Composition, synthesis and uses of EMM-73 molecular sieve

Abstract

A molecular sieve (designated EMM-73 and characterized by a unique powder XRD pattern), a method for producing such a molecular sieve, and uses of such a molecular sieve.

Description

[Technical field]

[0001] (CROSS REFERENCE TO RELATED APPLICATIONS) This application claims priority to and the benefit of U.S. Provisional Application No. 63 / 316293, filed March 3, 2022, the entire contents of which are incorporated herein by reference.

[0002] (Technical field) The present disclosure relates to compositions of molecular sieves, methods of making molecular sieves, and uses of molecular sieves. [Background technology]

[0003] BACKGROUND OF THEINVENTION Molecular sieve materials, whether natural or synthetic, can be used as adsorbents and can have catalytic properties in reactions for the conversion of hydrocarbons. Certain molecular sieves, e.g., zeolites, AlPO, and mesoporous materials, are ordered, porous, crystalline materials that have a well-defined crystal structure as determined by X-ray diffraction (XRD). A particular molecular sieve gives rise to an orderly and specific recognizable (or distinguishable or identifiable or identifiable) XRD pattern. Within a particular molecular sieve material, there may be a number of cavities (or voids or void spaces) which may be connected (or joined or linked or interconnected) to one another by a number of channels or pores (or holes or pores). Such cavities and pores are uniform in size (or dimension or size) within a particular molecular sieve material. Because the dimensions of the pores are such that, for example, they accept adsorbed molecules having certain dimensions while rejecting molecules having larger dimensions, such materials have come to be known as "molecular sieves" and are used in a variety of industrial processes (e.g., cracking, hydrocracking, disproportionation, alkylation, oligomerization, and isomerization).

[0004] Molecular sieves find use in catalysis and adsorption. Molecular sieves include both natural and synthetic crystalline molecular sieves. Examples of such molecular sieves include extra large pore zeolites, large pore zeolites, medium pore size zeolites, and small pore zeolites. Such zeolites and their isotypes have been classified by the Structure Commission of the International Zeolite Association according to the rules of the IUPAC Commission on Zeolite Nomenclature. By this classification, framework-type zeolites and other crystalline, microporous molecular sieves have been assigned three-letter codes (and therefore structures established) and are described in the following literature: "Atlas of Zeolite Framework Types," eds., Ch. Baerlocher, LB McCusker, and DH Olson, Elsevier, 6th ed., 2007, which is incorporated by reference into this disclosure. Such zeolites and their isotypes are also described below. http: / / america.iza-structure.org / IZA-SC / ftc_table.php.

[0005] The idealized inorganic framework structure of a zeolite is a silicate framework in which every tetrahedral atom is connected to the four next nearest tetrahedral atoms by oxygen atoms. The term "silicate" as used herein means a material that contains at least silicon atoms and oxygen atoms, the silicon atoms and the oxygen atoms being alternately bonded to each other (i.e., -O-Si-O-Si-), and optionally other atoms, such as boron, aluminum or other metals, such as transition metals, such as titanium, vanadium or zinc. In framework silicates, atoms other than silicon and oxygen occupy some of the lattice sites (or lattice sites), otherwise occupied by silicon atoms (or silica atoms), in "all-silica" framework silicates. Thus, the term "framework silicate" as used in this disclosure means a lattice of atoms (or atomic lattice) including any of silicate, borosilicate, gallosilicate, ferrisilicate, aluminosilicate, titanosilicate, zincosilicate, vanadosilicate, and the like.

[0006] In a given zeolite, the structure of the framework silicates determines the size (or magnitude or dimension) of the pores (or holes or pores) or channels present therein. The size (or size or dimension) of the pores (or holes or pores) or channels can determine the type (or type) of process (or step or method) for which a given zeolite is applicable (or adaptable or applicable). Currently, over 200 unique zeolite framework silicate structures are known. Such structures have been recognized by the Structure Commission of the International Zeolite Association, thereby defining a range of pore geometries and orientations.

[0007] Zeolite or molecular sieve framework silicates are commonly characterized with respect to their ring size, meaning the number of silicon atoms (or alternative atoms, such as those listed above) arranged tetrahedrally with oxygen atoms as loops that define pores or channels within the zeolite. For example, an "8-ring" zeolite means a zeolite having pores or channels defined by eight alternating tetrahedral atoms and eight oxygen atoms in a loop. The pores or channels defined in a given zeolite may be symmetric or asymmetric, depending on the various structural constraints present in the particular framework silicate.

[0008] Zeolites can be classified as having small pore, medium pore, large pore, and extra-large pore structures (which are structures with pore windows defined by 8, 10, 12, and more than 12 T-atoms, respectively). Extra-large pore zeolites (>12R) include, for example, AET (14R, e.g., ALPO-8), SFN (14R, e.g., SSZ-59), VFI (18R, e.g., VPI-5), CLO (20R, cloverite) and ITV (30R, ITQ-37) framework-type zeolites. Extra-large pore zeolites generally have a free pore size (or diameter or diameter) greater than about 0.8 nm. Large pore zeolites (12R) include, for example, LTL, MAZ, FAU, EMT, OFF, *BEA, MOR, and SFS framework type zeolites (e.g., mazzite, offretite, zeolite L, zeolite Y, zeolite X, omega (Ω), ZSM-2, zeolite T, beta (Β), and SSZ-56). Large pore zeolites generally have a free pore size (or diameter or diameter) of 0.6 to 0.8 nm. Medium (or intermediate) pore size zeolites (10R) include, for example, MFI, MEL, EUO, MTT, MFS, AEL, AFO, HEU, FER, MWW and TON framework type zeolites (e.g., ZSM-5, ZSM-11, ZSM-22, MCM-22, silicalite-1 and silicalite-2). Medium pore size zeolites generally have a free pore size (or diameter) (or free pore diameter) of 0.45 to 0.6 nm. Small pore size zeolites (8R) include, for example, CHA, RTH, ERI, KFI, LEV and LTA framework type zeolites (e.g., ZK-4, SAPO-34, SAPO-35, ZK-14, SAPO-42, ZK-21, ZK-22, ZK-5, ZK-20, zeolite A, chabazite and ALPO-17). Small pore size zeolites generally have a free pore size (or diameter or diameter) of 0.3 to 0.45 nm.

[0009] The synthesis of molecular sieve materials typically involves hydrothermal crystallization from a synthesis mixture that contains sources of all the elements present in the molecular sieve (e.g., a source of alumina as well as a source of silica). In many cases a structure directing agent (SDA) is also present. A structure directing agent is a compound that is believed to facilitate the formation of a molecular sieve, such a compound is believed to act as a template around which a particular molecular sieve structure can be formed, thereby facilitating the formation of a desired molecular sieve. A variety of compounds have been used as structure directing agents, including those containing various types of quaternary ammonium cations. Typically, molecular sieve (or zeolite) crystals form around a structure directing agent that occupies the pores in the molecular sieve once crystallization is complete. Thus, the "as-synthesized" molecular sieve contains a structure directing agent within its pores. Therefore, after crystallization, the "as-synthesized" (or "as-made") molecular sieves are typically subjected to a treatment step, such as a calcination step, to remove such structure directing agents.

[0010] For example, US2006 / 0292071 and US2007 / 0034549 disclose the preparation of the plate-like borosilicate molecular sieve SSZ-56 using a trans-fused N,N-diethyl-2-methyldecahydroquinolinium cation as the structure directing agent, while US2020 / 0062605 discloses the use of a benzyltributylammonium cation. US2013 / 0330272 discloses the preparation of a needle-like aluminosilicate molecular sieve, SSZ-56, using 1-butyl-1-(3,3,5-trimethylcyclohexyl)piperidinium cation as the structure directing agent. Summary of the Invention [Problem to be solved by the invention]

[0011] Although many different molecular sieves have been discovered, there is a continuing need for new molecular sieves (or zeolites) that have desirable characteristics (or properties) for gas separation and drying, organic conversion reactions, and other uses (or applications). New molecular sieves may contain new internal pore structures (or internal pore configurations or internal pore architectures) that may improve selectivity in such processes. It is also important to identify new structure directing agents and more efficient methods for synthesizing molecular sieves, thereby facilitating the preparation of new molecular sieves and / or reducing the cost of producing known molecular sieves. [Means for solving the problem]

[0012] (Abstract) The present disclosure relates to molecular sieves, methods for making molecular sieves, and uses of molecular sieves.

[0013] In a first aspect, the present disclosure relates to a molecular sieve having an X-ray diffraction pattern that, in its as-calcined form (e.g., having at least a portion of the SDA removed), comprises the peaks (2θ(°)) set out in Table 1 below.

[0014] [Table 1]

[0015] In a second aspect, the present disclosure relates to a molecular sieve having an X-ray diffraction pattern that, in its as-synthesized form (e.g., without SDA removal), comprises the peaks (2θ(°)) set forth in Table 2 below.

[0016] [Table 2]

[0017] In a third aspect, the present disclosure relates to a method for producing a molecular sieve, in particular a method for producing the molecular sieve of the first and / or second aspect, the method comprising the steps of: (a) A process (or step) for preparing (or producing or preparing or preparing) a synthetic mixture (or synthetic mixture or synthesis mixture or synthesis mixture), such synthetic mixture comprising the following components: water, a source of an oxide of a tetravalent element (Y); a source of an oxide of a trivalent element (X); Structure-directing agents (Q), Optionally, a source of hydroxide ions (OH), and Optionally, a source of alkali metal and / or alkaline earth metal elements (M) In the method, the structure directing agent (Q) comprises at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of formula I below and the benzimidazolium cation of formula II below:

[0018] [ka] (Formula I)

[0019] [ka] (Formula II)

[0020] During the ceremony, R and R' are the same or different, preferably the same. R and R' are selected from n-propyl and n-butyl. R'' is selected from methyl and ethyl, preferably methyl. (b) heating the synthesis mixture under crystallization conditions, such crystallization conditions comprising a temperature of 100-200° C. for a time sufficient to form crystals of the molecular sieve; (c) recovering at least a portion of the molecular sieve from step (b). (d) Optionally, treating the molecular sieve recovered in step (c) to remove at least a portion of the structure directing agent (Q).

