improve the fracture strength of the catalyst under commercial operating conditions. These materials (i.e., clay, oxides, etc.) serve as binders for the catalyst. Since it is desirable to prevent the catalyst from decomposing into powdered material for commercial use, it is desirable to provide a catalyst with excellent fracture strength. These clay and / or oxide binders have typically been used solely to improve the fracture strength of the catalyst.

[0063] Naturally occurring clays that can be compounded with SSZ-120 include montmorillonite and kaolin series, which include subbentonite and kaolin, commonly known as Dixie, McNamee, Georgia, and Florida clays, or others in which the major mineral components are halloysite, kaolinite, dicite, nakrite, or azozite. These clays may be used in their raw, unprocessed state as originally mined, or in a state that has undergone initial calcination, acid treatment, or chemical modification. Binders useful for compounding with SSZ-120 also include inorganic oxides, such as silica, zirconia, titania, magnesia, beryllia, alumina, and mixtures thereof.

[0064] In addition to the aforementioned materials, SSZ-120 can be composited with porous matrix materials such as silica-alumina, silica-magnesia, silica-zirconia, silica-thoria, silica-berilia, and silica-titania, as well as ternary compositions such as silica-alumina-thoria, silica-alumina-zirconia, silica-alumina-magnesia, and silica-magnesia-zirconia.

[0065] The relative ratio of SSZ-120 to the inorganic oxide matrix can vary widely, with an SSZ-120 content in the range of 1 to 90 weight% (e.g., 2 to 80 weight%) of the composite.

[0066] Examples

[0067] The following exemplary embodiments are intended to be non-limiting.

[0068] Example 1

[0069] 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H Synthesis of Imidazolium Dihydroxide

[0070] 5 g of 2,6-bis(bromomethyl)naphthalene, 3.83 g of 1,2-dimethylimidazole, and 100 mL of methanol were filled into a 250 mL round-bottom flask equipped with a magnetic stirring bar. A reflux condenser was then attached, and the mixture was heated at 65°C for 3 days. After cooling, the methanol was removed in a rotary evaporator to yield a white solid. The solid initially recovered from the rotary evaporation was further purified by recrystallization in cold ethanol. The recrystallized dibromide salt 1 H- and 13 It was purified by C-NMR spectroscopy.

[0071] The dibromide salt was exchanged with the corresponding dihydroxide salt by stirring overnight with a hydroxide exchange resin in deionized water. The solution was filtered, and a small sample was titrated with a standardized solution of 0.1 N HCl to analyze the filtrate for hydroxide concentration.

[0072] Example 2

[0073] Synthesis of SSZ-120

[0074] 0.27 g of Tosoh HSZ-390HUA Y-zeolite (SAR=500), 0.05 g of GeO2, and 2.5 mmol of aqueous 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1] were added to a metered 23 mL Parr reactor. H A solution of imidazolium dihydroxide was added. The reactor was then placed in an exhaust hood, and water was evaporated to achieve an H2O / (SiO2+GeO2) molar ratio of 7 (determined by the total mass of the suspension). Subsequently, 2.5 mmol of HF was added, and the reactor was heated to 160°C while tumbling at 43 rpm for approximately 7 days. The solid product was recovered by centrifugation, washed with deionized water, and dried at 95°C.

[0075] The powder XRD of the synthesized product exhibited the pattern shown in Figure 1, and the product showed a new phase, SSZ-120, in a pure form. A significantly reduced crystal size is inferred from the peak broadening in the powder XRD pattern.

[0076] Figures 2(a) to 2(d) show exemplary SEM images of the synthesized product at various magnifications.

[0077] When the product was determined by ICP-AES (Inductively Coupled Plasma - Atomic Emission Spectroscopy), the SiO2 / GeO2 molar ratio was 8.

[0078] Example 3

[0079] SSZ-120's Harso

[0080] The synthesized molecular sieve of Example 1 was heated to 550°C at a rate of 1°C / min and calcined inside a muffle furnace under an air flow maintained at 550°C for 5 hours, cooled, and then analyzed by powder XRD.

