Molecular Sieve SSZ-117x with High Acidity

Abstract

A novel synthetic crystalline aluminogermanosilicate molecular sieve material designated as SSZ-117x, which exhibits increased acidity, is provided. 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 increased acid sites. The SSZ-117x with increased acidity can be used in organic compound conversion reactions and / or sorption processes.

Description

Technical Field

[0001] This application claims the priority of U.S. Provisional Patent Application No. 63 / 365,514, filed on May 31, 2022, the entire disclosure of which is incorporated herein by reference in its entirety.

[0002] This application relates to a novel synthetic crystalline molecular sieve having increased acidity, designated SSZ-117x, and its synthesis.

Background Art

[0003] Zeolite materials are known to be useful as adsorbents and to have catalytic performance for various types of organic compound conversion reactions. Certain zeolite materials are ordered porous crystalline materials that have a certain crystal structure as measured by X-ray diffraction, with a large number of smaller cavities therein, which can be interconnected by some even smaller channels or pores. These cavities and pores are of uniform size within a particular zeolite material. Since the dimensions of these pores are such that they accept sorbate molecules of a particular dimension and not those of a larger dimension, these materials have come to be known as "molecular sieves" and are used in various ways that utilize these properties.

Summary of the Invention

Problems to be Solved by the Invention

[0004] There are currently over 250 known zeolite framework structures recognized by the International Zeolite Association. There is a need for new structures with properties different from those of known materials to improve the performance of many organic compound conversion and sorption processes. Each structure has unique pore, channel, and cage dimensions, giving it its specific properties as described above. Each framework structure has a specific composition. Improvements in preparing more pure single-phase materials are always important. Providing a molecular sieve with increased acid sites can be beneficial with respect to catalysis in organic compound conversion reactions.

Means for Solving the Problems

[0005] According to the present disclosure, a crystalline molecular sieve having increased acid sites, designated SSZ-117x, was synthesized using N,N,N,3,5-pentamethyladamantan-1-ammonium cation as a structure directing agent (SDA). The synthesis was carried out via a boron route, and the final molecular sieve contains some boron. In one embodiment, the amount of boron can range from 50 to 250 ppm.

[0006] This SSZ-117x molecular sieve, having increased acid sites and thus increased acidity, can have a chemical composition including the following molar relationships.

Table 1

[0007] In one embodiment, a method for synthesizing a molecular sieve having an increased acidity as described herein is provided. The method includes (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, and (b) then subjecting the reaction mixture to crystallization conditions sufficient for the reaction mixture to form crystals of an SSZ-117x boron molecular sieve.

[0008] The boron-containing molecular sieve is then treated to remove the structure directing agent (SDA) referred to as Q above. The SDA can be removed, for example, by calcination or by ozonation at 150 °C. It has also been found that the SDA can be removed by treating the molecular sieve with dimethylformamide.

[0009] Once the SDA is removed, the boron-containing SSZ-117x molecular sieve is treated to replace the boron in the framework with aluminum. The molecular sieve having increased acid sites is then recovered. The molecular sieve is SSZ-117x rich in acid sites.

[0010] In yet a further aspect, a process for converting a raw material containing an organic compound to a conversion product is provided, the process including contacting the raw material in organic compound conversion conditions with a catalyst comprising an SSZ-117x molecular sieve having an increased acid site as described herein.

[0011] Among other factors, the present process can provide an SSZ-117x molecular sieve with increased acid sites. By increased acid sites is meant that an SSZ-117x molecular sieve can be obtained with more acid sites than would be possible by preparing the molecular sieve in the conventional manner in a simple way having aluminum sites and no boron sites by using the present process together with its boron route. When the conventional route is utilized, it has been found that some amorphous phase occurs and a decrease in Al acid sites is experienced. Most surprisingly, it has been found that by first inserting boron into the framework and then replacing boron with aluminum, an SSZ-117x molecular sieve with a relatively increased number of acid sites can be obtained. Therefore, the SSZ-117x molecular sieve is acid-rich or has an increased acidity. The increased acid sites can result in improved catalytic properties of the present SSZ-117x molecular sieve. The present SSZ-117x molecular sieve also contains some boron.