[0021] In a fourth aspect, the present disclosure relates to a process for converting an organic compound to a transformation product, the process comprising contacting the organic compound with a molecular sieve according to the first or second aspect of the present disclosure or a molecular sieve prepared according to the process of the third aspect of the present disclosure.

[0022] These and other features and characteristics of the present disclosure and its advantageous applications and / or uses will become apparent from the following detailed description. Of course, it will be appreciated that features described in relation to one embodiment of the invention may be incorporated in other embodiments of the invention. In particular, any two or more of the features described in the specification of this application are included in this Summary, which may be taken together to form a combination of features, even if such combination is not specifically described in this disclosure. [Brief description of the drawings]

[0023] [Figure 1] FIG. 1 shows the powder XRD pattern of the as-synthesized (or post-synthesized) (or as-synthesized) product of Example 2. [Diagram 2] FIG. 2 shows the powder XRD pattern of the as-calcined (or calcined) (or as-calcined) product of Example 2. [Diagram 3] FIG. 3 shows the structure of EMM-73 (projections (or projections or plan views) in the

[0010] -12MR / b direction (left) and in the

[0001] -10MR / c direction (right)) [shown simply with oxygen atoms omitted]. [Figure 4] FIG. 4 shows an SEM image of the as-synthesized (or post-synthesized) (or as-synthesized) product of Example 2. [Diagram 5] FIG. 5 focuses on the first five XRD peaks (the as-calcined (or calcined) (or as-calcined) product of Example 2). [Figure 6] FIG. 6 shows an SEM image of the as-synthesized (or post-synthesized) (or as-synthesized) product of Example 6. [Figure 7] FIG. 7 shows an SEM image of the as-synthesized (or post-synthesized) (or as-synthesized) product of Example 9. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0024] (Detailed Description) The present disclosure relates to compositions of molecular sieves, methods of making molecular sieves, and uses of molecular sieves. The molecular sieve may be referred to as EMM-73 molecular sieve, or EMM-73 zeolite, or EMM-73 material.

[0025] In a first aspect, the present disclosure relates to a molecular sieve which, in its as-calcined (or calcined) form (e.g., having at least a portion of the SDA removed by heat or other treatment), has an X-ray diffraction pattern comprising the peaks set forth in Table 1 below.

[0026] [Table 3]

[0027] In a further embodiment, the molecular sieve may have an X-ray diffraction pattern in its as-calcined form, comprising the peaks shown in Table 1A below. In Table 1A, the values ​​of d-spacing have deviations. Such deviations are determined based on a corresponding deviation of ±0.20(2θ(°)), which are then converted to corresponding values ​​of d-spacing using Bragg's law.

[0028] [Table 4]

[0029] The XRD pattern has XRD peaks, which in this disclosure are described using Cu(Kα) radiation.

[0030] In one or more further embodiments, the molecular sieve, in its as-calcined (or calcined) form, may have a micropore volume (or micropore capacity or micropore volume or micropore volume) of 0.05 to 0.3, such as 0.1 to 0.25, for example 0.22 cc / g.

[0031] In one or more further embodiments, the molecular sieve, in its calcined form, has a micropore surface area of ​​100 to 800 m. 2 / g, e.g. 300-600m 2 / g, e.g. 573m 2 / g, and / or the external surface area is between 5 and 200 m 2 / g, e.g. 10-100m 2 / g, e.g. 13m 2 / g.

[0032] In one or more further embodiments, the molecular sieve, in its as-calcined form (or calcined form), may, as appropriate, be represented by the molecular formula of Formula III below: (m)X2O3:YO2 (Formula III) [In the formula, 0.005≦m≦0.1, X is a trivalent element, Y is a tetravalent element. Y may include one or more of Si, Ti, and Ge. For example, Y may include or be Si. X may include one or more of Al, B, Fe, or Ga. In particular, X may include or be Al and / or B. For example, X may include or be Al. In some embodiments, when Y is Si and X is Al, such molecular sieves are aluminosilicates. In some embodiments, when Y is Si and X is B, such molecular sieves are borosilicates. The oxygen atom in formula III may be replaced by a carbon atom (e.g., in the form of CH2), such carbon atom may be derived from the source of the ingredient (or component) used to prepare (or manufacture) the molecular sieve (as-produced (or post-produced)). Also, the oxygen atom of formula III may be replaced with a nitrogen atom (eg, after SDA is removed). Formula III may represent the framework (as defined in this disclosure) of a typical molecular sieve, and does not correspond to a representation of such a molecular sieve alone (or solo) in its calcined form (or calcined form). Such molecular sieves, in their as-calcined form, may contain SDA and / or impurities (after appropriate treatment to remove SDA and impurities). Such SDA and / or impurities are not accounted for in formula III. Furthermore, Formula III does not include protons and charges (protons and charges compensating ions that may be present on the molecular sieve upon (or after) calcination).

[0033] The variable m represents the molar ratio relationship of X2O3 / YO2 in formula III. For example, when m is 0.025, the molar ratio of YO2 / X2O3 is 40 and the molar ratio of Y / X is 20 (eg, the molar ratio of Si / Al is 20). m may vary from 0.005 to 0.1 (e.g. at least 0.005, or at least 0.007, or at least 0.01 to up to 0.1, or up to 0.07, or up to 0.05, e.g., 0.01 to 0.05 or 0.01 to 0.025). The molar ratio of Y / X may be from 5 to 100 (e.g., at least 5, or at least 7, or at least 10, or at least 15, up to 100, or up to 75, or up to 50, e.g., 10-50 or 15-50).

[0034] In a second aspect, the present disclosure relates to a molecular sieve, in particular a molecular sieve as defined in the first aspect, which molecular sieve, in its as-synthesized form (e.g., without SDA removed), has an X-ray diffraction pattern comprising the peaks (2θ(°)) set out in Table 2 below.

[0035] [Table 5]

[0036] In a further embodiment, the molecular sieve described above, in its as-synthesized form (or post-synthesized form), may have an X-ray diffraction pattern comprising the peaks shown in Table 2A below. In Table 2A, the values ​​of the distance d (or d-spacing) have deviations. Such deviations are determined based on a corresponding deviation of ±0.20 (2θ(°)). Then, Bragg's law is used to convert the values ​​of the distance d (d-spacing) to the corresponding values.

[0037] [Table 6]

[0038] The XRD patterns with XRD peaks described in this disclosure use Cu(Kα) radiation.

[0039] In one or more further embodiments, the molecular sieve, in its as-synthesized form (or post-synthesized form), may be represented by the molecular formula of Formula IV, as appropriate: (q)Q:(m)X2O3:YO2 (Formula IV) [In the formula, 0 <q≦0.7であり、 0.005≦m≦0.1, Q comprises at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of Formula I and the benzimidazolium cation of Formula II.

[0040] [ka] (Formula I)

[0041] [ka] (Formula II)

[0042] During the ceremony, R and R' are the same or different, preferably the same, and R and R' are selected from n-propyl and n-butyl. R'' is selected from methyl and ethyl, preferably methyl. X is a trivalent element (as defined in formula III). Y is a tetravalent element (as defined in formula III). Formula IV may represent a typical molecular sieve framework as defined in this disclosure, in its as-synthesized form (and thus including the structure directing agent (Q)) (not intended to represent such material alone). The molecular sieve may contain impurities in its as-synthesized form. Such impurities are not accounted for in Formula IV. Additionally, Formula IV does not include protons and charges that compensate for ions that may be present on the as-synthesized molecular sieve.

[0043] The variable m represents the molar ratio relationship of X2O3 / YO2 in formula IV. The value of the variable m in formula IV is the same as that described in this disclosure for formula III.

[0044] The variable q represents the molar relationship of Q / YO2 in formula IV. For example, when q is 0.1, the molar ratio of Q / YO2 is 0.1. The molar ratio of Q / YO2 may be 0 (greater than zero) to 0.7, for example, 0.1 to 0.6, for example, 0.1 to 0.4.

[0045] In a further embodiment, the framework structure (or skeletal structure or framework structure or framework structure) of the molecular sieve of the first and / or second aspect of the present disclosure (in its as-synthesized form or in its as-calcined form) may be identified (or assigned or identified) as being of the SFS framework type. In particular, the framework structure of the molecular sieve of the present disclosure may be identified as having a two-dimensional channel system in which 10-ring pores intersect with 12-ring pores (12MR×10MR zeolite) with dimensions of 8.4±0.20 Å×5.8±0.20 Å and 5.5±0.20 Å×5.1±0.20 Å.

[0046] In yet further embodiments, at least a portion of the crystals of the molecular sieve of the present disclosure may have either an as-synthesized form or an as-calcined form, and may have a square-like morphology (or morphology) (or a roughly square or roughly rectangular morphology or a rectangular-like morphology). "At least a portion" of the molecular sieve crystals may have a square (or rectangular)-like morphology (or morphology) (or approximately square (or approximately rectangular) morphology (or morphology) or rectangular-like morphology) means that at least about 50% (e.g., at least 60%, at least 75%, or at least 85%) of the molecular sieve crystals can have a square (or rectangular)-like morphology (or morphology) (or approximately square (or approximately rectangular) morphology (or morphology) or rectangular-like morphology). By "rectangular-like morphology" is meant that the crystal is substantially rectangular parallelepiped (or rectangular prism or rectangular cuboid) in shape or form. That is, parallelepiped means a shape in which all six faces are substantially rectangular (or rectangular) in shape, in particular having one long dimension and two short dimensions. Here, one longer dimension can be referred to as the length (l) of the square (or rectangular) parallelepiped (i.e., the longest side of the largest face). The two shorter dimensions can be referred to as the width (w) and height (h) of the square (or rectangular) parallelepiped (i.e., the largest dimension of the particle perpendicular to the length (l), respectively). The morphology and percentage (vol%) of crystals having such morphologies can be determined by image analysis (e.g., scanning electron microscopy (SEM) micrographs (e.g., using ImageJ software)).