[0081] The powder XRD pattern of the calcined material is shown in Figure 3 and indicates that the material remains stable after calcination, thereby removing the structure-inducing agent.

[0082] Example 4

[0083] Example 2 was repeated using Zeolyst CBV780 Y-zeolite (SAR=80) as the FAU source. Powder XRD showed that the product was SSZ-120.

[0084] Example 5

[0085] Example 2 was repeated using Zeolyst CBV760 Y-zeolite (SAR=60) as the FAU source. Powder XRD showed that the product was SSZ-120.

[0086] The product was calcined as described in Example 2. The surface area of ​​the sample was measured using nitrogen physical absorption, and the data were analyzed by the t-plot method. The determined total surface area was 693 m². 2 / g and the external surface area is 144 m² 2 / g. The micropore volume was 0.2666 cm³ 3 / g was.

[0087] Example 6

[0088] Example 2 was repeated using Zeolyst CBV720 Y-zeolite (SAR=30) as the FAU source. Powder XRD showed that the product was SSZ-120.

[0089] Example 7

[0090] Brønsted Sando

[0091] The Brønsted acidity of the molecular sieve of Example 5 in the calcined form is [TJ Gricus Kofke et al. ( J. Catal . 1988, 114, 34-45); TJ Gricus Kofke et al. ( J. Catal . 1989, 115, 265-272); and JG Tittensor et al. ( J. Cataln-propylamine temperature-programmed desorption (TPD) was measured as adopted from the description published by [1992, 138, 714-720]. Samples were pretreated in fluid-drying H2 at 400°C to 500°C for 1 hour. Then, the dehydrated samples were cooled to 120°C in fluid-drying helium and maintained at 120°C for 30 minutes in fluid-drying helium saturated with n-propylamine for adsorption. Subsequently, the n-propylamine-saturated samples were heated to 500°C in fluid-drying helium at a rate of 10°C / min. Brønsted acidity was calculated based on weight loss versus temperature by thermogravimetric analysis (TGA) and effluent NH3 and propene by mass spectrometry. The Brønsted acidity of the samples was 250 μmol / g, indicating that aluminum sites were incorporated into the molecular sieve framework.

[0092] Example 8

[0093] Constraint Index Test

[0094] The constraint index is a test to determine shape-selective catalytic behavior in molecular sieves. The reaction rates for cracking of n-hexane (n-C6) and its isomer 3-methylpentane (3-MP) are compared under competitive conditions (Reference [VJ Frillette et al., J. Catal [See . 1981, 67, 218-222]

[0095] The hydrogen-form molecular sieve prepared according to Example 5 was pelletized at 4 kpsi, ground, and granulated to 20-40 mesh. A 0.6 g sample of the granulated material was calcined in air at 540°C for 4 hours and cooled in a desiccator to be completely dried. Then, 0.47 g of the material was loaded into a ¼-inch stainless steel tube with alundum on both sides of the molecular sieve bed. The reactor tube was heated using a furnace (Applied Test Systems, Inc.). Nitrogen was introduced into the reactor tube at 9.4 mL / min at atmospheric pressure. The reactor was heated to approximately 700°F (371°C), and a 50 / 50 feed of n-hexane and 3-methylpentane was introduced into the reactor at a rate of 8 μL / min. The feed was delivered by an ISCO pump. Direct sampling to the GC was initiated 15 minutes after the feed was introduced. The test data results after 15 minutes at the stream (700℉) are presented in Table 5.

[0096]

[0097] Example 9

[0098] Hydrogenation of n-decane

[0099] The material of Example 5 was calcined in air at 595°C for 5 hours. After calcination, 4.5 g of 0.148 N NH4OH solution was mixed with 5.5 g of deionized water at room temperature for 3 days, and then (NH3)4Pd(NO3)2 solution (buffered at pH 9.5) was mixed to load palladium onto the material, thereby providing 0.5 wt% Pd loading in 1 g of this solution mixed with 1 g of molecular sieve. The recovered Pd / SSZ-120 material was washed with deionized water and dried at 95°C, and then calcined at 300°C for 3 hours. The calcined Pd / SSZ-120 catalyst was then pelletized, ground, and sieved through a 20-40 mesh.

