Method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals

Abstract

The invention discloses a method for synthesizing a high-crystallinity zeolite molecular sieve through in-situ crystallization of aluminosilicate minerals, and belongs to the technical field of zeolite molecular sieve synthesis. The preparation method comprises the following steps: preparing a crystal nucleus liquid containing zeolite molecular sieve microcrystals and a solid-phase wafer; mixing aluminosilicate minerals with the crystal nucleus liquid, and respectively roasting at 850-1000 DEG C and 650-800 DEG C to prepare an active mineral silicon source and an active mineral aluminum source; and mixing the active mineral source with additional silicon species, NaOH, a template agent, a crystal nucleus liquid, a solid-phase wafer and water, crystallizing at 90-150 DEG C, and post-processing to obtain the high-crystallinity zeolite molecular sieve. By introducing the crystal nucleus liquid and the solid-phase wafer, silicon and aluminum components in the aluminosilicate mineral are promoted to be converted into the target molecular sieve in situ, the crystallinity of the product is remarkably improved, the synthesis cost is reduced, and the method is suitable for the fields of petrochemical engineering, environmental protection and the like.

Description

Technical Field

[0001] The invention belongs to the technical field of zeolite molecular sieve synthesis, and particularly relates to a method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals. Background Art

[0002] Aluminosilicate minerals are a class of layered minerals primarily composed of silicon oxide (SiO2) and aluminum oxide (Al2O3). Their crystal structure consists of silicon tetrahedral sheets tightly connected by hydrogen bonds with aluminum octahedral sheets, forming a 1:1, non-expandable layered structure. These minerals primarily include kaolin, halloysite, dickite, perlite, and bentonite. They are widely available and inexpensive. The in situ crystallization method for synthesizing zeolites from aluminosilicate minerals uses aluminosilicate minerals as the primary source of silicon and aluminum. In the presence of a directing agent, the silicon and aluminum species in the aluminosilicate minerals undergo in-situ crystallization to form zeolites. Compared to hydrothermal synthesis, this method uses inexpensive aluminosilicate minerals as raw materials, significantly reducing the cost of zeolite synthesis. However, a major limitation of existing methods is the relatively low crystallinity (content) of the synthesized zeolites, which significantly affects their performance, particularly for Y-type and ZSM-5 zeolites.

[0003] Y-type molecular sieve is a zeolite molecular sieve with a faujasite-type crystal structure, an average effective pore size of about 0.74nm, a high silicon-aluminum ratio, strong hydrothermal stability, excellent adsorption selectivity and catalytic activity, and is widely used in the fields of petrochemicals, adsorption separation, environmental protection, and fine chemicals. The synthesis of Y-type zeolite molecular sieve currently mainly adopts a hydrothermal synthesis method, which usually uses water glass as a silicon source and sodium metaaluminate or aluminum salt as an aluminum source, and synthesizes Y-type zeolite molecular sieve through a hydrothermal crystallization process under the action of alkali solution and a directing agent. However, since the raw materials all come from finished chemical reagents, the synthesis cost of Y-type zeolite molecular sieve is relatively high. The synthesis of ZSM-5 zeolite molecular sieve currently mainly adopts a hydrothermal synthesis method, which usually uses water glass as a silicon source and sodium metaaluminate or aluminum salt as an aluminum source, and synthesizes through a hydrothermal crystallization process under the action of alkali and a template. However, since the raw materials all come from finished chemical reagents, the synthesis cost of current ZSM-5 zeolite molecular sieve is increased.

[0004] Therefore, how to improve the crystallinity of the synthesized zeolite molecular sieve is a technical problem currently faced in the field of in-situ crystallization synthesis of zeolite molecular sieves by aluminosilicate minerals. Summary of the Invention

[0005] To address these technical challenges, the present invention aims to provide a method for synthesizing highly crystalline zeolite molecular sieves by in-situ crystallization of aluminosilicate minerals. Compared to existing methods for synthesizing zeolite molecular sieves by in-situ crystallization of aluminosilicate minerals, the present invention significantly improves the crystallinity of the synthesized zeolite molecular sieve, thereby endowing it with excellent application properties.

[0006] In order to achieve the above-mentioned object of the invention, the present invention provides the following technical solutions: The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) Zeolite molecular sieve, NaOH (sodium hydroxide), silicon source, aluminum source and water are mixed and hydrothermally treated, and then filtered. The filtrate obtained is used as the crystal nucleus liquid, and the solid obtained is dried as the solid phase crystal element; (2) mixing the aluminosilicate mineral, the crystal nucleus solution obtained in step (1) and water, drying the mixture, and then calcining the mixture at 850-1000° C. to obtain an active mineral silicon source; (3) mixing the aluminosilicate mineral, the crystal nucleus solution obtained in step (1) and water, drying the mixture, and then calcining the mixture at 650-800° C. to obtain an active mineral aluminum source; (4) The active mineral silicon source obtained in step (2), the active mineral aluminum source obtained in step (3), the added silicon species, NaOH, the template, the crystal nucleus solution obtained in step (1), the solid phase crystal element obtained in step (1) and water are mixed and placed in an autoclave for crystallization, and then filtered, washed and dried to obtain a high-crystallinity zeolite molecular sieve.