[0047] Molecular sieve crystals having a square (or rectangular)-like morphology (or nearly square (or nearly rectangular) morphology or rectangular-like morphology) according to the present disclosure may typically have a length (or length) (l) / width (or width) (w) ratio of 1 to less than 10 (e.g., 1 to 6, e.g., 2 to 3) and a length (or length) (l) / height (or height) (h) ratio of 1 to less than 10 (e.g., 1 to 6, e.g., 2 to 3). The width (w) / height (h) ratio may vary from 1 to 3 (eg, 1 to 2). In a specific embodiment, the molecular sieve is an aluminosilicate and the length (l) of the molecular sieve crystallites is between 0.1 and 2 μm (or microns). In another specific embodiment, the molecular sieve is a borosilicate and the crystal length (l) of the molecular sieve is from 50 nm to less than 1 μm (or micron), preferably less than 500 nm, and more preferably less than 400 nm.

[0048] Rectangular-like morphologies are particularly advantageous in catalysis and adsorption applications as compared to plate-like, needle-like or rod-like morphologies. Indeed, the diffusion velocity (or diffusion rate) through the largest dimension of a zeolite catalyst is faster in rectangular-like particles due to their smaller aspect ratio (length / width and / or length / height). Additionally, needle-shaped or needle-like crystals have been produced, which have raised concerns about the health effects of inhalation over long periods of time.

[0049] Also, without wishing to be bound by theory, it is believed that in the crystals of the molecular sieves of the present disclosure having a rectangular-like morphology, the two short dimensions correspond to two short diffusion lengths, particularly the 12-ring pores in the a- and b-directions, and the one long dimension corresponds to one long diffusion length, particularly the 10-ring pore in the c-direction. Such a configuration is particularly advantageous because it results in faster diffusion of the molecules in the 12MR direction.

[0050] In a third aspect, the present disclosure relates to a method for producing a molecular sieve, in particular a method for producing a molecular sieve as defined in the first and / or second aspect of the present disclosure, the method comprising the following steps (or stages) (a) to (d): (a) A process (or step) for preparing (or producing or preparing or preparing) a synthetic mixture (or synthetic mixture or synthesis mixture or synthesis mixture), such synthetic mixture comprising the following components: water A source of oxide of a tetravalent element (Y) A source of an oxide of a trivalent element (X) Structure Directing Agents (Q) Optionally, a source of hydroxide ions (OH) Optionally, a source of alkali metal and / or alkaline earth metal elements (M) The structure directing agent (Q) comprises at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of formula I and the benzimidazolium cation of formula II.

[0051] [ka] (Formula I)

[0052] [ka] (Formula II)

[0053] During the ceremony, R and R' are the same or different, preferably the same. R and R' are selected from n-propyl and n-butyl. R'' is selected from methyl and ethyl, preferably methyl. (b) A process (or step) of heating a synthesis mixture (or synthesis mixture) under crystallization conditions, such conditions including a temperature of 100°C to 200°C for a time sufficient to form crystals of the molecular sieve. (c) recovering at least a portion of the molecular sieve from step (b); and (d) Optionally, treating the molecular sieve recovered in step (c) to remove at least a portion of the structure directing agent (Q).

[0054] The structure directing agent (Q) may be selected from the group consisting of the cations of formula I and / or formula II as defined above, in particular the 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation, the 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium cation, the 2-methyl-1,3-dipropylbenzimidazolium cation, the 2-methyl-1,3-di-n-butylbenzimidazolium cation, and mixtures thereof. The structure directing agent (Q) may be present in any suitable form. For example, it may be present as a halide, such as a fluoride, chloride, iodide, or bromide, as a hydroxide, or as a nitrate. For example, it may be present in the form of a hydroxide. A structure directing agent (Q) may be present in the synthesis mixture, the molar ratio of Q / Y may be from 0.05 to 1.0, such as at least 0.1, or at least 0.15, up to 0.8, or up to 0.7, or up to 0.6, such as from 0.1 to 0.8, or from 0.15 to 0.7, such as from 0.15 to 0.6.

[0055] The synthesis mixture includes at least one source of an oxide of a tetravalent element (Y) (eg, Si, Ti and / or Ge). Preferably, Y comprises Si. More preferably, Y is Si. Suitable sources of tetravalent element (Y) that can be used to prepare the synthesis mixture will depend on the element (Y) selected. In some embodiments, when Y is silicon, suitable sources of Si (e.g., sources of silicon oxide (or silicon oxide sources)) for use in the method include silicates, such as tetraalkylorthosilicates, such as tetramethylorthosilicate (TMOS) and tetraethylorthosilicate (TEOS), fumed silica, such as Examples include Aerosil® (available from Evonik), Cabosperse® (available from Cabot), and Cabosil® (available from DMS), precipitated silicas such as Ultrasil® and Sipernat® 340 (available from Evonik), alkali metal silicates such as potassium silicate and sodium silicate, and aqueous suspensions of colloidal silica such as those sold by EI du Pont de Nemours under the trade name Ludox® or those sold by Evonik under the trade name Aerodisp®. Preferred are silicates, fumed silicas, precipitated silicas, faujasite zeolites, alkali metal silicates, and colloidal silicas. In some embodiments, when Y is germanium, suitable sources of Ge include germanium oxide. In some embodiments, when Y is titanium, suitable sources of Ti include titanium dioxide and titanium tetraalkoxides, such as titanium(IV) tetraethoxide and titanium(IV) tetrachloride.

[0056] The synthesis mixture includes at least one source of an oxide of a trivalent element (X) (e.g., Al, B, F, and / or Ga). Preferably, X includes Al and / or B (e.g., Al). More preferably, X is Al and / or B (e.g., Al). Suitable sources of trivalent element (X) that can be used to prepare the synthetic mixture will depend on the element (X) selected. In some embodiments, when X is aluminum, suitable sources of Al (e.g., sources of aluminum oxide) for use in the method include aluminum hydroxide (or aluminum hydroxide), aluminum salts, particularly water-soluble salts, such as aluminum sulfate (or aluminum sulfate), aluminum nitrate (or aluminum nitrate), alkali metal aluminates, such as sodium aluminate (or sodium aluminate), and aluminum hydroxides (or aluminum alkoxides), such as aluminum isopropoxide, as well as hydrated aluminum oxides (or hydrous aluminum oxides or hydrated aluminum oxides), such as boehmite, gibbsite, and pseudoboehmite, and mixtures thereof. Other sources of aluminum include, but are not limited to, other water soluble aluminum salts, sodium aluminate, aluminum hydroxide, e.g., aluminum isopropoxide, or aluminum metal, e.g., aluminum in the form of chips. In particular, suitable sources of alumina are aluminum hydroxide (or aluminum hydroxide), water-soluble salts such as aluminum sulfate (or aluminum sulfate), aluminum nitrate (or aluminum nitrate), and alkali metal aluminates such as sodium aluminate (or sodium aluminate) and potassium aluminate (or potassium aluminate). In some embodiments, when X is boron, suitable sources of B include boric acid and borate salts, such as sodium tetraborate or borax and potassium tetraborate. Boron sources tend to be more suitable than aluminum sources in hydroxide-mediated synthesis systems.

[0057] Alternatively or in addition to the sources of Y and X mentioned above, sources containing both elements Y and X (e.g., sources of Si and Al) can also be used. Examples of suitable sources containing both Si and Al elements include amorphous silica-alumina gels or dried silica-alumina powders, silica-aluminas, clays such as kaolin, metakaolin, and zeolites, particularly aluminosilicates such as synthetic faujasite and ultrastable faujasite, e.g., Ultrastable Y (USY), beta (β) or other large to medium pore zeolites.

[0058] The molar ratio of Y / X in the synthesis mixture may be 5-100, such as 5-75, for example 10-50 or 15-50.

[0059] In a preferred embodiment, Y is Si. X is Al or B. Such molecular sieves are aluminosilicates or borosilicates.

[0060] Optionally, the synthesis mixture may include at least one source of hydroxide ions (OH). For example, hydroxide ions may be present as counter ions to the structure directing agent (Q), or may be present by using aluminum hydroxide or sodium aluminate as a source of Al. Also, a suitable source of hydroxide ions may be selected from the group consisting of alkali metal hydroxides, alkaline earth metal hydroxides, ammonium hydroxide, and mixtures thereof; for example, may be selected from the group consisting of sodium hydroxide, potassium hydroxide, lithium hydroxide, rubidium hydroxide, calcium hydroxide, magnesium hydroxide, ammonium hydroxide, and mixtures thereof; more frequently, may be selected from the group consisting of sodium hydroxide, potassium hydroxide, lithium hydroxide, ammonium hydroxide, and mixtures thereof; and most frequently, may be selected from sodium hydroxide and / or potassium hydroxide. The synthesis mixture may include a source of hydroxide ions, the OH / Y molar ratio of which may be from 0 to 1.0, such as from 0.05 to 0.8, or from 0.1 to 0.7, such as from 0.15 to 0.6. Alternatively, the synthesis mixture may be substantially free of (or substantially free of) hydroxide (or hydroxide) sources.