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 "zeolite" generally refers to a synthetic aluminosilicate molecular sieve having a framework composed of alumina and silica (i.e., repeating SiO 4 and AlO 4 tetrahedral units).

[0014] The term "aluminogermanosilicate" refers to a crystalline microporous solid that contains aluminum, germanium, and silicon oxide within its framework structure. Aluminogermanosilicates may be either "pure aluminogermanosilicates" (i.e., without other detectable metal oxides along with their framework structure) or optionally substituted. When described as "optionally substituted", each framework may contain other atoms (e.g., B, Ga, In, Fe, Ti, Zr) that replace one or more of the atoms that are not yet present in the parent framework.

[0015] 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.

[0016] As used herein, the term "anhydrous" refers to a molecular sieve that is substantially free of both physically adsorbed and chemisorbed water.

[0017] As used herein, the group numbering scheme of the periodic table is as disclosed in Chem. Eng. News 1985, 63(5), 26 - 27.

[0018] "Increased" or "more" acid sites means that the SSZ-117x molecular sieve prepared by the present process contains more acid sites than would be possible by preparing the molecular sieve conventionally without using this boron route. When a conventional simple method using aluminum is utilized, it has been found that an amorphous phase is generated, causing a decrease in the Al acid sites. Extremely surprisingly, by first inserting boron into the SSZ-117x framework and then replacing the boron with aluminum, an SSZ-117x molecular sieve having a relatively larger number of aluminum acid sites than would be obtained if boron were not introduced into the initial preparation of the molecular sieve has been found. This increased acidity affects the catalytic properties of the molecular sieve and can be improved. The molecular sieve will be extremely useful, for example, in converting raw materials containing organic compounds into products. Due to the boron route, some boron remains within the SSZ-117x molecular sieve.

[0019] Synthesis of Molecular Sieve This molecular sieve SSZ-117x is synthesized using a boron route. The process includes (a) providing a reaction mixture including (1) a silicon oxide source such as a 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. In one embodiment, the FAU framework zeolite has very little Al 2 O 3 and only has. SiO 2 / Al 2 O 3 The ratio can be 300 or more. Therefore, the framework contains a predominant amount of boron.

[0020] SDA is removed from the molecular sieve, for example, by either calcination or ozonation treatment, and then the molecular sieve is treated to replace at least a part, if not most, of the boron sites with aluminum. Then, the SSZ-117x molecular sieve with increased acid sites can be recovered.

[0021] The reaction mixture has a composition with respect to the molar ratios within the ranges described in Table 2: [Table 2] (wherein T and Q are as described above herein) may be included.

[0022] Suitable sources of silicon oxide may include any suitable known sources 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 SiO 2 / Al 2 O 3 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 SiO 2 / Al 2 O 3 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.

[0023] Sources of germanium may include germanium oxide and germanium alkoxides (e.g., germanium ethoxide, germanium isopropoxide).

[0024] Silicon and germanium have a SiO 2 / GeO 2It can be present in the reaction mixture in molar ratio.

[0025] The source of boron can include boric acid, which is preferred. Other suitable sources can be used, but are not preferred.

[0026] The source of fluoride ions can include, for example, hydrogen fluoride, ammonium fluoride, and ammonium bifluoride.

[0027] Boron-containing SSZ-117x has the following structure (1):

Chemical formula

[0028] 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).

[0029] The reaction mixture can 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 obtained product by promoting the nucleation and / or formation of boron SSZ-117x over undesirable phases.

[0030] It is noted that the reaction mixture components can be supplied by 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.

[0031] The reaction mixture can be prepared either batchwise or continuously, and the crystal size, morphology, and crystallization time of the molecular sieves described herein can vary depending on the nature of the reaction mixture and the crystallization conditions.