[0007] In the step (1), the mass ratio of zeolite molecular sieve (dry basis), NaOH, silicon source (calculated as SiO2), aluminum source (calculated as Al2O3) and water is 1: (0.1-0.3): (0.05-0.5): (0-0.1): (4-8).

[0008] In the step (1), the hydrothermal treatment temperature is 40-160° C., and the hydrothermal treatment time is 4-24 hours.

[0009] In the step (1), the zeolite molecular sieve is a zeolite molecular sieve with a SiO2 / Al2O3 molar ratio of ≥10; the silicon source is at least one of silica sol, silica gel, white carbon black and water glass, preferably water glass; and the aluminum source is at least one of aluminum sulfate, sodium aluminate, aluminum nitrate, pseudo-boehmite, boehmite and aluminum chloride, preferably sodium aluminate.

[0010] The mass ratio of the aluminosilicate mineral, the crystal nucleus liquid and the water in the steps (2) and (3) is: 1: (0.1-0.3): (0.5-1); the aluminosilicate mineral is at least one of kaolin, diatomaceous earth, halloysite, montmorillonite, bentonite, attapulgite, pyrophyllite and perlite.

[0011] The roasting time in step (2) is 1 to 3 hours; the roasting time in step (3) is 1 to 3 hours.

[0012] In the step (4), the dry mass ratio of the active mineral silicon source to the active mineral aluminum source is (1-10): (1-5).

[0013] In the step (4), the total mass (dry basis) of the active mineral silicon source and the active mineral aluminum source, the added silicon species (calculated by SiO2 mass), NaOH, the template, the crystal nucleus solution obtained in the step (1), the solid phase crystal element obtained in the step (1) and the water are in a mass ratio of 1: (0.05~0.5): (0.05~0.3): (0~0.15): (0.05~0.15): (0.01~0.10): (4~8).

[0014] The added silicon species in step (4) is at least one of silica sol, silica gel, white carbon black and water glass, preferably water glass; the template in step (4) is at least one of tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrapropylammonium bromide, n-butylamine, triethylamine and diethylammonium, preferably tetrapropylammonium hydroxide.

[0015] In the step (4), the crystallization temperature is 90-150° C., and the crystallization time is 12-48 hours.

[0016] In the step (1), the zeolite molecular sieve is preferably one of high-silicon USY zeolite molecular sieve and ZSM-5 zeolite molecular sieve.

[0017] In the method of the present invention, the filtering, washing and drying steps adopt technical solutions well known to those skilled in the art and are not particularly limited.

[0018] This method hydrothermally treats high-silicon zeolite molecular sieves (such as USY and ZSM-5) with silicon and aluminum sources under alkaline conditions to partially form the molecular sieve structure. After filtration, the filtrate becomes a nucleation liquid containing microcrystals, and the solid, after drying, becomes solid-phase crystal elements. These two serve as "seeds" for subsequent crystallization. An aluminosilicate mineral is mixed with the nucleation liquid and then calcined at different temperatures: 850-1000°C to generate an active mineral silicon source. At high temperatures, the microcrystals in the nucleation liquid induce the silicon component in the mineral to convert into the target molecular sieve microstructure units; and 650-800°C to generate an active mineral aluminum source. At moderate temperatures, the microcrystals induce the aluminum component in the mineral to convert into the target molecular sieve microstructure units. The active mineral silicon source and aluminum source are then mixed with an external silicon species, an alkali, a template, a nucleation liquid, and solid-phase crystal elements, and crystallized in an autoclave. The pre-set microstructure units, the nucleation liquid, and the solid-phase crystal elements work together to accelerate the nucleation and growth of the target molecular sieve, ultimately forming a highly crystalline product.

[0019] When preparing high-crystalline Y-type zeolite molecular sieve, the high-silicon USY zeolite molecular sieve, a silicon source, and an aluminum source are first hydrothermally treated in an alkaline aqueous solution. During this process, some structural units of the high-silicon USY zeolite molecular sieve dissociate in the alkaline medium. Furthermore, under the guidance of the high-silicon USY molecular sieve structure, the silicon source and the aluminum source undergo a crystallization reaction to form Y-type zeolite molecular sieve microstructure units (crystals). After filtration and separation, a crystal nucleus solution containing a high concentration of Y-type zeolite molecular sieve microcrystals and solid-phase crystals are obtained. Subsequently, an aluminosilicate mineral is mixed with the prepared crystal nucleus solution and water, dried, and calcined to obtain the active mineral silicon source and active mineral aluminum source, respectively. During the above-mentioned roasting process, part of the silicon and aluminum components in the aluminosilicate mineral will generate Y-type molecular sieve microstructure units through solid-phase reaction under the structural mutagenic effect of the USY zeolite molecular sieve microcrystals contained in the crystal nucleus liquid, thereby pre-setting the Y-type molecular sieve microstructure units in the prepared active mineral silicon source and active mineral aluminum source structure; finally, with the active mineral silicon source and active mineral aluminum source of the above-mentioned pre-set Y-type molecular sieve microstructure units as the main silicon and aluminum sources, under the action of external silicon species, NaOH, crystal nucleus liquid and solid phase crystal elements, Y-type zeolite molecular sieve is in situ synthesized through an in-situ crystallization process. In this way, as the inducing crystallization active species, the pre-set Y-type molecular sieve microstructure units in the above-mentioned system and the USY zeolite molecular sieve microcrystals contained in the crystal nucleus liquid and solid phase crystal elements will be able to greatly promote the nucleation, growth and crystallization process of the Y-type zeolite molecular sieve during the in-situ crystallization process, thereby significantly improving the crystallinity of the Y-type zeolite molecular sieve product synthesized by in-situ crystallization of the aluminosilicate mineral, and giving the synthesized Y-type zeolite molecular sieve excellent application performance.

