Molecular sieve boron SSZ-117x

Abstract

Provided is a novel synthetic crystalline boron germanosilicate molecular sieve material designated as boron SSZ-117x. Boron SSZ-117x can be synthesized using the N,N,N,3,5-pentamethyladamantan-1-ammonium cation as a structure directing agent. The synthesis utilizes a boron route to obtain a boron molecular sieve. Boron SSZ-117x can be used in organic compound conversion reactions such as reforming and / or sorption processes.

Description

Technical Field

[0001] This application claims the benefit of U.S. Provisional Patent Application No. 63 / 365,534, filed May 31, 2022, the entire disclosure of which is incorporated herein by reference in its entirety.

[0002] The present disclosure relates to a novel synthetic crystalline molecular sieve, designated SSZ-117x, that contains boron within its framework. The present disclosure also relates to its synthesis.

Background Art

[0003] Molecular sieves are a commercially important class of materials having a unique crystal structure with a distinct pore structure as indicated by a unique X-ray diffraction (XRD) pattern. Molecular sieves also have a specific chemical composition. The crystal structure defines cavities and pores that are characteristic of a particular type of molecular sieve. Providing new molecular sieves that differ in crystal structure as well as composition can lead to unique catalysts or adsorption / separation materials. Altering the crystal structure is always difficult, but if successful, can provide benefits for new catalysts for organic compound conversion reactions. U.S. Patent Application Publication No. 2022 / 0072520 discloses the preparation of SSZ-117x. However, it does not disclose boron SSZ-117x.

Summary of the Invention

Means for Solving the Problems

[0004] According to the present disclosure, a crystalline molecular sieve designated boron SSZ-117x is synthesized using N,N,N,3,5-pentamethyladamantan-1-ammonium cation as a structure directing agent (SDA). It has been found that the synthesis was successful in providing a boron-containing molecular sieve having the SSZ-117x crystal structure.

[0005] In one aspect, a boron SSZ-117x molecular sieve having a powder X-ray diffraction pattern containing at least the peaks in Table 3 below is prepared in its as-synthesized form.

[0006] In its as-synthesized and anhydrous form, the boron molecular sieve has the following molar relationships: [Table 1] (wherein T is a tetravalent element including silicon and germanium; Q + is N,N,N,3,5-pentamethyladamantan-1-ammonium cation) and may have a chemical composition. In one embodiment, the ratio of TO2 / B2O3 is in the range of 15 to 20.

[0007] In its calcined or ozone-treated form, the boron SSZ-117x molecular sieve has the following molar relationships: B2O3:(n)TO2 (wherein n is ≧10; T is a tetravalent element including silicon and germanium) and may have a chemical composition.

[0008] In a further aspect, a method for synthesizing a boron SSZ-117x molecular sieve is provided. The method comprises (a) providing a reaction mixture comprising: (1) an FAU framework type zeolite; (2) a source of germanium; (3) a source of boron; (4) N,N,N,3,5-pentamethyladamantan-1-ammonium hydroxide (Q); (5) a source of fluoride ions; and (6) water. The reaction mixture is then subjected to crystallization conditions sufficient to form crystals of the SSZ-117x boron molecular sieve. T is as described above.

[0009] Next, the boron-containing molecular sieve is treated to remove the structure-directing agent (SDA) referred to above as Q. The SDA can be removed, for example, by calcination or by ozone treatment at 150 °C. It has also been found that the SDA can be removed by treating the molecular sieve with dimethylformamide.

[0010] In yet a further aspect, there is provided a process for converting a raw material containing an organic compound into a conversion product, the process comprising contacting the raw material under organic compound conversion conditions with a catalyst comprising a boron SSZ-117x molecular sieve.