[0061] Optionally, the synthesis mixture may include one or more sources of alkali metal or alkaline earth metal cations (M). When present, M is preferably selected from the group consisting of sodium, potassium, lithium, rubidium, calcium, magnesium, and mixtures thereof, preferably selected from sodium and / or potassium, more preferably sodium. If present, the source of sodium may be sodium hydroxide, sodium aluminate, sodium silicate, sodium aluminate or a sodium salt, for example, NaCl, NaBr, or sodium nitrate. If present, the source of potassium may be potassium hydroxide, potassium aluminate, potassium silicate, a potassium salt, such as KCl or KBr, or potassium nitrate. The source of lithium, if present, may be lithium hydroxide or a lithium salt, such as LiCl, LiBr, LiI, lithium nitrate, or lithium sulfate. The source of rubidium, if present, may be rubidium hydroxide or a rubidium salt, such as RbCl, RbBr, RBI, or rubidium nitrate. The source of calcium, if present, may be, for example, calcium hydroxide. The source of magnesium, if present, may be, for example, magnesium hydroxide. Additionally, the alkali metal or alkaline earth metal cation (M) may be present in one or more sources of trivalent element (X) (e.g., sodium aluminate, sodium tetraborate, potassium tetraborate) and / or one or more sources of tetravalent element (Y) (e.g., potassium silicate and / or sodium silicate). The synthesis mixture may include a source of alkali metal or alkaline earth metal cations (M), the molar ratio of M / Y being from 0 to 1.0, such as from 0.05 to 0.5, or from 0.05 to 0.2, such as from 0.08 to 0.15. Alternatively, the synthesis mixture may be substantially free of alkali metal or alkaline earth metal cations (M) (or may be substantially free of alkali metal or alkaline earth metal cations (M)).

[0062] The synthesis mixture may optionally further comprise at least one source of halide ions (W), which may be selected from the group consisting of fluoride, chloride, bromide or iodide. The source of halide ions (W) may be any compound capable of releasing halide ions in the synthesis mixture of the molecular sieve. For example, a halide ion can be present as a counter ion of a structure directing agent (Q). Non-limiting examples of sources of halide ions include hydrogen fluoride (HF), hydrogen chloride (HCl), hydrogen bromide (HBr), hydrogen iodide (HI); a salt containing one or more halide ions (e.g., a metal halide) (preferably where the metal is sodium, potassium, calcium, magnesium, strontium, or barium, or a metal such as aluminum (e.g., AlF3, Al2F6) or tin (e.g., SnF2); an ammonium halide (e.g., NH4Cl, NH4Br, NHI, NH4F, NH4HF2); or a tetraalkylammonium halide (e.g., tetramethylammonium halide or tetraethylammonium halide). Also, small amounts of halide ions (W) may be present as impurities, for example in any source of alkali metal or alkaline earth metal cations (M). The halide ions (or halide ions) (W) may be present in a molar ratio of W / Y from 0 to 0.2, such as from 0 to 0.1, for example less than 0.1 (or may be 0). In a preferred embodiment, the synthesis mixture may be substantially free of halide ions (W) (or may be substantially free of halide ions (W)).

[0063] The synthesis may be carried out with or without the addition of nucleating seeds. When nucleating seeds are added to the synthesis mixture, the nucleating seeds may have the same or different structure as the molecular sieves of the present disclosure (e.g., the EMM-73 material obtained by the synthesis described above) and may be suitably present in an amount of about 0.01 ppm to about 10,000 ppm by weight, based on the weight of the synthesis mixture, for example, about 100 ppm to about 5,000 ppm by weight, based on the weight of the synthesis mixture.

[0064] The synthesis mixture typically contains water, with the molar ratio of H2O / Y being 1-100, such as 5-80 or 10-50, such as 10-40. Depending on the nature of the components contained in the base mixture, a certain amount of solvent (e.g., water from a hydroxide solution, methanol and ethanol from hydrolysis of a silica source, if necessary) contained in the base mixture may be removed to achieve a desired solvent / Y molar ratio in the synthesis mixture. Suitable methods for reducing the solvent content may include evaporation in a static or dynamic atmosphere (e.g., ambient air, dry nitrogen, dry air), or by spray drying or freeze drying. Water may be added to the resulting mixture to achieve the desired H2O / Y molar ratio, with excess water being removed during the solvent removal process. In some instances, removal of water is not necessary, where the preparation has a sufficient H2O / Y molar ratio.

[0065] Carbon, in the form of CH2, may be present in a variety of sources, and components of such sources are used to prepare the molecular sieves of the present disclosure (e.g., a source of a tetravalent element (silica source) or a source of a trivalent element (alumina source)), and carbon is incorporated into the framework of the molecular sieve as a bridging atom. The nitrogen atom may be incorporated as a bridging atom into the framework of the molecular sieve after removal of the SDA.

[0066] In one or more embodiments, the synthesis mixture after adjusting the solvent (e.g., achieving a desired water / silica ratio) can be mixed by a mechanical process (e.g., stirring or high shear mixing) to ensure proper homogenization of the base mixture. For example, dual asymmetric centrifugal mixing (e.g., a FlackTek speedmixer) can be used. The mixing speed is 1000 rpm to 3000 rpm (e.g., 2000 rpm).

[0067] The synthesis mixture is then subjected to suitable crystallization conditions to produce (or form) molecular sieves. Crystallization of the molecular sieves may be carried out under static or dynamic (or agitated) conditions in a suitable reaction vessel, such as a Teflon-lined or stainless steel autoclave placed in a convection oven maintained at a suitable temperature.

[0068] The crystallization in step (b) of the process is typically carried out at a temperature of from 100° C. to 200° C., for example from 120° C. to 180° C., preferably from 150° C. to 170° C. The time is sufficient for crystallization to occur at the temperature employed. For example, at higher temperatures, the crystallization time may be shorter. For example, the conditions for crystallization in process (b) of the method may comprise heating for a period of from 1 to 100 days, such as from 1 to 50 days, for example from 1 to 30 days, for example at least 1 day or at least 4 days, up to 30 days or 20 days. The time of crystallization can be established by methods known in the art, for example by sampling the synthesis mixture at various times and determining the yield and X-ray crystallinity of the precipitated solid. Unless otherwise stated in this disclosure, the measured temperature is the temperature of the environment surrounding the material being heated (e.g., the temperature of the atmosphere in which the material is heated).

[0069] Typically, the molecular sieves are formed in solution and can be recovered by standard means (e.g., centrifugation or filtration). Alternatively, the separated molecular sieves can be washed, recovered by centrifugation or filtration, and dried.

[0070] The molecular sieves of the present disclosure may be at least partially dehydrated (e.g., dried) when employed as catalysts or adsorbents in organic compound conversion processes. This may be done by heating to a temperature in the range of 80°C to 500°C (e.g., 90°C to 370°C) under ambient (e.g., air, nitrogen, etc., and atmospheric, reduced or elevated pressure for 30 minutes to 48 hours. Dehydration may also be performed at room temperature, i.e., by subjecting the molecular sieves to reduced pressure, but longer times are required to obtain a sufficient amount of dehydration.

[0071] As a result of the crystallization process, the product recovered contains within its pores at least a portion of the structure directing agent used in the synthesis. Thus, the molecular sieve recovered from process (or step) (c) (as-synthesized molecular sieve) may be subjected to a heat treatment (or thermal treatment) or other treatment (or treatments) to remove some or all of the SDA that was trapped in the pores during synthesis. Thermal treatment (e.g., calcination) of molecular sieves (as-synthesized molecular sieves) typically involves subjecting such materials to elevated temperatures sufficient to remove some or all of the SDA in a furnace with an atmosphere selected from air, nitrogen, ozone, or mixtures thereof. Although reduced pressure may be employed in such heat treatments (or thermal treatments), for reasons of simplicity, atmospheric pressure is preferred. Such heat treatment (or thermal treatment) may be carried out at a temperature up to 925°C, for example between 300°C and 700°C, or between 400°C and 600°C. The measured temperature is the temperature of the environment surrounding the sample (or specimen). Such thermal treatments (e.g. calcination) may be carried out in a box furnace (dry air). The box furnace is exposed to a drying tube. Such a drying tube contains a desiccant that removes water from the air. Heating is typically for calcination (or calcination) for at least one minute (generally from as little as one day up to several days). Initially, such heating may be carried out under a nitrogen atmosphere, which may then be replaced (or switched) to air and / or ozone.

[0072] The molecular sieve may also be subjected to an ion exchange treatment, for example with aqueous ammonium salts such as ammonium nitrate, ammonium chloride and ammonium acetate, in order to remove the remaining alkali metal and / or alkaline earth metal cations (if present in the synthesis mixture) and thereby exchange them for protons, thereby producing the acid form of the molecular sieve. To the extent desired, the original cations (e.g., alkali metal cations) of the as-synthesized material can be replaced by other cations by ion exchange. Preferred replacement cations include hydrogen ions, hydrogen precursors (or hydrogen precursors) such as ammonium ions, and mixtures thereof. The ion exchange process (or step) may be performed after drying the as-made (or post-manufactured) molecular sieves. The ion exchange process (or step) may be carried out before or after the calcination process (or calcination step or calcination step).

[0073] Optionally, aluminum atoms may be introduced into the molecular sieve framework (from which some or all of the SDA has been removed) during an exchange process following the hydrothermal synthesis reaction. Framework silicates that contain boron atoms (eg, borosilicates) may be particularly effective at undergoing exchange with aluminum atoms. Such an exchange process may include exposing the molecular sieve to a source of aluminum (e.g., an aqueous solution containing an aluminum salt) under conditions sufficient to exchange at least a portion, and up to substantially all, of the boron atoms contained in the framework silicate with aluminum atoms. For example, calcined molecular sieves containing boron can be converted to aluminosilicate molecular sieves by heating the calcined molecular sieves containing boron with a solution containing aluminum sulfate, aluminum nitrate, aluminum chloride, and / or aluminum acetate (e.g., in a closed autoclave, in a convection oven at 100°C, or at boiling temperature in an open system). The aluminized molecular sieves may then be recovered by filtration and washed with deionized water.