[0020] To prepare high-crystallinity ZSM-5 zeolite, the ZSM-5 zeolite and a silicon source are first hydrothermally treated in an alkaline aqueous solution. During this hydrothermal process, some structural units of the ZSM-5 zeolite dissociate, while the ZSM-5 zeolite structure guides the SiO2 in the silicon source to form ZSM-5 zeolite microstructure units (crystals). After filtration and separation, a nucleus solution containing a high concentration of ZSM-5 zeolite microcrystals and solid-phase crystals are obtained. The aluminosilicate mineral is then mixed with the prepared guiding agent (nucleus solution) and water, dried, and calcined to produce the active mineral silicon source and active mineral aluminum source, respectively. During the calcination process, some of the silicon and aluminum components in the aluminosilicate mineral, guided by the structure of the ZSM-5 zeolite molecular sieve microcrystals contained in the crystal nucleus solution, undergo a solid-phase reaction to form ZSM-5 zeolite molecular sieve microstructure units, thereby pre-setting the ZSM-5 zeolite molecular sieve microstructure units within the structures of the prepared active mineral silicon source and active mineral aluminum source. Finally, using the active mineral silicon source and active mineral aluminum source with the pre-set ZSM-5 zeolite molecular sieve microstructure units as the primary silicon and aluminum sources, and under the action of an external silicon source, NaOH, a template, and a solid-phase crystal element, a ZSM-5 zeolite molecular sieve is synthesized through an in-situ crystallization process. In this way, as active species inducing crystallization, pre-setting ZSM-5 zeolite molecular sieve microstructure units and solid phase crystal elements in the active mineral source will be able to greatly promote the nucleation, growth and crystallization process of ZSM-5 zeolite molecular sieve during the in situ crystallization process, thereby significantly improving the crystallinity of the ZSM-5 zeolite molecular sieve product synthesized by in situ crystallization of aluminosilicate minerals, and will give the synthesized in situ crystallized ZSM-5 zeolite molecular sieve excellent application performance.

[0021] Compared with the prior art, the present invention has the following beneficial effects: (1) By introducing nucleation liquid and solid-phase crystal elements, the nucleation, growth, and crystallization processes of the zeolite molecular sieve are promoted. The crystallinity of the Y-type and ZSM-5 zeolite molecular sieves synthesized by the present invention is significantly higher than that of existing methods. The crystallinity of the Y-type zeolite molecular sieve synthesized by the present invention reaches up to 66%, while the maximum crystallinity of the existing method is 46%; the crystallinity of the ZSM-5 zeolite molecular sieve reaches up to 62%. The high crystallinity gives the zeolite molecular sieve better adsorption selectivity, catalytic activity, and hydrothermal stability, broadening its application in petrochemicals, adsorption separation, environmental protection and other fields.

[0022] (2) The present invention uses widely available and low-cost aluminosilicate minerals (such as kaolin, halloysite, etc.) as the main source of silicon and aluminum, replacing the finished chemical reagents used in traditional hydrothermal synthesis, thereby significantly reducing the cost of raw materials. The present invention can adapt to different types of aluminosilicate minerals and target zeolite molecular sieves by adjusting parameters such as raw material ratio, roasting temperature, and crystallization conditions. BRIEF DESCRIPTION OF THE DRAWINGS

[0023] Figure 1 This is the XRD pattern of the Y-type zeolite molecular sieve (C1) synthesized in Example 1 of the present invention.

[0024] Figure 2 This is the XRD pattern of the Y-type zeolite molecular sieve (D1) synthesized in Comparative Example 1 of the present invention.

[0025] Figure 3 This is the XRD pattern of the ZSM-5 zeolite molecular sieve (C10) synthesized in Example 10 of the present invention.

[0026] Figure 4 This is the XRD pattern of the ZSM-5 zeolite molecular sieve (D4) synthesized in Comparative Example 4 of the present invention. DETAILED DESCRIPTION

[0027] The technical solutions of the present invention will be described clearly and completely below in conjunction with the embodiments of the present invention.

[0028] USY zeolite molecular sieve: Nankai University Catalyst Plant; ZSM-5 zeolite molecular sieve: Nankai University Catalyst Plant.

[0029] (1) Raw material specifications Kaolin (solid content 85.6%), halloysite (solid content 86.7%), bentonite (solid content 76.8%), USY zeolite molecular sieve (solid content 89.7%, SiO2 / Al2O3=11), ZSM-5 zeolite molecular sieve (solid content 89.7%, SiO2 / Al2O3=40), water glass (modulus 3.3, SiO2 content 20%) and directing agent (15SiO2:Al2O3:15Na2O:320H2O), qualified industrial products.