[0032] Crystallization and synthetic post-treatment In line with the boron route, crystallization of the molecular sieve from the above reaction mixture can be carried out under static, rotating, or stirring conditions, in a suitable reactor vessel (e.g., a polypropylene jar or a Teflon(trademark)-processed or stainless-steel autoclave), at a temperature of 125 °C to 200 °C (e.g., 150 °C to 170 °C), 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.

[0033] When molecular sieve crystals containing boron are 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 step 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 step can be carried out either under vacuum or at atmospheric pressure.

[0034] 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.

[0035] The 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.

[0036] Alternatively, or in addition, 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.

[0037] The molecular sieve crystals can then be treated to replace at least some, preferably almost all (at least 90%) but not all of the boron with aluminum. In one embodiment, the amount of boron remaining after the exchange procedure can be an amount in the range of 50 to 250 ppm boron. For example, conventional techniques by ion exchange can be used. However, treating the molecular sieve with an aqueous solution of aluminum nitrate is a preferred way to replace boron in the framework with aluminum. The treatment can be carried out by contacting the molecular sieve with a refluxing aluminum nitrate solution.

[0038] Characterization of the Molecular Sieve The final SSZ-117x molecular sieve has the following molar relationship: Al 2 O 3 :(n)TO 2 (where n is ≥ 150; T is a tetravalent element containing silicon and germanium) has a composition. In one embodiment, n in the above relationship is 300 or more, and in one embodiment, it is in the range of 300 to 600.

[0039] The molecular sieve has the following molar relationships as described in Table 1: **Table 1** (where T is a tetravalent element consisting of silicon and germanium) may have a chemical composition. This SSZ-117x also has relatively increased acid sites and some boron in the framework. SiO 2 / GeO 2 The ratio can also be in the range of 4 to 12, or in one embodiment, 7 to 10.

[0040] The SSZ-117x with increased acid has the following peaks: **Table 3** will have a powder XRD diffraction pattern including. As understood by those skilled in the art, the measurement of the parameter 2-theta (2θ) is subject to both human error and mechanical error, and together they can give an uncertainty of about ±0.30° to each reported value of 2-theta. The relative intensity (100×I / I o ) is recorded as the ratio of the peak intensity to the intensity of the strongest peak designated as the value of 100. The relative intensity of the d-spacing is indicated by the notations VS, S, M, and W, representing very strong, strong, medium, and weak, respectively. Regarding the relative intensity, the above names are as follows: W (weak) is less than 20; M (medium) is greater than 20 and less than 40; S (strong) is from 40 to less than 60; VS (very strong) is 60. When the intensity is close to the endpoint of a certain range, the intensity can be characterized as being within that range. For example, an intensity of 18 - 22 can be listed as W - M. However, due to the variation in the intensity of the lines, as is known in the art, one or more lines can have intensities in the adjacent ranges.

[0041] The powder X-ray diffraction patterns presented in this specification 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 intensity of the peaks (adjusted with respect to the background), and the lattice plane spacing d corresponding to the recorded lines could be calculated.

[0042] 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.

[0043] The increased acidity of this molecular sieve can be measured, for example, by measuring its Brønsted acidity.

[0044] Adsorption and Catalysis This molecular sieve SSZ-117x (where some or all of the Q+ has been removed) can be used as an adsorbent or as a catalyst to catalyze a variety of organic compound conversion processes, including many that currently have commercial / industrial importance. Examples of chemical conversion processes effectively catalyzed by acid-rich SSZ-117x alone or in combination with one or more other catalytically active substances, including other crystalline catalysts, are those that have acid activity or require a catalytic metal. Examples of organic conversion processes that can be catalyzed by acid-rich SSZ-117x include cracking, hydrocracking, disproportionation, alkylation, oligomerization, aromatization, and isomerization. The molecular sieve can also be used when exchanging heavy metals such as copper, which can be useful in reducing nitrous oxide pollutants.