[0011] Among other factors, the process can provide a boron SSZ-117x molecular sieve that is a borongermanosilicate. This new molecular sieve prepared by the process imparts unique capabilities as a catalyst in organic compound conversion reactions such as reforming. The molecular sieve also finds significant value as an adsorption / separation material. **DETAILED DESCRIPTION OF THE INVENTION**

[0012] Definitions The term "framework type" has the meaning described in "Atlas of Zeolite Framework Types" by Ch. Baerlocher and L.B. McCusker and D.H. Olsen (Elsevier, Sixth Revised Edition, 2007).

[0013] The term "boron germanosilicate" refers to a crystalline microporous solid containing boron, germanium, and silicon oxide within its framework structure. The boron germanosilicate may be either "pure boron germanosilicate" (i.e., without other detectable metal oxides along with its framework structure) or optionally substituted. When described as "optionally substituted", each framework may contain other atoms (e.g., Al, Ga, In, Fe, Ti, Zr) that replace one or more atoms that are not yet present in the parent framework.

[0014] As used herein, the term "as-synthesized" refers to the molecular sieve in that form after crystallization and before removal of the structure-directing agent.

[0015] As used herein, the term "anhydrous" refers to a molecular sieve substantially free of both physically adsorbed water and chemically adsorbed water.

[0016] As used herein, the Group numbering scheme of the Periodic Table is as disclosed in Chem. Eng. News 1985, 63(5), 26 - 27.

[0017] Synthesis of Molecular Sieve This molecular sieve boron SSZ - 117x is synthesized by (a) providing a reaction mixture comprising (1) a silicon oxide source such as an FAU framework type zeolite; (2) a source of germanium; (3) a source of boron; (4) N,N,N,3,5 - pentamethyladamantan - 1 - ammonium hydroxide (Q); (5) a source of fluoride ions; and (6) water; and then (b) subjecting the reaction mixture to crystallization conditions sufficient to form crystals of the SSZ - 117x boron molecular sieve. T is as described above herein. In one embodiment, the FAU framework zeolite has very little Al2O3. The SiO2 / Al2O3 ratio can be 300 or more. Thus, the framework contains a predominant amount of boron.

[0018] The reaction mixture has a composition with respect to molar ratios within the ranges set forth in Table 2: [[Table 2]] (wherein T and Q are as described above herein) may be included.

[0019] Suitable sources of silicon oxide may include any suitable known source such as colloidal silica, fumed silica, precipitated silica, or alkali metal silicates. FAU framework type zeolites, such as zeolite Y, may also be a source of silicon oxide. In such cases, the FAU framework type zeolite has a very high SiO2 / Al2O3 molar ratio of at least 250, preferably at least 300 (e.g., from 300 to 500). The FAU framework type zeolite may include two or more FAU framework type zeolites having different SiO2 / Al2O3 molar ratios. The FAU framework type zeolite may be either zeolite Y or any of its various post-synthetic modified forms, as is known in the art. The inclusion of boron within the final framework by this process is of utmost importance.

[0020] Sources of germanium may include germanium oxide and germanium alkoxides (e.g., germanium ethoxide, germanium isopropoxide), germanium hydroxide, and germanium carboxylate.

[0021] Silicon and germanium may be present in the reaction mixture at a SiO2 / GeO2 molar ratio of from 4 to 12 (e.g., from 6 to 10).

[0022] The source of boron may include boric acid, which is preferred. Other suitable sources may be used, but are not preferred.

[0023] Sources of fluoride ions may include, for example, hydrogen fluoride, ammonium fluoride, and ammonium bifluoride.

[0024] SSZ-117x having boron has the following structure (1): [Chemical formula] It is synthesized using a structure-directing agent containing the N,N,N,3,5-pentamethyladamantan-1-ammonium cation (Q+) represented by:

[0025] The reaction mixture typically has a Q / F molar ratio in the range of 0.80 to 1.20 (e.g., 0.85 to 1.15, 0.90 to 1.10, 0.95 to 1.05, or 1 to 1).