[0030] Sodium hydroxide (NaOH) and sodium metaaluminate (NaAlO2, Al2O3 content 62%) were analytically pure reagents purchased from Sinopharm Chemical Reagent Co., Ltd.; tetrapropylammonium hydroxide (TPAOH) was analytically pure reagent purchased from Sinopharm Chemical Reagent Co., Ltd.

[0031] (2) Analysis and testing The phase and crystallinity of the product were analyzed and tested on a D / max-2200PC X-ray diffractometer produced by Rigaku Corporation of Japan.

[0032] Example 1 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 50 g of USY zeolite molecular sieve (dry basis), 5 g of NaOH, 25 g of water glass, 0.81 g of sodium metaaluminate and 200 g of water were mixed and hydrothermally treated (40 ° C, 24 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of kaolin (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 850° C. for 3 h to obtain an active mineral silicon source; (3) 1000 g of kaolin (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 800° C. for 1 h to obtain an active mineral aluminum source; (4) 250 g of the active mineral silicon source (dry basis) obtained in step (2), 250 g of the active mineral aluminum source (dry basis) obtained in step (3), 250 g of water glass, 25 g of NaOH, 25 g of the crystal nucleus solution obtained in step (1), 12.5 g of the solid phase crystal element obtained in step (1) and 2000 g of water were mixed and placed in an autoclave for crystallization (90°C, 48 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C1.

[0033] Example 2 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 70 g USY zeolite molecular sieve (dry basis), 14 g NaOH, 105 g water glass, 5.65 g sodium aluminate and 420 g water were mixed and hydrothermally treated (70 ° C, 12 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of kaolin (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 900° C. for 2 h to obtain an active mineral silicon source; (3) 1000 g of kaolin (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 700 ° C for 2 h to obtain an active mineral aluminum source; (4) 300 g of the active mineral silicon source (dry basis) obtained in step (2), 200 g of the active mineral aluminum source (dry basis) obtained in step (3), 500 g of water glass, 50 g of NaOH, 50 g of the crystal nucleus solution obtained in step (1), 25 g of the solid phase crystal element obtained in step (1) and 3000 g of water were mixed and placed in an autoclave for crystallization (110° C., 24 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C2.

[0034] Example 3 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 90 g USY zeolite molecular sieve (dry basis), 27 g NaOH, 225 g water glass, 14.52 g sodium aluminate and 720 g water were mixed and hydrothermally treated (95 ° C, 4 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of kaolin (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 1000° C. for 1 h to obtain an active mineral silicon source; (3) 1000 g of kaolin (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 650° C. for 3 h to obtain an active mineral aluminum source; (4) 350 g of the active mineral silicon source (dry basis) obtained in step (2), 150 g of the active mineral aluminum source (dry basis) obtained in step (3), 750 g of water glass, 100 g of NaOH, 75 g of the crystal nucleus solution obtained in step (1), 50 g of the solid phase crystal element obtained in step (1) and 4000 g of water were mixed and placed in an autoclave for crystallization (130° C., 16 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C3.

[0035] Example 4 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 50 g of USY zeolite molecular sieve (dry basis), 7 g of NaOH, 75 g of water glass, 4.03 g of sodium aluminate and 300 g of water were mixed and hydrothermally treated (70 ° C, 12 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of halloysite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 900° C. for 2 h to obtain an active mineral silicon source; (3) 1000 g of halloysite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 700° C. for 2 h to obtain an active mineral aluminum source; (4) 300 g of the active mineral silicon source (dry basis) obtained in step (2), 200 g of the active mineral aluminum source (dry basis) obtained in step (3), 500 g of water glass, 50 g of NaOH, 50 g of the crystal nucleus solution obtained in step (1), 25 g of the solid phase crystal element obtained in step (1) and 3000 g of water were mixed and placed in an autoclave for crystallization (110° C., 24 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C4.

[0036] Example 5 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 70 g USY zeolite molecular sieve (dry basis), 18 g NaOH, 175 g water glass, 11.29 g sodium aluminate and 560 g water were mixed and hydrothermally treated (95 ° C, 4 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of halloysite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 1000° C. for 1 h to obtain an active mineral silicon source; (3) 1000 g of halloysite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and calcined at 650° C. for 3 h to obtain an active mineral aluminum source; (4) 350 g of the active mineral silicon source (dry basis) obtained in step (2), 150 g of the active mineral aluminum source (dry basis) obtained in step (3), 750 g of water glass, 100 g of NaOH, 75 g of the crystal nucleus solution obtained in step (1), 50 g of the solid phase crystal element obtained in step (1) and 4000 g of water were mixed and placed in an autoclave for crystallization (130° C., 16 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C5.