[0074] The molecular sieves may also be subjected to other treatments (eg, steaming and / or washing with a solvent). Such treatments are well known to those skilled in the art and are carried out to modify the properties of the molecular sieve as desired.

[0075] The molecular sieves of the present disclosure, when some or all of the SDA has been removed, may be used as a catalyst support or catalyst or as an adsorbent (or adsorbent or adsorbent) in the conversion of a wide variety of hydrocarbons, for example, the conversion of organic compounds to conversion products (or conversion products or conversion products or conversion products). Thus, in a fourth aspect, the present disclosure relates to a process (or step or method) of converting (or converting or converting or converting) an organic compound to a transformation product (or transformation product or conversion product or conversion product), the process (or step or method) comprising contacting (or contacting) the organic compound with a molecular sieve according to the first or second aspect of the present disclosure or a molecular sieve prepared (or produced or produced) according to the process (or step or method) of the third aspect of the present disclosure.

[0076] The molecular sieves of the present disclosure (in which some or all of the SDA has been removed) may be used as adsorbents (e.g., adsorbents for separating at least one component from a mixture of multiple components contained in a gas or liquid phase having differential adsorption properties with respect to such material). Thus, with respect to molecular sieves, at least one component may be partially or substantially completely separated from a mixture of components having differential adsorption properties by selectively adsorbing one component by contacting the mixture with the molecular sieve. For example, in a process for selectively separating one or more desired components of a feedstock from the remaining components of the feedstock, the feedstock may be contacted with an adsorbent comprising a molecular sieve of the present disclosure under effective adsorption conditions to form an adsorbed product and an effluent product. One or more desired components are recovered from the adsorbed or effluent product.

[0077] Additionally, the molecular sieves of the present disclosure (when some or all of the SDA has been removed) may be used as catalysts to catalyze the conversion processes of a wide variety of organic compounds. Examples of chemical conversion processes that may be effectively catalyzed by the molecular sieves described herein include those that require acid-activated catalysis, either alone or in combination with one or more other catalytically active substances, including other crystalline catalysts. Examples of organic conversion processes that may be catalyzed by the molecular sieves described in this disclosure include cracking (or cracking), hydrocracking (or hydrocracking), isomerization (or isomerization), polymerization (or polymerization), reforming (or reforming), hydrogenation (or hydrogenation), dehydrogenation (or dehydrogenation), dewaxing (or dewaxing), hydrodewaxing (or hydrodewaxing), and the like. rodewaxing), adsorption, alkylation, transalkylation, dealkylation, hydrodesilylation, disproportionation, oligomerization, dehydrocyclization, conversion of methanol to olefins, deNOx x (deNOx) uses (or applications or applications) and combinations thereof. The conversion of the hydrocarbon feed (or feed) may be carried out in any convenient mode, for example in a fluidized bed, moving bed or fixed bed reactor, depending on the type of process (or step or method) desired.

[0078] The molecular sieves of the present disclosure may be formulated into product compositions by combination with other materials, such as binders and / or matrix materials (which impart additional hardness to the final product). Such other materials may be inert or may be catalytically active materials.

[0079] For example, it may be desirable to incorporate another material into the molecular sieves of the present disclosure that is resistant to the temperatures and other conditions employed during use. Such materials include synthetic or natural zeolites as well as inorganic materials such as clays, silica and / or metal oxides (e.g., alumina) and mixtures thereof. The metal oxides may be naturally occurring or may be in the form of gelatinous precipitates or gels (including mixtures of silica and metal oxides). The use of a resistant material (i.e., combined with the molecular sieve of the present disclosure or present during the synthesis of the as-made molecular sieve) in conjunction with the molecular sieve of the present disclosure (the crystals of which are active) tends to change the selectivity and / or conversion of the catalyst in a particular organic conversion process. An inactive resistant material is suitably useful as a diluent to control the amount of conversion in a given process, so that the product can be obtained in an economical and orderly manner without employing other means to control the rate of reaction. These materials may be incorporated into naturally occurring clays (eg, bentonite and kaolin). The breaking strength (or crush strength) of a product (or article or product) can be improved (or enhanced) under commercial (or market) operating conditions. The above inactive resistant materials, i.e. clays, oxides, etc., function as binders for the catalyst. A catalyst having good crush strength can be beneficial because in commercial use it is desirable to inhibit (or prevent) the catalyst from breaking down into powder-like material.

[0080] Natural clays that can be used include the montmorillonite and kaolin families, including subbentonites (or subbentonites), and kaolins (such as those commonly known as Dixie, McNamee, Georgia, and Florida clays), where the major inorganic constituents are halloysite, kaolinite, dickite, nacrite, or anauxite. Such clays can be used in the raw state in which they were originally mined, or after being subjected to calcination, acid treatment or chemical modification. Binders useful for composition with the molecular sieves of the present disclosure also include inorganic oxides selected from silica, zirconia, titania, magnesia, beryllia, alumina, yttria, gallium oxide, zinc oxide, and mixtures thereof.

[0081] In addition to the materials described above, the molecular sieves of the present disclosure may be formulated with porous matrix materials (e.g., 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).

[0082] These binder materials are resistant to temperature and other conditions, such as mechanical attrition, that occur during the various hydrocarbon separation processes. Thus, the molecular sieves of the present disclosure can be used in extrudate form (or foam) along with a binder. These are typically joined (or bonded or bonded) by forming (or producing) a tablet (or pill), sphere (or sphere) or extrudate (or extrudate or extrude). The extrudates (or extrudates or extrudes) are typically formed (or produced) by extruding molecular sieves, optionally in the presence of a binder, followed by drying and calcination (or calcination) of the resulting extrudates (or extrudates or extrudes). Further treatment (eg, steaming) and / or ion exchange may be performed as required. The molecular sieve may be optionally bound (or bonded) to a binder. The binder has a surface area of ​​at least 100 m2 / g, e.g., at least 200m 2 / g, if necessary, at least 300m 2 / g.

[0083] The relative proportions of the molecular sieve and inorganic oxide matrix may vary widely, with the molecular sieve content being in the range of about 1 to about 100% by weight, more usually in the range of about 2 to about 95% by weight, optionally in the range of about 20 to about 90% by weight, based on the composite, particularly when such composite is prepared in extrudate form.

[0084] The molecular sieves of the present disclosure may also be used in intimate combination with a hydrogenation component (e.g., tungsten, vanadium, molybdenum, rhenium, nickel, cobalt, chromium, manganese, or a precious metal (e.g., platinum or palladium)) in which a hydrogenation-dehydrogenation function may be performed. Such hydrogenation components may be incorporated into the composition by one or more of the following processes: Cocrystallization (the composition is exchanged to the extent that a Group IIIA element (e.g., aluminum) is present in the structure) or intimately physically mixed (or blended) with such a hydrogenation component. Such hydrogenation components may also be impregnated in or on the molecular sieve, for example by treating the molecular sieve with hydride metal-containing ions. For example, in the case of platinum, suitable platinum compounds for this purpose include a variety of compounds including chloroplatinic acid, platinum chloride, and platinum amine complexes. Also, combinations of metals and methods for their introduction can be used.

[0085] One of ordinary skill in the art will appreciate that the molecular sieves of the present disclosure may contain impurities (e.g., amorphous materials, unit cells having different topologies (e.g., molecular sieves or quartz having different framework types) that may or may not affect the performance of the resulting catalyst) and / or other impurities (e.g., heavy metals and / or organic hydrocarbons). Typical examples of molecular sieves having different framework types that may coexist with the molecular sieves of the present disclosure are, for example, molecular sieves having framework types FER or IWV (eg, ITQ-27). The molecular sieves of the present disclosure are preferably substantially free of impurities. The term "substantially free of impurities" (or the alternative term "substantially pure"), as used herein, means that the molecular sieve has a small or minor proportion of such impurities (e.g., less than 50% by weight of such impurities). Such impurities are preferably less than 20% by weight, more preferably less than 10% by weight, even more preferably less than 5% by weight, and most preferably less than 1% by weight (e.g., less than 0.5% by weight or less than 0.1% by weight). Such weight percent (wt%) values ​​are based on the combined weight of impurities and pure molecular sieve. The amount of impurities can be suitably determined by powder XRD, rotational electron diffraction and / or SEM / TEM (eg, different crystal morphologies (or crystal forms)).

[0086] The molecular sieves described in this disclosure are substantially crystalline (or crystalline or crystal or crystalline). The term "crystalline" as used herein means that the material is in a crystalline solid form, including, but not limited to, single-component or multi-component crystalline forms (e.g., solvates, hydrates, and co-crystals). Crystalline (or crystalline or crystal or crystalline) can mean having a regular repetition of molecules and / or an orderly arrangement of molecules and having a distinct crystal lattice. For example, molecular sieves may differ in their water or solvent content. The lattices of different crystalline materials can be identified by characterization methods in the solid state, such as XRD (e.g., powder XRD). Other characterization methods known to those of skill in the art can further aid in the identification of the crystalline form and can further aid in the determination of stability and solvent / water content. The term "substantially crystalline" as used in this disclosure means that the majority (50% or more by weight) of a sample of the material being described is in crystalline form, with the remainder of the sample being in a non-crystalline form (amorphous form or non-crystalline form). In one or more embodiments, a substantially crystalline sample has at least 95% crystallinity (e.g., 5% is in non-crystalline form); having at least 96% crystallinity (e.g., 4% is in non-crystalline form); having at least 97% crystallinity (e.g., 3% is in a non-crystalline form); having at least 98% crystallinity (e.g., about 2% is in a non-crystalline form); having at least 99% crystallinity (e.g., 1% is in a non-crystalline form); It has 100% crystallinity (eg, 0% is a non-crystalline form).

[0087] Aspects of the present disclosure will now be described in further detail by way of specific examples. The following examples are offered for illustrative purposes and are not intended to limit (or restrict) the present disclosure in any way (or manner). Those skilled in the art will readily understand that the various parameters can be changed or modified while still achieving essentially the same results. EXAMPLES

[0088] (Example) The present invention is further described below, but is not limited to the scope thereof.