[0026] The reaction mixture may contain seed crystals of a molecular sieve material such as boron SSZ-117x obtained from a previous synthesis in an amount of 0.01 to 10,000 ppm by weight of the reaction mixture (e.g., 100 to 5000 ppm by weight). The addition of seed crystals can be advantageous in reducing the time required for complete crystallization. Further, the addition of seed crystals can result in an increase in the purity of the resulting product by promoting the nucleation and / or formation of boron SSZ-117x over undesirable phases.

[0027] It is noted that the reaction mixture components can be supplied from two or more sources. Also, two or more reaction components can be provided by one source. The reaction mixture can be prepared batchwise or continuously.

[0028] Crystallization and Synthetic Post-Treatment The crystallization of the boron molecular sieve from the above reaction mixture can be carried out at a temperature of 125°C to 200°C (e.g., 150°C to 170°C) in a suitable reactor vessel (e.g., a polypropylene jar or a Teflon(trademark)-processed or stainless steel autoclave) under static, rotating, or stirring conditions for a time sufficient for crystallization to occur at the temperature used (e.g., 1 day to 20 days, or 2 days to 10 days). The hydrothermal crystallization process is typically carried out under pressure, such as in an autoclave, and preferably under autogenous pressure.

[0029] When a molecular sieve crystal containing boron is formed, the solid product can be recovered from the reaction mixture by standard mechanical separation techniques such as centrifugation or filtration. The recovered crystals are washed with water and then dried to obtain as-synthesized molecular sieve crystals of SSZ-117x boron. The drying process can be carried out at a high temperature (e.g., 75 °C to 150 °C) for several hours (e.g., about 4 to 24 hours). The drying process can be carried out under vacuum or at atmospheric pressure.

[0030] As a result of the crystallization process, the recovered crystalline molecular sieve product contains at least a portion of the structure-directing agent used in the synthesis within its pore structure. The as-synthesized molecular sieve is subjected to a treatment to remove some or all of the structure-directing agent used in its synthesis.

[0031] Removal of the structure-directing agent can be carried out by a heat treatment (e.g., calcination) in which the as-synthesized molecular sieve is heated at a temperature sufficient to remove some or all of the structure-directing agent. A pressure lower than atmospheric pressure can be used for the heat treatment, but atmospheric pressure is desirable for simplicity. The heat treatment can be carried out at a temperature of at least 370 °C for at least 1 minute and generally less than 20 hours (e.g., 1 to 12 hours). The heat treatment can be carried out at a temperature up to 925 °C. For example, the heat treatment can be carried out at a temperature of 400 °C to 600 °C in the presence of an oxygen-containing gas.

[0032] Furthermore, or alternatively, the structure-directing agent can be removed by treatment with ozone. See, for example, A.N. Parikh et al., Micropor. Mesopor. Mater. 2004, 76, 17 - 22. In one embodiment, the use of ozone is preferred in that it gives a higher micropore volume. It has also been found that the SDA can be removed by treatment with dimethylformamide, for example, by treatment at about 150 °C.

[0033] Characterization of the Molecular Sieve As-synthesized and in anhydrous form, molecular sieve SSZ-117x having boron may have a chemical composition comprising the following molar relationships set forth in Table 1: [Table 1] (wherein T is a tetravalent element including silicon and germanium; and Q+ may include the N,N,N,3,5-pentamethyladamantan-1-ammonium cation). In some embodiments, the molecular sieve may have an SiO2 / GeO2 molar ratio in the range of 4 to 12 (e.g., 6 to 10). In one embodiment, the SiO2 / GeO2 molar ratio ranges from 7 to 10, preferably about 9. In one embodiment, the ratio of TO2 / B2O3 is in the range of 15 - 20.

[0034] It should be noted that as-synthesized molecular sieve SSZ-117x having boron may have a molar ratio different from the molar ratio of the reactants of the reaction mixture used to prepare it in the as-synthesized form. This result can occur because 100% of the reactants of the reaction mixture are not completely incorporated into the crystals formed (from the reaction mixture).