[0037] Example 6 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 90 g of USY zeolite molecular sieve (dry basis), 15 g of NaOH, 45 g of water glass, 1.45 g of sodium aluminate and 360 g of water were mixed and hydrothermally treated (40 ° C, 24 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of halloysite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 850° C. for 3 h to obtain an active mineral silicon source; (3) 1000 g of halloysite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and calcined at 800° C. for 1 h to obtain an active mineral aluminum source; (4) 250 g of the active mineral silicon source (dry basis) obtained in step (2), 250 g of the active mineral aluminum source (dry basis) obtained in step (3), 250 g of water glass, 25 g of NaOH, 25 g of the crystal nucleus solution obtained in step (1), 12.5 g of the solid phase crystal element obtained in step (1) and 2000 g of water were mixed and placed in an autoclave for crystallization (90°C, 48 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C6.

[0038] Example 7 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 50 g of USY zeolite molecular sieve (dry basis), 9 g of NaOH, 125 g of water glass, 8.06 g of sodium aluminate and 400 g of water were mixed and hydrothermally treated (95 ° C, 4 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of bentonite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 1000° C. for 1 h to obtain an active mineral silicon source; (3) 1000 g of bentonite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and calcined at 650° C. for 3 h to obtain an active mineral aluminum source; (4) 350 g of the active mineral silicon source (dry basis) obtained in step (2), 150 g of the active mineral aluminum source (dry basis) obtained in step (3), 750 g of water glass, 100 g of NaOH, 75 g of the crystal nucleus solution obtained in step (1), 50 g of the solid phase crystal element obtained in step (1) and 4000 g of water were mixed and placed in an autoclave for crystallization (130° C., 16 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C7.

[0039] Example 8 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 70 g USY zeolite molecular sieve (dry basis), 10 g NaOH, 35 g water glass, 1.13 g sodium aluminate and 280 g water were mixed and hydrothermally treated (40 ° C, 24 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of bentonite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 850° C. for 3 h to obtain an active mineral silicon source; (3) 1000 g of bentonite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and then calcined at 800° C. for 1 h to obtain an active mineral aluminum source; (4) 250 g of the active mineral silicon source (dry basis) obtained in step (2), 250 g of the active mineral aluminum source (dry basis) obtained in step (3), 250 g of water glass, 25 g of NaOH, 25 g of the crystal nucleus solution obtained in step (1), 12.5 g of the solid phase crystal element obtained in step (1) and 2000 g of water were mixed and placed in an autoclave for crystallization (90°C, 48 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C8.

[0040] Example 9 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 90 g of USY zeolite molecular sieve (dry basis), 21 g of NaOH, 135 g of water glass, 7.26 g of sodium aluminate and 540 g of water were mixed and hydrothermally treated (70 ° C, 12 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of bentonite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 900° C. for 2 h to obtain an active mineral silicon source; (3) 1000 g of bentonite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 700° C. for 2 h to obtain an active mineral aluminum source; (4) 300 g of the active mineral silicon source (dry basis) obtained in step (2), 200 g of the active mineral aluminum source (dry basis) obtained in step (3), 500 g of water glass, 50 g of NaOH, 50 g of the crystal nucleus solution obtained in step (1), 25 g of the solid phase crystal element obtained in step (1) and 3000 g of water were mixed and placed in an autoclave for crystallization (110° C., 24 h), and then filtered, washed and dried to obtain the Y-type zeolite molecular sieve C9.

[0041] Example 10 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 50 g ZSM-5 zeolite molecular sieve (dry basis), 5 g NaOH, 25 g water glass and 200 g water were mixed and placed in an autoclave for hydrothermal treatment (80 ° C, 24 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of kaolin (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 850° C. for 3 h to obtain an active mineral silicon source; (3) 1000 g of kaolin (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 800° C. for 1 h to obtain an active mineral aluminum source; (4) 900 g of the active mineral silicon source (dry basis) obtained in step (2), 100 g of the active mineral aluminum source (dry basis) obtained in step (3), 500 g of water glass, 100 g of NaOH, 50 g of TPAOH, 10 g of the solid phase crystal element obtained in step (1) and 4000 g of water were mixed and placed in an autoclave for crystallization (100° C., 48 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C10.

[0042] Example 11 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 75 g of ZSM-5 zeolite molecular sieve (dry basis), 15 g of NaOH, 112.5 g of water glass and 450 g of water were mixed and placed in an autoclave for hydrothermal treatment (130 ° C, 12 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of kaolin (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 900° C. for 2 h to obtain an active mineral silicon source; (3) 1000 g of kaolin (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 700 ° C for 2 h to obtain an active mineral aluminum source; (4) 750 g of the active mineral silicon source (dry basis) obtained in step (2), 250 g of the active mineral aluminum source (dry basis) obtained in step (3), 1500 g of water glass, 200 g of NaOH, 100 g of TPAOH, 50 g of the solid phase crystal element obtained in step (1) and 6000 g of water were mixed and placed in an autoclave for crystallization (120° C., 24 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C11.

[0043] Example 12 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 100 g of ZSM-5 zeolite molecular sieve, 30 g of NaOH, 250 g of water glass and 800 g of water were mixed and placed in an autoclave for hydrothermal treatment (160 ° C, 6 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of kaolin (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 1000° C. for 1 h to obtain an active mineral silicon source; (3) 1000 g of kaolin (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 650° C. for 3 h to obtain an active mineral aluminum source; (4) 600 g of the active mineral silicon source (dry basis) obtained in step (2), 400 g of the active mineral aluminum source (dry basis) obtained in step (3), 2500 g of water glass, 300 g of NaOH, 150 g of TPAOH, 100 g of the solid phase crystal element obtained in step (1) and 8000 g of water were mixed and placed in an autoclave for crystallization (150° C., 12 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C12.