[0089] In these examples, X-ray diffraction (XRD) patterns of the as-synthesized and as-calcined materials were recorded (2θ range, 2-50°) using an X-Ray Powder Diffractometer (Bruker DaVinci D8 Discovery instrument), continuum mode (CuKα radiation), Bragg-Bentano geometry (with a Vantec 500 detector). The interplanar spacing (d spacing) was calculated in Angstroms, and the relative intensity (I / Io) of a line is the ratio of the peak intensity to the peak intensity of the longest line (above background). These intensities remain uncorrected (or uncalibrated) for the Lorentz effect and the polarization effects. The positions (locations) of the diffraction peaks (2θ) and the relative peak area intensities (I / I(o)) of the lines (where I(o) is the intensity of the longest line (above background) were determined (using the MDI Jade peak search algorithm). It should be understood that diffraction data listed as a single line may consist of multiple overlapping lines. Under certain conditions (e.g., differences in crystallographic changes), these lines may be resolved or appear as partially resolved lines. Typically, such crystallographic changes may involve minor changes in unit cell parameters and / or changes in crystal symmetry, without altering the framework connectivity. Additionally, such minor effects (including changes in relative intensity) may result from differences in cation content, framework composition, the nature and degree of pore filling, crystal size and shape, preferred orientation, and thermal and / or hydrothermal history.

[0090] Scanning electron microscopy (SEM) images were obtained of the as-synthesized materials (Hitachi 4800 Scanning Electron Microscope). SEM images were used to aid in the assessment of product purity. The presence of distinctly different crystal morphologies (or crystal forms or crystal structures) in SEM images can indicate impurities in the form of other crystalline (or crystalline or crystal or crystalline) materials (or materials). Such approximate analysis may be particularly useful in recognizing (or identifying or identifying) the presence of relatively small amounts of crystalline (or crystalline or crystal or crystalline) impurity formations, even if such presence is not discernible (or discernible or identifiable or unidentifiable) from the XRD pattern of the product (or article or product).

[0091] The BET method determines the total BET surface area (S BET The BET method is as described in S. Brunauer et al., (1938), J. Am. Chem. Soc., v. 60, pg. 309, which is incorporated herein by reference, and utilizes nitrogen adsorption-desorption (or desorption) at liquid nitrogen temperatures. The external surface area (S) of a material ext ) was obtained from the t-plot method. The micropore surface area (S) of a material micro ) to the total BET surface area (S BET ) to the external surface area (S ext ) was calculated by subtracting

[0092] Using methods known in the relevant art, the micropore volume (V) of a material may be determined. micro ) can be determined. For example, the pore volume of a material can be measured by nitrogen physical adsorption. The data can be analyzed by the t-plot method, which is described in Lippens, BC et al., (1965), "Studies on pore system in catalysts: V. The t method," J. Catal., v.4, pg. 319, which describes the micropore volume method and is incorporated herein by reference.

[0093] The molar ratios and conditions used in the synthesis of Examples 2-11 and the resulting products are detailed below and summarized in Table 3.

[0094] Example 1a 2-Methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenz Synthesis of imidazolium cation (SDA-1) 2-Methyl-4,5,6,7-tetrahydrobenzimidazole 40 g of 2-methylbenzimidazole were dissolved in 320 ml of glacial acid. 15 g of palladium (10% by weight on carbon) were added and the reaction mixture was treated with hydrogen (temperature 120° C., pressure 80 bar, 24 h). The solution was filtered through celite and washed with glacial acid. The solvent was evaporated under reduced pressure, and then sodium hydroxide solution was added to adjust the pH of the solution to 9-10. The precipitate was filtered, washed with water, then dissolved in chloroform and extracted with saturated sodium chloride solution. Dry the organic phase over sodium sulfate, filter and concentrate under reduced pressure.

[0095] 2-Methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium iodide 13.6 g of 2-methyl-4,5,6,7-tetrahydro-1H-benzimidazole, 55 g of 1-iodobutane, and 20 g of potassium carbonate were added to 150 ml of acetonitrile (CH3CN) in a 500 mL round bottom flask equipped with a magnetic stir bar. The suspension was then refluxed for 18 hours and then cooled to room temperature. The solution was then filtered through a Buchner funnel and the filtrate was concentrated on a rotovap. Dichloromethane was added to the concentrated solution to remove residual potassium salts. The filtrate (in dichloromethane) was concentrated on a rotovap and dried under reduced pressure to give 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium iodide.

[0096] 2-Methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium hydroxide The iodide salt was ion-exchanged to the hydroxide form using Amberlite® IRN78 OH (hydroxide form) (iodide:resin:water ratio 1:3.5:5) at room temperature overnight.

[0097] Example 1b Synthesis of 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation (SDA-2) The three-step process of Example 1a was followed except that 51 g of 1-iodopropane was used instead of 55 g of 1-iodobutane.

[0098] Example 1c Synthesis of 2-methyl-1,3-di-n-butylbenzimidazolium cation (SDA-3) 2-Methyl-1,3-di-n-butyl-benzimidazolium iodide 15 g of 2-methyl-benzimidazole, 63 g of 1-iodobutane, and 22 g of potassium carbonate were added to 200 ml of acetonitrile (CH3CN) (500 mL round bottom flask equipped with a magnetic stir bar). The suspension was then refluxed for 18 hours and then cooled to room temperature. The solution was then filtered through a Buchner funnel and the filtrate was concentrated on a rotovap. Dichloromethane was added to the concentrated solution to remove residual potassium salts. The filtrate (in dichloromethane) was concentrated on a rotovap and dried under reduced pressure to give 2-methyl-1,3-di-n-butyl-benzimidazolium iodide.

[0099] 2-Methyl-1,3-di-n-butyl-benzimidazolium hydroxide The iodide salt was ion-exchanged to the hydroxide form using ion exchange resin Amberlite® IRN78 OH (hydroxide form) (iodide:resin:water ratio=1:3.5:5). Such ion exchange was carried out overnight at room temperature.

[0100] Example 1d Synthesis of 2-methyl-1,3-dipropylbenzimidazolium cation (SDA-4) The two-step process of Example 1c was followed except that 58 g of 1-iodopropane was used instead of 63 g of 1-iodobutane.

[0101] Example 2 SDA-1, USY zeolite, Si / Al=30 In a PTFE liner of a 23 mL SteelParr autoclave, 7.31 g of SDA-1 solution (16.4 wt%) and 0.46 g of Ultrastable Y (USY) zeolite (Si / Al molar ratio=30) (available from Zeolyst as CBV760) were then mixed together and stirred at 50° C. with a loss of 3.8 g of HO to produce a synthesis mixture having the following molar ratio composition: 18H2O:1SiO2:0.017Al2O3:0.6QOH

[0102] The liner was then capped and sealed in a 23 mL Parr autoclave and placed on the spit inside a convection oven (or convection over). The reactor was heated at 160° C. under tumbling conditions (approximately 30 rpm) for three weeks. The product was isolated by filtration, rinsed with deionized water and dried. The as-synthesized material was isolated by filtration and rinsed with deionized water. The product was dried at 90°C in a ventilated drying oven. The as-synthesized material was then calcined in air (up to 580 °C) (box furnace, ramp rate = 3 °C / min). The temperature remained at 580° C. for 8 hours. The box furnace was then cooled.

[0103] XRD analysis of the as-synthesized and as-calcined products showed that the materials had powder XRD patterns, in terms of 2θ (°) and d spacing, similar to the as-synthesized and as-calcined SSZ-56 molecular sieves, respectively, although the relative intensities differ (e.g., as shown in Tables 1 / 1A and 2 / 2A of US2006 / 0292071 and Tables 3 and 4 of US2013 / 0330272, which are incorporated herein by reference in their entireties). Such a new product was identified as EMM-73. 1 and 2 show the powder XRD patterns of the as-synthesized (or after-synthesized) and as-calcined (or after-calcined) materials. Tables 4 and 5 below provide a list of peaks and intensities for the as-synthesized (or after-synthesized) and as-calcined (or after-calcined) materials.

[0104] The EMM-73 material was shown to have an SFS framework type. EMM-73 has a two-dimensional channel system in which 10-ring pores and 12-ring pores intersect (12MR x 10MR zeolite). FIG. 3 shows projections (or projections or plan views) of EMM-73 along the

[0010] -12MR (left) and the

[0001] -10MR (right) (oxygen atoms have been omitted for brevity). The pore along the d direction (Figure 3, left) is a straight channel, bounded by 12 tetrahedral atoms, and has dimensions of 8.4 × 5.8 Å (angstroms). The pore along the c-direction (Figure 3, right) is constrained by a 10-ring window and has dimensions of 5.5 × 5.1 Å (angstroms).

[0105] The EMM-73 material has a unique rectangular-like morphology having two short diffusion lengths (i.e., width and thickness) and one long diffusion length (i.e., length). Such a morphology is shown in FIG. 4, which shows an SEM image of the as-synthesized product of Example 2. More specifically, two short diffusion lengths are in the a and b directions (12 MR direction), and a long diffusion length (i.e., up to 2 μm (or microns) long) is in the c direction (10 MR direction), resulting in faster diffusion of molecules in the 12 MR direction. Such a form (or morphology) is highly preferred in catalysis and adsorption applications as compared to plate-like or needle-like forms (or morphologies). Also, the effect of crystal size anisotropy (resulting from a particular rectangular-like morphology) is reflected in the distinct relative intensities of the first five XRD peaks of EMM-73 as-calcined, as shown in Table 4 and Figures 2 and 5.

[0106] The micropore surface area (S micro ) is 573m 2 / g. Its external surface area (or outer surface area or external surface area) (S ext ) is 13m 2 / g. The micropore volume (or micropore volume or micropore volume) (V micro ) was 0.22 cc / g.