[0045] As with many catalysts, it may be desirable to combine acid-rich SSZ-117x with another material that is resistant to temperature and other conditions utilized in the organic conversion process. Such materials include active and inert materials, as well as synthetic or naturally occurring zeolites and inorganic materials such as clays, silica, and / or metal oxides such as alumina. The latter may be naturally occurring or in the form of gelatinous precipitates or gels containing mixtures of silica and metal oxides. The use of materials combined with active acid-rich SSZ-117x (i.e., combined with the new material or present during its synthesis) tends to change the conversion rate and / or selectivity of the catalyst in a particular organic conversion process. Inert materials preferably act as diluents that control the amount of conversion in a given process so that products can be obtained in an economical and orderly manner without using other means to control the reaction rate. These materials can be incorporated into naturally occurring clays (e.g., bentonite and kaolin) to improve the crushing strength of the catalyst under commercial operating conditions. These materials (i.e., clays, oxides, etc.) function as binders for the catalyst. In commercial use, it is desirable to prevent the disintegration of the catalyst into a powdered material, so it is desirable to provide a catalyst with good crushing strength. These clay and / or oxide binders have typically been utilized only for the purpose of improving the crushing strength of the catalyst.

[0046] Naturally occurring clays that can be complexed with SSZ-117x include the montmorillonite and kaolin families, which include sub-bentonite, and kaolins or the major mineral constituents commonly known as Dixie, McNamee, Georgia, and Florida clays, and others where the halloysite, kaolinite, dickite, nacrite, or anauxite. Such clays can be used as-mined in their raw state or first subjected to calcination, acid treatment, or chemical modification. Binders useful for complexing with this acid-rich SSZ-117x also include inorganic oxides such as silica, zirconia, titania, magnesia, beryllia, alumina, and mixtures thereof.

[0047] In addition to the above materials, acid-rich SSZ-117x can be combined with porous matrix materials such as silica-alumina, silica-magnesia, silica-zirconia, silica-thoria, silica-beryllia, silica-titania, and ternary compositions such as silica-alumina-thoria, silica-alumina-zirconia, silica-alumina-magnesia, and silica-magnesia-zirconia.

[0048] The relative ratios of acid-rich SSZ-117x to the inorganic oxide matrix can vary widely, and the SSZ-117x content ranges from 1 to 90 wt% (e.g., 2 to 80 wt%) of the composite.

Examples

[0049] The following examples are intended to be non-limiting.

[0050] (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 3-fold excess methyl iodide and 2 equivalents of potassium hydrogen carbonate in methanol for 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.

[0051] The resulting iodide salt was exchanged with 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.

[0052] (Example 2) Synthesis of SSZ-117x with Boron Into a tared 23 mL Parr reactor, 0.27 g of Tosoh Corporation's 390HUA Y-zeolite (approx. 500 SiO 2 / Al 2 O 3 molar ratio), 0.05 g of GeO 2 , 0.02 g of H 3 BO 3 , and 2.5 millimoles of an aqueous solution of N,N,N,3,5-pentamethyladamantan-1-ammonium hydroxide were added. Then, the reactor was placed in an exhaust hood and water was evaporated to make the H 2 O / (SiO 2 +GeO 2 ) molar ratio 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.

[0053] Powder XRD will show that the final product is a new phase in pure form called SSZ-117x boron and exhibits the characteristic peaks in Table 3.

[0054] (Example 3) SSZ117x with Increased Acid When all or part of the SDA was removed by either calcination or ozone treatment and then the recovered product was treated with an aqueous solution of aluminum nitrate while refluxing, a final SSZ-117x product with increased acid sites was obtained, and the product also contained some boron.