[0044] Example 13 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 50 g ZSM-5 zeolite molecular sieve (dry basis), 10 g NaOH, 75 g water glass and 300 g water were mixed and placed in an autoclave for hydrothermal treatment (130 ° C, 12 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of halloysite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 900° C. for 2 h to obtain an active mineral silicon source; (3) 1000 g of halloysite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 700° C. for 2 h to obtain an active mineral aluminum source; (4) 750 g of the active mineral silicon source (dry basis) obtained in step (2), 250 g of the active mineral aluminum source (dry basis) obtained in step (3), 1500 g of water glass, 200 g of NaOH, 100 g of TPAOH, 50 g of the solid phase crystal element obtained in (1) and 6000 g of water were mixed and placed in an autoclave for crystallization (130° C., 24 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C13.

[0045] Example 14 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 75 g ZSM-5 zeolite molecular sieve (dry basis), 22.5 g NaOH, 187.5 g water glass and 600 g water were mixed and placed in an autoclave for hydrothermal treatment (160 ° C, 6 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of halloysite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 1000° C. for 1 h to obtain an active mineral silicon source; (3) 1000 g of halloysite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and calcined at 650° C. for 3 h to obtain an active mineral aluminum source; (4) 600 g of the active mineral silicon source (dry basis) obtained in step (2), 400 g of the active mineral aluminum source (dry basis) obtained in step (3), 2500 g of water glass, 300 g of NaOH, 150 g of TPAOH, 100 g of the solid phase crystal element obtained in step (1) and 8000 g of water were mixed and placed in an autoclave for crystallization (150° C., 12 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C14.

[0046] Example 15 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 100 g ZSM-5 zeolite molecular sieve (dry basis), 10 g NaOH, 50 g water glass and 400 g water were mixed and placed in an autoclave for hydrothermal treatment (80 ° C, 24 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of halloysite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 850° C. for 3 h to obtain an active mineral silicon source; (3) 1000 g of halloysite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and calcined at 800° C. for 1 h to obtain an active mineral aluminum source; (4) 900 g of the active mineral silicon source (dry basis) obtained in step (2), 100 g of the active mineral aluminum source (dry basis) obtained in step (3), 500 g of water glass, 100 g of NaOH, 50 g of TPAOH, 10 g of the solid phase crystal element obtained in step (1) and 4000 g of water were mixed and placed in an autoclave for crystallization (100° C., 48 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C15.

[0047] Example 16 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 50 g ZSM-5 zeolite molecular sieve (dry basis), 15 g NaOH, 125 g water glass and 400 g water were mixed and placed in an autoclave for hydrothermal treatment (160 ° C, 6 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of bentonite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and then calcined at 1000° C. for 1 h to obtain an active mineral silicon source; (3) 1000 g of bentonite (dry basis), 300 g of the crystal nucleus solution obtained in step (1) and 1000 g of water were mixed, dried and calcined at 650° C. for 3 h to obtain an active mineral aluminum source; (4) 600 g of the active mineral silicon source (dry basis) obtained in step (2), 400 g of the active mineral aluminum source (dry basis) obtained in step (3), 2500 g of water glass, 300 g of NaOH, 150 g of TPAOH, 100 g of the solid phase crystal element obtained in step (1) and 8000 g of water were mixed and placed in an autoclave for crystallization (150° C., 12 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C16.

[0048] Example 17 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 75 g ZSM-5 zeolite molecular sieve (dry basis), 7.5 g NaOH, 37.5 g water glass and 300 g water were mixed and placed in an autoclave for hydrothermal treatment (80 ° C, 24 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of bentonite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and calcined at 850° C. for 3 h to obtain an active mineral silicon source; (3) 1000 g of bentonite (dry basis), 100 g of the crystal nucleus solution obtained in step (1) and 500 g of water were mixed, dried and then calcined at 800° C. for 1 h to obtain an active mineral aluminum source; (4) 900 g of the active mineral silicon source (dry basis) obtained in step (2), 100 g of the active mineral aluminum source (dry basis) obtained in step (3), 500 g of water glass, 100 g of NaOH, 50 g of TPAOH, 10 g of the solid phase crystal element obtained in step (1) and 4000 g of water were mixed and placed in an autoclave for crystallization (100° C., 48 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C17.

[0049] Example 18 A method for synthesizing a high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals comprises the following steps: (1) 100 g ZSM-5 zeolite molecular sieve (dry basis), 20 g NaOH, 150 g water glass and 600 g water were mixed and placed in an autoclave for hydrothermal treatment (130 ° C, 12 h), and then filtered. The filtrate was used as the crystal nucleus liquid, and the solid was dried as the solid phase crystal element; (2) 1000 g of bentonite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 900° C. for 2 h to obtain an active mineral silicon source; (3) 1000 g of bentonite (dry basis), 200 g of the crystal nucleus solution obtained in step (1) and 700 g of water were mixed, dried and then calcined at 700° C. for 2 h to obtain an active mineral aluminum source; (4) 750 g of the active mineral silicon source (dry basis) obtained in step (2), 250 g of the active mineral aluminum source (dry basis) obtained in step (3), 1500 g of water glass, 200 g of NaOH, 100 g of TPAOH, 50 g of the solid phase crystal element obtained in step (1) and 6000 g of water were mixed and placed in an autoclave for crystallization (130° C., 24 h), and then filtered, washed and dried to obtain the ZSM-5 zeolite molecular sieve C18.