[0035] In its calcined form, molecular sieve boron SSZ-117x may have the following molar relationship: B2O3:(n)TO2 (wherein n is ≧10 (e.g., 15 or more, or in the range of 15 - 20); and T is a tetravalent element including silicon and germanium).

[0036] Molecular sieve boron SSZ-117x is characterized by a powder XRD pattern comprising at least the peaks set forth in Table 3 below in the as-synthesized form of the molecular sieve. In another embodiment, boron SSZ-117x has a unique XRD pattern comprising at least the peaks set forth in Table 4 below after being subjected to ozonalysis. [Table 3]

Table 4

[0037] The powder X-ray diffraction patterns presented herein were collected by standard techniques. The radiation was CuKα radiation. The peak height and position as a function of 2θ where θ is the Bragg angle were read from the relative intensities of the peaks (adjusted with respect to the background), and the lattice plane spacing d corresponding to the recorded lines could be calculated.

[0038] Small variations in the diffraction pattern can result from variations in the molar ratio of the framework species of the sample due to changes in the lattice constant. Additionally, irregular substances and / or sufficiently small crystals will affect the shape and intensity of the peaks, resulting in significant peak broadening. Small variations in the diffraction pattern can also result from variations in the organic compounds used in the preparation. Calcination can also cause a small shift in the XRD pattern. Despite these small perturbations, the basic crystal lattice structure remains unchanged.

[0039] Adsorption and Catalysis This molecular sieve boron SSZ-117x (where part or all of Q+ has been removed) can be used as an adsorbent or as a catalyst for catalyzing a wide variety of organic compound conversion processes. There is a particular potential for use as a catalyst in the modification process of boron SSZ-117x. In one embodiment, the catalyst also contains platinum.

[0040] Catalytic reforming is one of the basic petroleum refining processes for reforming light hydrocarbon raw materials, often referred to as naphtha feedstocks. The products obtained from catalytic reforming can include high-octane gasoline useful as automotive fuel, aromatics (e.g., benzene, toluene, xylene, and ethylbenzene), and / or hydrogen. Reactions typically involved in catalytic reforming include dehydrocylization, isomerization, and dehydrogenation of naphtha-range hydrocarbons, and the dehydrogenation cyclization and dehydrogenation of straight-chain and slightly branched alkanes and the dehydrogenation of cyclic paraffins result in the production of aromatics. Dealkylation and hydrocracking are generally not desirable due to the low value of the resulting light hydrocarbon products.

[0041] The boron SSZ-117x catalyst used in catalysts commonly used for commercial reforming reactions often contains a Group VIII metal such as platinum or palladium, or a second catalytic metal that acts as a promoter in addition to the Group VIII metal. Examples of metals useful as promoters include rhenium, tin, tungsten, germanium, cobalt, nickel, rhodium, ruthenium, iridium, or combinations thereof. The catalytic metal or metals can be dispersed on a support such as alumina, silica, or silica-alumina.

[0042] The boron SSZ-117x modified catalyst can be used by being arranged as a fixed bed in the reaction zone in the form of pellets, pellets, granules, fragments, or various special shapes, and the feedstock can pass through in any of upward, downward, or radial flow through the liquid phase, gas phase, or mixed phase. Alternatively, the modified catalyst can be used in a moving bed or fluidized solid process where the feedstock rises and passes through a turbulent bed of finely divided catalyst. However, a fixed bed system or a dense phase moving bed system is preferred due to less catalyst consumption and other operating advantages. In a fixed bed system, the feed material is preheated to the desired reaction temperature (by any suitable heating means) and then passed through a reaction zone containing a fixed bed of catalyst. This reaction zone can be one or more separate reactors having suitable means for maintaining the desired temperature at the reactor inlet. Since the reforming reaction is typically endothermic in nature, the temperature must be maintained.