[0107] Example 3 SDA-1, USY zeolite, Si / Al=30 Example 3 was carried out under similar conditions to Example 2, except that the synthesis mixture contained less SDA-1, more water (i.e., more water was added than removed), and more NaOH, resulting in the following compositions in terms of molar ratios: 35.5H2O:1SiO2:0.017Al2O3:0.27QOH:0.125NaOH

[0108] After heating at 160° C. for 3 weeks, a pure EMM-73 product was obtained, which was identified by its XRD pattern.

[0109] Example 4 SDA-1, USY zeolite, Si / Al=30 Example 4 was carried out under similar conditions to Example 3, except that the synthesis mixture contained less SDA-1 and more NaOH. In terms of molar ratios, the following compositions were obtained: 35.5H2O:1SiO2:0.017Al2O3:0.18QOH:0.18NaOH

[0110] After heating at 160° C. for one week, a pure EMM-73 product was obtained, which was identified by its XRD pattern.

[0111] Example 5 SDA-1, colloidal silica (or colloidal silica or colloidal silica), sodium aluminate (or sodium aluminate), Si / Al=17 Example 5 was carried out under the same conditions as Example 2, except that Ludox HS40 (a suspension of 40 wt% colloidal silica) was used as the source of Si and sodium aluminate (NaAlO2, 25 wt% Al2O3, 19.3 wt% Na2O) was used as the source of Al to obtain a synthesis mixture having the following composition in terms of molar ratios: 21H2O:1SiO2:0.029Al2O3:0.2QOH:0.08NaOH

[0112] After heating at 160° C. for two weeks, a product of EMM-73 was obtained, which contained a small amount of FER material, and was identified by its XRD pattern.

[0113] Example 6 SDA-1, colloidal silica (or colloidal silica or colloidal silica), boric acid, Si / B=10 Example 6 was carried out under the same conditions as Example 2, except that Ludox LS30 (a 30 wt% suspension of colloidal silica) was used as the source of Si and boric acid (H3BO3, 3.9 wt%) was used as the source of B to obtain a synthesis mixture having the following composition in terms of molar ratios: 10H2O:1SiO2:0.05B2O3:0.4QOH

[0114] After heating at 160° C. for 6 weeks, a pure EMM-73 product was obtained, which was identified by its XRD pattern.

[0115] As can be seen from FIG. 6, which shows an SEM image of the product as-synthesized in Example 6, the EMM-73 borosilicate has a square (or rectangular)-like morphology (or nearly square (or nearly rectangular) morphology or rectangular-like morphology). However, the particle size (or size or dimension) (or particle diameter or particle size) is significantly smaller than that of the EMM-73 aluminosilicate. Also, the length (or length) is less than 400 nm, for example, about 100 to 200 nm.

[0116] Example 7 SDA-2, colloidal silica (or colloidal silica or colloidal silica), sodium aluminate (or sodium aluminate), Si=Al=50 Example 7 was carried out under the same conditions as Example 5, except that SDA-2 was used instead of SDA-1. The synthesis mixture had the following composition, in terms of molar ratios: 25H2O:1SiO2:0.01Al2O3:0.15QOH:0.1NaOH

[0117] After heating at 175° C. for 4 days, a product of EMM-73 was obtained, which contained a small amount of ITQ-27 material, and was identified by its XRD pattern.

[0118] Example 8 SDA-2, colloidal silica (or colloidal silica or colloidal silica), aluminum hydroxide, Si / Al=50 Example 8 was carried out under the same conditions as Example 7, except that aluminum hydroxide (Sigma, 54 wt% Al2O3) was used as the source of Al. The synthesis mixture had the following composition, in terms of molar ratios: 15H2O:1SiO2:0.01Al2O3:0.15QOH:0.1NaOH

[0119] After heating at 175° C. for 4 days, a product of EMM-73 was obtained, which contained a small amount of quartz. Such a product was identified by its XRD pattern.

[0120] Example 9 SDA-2, colloidal silica (or colloidal silica or colloidal silica), boric acid, Si / B=10 Example 9 was carried out under the same conditions as Example 6, except that SDA-2 was used instead of SDA-1. The synthesis mixture had the following composition, in terms of molar ratios: 10H2O:1SiO2:0.05B2O3:0.4QOH

[0121] After heating at 160° C. for 4 weeks, a pure EMM-73 product was obtained, which was identified by its XRD pattern.

[0122] FIG. 7 shows an SEM image of the product (or article or product) during (or after) synthesis of Example 9. As in Example 6, the resulting EMM-73 borosilicate has a square (or rectangular)-like morphology (or nearly square (or nearly rectangular) morphology or rectangular-like morphology). The length of such a morphology is less than 400 nm (e.g., about 50-100 nm).

[0123] Example 10 SDA-3, colloidal silica (or colloidal silica or colloidal silica), aluminum hydroxide (or aluminum hydroxide), Si / Al=39 Example 10 was carried out under the same conditions as Example 8 (in Example 8, colloidal silica and aluminum hydroxide were used as the source of Si and Al), except that SDA-3 was used instead of SDA-2. The synthesis mixture had the following composition, in terms of molar ratios: 30H2O:1SiO2:0.013Al2O3:0.15QOH:0.1NaOH

[0124] After heating at 160° C. for 3 weeks, a pure EMM-73 product was obtained, which was identified by its XRD pattern.

[0125] Example 11 SDA-4, colloidal silica (or colloidal silica or colloidal silica), aluminum hydroxide (or aluminum hydroxide), Si / Al=39 Example 11 was carried out under the same conditions as Example 10 (in which colloidal silica and aluminum hydroxide were used as the source of Si and Al), except that SDA-4 was used instead of SDA-3 to obtain a synthesis mixture. The synthesis mixture had the following composition, in terms of molar ratios: 30H2O:1SiO2:0.013Al2O3:0.15QOH:0.1NaOH

[0126] After heating at 160° C. for two weeks, a pure EMM-73 product was obtained, which was identified by its XRD pattern.

[0127] [Table 7]

[0128] * SDA-1 = 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium cation SDA-2 = 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation SDA-3 = 2-methyl-1,3-di-n-butylbenzimidazolium cation SDA-4 = 2-methyl-1,3-dipropylbenzimidazolium cation

[0129] [Table 8]

[0130] [Table 9]

[0131] While the present invention has been described and illustrated with reference to specific embodiments, it will be understood by those skilled in the art that the present invention is susceptible to many different alterations, modifications and variations thereon that are not specifically set forth in the present disclosure. Furthermore, when a lower limit and an upper limit of a numerical value are described in the present disclosure, it will be apparent to a person skilled in the art that a range from any lower limit to any upper limit is also contemplated. Additionally, all numerical values ​​set forth in the detailed description of the present disclosure are modified by "about" to indicate that the stated value takes into account experimental error and variations, and may be predicted (or expected) by one of ordinary skill in the art.

[0132] In the above description, wholes or elements are described which have known, obvious, or foreseeable equivalents (or equivalents), and such equivalents are then incorporated in this disclosure as if each was described. The following claims should be referenced to determine the true scope of the invention, which should be construed to encompass any such equivalents. It is also understood that any features or wholes of the invention described as being preferred, advantageous, convenient, or the like are optional for the reader and do not limit the scope of the independent claims. Further, it should be understood that any such feature or features may be beneficial in some embodiments of the present invention, while in other embodiments, it may be undesirable and therefore may not be present.

[0133] Additionally or alternatively, the invention relates to the following embodiments:

[0134] EMBODIMENT 1 A molecular sieve, which in its as-calcined (or calcined) form (or calcined form) has an X-ray diffraction pattern including the peaks shown in Table 1.

[0135] EMBODIMENT 2 2. The molecular sieve of embodiment 1, having a molecular formula of Formula III: (m)X2O3:YO2 (Formula III) [In the formula, 0.005 <m≦0.1であり、 X is a trivalent element, Y is a tetravalent element.

[0136] EMBODIMENT 3 The molecular sieve of embodiment 2, wherein X comprises one or more of aluminum, boron, iron and gallium, preferably X comprises or is aluminum and / or boron.

[0137] EMBODIMENT 4 The molecular sieve according to embodiment 2 or 3, wherein Y comprises one or more of silicon, titanium and germanium, and preferably Y comprises or is silicon.

[0138] EMBODIMENT 5 A molecular sieve, the X-ray diffraction pattern of which in its as-synthesized (or post-synthesized) form (or as-synthesized form) includes the peaks shown in Table 2.

[0139] EMBODIMENT 6 6. The molecular sieve of embodiment 5, having a molecular formula of Formula IV: (q)Q:(m)X2O3:YO2 (Formula IV) [In the formula, 0 <q≦0.7であり、 0.005≦m≦0.1, X is a trivalent element, Y is a tetravalent element, Q comprises at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of formula I below and the benzimidazolium cation of formula II below.

[0140] [ka] (Formula I)

[0141] [ka] (Formula II)

[0142] During the ceremony, R and R' are the same or different, preferably the same. R and R' are selected from n-propyl and n-butyl. R'' is selected from methyl and ethyl, preferably methyl.

[0143] EMBODIMENT 7 7. The molecular sieve of embodiment 6, wherein X comprises one or more of aluminum, boron, iron and gallium, preferably X comprises or is aluminum and / or boron.

[0144] EMBODIMENT 8 The molecular sieve according to embodiment 6 or 7, wherein Y comprises one or more of silicon, titanium and germanium, preferably Y comprises or is silicon.

[0145] EMBODIMENT 9 The molecular sieve according to any one of embodiments 6 to 8, wherein the structure directing agent (Q) comprises at least one cation selected from the group consisting of 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-dipropylbenzimidazolium cation, 2-methyl-1,3-di-n-butylbenzimidazolium cation, and mixtures thereof.