[0050] Comparative Example 1 The method of zeolite molecular sieve comprises the following steps: (1) Calcinate 1000 g of kaolin (dry basis) at 850°C for 3 h to obtain an active mineral silicon source; (2) Calcinate 1000 g of kaolin (dry basis) at 800 °C for 1 h to obtain an active mineral aluminum source; (3) 250 g of the active mineral silicon source (dry basis) obtained in step (1), 250 g of the active mineral aluminum source (dry basis) obtained in step (2), 250 g of water glass, 25 g of NaOH, 25 g of a directing agent and 2000 g of water were mixed and placed in an autoclave for crystallization (90°C, 48 h). The mixture was then filtered, washed and dried to obtain the comparative Y-type zeolite molecular sieve D1.

[0051] Comparative Example 2 The method of zeolite molecular sieve comprises the following steps: (1) Calcinate 1000 g of halloysite (dry basis) at 900 °C for 2 h to obtain an active mineral silicon source; (2) Calcinate 1000 g of halloysite (dry basis) at 700 °C for 2 h to obtain an active mineral aluminum source; (3) 300 g of the active mineral silicon source (dry basis) obtained in step (1), 200 g of the active mineral aluminum source (dry basis) obtained in step (2), 500 g of water glass, 50 g of NaOH, 50 g of a directing agent and 3000 g of water were mixed and placed in an autoclave for crystallization (110°C, 24 h). The mixture was then filtered, washed and dried to obtain a comparative Y-type zeolite molecular sieve D2.

[0052] Comparative Example 3 The method of zeolite molecular sieve comprises the following steps: (1) Calcinate 1000 g of bentonite (dry basis) at 1000°C for 1 h to obtain an active mineral silicon source; (2) Calcinate 1000 g of bentonite (dry basis) at 650°C for 3 h to obtain an active mineral aluminum source; (3) 350 g of the active mineral silicon source (dry basis) obtained in step (1), 150 g of the active mineral aluminum source (dry basis) obtained in step (2), 750 g of water glass, 100 g of NaOH, 75 g of a directing agent and 4000 g of water were mixed and placed in an autoclave for crystallization (130° C., 16 h). The mixture was then filtered, washed and dried to obtain comparative Y-type zeolite molecular sieve D3.

[0053] Comparative Example 4 The method of zeolite molecular sieve comprises the following steps: (1) Calcinate 1000 g of kaolin (dry basis) at 850°C for 3 h to obtain an active mineral silicon source; (2) Calcinate 1000 g of kaolin (dry basis) at 800 °C for 1 h to obtain an active mineral aluminum source; (3) 900 g of the active mineral silicon source (dry basis) obtained in step (1), 100 g of the active mineral aluminum source (dry basis) obtained in step (2), 500 g of water glass, 100 g of NaOH, 50 g of TPAOH and 4000 g of water were mixed and placed in an autoclave for crystallization (100°C, 48 h). The mixture was then filtered, washed and dried to obtain the comparative ZSM-5 zeolite molecular sieve D4.

[0054] Comparative Example 5 The method of zeolite molecular sieve comprises the following steps: (1) Calcinate 1000 g of halloysite (dry basis) at 900 °C for 2 h to obtain an active mineral silicon source; (2) Calcinate 1000 g of halloysite (dry basis) at 700 °C for 2 h to obtain an active mineral aluminum source; (3) 750 g of the active mineral silicon source (dry basis) obtained in step (1), 250 g of the active mineral aluminum source (dry basis) obtained in step (2), 1500 g of water glass, 200 g of NaOH, 100 g of TPAOH and 6000 g of water were mixed and placed in an autoclave for crystallization (130°C, 24 h). The mixture was then filtered, washed and dried to obtain the comparative ZSM-5 zeolite molecular sieve D5.

[0055] Comparative Example 6 The method of zeolite molecular sieve comprises the following steps: (1) Calcinate 1000 g of bentonite (dry basis) at 1000°C for 1 h to obtain an active mineral silicon source; (2) Calcinate 1000 g of bentonite (dry basis) at 650°C for 3 h to obtain an active mineral aluminum source; (3) 600 g of the active mineral silicon source (dry basis) obtained in step (1), 400 g of the active mineral aluminum source (dry basis) obtained in step (2), 2500 g of water glass, 300 g of NaOH, 150 g of TPAOH and 8000 g of water were mixed and placed in an autoclave for crystallization (150°C, 12 h). The mixture was then filtered, washed and dried to obtain the comparative ZSM-5 zeolite molecular sieve D6.

[0056] The XRD pattern of Y-type zeolite molecular sieve (C1) synthesized in Example 1 is as follows: Figure 1 shown.

[0057] The XRD pattern of Y-type zeolite molecular sieve (D1) synthesized in Comparative Example 1 is as follows: Figure 2 shown.