[0043] The actual reforming conditions often depend, at least in part, on the feedstock used, whether highly aromatic, paraffinic, or naphthenic, and on the desired octane number of the product and the desired amount of hydrogen production.

Examples

[0044] The following examples are intended to be non-limiting.

[0045] (Example 1) Synthesis of N,N,N,3,5-pentamethyladamantan-1-ammonium hydroxide 3,5-Dimethyladamantan-1-amine was permethylated by treatment with more than three-fold excess methyl iodide and 2 equivalents of potassium hydrogen carbonate in methanol over several days. The reaction mixture was concentrated under reduced pressure, and the resulting solid was extracted twice with chloroform. The crude product was recovered by rotary evaporation of chloroform under reduced pressure. The crude product was recovered by removal of chloroform. The crude product was heated in a minimum amount of 95% ethanol at 70 °C to obtain a clear solution. The solution was allowed to cool to room temperature to obtain the iodide salt as very clear crystals. The purity of the product was then confirmed by both chemical analysis and H and C NMR in CDCl3.

[0046] The resulting iodide salt was exchanged for the corresponding hydroxide salt by stirring overnight in deionized water with a hydroxide exchange resin (AMBERLITE(C) IRN78). The solution was filtered and the filtrate was analyzed for hydroxide concentration by titration with a standard solution of 0.1 N HCl of a small sample.

[0047] (Example 2) Synthesis of SSZ-117x Containing Boron To a weighed 23 mL Parr reactor was added 0.27 g of Tosoh Corporation's 390HUA Y-zeolite (approximate SiO2 / Al2O3 molar ratio of 500), 0.05 g of GeO2, 0.02 g H3BO3, and 2.5 millimoles of an aqueous solution of N,N,N,3,5-pentamethyladamantan-1-ammonium hydroxide. The reactor was then placed in an exhaust hood and water was evaporated to give an H2O / (SiO2 + GeO2) molar ratio of 7 (determined by the total mass of the suspension). Then HF (2.5 millimoles) was added and the reactor was heated to 160 °C for about 7 days while rotating at 43 rpm. The solid product was recovered by centrifugation, washed with deionized water, and dried at 95 °C.

[0048] Powder XRD will show that the final product is a new phase in pure form designated as SSZ-117x boron and exhibiting the characteristic peaks of Table 3.

[0049] (Example 3) The as-synthesized boron SSZ-117x of Example 2 was heated in excess dimethylformamide in a sealed reactor at 150 °C for 5 days. Upon cooling, the solid was washed to remove the solvent and then washed with water and dried at 95 °C. The mass loss was 20% with this extraction. The dried solid was then subjected to ozonolysis at 150 °C overnight to remove all of the residual SDA in the pores. The opened structure now had a significantly changed XRD pattern as shown in Table 4.

Table 4

[0050] (Example 4) An as-synthesized sample of SSZ-117 having boron and Ge is treated at 150 °C for 3 days in a sealed reactor with 10 cc of dimethylformamide per gram of zeolite. The material is collected by filtration and then washed with water. After drying, the material (whose XRD pattern has changed from SSZ-117 to 117x) is then treated with flowing ozone at 150 °C overnight to complete the removal of the organics used in the production of the zeolite.

[0051] Next, the material (0.825 grams) is treated with 0.128 grams of 50% CsOH in 12 ml of water to neutralize the acidity. The treatment is carried out at room temperature for 25 hours and then filtered. The collected solid is then calcined at 300 °C in air.

[0052] The calcined boron SSZ-117x is then redispersed in 18 ml of water with 0.0155 grams of platinum tetramine chloride and stirred at room temperature for 24 hours. The material is then collected, calcined at 300 °C, and then compressed and sieved to 24 / 40 pieces for charging into the reactor.