[0146] EMBODIMENT 10 A molecular sieve according to any one of embodiments 1 to 9, wherein at least a portion of the crystals of the molecular sieve have a square (or rectangular)-like morphology (or morphology) (or a roughly square (or roughly rectangular) morphology or rectangular-like morphology).

[0147] EMBODIMENT 11 A molecular sieve according to embodiment 10, wherein at least a portion of the crystals of such molecular sieve have a square (or rectangular)-like morphology (or quasi-square (or approximately rectangular) morphology or rectangular-like morphology), the ratio of length (l) / width (w) is between 1 and 10 and less, preferably between 1 and 6, and the ratio of length (l) / height (h) is between 1 and 10 and less, preferably between 1 and 6.

[0148] EMBODIMENT 12 A molecular sieve according to embodiment 10 or 11, wherein at least a portion of the crystals of such molecular sieve have a square (or rectangular)-like morphology (or quasi-square (or approximately rectangular) morphology or rectangular-like morphology) and the ratio of width (w) / height (h) is between 1 and 3, preferably between 1 and 2.

[0149] EMBODIMENT 13 13. The molecular sieve of any one of embodiments 1 to 12, wherein the molecular sieve is an aluminosilicate and the crystals of the molecular sieve have a length of 0.1 to 2 μm (or microns).

[0150] EMBODIMENT 14 A molecular sieve according to any one of embodiments 1 to 12, wherein the molecular sieve is a borosilicate and the crystals of the molecular sieve have a length of 50 nm to less than 1 μm (or micron), preferably less than 500 nm, more preferably less than 400 nm.

[0151] EMBODIMENT 15 The molecular sieve according to any one of the first to fourth embodiments, wherein the molecular sieve is an aluminosilicate or a borosilicate, and the molar ratio of Si / Al or Si / B of the molecular sieve is less than 100, preferably 5-75, more preferably 10-50 or 15-50.

[0152] EMBODIMENT 16 A method for producing the molecular sieve according to any one of embodiments 1 to 15, comprising the steps of: (a) preparing a molecular sieve from a mixture of 100% ethanol and 100% ethanol; (a) A process for preparing (or producing or preparing or preparing) a synthetic mixture (or synthetic mixture or synthesis mixture or synthesis mixture), such synthetic mixture comprising: Water, a source of an oxide of a tetravalent element (Y); a source of an oxide of a trivalent element (X); A structure directing agent (Q); Optionally, a source of hydroxide ions (OH); Optionally, a source of alkali metal and / or alkaline earth metal elements (M), Including, The structure directing agent (Q) comprises at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of formula I below and the benzimidazolium cation of formula II below,

[0153] [ka] (Formula I)

[0154] [ka] (Formula II)

[0155] During the ceremony, R and R' are the same or different, preferably the same. R and R' are selected from n-propyl and n-butyl. R'' is selected from methyl and ethyl, preferably methyl. (b) heating the synthesis mixture under crystallization conditions, such conditions including a temperature of 100°C to 200°C for a time sufficient to form crystals of the molecular sieve; (c) recovering at least a portion of the molecular sieve from step (b). (d) Optionally, treating the molecular sieve recovered in step (c) to remove at least a portion of the structure directing agent (Q).

[0156] EMBODIMENT 17 17. The method according to embodiment 16, wherein the structure directing agent (Q) comprises at least one cation selected from the group consisting of 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-dipropylbenzimidazolium cation, 2-methyl-1,3-di-n-butylbenzimidazolium cation, and mixtures thereof.

[0157] EMBODIMENT 18 The method according to embodiment 16 or 17, wherein the structure directing agent (Q) is in the form of a halide, hydroxide or nitrate, preferably the structure directing agent (Q) is in the form of a hydroxide.

[0158] EMBODIMENT 19 The method according to any one of embodiments 16 to 18, wherein the tetravalent element (Y) is selected from the group consisting of silicon, titanium, germanium, and mixtures thereof, preferably, the tetravalent element (Y) comprises silicon, more preferably, the tetravalent element (Y) is silicon.

[0159] EMBODIMENT 20 The method according to any one of embodiments 16 to 19, wherein the trivalent element (X) is selected from the group consisting of aluminum, boron, iron, gallium, and mixtures thereof, preferably the trivalent element (X) comprises aluminum and / or boron, more preferably the trivalent element (X) is aluminum and / or boron, in particular aluminum.

[0160] EMBODIMENT 21 The method according to any one of embodiments 16 to 20, wherein the synthesis mixture has the following composition, in terms of molar ratios:

[0161] [Table 10]

[0162] EMBODIMENT 22 A process (or step or method) for converting (or converting or converting or converting) an organic compound to a transformation product (or transformation product or conversion product or conversion product), the process comprising contacting (or contacting) the organic compound with a molecular sieve according to any one of embodiments 1 to 15.

Claims

1. A molecular sieve in its as-calcined form having an X-ray diffraction pattern showing the peaks shown in Table 1 below: 【Table 1】 including molecular sieves.

2. The molecular formula of Formula III: (m)X ２ O ３ ::YO ２ (Formula III) [In the formula, 0.005<m≦0.1, X is a trivalent element, in particular X comprises one or more of aluminum, boron, iron and gallium, preferably X comprises or is aluminum and / or boron; Y is a tetravalent element, in particular Y comprises one or more of silicon, titanium and germanium, and preferably Y comprises or is silicon.

2. The molecular sieve of claim 1 having the formula:

3. A molecular sieve, in its as-synthesized form, having an X-ray diffraction pattern with the peaks shown in Table 2 below: 【Table 2】 including molecular sieves.

4. The molecular formula of Formula IV: (q)Q:(m)X ２ O ３ :YO ２ (Formula IV) [In the formula, 0<q≦0.7, 0.005≦m≦0.1, X is a trivalent element, in particular X comprises one or more of aluminum, boron, iron and gallium, preferably X comprises or is aluminum and / or boron; Y is a tetravalent element, in particular Y comprises one or more of silicon, titanium and germanium, preferably Y comprises or is silicon; Q comprises at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of formula I below and the benzimidazolium cation of formula II below. having 【Chemistry 1】 (Formula I) 【Chemistry 2】 (Formula II) During the ceremony, R and R' are the same or different, preferably the same, and R and R' are selected from n-propyl and n-butyl; R″ is selected from methyl and ethyl, preferably methyl; The molecular sieve of claim 3.

5. 5. The molecular sieve of claim 4, wherein the structure directing agent (Q) comprises at least one cation selected from the group consisting of 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-dipropylbenzimidazolium cation, 2-methyl-1,3-di-n-butylbenzimidazolium cation, and mixtures thereof.

6. 6. The molecular sieve of any one of claims 1 to 5, wherein at least a portion of the crystals of the molecular sieve have a rectangular-like morphology.

7. 7. The molecular sieve of claim 6, wherein the molecular sieve is an aluminosilicate and the crystals of the molecular sieve have a length of 0.1 to 2 μm.

8. 7. The molecular sieve of claim 6, wherein the molecular sieve is a borosilicate and the crystals of the molecular sieve have a length of 50 nm to less than 1 μm, preferably less than 500 nm, more preferably less than 400 nm.

9. 9. The molecular sieve of claim 1, wherein the molecular sieve is an aluminosilicate or a borosilicate and the Si / Al or Si / B molar ratio of the molecular sieve is less than 100, preferably 5-75, more preferably 10-50 or 15-50.

10. A method for producing the molecular sieve of any one of claims 1 to 9, comprising the following steps (a) to (d): (a) Preparing a synthesis mixture, the synthesis mixture comprising: Water, a source of an oxide of a tetravalent element (Y); a source of an oxide of a trivalent element (X); A structure directing agent (Q); optionally a source of hydroxide ions (OH); Optionally, a source of alkali metal and / or alkaline earth metal element (M); Including, said structure directing agent (Q) comprising at least one cation selected from the 4,5,6,7-tetrahydrobenzimidazolium cation of formula I below and the benzimidazolium cation of formula II below; 【Chemistry 3】 (Formula I) 【Chemistry 4】 (Formula II) [In the formula, R and R' are the same or different, preferably the same, and R and R' are selected from n-propyl and n-butyl; R″ is selected from methyl and ethyl, preferably methyl; (b) heating the synthesis mixture under crystallization conditions, said conditions comprising a temperature of from 100° C. to 200° C. for a time sufficient to form crystals of the molecular sieve; (c) recovering at least a portion of the molecular sieve from step (b); (d) Optionally, treating the molecular sieve recovered in step (c) to remove at least a portion of the structure directing agent (Q). A method comprising:

11. 11. The method of claim 10, wherein the structure directing agent (Q) comprises at least one cation selected from the group consisting of 2-methyl-1,3-dipropyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-di-n-butyl-4,5,6,7-tetrahydrobenzimidazolium cation, 2-methyl-1,3-dipropylbenzimidazolium cation, 2-methyl-1,3-di-n-butylbenzimidazolium cation, and mixtures thereof.

12. 12. The method according to claim 10 or 11, wherein the structure directing agent (Q) is in the form of a halide, hydroxide or nitrate, preferably the structure directing agent (Q) is in the form of a hydroxide.

13. The tetravalent element (Y) is selected from the group consisting of silicon, titanium, germanium, and mixtures thereof, preferably, the tetravalent element (Y) comprises silicon, more preferably, the tetravalent element (Y) is silicon; 13. The method according to any one of claims 10 to 12, wherein the trivalent element (X) is selected from the group consisting of aluminium, boron, iron, gallium and mixtures thereof, preferably the trivalent element (X) comprises aluminium and / or boron, more preferably the trivalent element (X) is aluminium and / or boron, in particular aluminium.

14. The synthesis mixture had the following composition, in terms of molar ratio: 【Table 3】 The method according to any one of claims 10 to 13, comprising:

15. A process for converting an organic compound to a conversion product, the process comprising contacting the organic compound with a molecular sieve according to any one of claims 1 to 9.

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