[0058] The XRD pattern of the ZSM-5 zeolite molecular sieve (C10) synthesized in Example 10 is as follows: Figure 3 shown.

[0059] The XRD pattern of ZSM-5 zeolite molecular sieve (D4) synthesized in Comparative Example 4 is as follows: Figure 4 shown.

[0060] The crystallinity of the Y-type zeolite molecular sieves synthesized in Examples 1 to 9 and Comparative Examples 1 to 3 is shown in Table 1.

[0061] The crystallinity of the ZSM-5 zeolite molecular sieves synthesized in Examples 10 to 18 and Comparative Examples 4 to 6 is shown in Table 2.

[0062] Table 1: Crystallinity of Y-type zeolite molecular sieves synthesized in Examples 1 to 9 and Comparative Examples 1 to 3

[0063] As shown in Table 1, compared with the existing method for synthesizing Y-type zeolite molecular sieve, the Y-type zeolite molecular sieve synthesized by the method of the present invention has significantly higher crystallinity, indicating that the method of the present invention can significantly increase the crystallinity of Y-type zeolite molecular sieve synthesized by in situ crystallization of aluminosilicate minerals, thereby giving the synthesized Y-type zeolite molecular sieve excellent application performance.

[0064] Table 2: Crystallinity of ZSM-5 zeolite molecular sieves synthesized in Examples 10 to 18 and Comparative Examples 4 to 6

[0065] As shown in Table 2, compared with the existing method for synthesizing ZSM-5 zeolite molecular sieve, the ZSM-5 zeolite molecular sieve synthesized by the method of the present invention has a significantly higher crystallinity, indicating that the method of the present invention can significantly increase the crystallinity of ZSM-5 zeolite molecular sieve synthesized by in situ crystallization of aluminosilicate minerals, thereby giving the synthesized ZSM-5 zeolite molecular sieve excellent application performance.

Claims

1. A method for synthesizing high-crystallinity zeolite molecular sieves by in-situ crystallization of aluminosilicate minerals, characterized in that: The following steps are involved: (1) Zeolite molecular sieve, NaOH, silicon source, aluminum source and water are mixed and hydrothermally treated, and then filtered. The obtained filtrate is used as the crystal nucleus liquid, and the obtained solid is dried as the solid phase crystal element; (2) mixing the aluminosilicate mineral, the crystal nucleus solution obtained in step (1) and water, drying the mixture, and then calcining the mixture at 850-1000° C. to obtain an active mineral silicon source; (3) mixing the aluminosilicate mineral, the crystal nucleus solution obtained in step (1) and water, drying the mixture, and then calcining the mixture at 650-800° C. to obtain an active mineral aluminum source; (4) The active mineral silicon source obtained in step (2), the active mineral aluminum source obtained in step (3), the added silicon species, NaOH, the template, the crystal nucleus solution obtained in step (1), the solid phase crystal element obtained in step (1) and water are mixed and placed in an autoclave for crystallization, and then filtered, washed and dried to obtain a high-crystallinity zeolite molecular sieve.

2. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: In the step (1), the mass ratio of zeolite molecular sieve, NaOH, silicon source, aluminum source and water is 1: (0.1-0.3): (0.05-0.5): (0-0.1): (4-8).

3. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: In the step (1), the hydrothermal treatment temperature is 40-160° C., and the hydrothermal treatment time is 4-24 hours.

4. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: In the step (1), the zeolite molecular sieve is a zeolite molecular sieve with a SiO2 / Al2O3 molar ratio of ≥10; the silicon source is at least one of silica sol, silica gel, white carbon black and water glass; and the aluminum source is at least one of aluminum sulfate, sodium metaaluminate, aluminum nitrate, pseudo-boehmite, boehmite and aluminum chloride.

5. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: The mass ratio of the aluminosilicate mineral, the crystal nucleus liquid and the water in the steps (2) and (3) is: 1: (0.1-0.3): (0.5-1); the aluminosilicate mineral is at least one of kaolin, diatomaceous earth, halloysite, montmorillonite, bentonite, attapulgite, pyrophyllite and perlite.

6. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: The roasting time in step (2) is 1 to 3 hours; the roasting time in step (3) is 1 to 3 hours.

7. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: In the step (4), the dry mass ratio of the active mineral silicon source to the active mineral aluminum source is (1-10): (1-5).

8. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: In the step (4), the total mass ratio of the active mineral silicon source and the active mineral aluminum source, the added silicon species, NaOH, the template, the crystal nucleus solution obtained in the step (1), the solid phase crystal element obtained in the step (1) and water is 1: (0.05~0.5): (0.05~0.3): (0~0.15): (0.05~0.15): (0.01~0.10): (4~8).

9. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: The added silicon species in step (4) is at least one of silica sol, silica gel, white carbon black and water glass; the template in step (4) is at least one of tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrapropylammonium bromide, n-butylamine, triethylamine and diethylammonium.

10. The method for synthesizing high-crystallinity zeolite molecular sieve by in-situ crystallization of aluminosilicate minerals according to claim 1, characterized in that: In the step (4), the crystallization temperature is 90-150° C., and the crystallization time is 12-48 hours.

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