[0053] (Example 5) Pretreatment of Naphtha Reforming Catalyst The naphtha catalytic reforming catalyst prepared in Example 4 is sulfided. The sulfidation reaction was carried out in a downflow fixed bed reactor system. The procedure is described as follows:

[0054] The catalyst was sieved to 24 - 40 mesh and then placed in the center of a stainless steel tubular reactor. The catalyst (dry weight of 0.6 g measured by TGA (thermogravimetric analysis) at 1112°F) was first dried in a N2 flow (300 ml / min) from room temperature to 400°F at a heating rate of 10°F / min and maintained at 400°F for 30 minutes. For the reduction of platinum in the catalyst, thereafter, the catalyst was heated in a H2 flow (300 ml / min) from 400°F to 900°F at a heating rate of 5°F / min and maintained at 900°F for 30 minutes. Finally, the catalyst was cooled to 800°F and the sulfidation reaction was started.

[0055] The feedstock applied to the sulfidation reaction was anhydrous n - octane containing 200 ppm sulfur (as dimethyldisulfide). The sulfidation was carried out at 800°F and atmospheric pressure for 60 minutes. The flow rates of H2 and the liquid feedstock were 30 ml / min and 0.43 ml / min, respectively. After sulfidation, to remove excess sulfur species occluded in and / or on the surface of the catalyst pores, the catalyst was heated in a H2 flow (300 ml / min) from 800 to 900°F within a few minutes and then further heated at 900°F for 30 minutes. Finally, the catalyst was heated or cooled to the preset reaction temperature (e.g., 850 or 950°F) in the same H2 flow (300 ml / min) within 2 hours in preparation for the start of the naphtha catalytic reforming test of Example 6.

[0056] (Example 6) Procedure for the naphtha catalytic reforming test After the sulfidation procedure described in Example 5, the naphtha catalytic reforming reaction was carried out as described below.

[0057] The catalyst was heated or cooled to a pre-set reaction temperature (950°F in Example 8) in the same H2 flow (300 ml / min) within 2 hours to prepare for the start of the naphtha catalytic reforming test in this example as described in Example 5. At the same time, the reactor system was pressurized to a pre-set pressure (150 psig in Example 8). During that time, the H2 flow was adjusted to a pre-set flow rate (16 ml / min in Example 8). The feed rate was 1.75 ml / hr (in Example 8).

[0058] In the following examples, the naphtha catalytic reforming experiment was carried out at a hydrocarbon WHSV of 2.2 and a molar ratio of hydrogen to hydrocarbon of 3.0 using the naphtha feedstock described in Example 7.

[0059] (Example 7) Feedstock for the naphtha catalytic reforming test The GC analysis data obtained from the feedstock used in the naphtha catalytic reforming test is given in Table 5 together with the GC results of Example 8 for the products of that naphtha catalytic reforming test on the catalyst described in Example 4. The GC data was obtained by on-line analysis.

[0060] (Example 8) Products obtained from the naphtha catalytic reforming test The GC analysis data obtained from the feedstock of Example 7 used in the naphtha catalytic reforming test is given in Table 5 together with the results of this example for the products of that naphtha catalytic reforming test on the catalyst described in Example 4. The naphtha catalytic reforming experiment was carried out at 950°F, 150 psig, a hydrocarbon WHSV of 2.2 and a molar ratio of hydrogen to hydrocarbon of 3.0.

[0061] The GC results obtained from the feedstock (Example 7) used in the naphtha catalytic reforming test and from the products of that naphtha catalytic reforming test (Example 8) on the catalyst described in Example 4 are shown in Table 5 below. Reaction conditions: 950°F, 150 psig, a hydrocarbon WHSV of 2.2 and a molar ratio of hydrogen to hydrocarbon of 3.0.

Table 5

[0062] As shown in Table 5, the product shows a significant increase in aromatics useful for high-octane gasoline. Boron SSZ-117x was successful in reforming the raw materials of Example 7.