[0055] (Example 4) Bronsted Acidity The Brønsted acidity of the molecular sieve of Example 3 was measured by temperature-programmed desorption (TPD) of n-propylamine, which was modified from the published descriptions by T.J. Gricus Kofke et al. (J. Catal. 1988, 114, 34 - 45); T.J. Gricus Kofke et al. (J. Catal. 1989, 115, 265 - 272); and J.G. Tittensor et al. (J. Catal. 1992, 138, 714 - 720). The sample was pretreated in a dry H 2 flow at 400 °C to 500 °C for 1 hour. Then, the dehydrated sample was cooled to 120 °C in a dry helium flow and maintained for adsorption in a helium flow saturated with n-propylamine at 120 °C for 30 minutes. Next, the n-propylamine-saturated sample was heated in a dry helium flow at a rate of 10 °C / min up to 500 °C. The Brønsted acidity was calculated based on the weight loss with respect to temperature by thermogravimetric analysis (TGA) and the effluent NH 3 and propene by mass spectrometry. The sample had a Brønsted acidity of 77.72 μmol / g, indicating that the aluminum sites were incorporated within the framework of the molecular sieve.

[0056] (Example 5) The as-synthesized boron SSZ-117x of Example 2 was heated in an excess of 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% in this extraction. Then, the dried solid was subjected to ozonolysis at 150 °C overnight to remove all the residual SDA in the pores. The opened structure now had a significantly changed XRD pattern as shown in Table 3.

Table 3

[0057] Next, the ozonated product can be treated to replace boron with aluminum, for example, by refluxing with an aqueous solution of aluminum nitrate. The resulting molecular sieve is SSZ-117x having boron and increased acid sites.

[0058] As used herein, the term "comprises" or "comprising" is intended to be a non-limiting transition that means the inclusion of the recited elements but does 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 transition that means the exclusion of all except the recited elements, except for trace impurities.

[0059] 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 merely included herein 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 actually departing from the spirit and scope of the invention as defined by the appended claims.

Claims

1. A molecular sieve having a powder X-ray diffraction pattern comprising the following peaks: 【Table A】 and containing boron and having increased acid sites.

2. A molecular sieve according to claim 1, having a composition comprising the following molar relationship: Al ２ O ３ :(n)TO ２ (wherein n is ≥ 150; 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: Al ２ O ３ :(n) TO ２ (wherein n is ≥ 300; and T is a tetravalent element including silicon and germanium).

4. A molecular sieve according to claim 1, having a chemical composition comprising the following molar relationship: 【Table B】 (wherein T is a tetravalent element including silicon and germanium).

5. The molecular sieve according to claim 1, wherein the amount of boron in the molecular sieve is in the range of 50 to 250 ppm.

6. A method for synthesizing the molecular sieve according to claim 1, comprising: (a) providing a reaction mixture comprising: (1) FAU framework type zeolite having an SiO ２ / Al ２ O ３ molar ratio of 300 or more; ２ / Al ２ O ３ and a molar ratio of; (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 boron-containing molecular sieve; (c) removing Q from the molecular sieve framework; and (d) replacing a part of the boron in the molecular sieve crystals with aluminum. The above method.

7. The method according to claim 6, wherein the reaction mixture has a composition with respect to molar ratios as follows: 【Table C】 (wherein T is a tetravalent element including silicon and germanium).

8. The method according to claim 6, wherein the reaction mixture has a composition with respect to molar ratios as follows: 【Table D】 (wherein T is a tetravalent element including silicon and germanium).

9. The method according to claim 6, wherein the FAU framework type zeolite is zeolite Y or a post-synthetic modified form.

10. The method according to claim 6, wherein the crystallization conditions include a temperature of 125°C to 200°C.

11. The method according to claim 6, wherein the reaction mixture has a Q / F molar ratio in the range of 0.8 to 1.

2.

12. The method according to claim 6, wherein the Q is removed by calcination.

13. The method according to claim 6, wherein Q is removed by treatment with ozone.

14. The method according to claim 6, wherein replacing boron with aluminum comprises refluxing the molecular sieve crystal together with a solution of aluminum nitrate.

15. 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 1 under organic compound conversion conditions.

16. 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 4 under organic compound conversion conditions.

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 1.

18. 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.

19. A product prepared by the method according to claim 6.

20. A product prepared by the method according to claim 14.

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