[0100] 0.5 g of Pd / SSZ-120 catalyst was loaded into the center of a 23-inch long x ¼-inch outer diameter stainless steel reactor tube, with alundum loaded upstream of the catalyst to preheat the feed (total pressure 1200 psig; measured at 1 atm and 25°C, downflow hydrogen rate 160 mL / min; and downflow liquid feed rate 1 mL / h). All materials were first reduced in flowing hydrogen at approximately 315°C for 1 hour. The products were analyzed by online capillary GC once every 60 minutes. Raw data from the GC was collected by an automated data acquisition / processing system, and hydrocarbon conversion rates were calculated from the raw data. Conversion is defined as the amount of n-decane reacted to produce other products (including iso-C10). Yield is expressed as the molar percentage of products other than n-decane, including iso-C10 isomers as yield products. The results are shown in Figure 4 and indicate that the catalyst is highly active and not particularly selective for isomerization, allowing for the production of significant decomposition products from n-decane.

Claims

Claim 1 Aluminogermanosilicate molecular sieve having a powder X-ray diffraction pattern including the peaks in the table below in a calcined form: . Claim 2 In claim 1, the molecular sieve has a total surface area of ​​at least 500 m² when determined by the t-plot method for nitrogen physical adsorption. 2 / g and / or, when determined from the t-plot method of nitrogen physical adsorption, the external surface area is at least 100 m² 2 Aluminogermanosilicate molecular sieve containing crystals in the range of / g. Claim 3 In paragraph 2, the total surface area is 500 to 800 m² 2 Aluminogermanosilicate molecular sieve in the range of / g. Claim 4 In paragraph 2, the external surface area is 100 to 300 m² 2 Aluminogermanosilicate molecular sieve in the range of / g. Claim 5 In claim 1, an aluminogermanosilicate molecular sieve having a composition including the following molar relationship: Al2O3: ( n )(SiO2+GeO2)where n is ≥30. Claim 6 Aluminogermanosilicate molecular sieve having a powder X-ray diffraction pattern including the peaks in the table below in the synthesized form: . Claim 7 In claim 6, an aluminogermanosilicate molecular sieve having a composition in the following molar ratios: Here, Q is 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] Contains divalent cations. Claim 8 In claim 6, an aluminogermanosilicate molecular sieve having a chemical composition including the following molar relationship: Here, Q is 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H -Imidazolium] Contains divalent cations. Claim 9 A method for synthesizing an aluminogermanosilicate molecular sieve, wherein the method comprises the step of providing a reaction mixture comprising: (1) a FAU framework type zeolite; (b) a source of germanium; (c) 3,3'-[2,6-naphthalenebis(methylene)]bis[1,2-dimethyl-1 H A method comprising: (d) a structure-inducing agent (Q) containing a divalent cation [imidazolium]; a source of fluoride ions; and (e) water; and (2) applying a reaction mixture to crystallization conditions sufficient to form crystals of an aluminogermanosilicate molecular sieve, wherein the crystallization conditions include heating the reaction mixture at a temperature of 100°C to 200°C under self-generating pressure for a period of 1 to 14 days. Claim 10 In claim 9, the method wherein the reaction mixture has a composition in the following molar ratios: . Claim 11 In claim 9, the method wherein the reaction mixture has a composition in the following molar ratios: . Claim 12 In claim 9, the above FAU framework type zeolite is zeolite Y, method. Claim 13 delete Claim 14 A method for converting a feedstock containing an organic compound into a conversion product, comprising the step of contacting the feedstock with a catalyst comprising the aluminogermanosilicate molecular sieve of claim 1 under organic compound conversion conditions. Claim 15 delete

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