[0063] As used in this disclosure, the terms "comprises" or "comprising" are intended to be non-limiting transitional terms that mean the inclusion of the recited elements but do not necessarily exclude other unrecited elements. The phrase "consists essentially of" or "consisting essentially of" is intended to mean the exclusion of other elements that have essential significance to the composition. The phrase "consisting of" or "consists of" is intended to be a transitional term that means the exclusion of all except the recited elements, except for trace impurities.

[0064] All patents and publications cited herein are incorporated herein by reference to the extent not inconsistent herewith. It will be understood that some of the structures, functions, and operations of the above-described embodiments are not necessary to practice the present invention and are included herein merely for purposes of illustration of exemplary embodiments or completeness of one or more embodiments. Further, it will be understood that the specific structures, functions, and operations described in the above-cited patents and publications can be practiced in conjunction with the present invention, but they are not essential thereto. Accordingly, it is to be understood that the present invention can be practiced otherwise than as specifically described without departing from the spirit and scope of the invention as defined by the appended claims.

Claims

1. A molecular sieve containing boron, having a powder X-ray diffraction pattern in its as-synthesized form with the following peaks: 【Table 3】

2. A molecular sieve according to claim 1, having a composition comprising the following molar relationship: B ２ O ３ :(n) TO ２ (wherein n is ≧ 10; and T is a tetravalent element including silicon and germanium).

3. A molecular sieve according to claim 1, having a composition comprising the following molar relationship: B ２ O ３ :(n) TO ２ (wherein n is ≧ 15; and T is a tetravalent element including silicon and germanium).

4. The following molar relationship: 【Table 1A】 (wherein T is a tetravalent element containing silicon and germanium; Q － is a molecular sieve according to claim 1, having a chemical composition comprising (including the N,N,N,3,5-pentamethyladamantan-1-ammonium cation).

5. A molecular sieve according to claim 4, which is sulfided and contains a Group VIII metal.

6. A molecular sieve according to claim 5, wherein the Group VIII metal is platinum or palladium.

7. A method for synthesizing a molecular sieve according to claim 1, comprising: (1) FAU framework type zeolite having a SiO ２ / Al ２ O ３ molar ratio of at least 300; (a) preparing a reaction mixture comprising: (2) a source of germanium; (3) a source of boron; (4) N,N,N,3,5-pentamethyladamantan-1-ammonium hydroxide (Q); (5) a source of fluoride ions; and (6) water; (b) subjecting the reaction mixture to crystallization conditions sufficient to form crystals of the molecular sieve; and (c) removing Q from the molecular sieve framework.

8. The method according to claim 7, wherein the reaction mixture has a composition with respect to molar ratios as follows: 【Table 2A】 (wherein T is a tetravalent element including silicon and germanium).

9. The method according to claim 7, wherein the reaction mixture has a composition with respect to molar ratios as follows: 【Table 2B】 (wherein T is a tetravalent element including silicon and germanium).

10. The method according to claim 7, wherein the FAU framework type zeolite is zeolite Y or a post-synthetic modified form.

11. The method according to claim 7, wherein the crystallization conditions include a temperature of 125 °C to 200 °C.

12. The method according to claim 7, wherein the reaction mixture has a Q / F molar ratio in the range of 0.8 to 1.

2.

13. A method for converting a raw material containing an organic compound into a conversion product, the method comprising contacting the raw material with a catalyst comprising the molecular sieve according to claim 5 under organic compound conversion conditions.

14. A method for converting a raw material containing an organic compound into a conversion product, the method comprising contacting the raw material with a catalyst comprising the molecular sieve according to claim 6 under organic compound conversion conditions.

15. The method according to claim 13, wherein the conversion reaction is reforming.

16. The method according to claim 14, wherein the conversion reaction is reforming.

17. A method for ion-exchanging a metal, the method comprising contacting a stream containing a heavy metal with the molecular sieve according to claim 4.

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