A particle of sodalite molecular sieve with multi-level pore channels and a preparation method and application thereof

Abstract

This invention provides a hierarchical interconnected sodalite molecular sieve particle, its preparation method, and its application, belonging to the field of molecular sieve technology. The preparation method of the hierarchical interconnected sodalite molecular sieve particle provided by this invention includes the following steps: mixing an aluminum source, an alkali source, a silicon source, a first solvent, and a mesoporous template agent to obtain a silica-alumina gel solution; aging and drying the silica-alumina gel solution sequentially to obtain a silica-alumina dry gel; mixing the silica-alumina dry gel, a molding aid, and a second solvent, and kneading to obtain silica-alumina gel particles; and crystallizing and calcining the silica-alumina gel particles sequentially to obtain hierarchical interconnected sodalite molecular sieve particles. This invention uses a dry gel conversion method to synthesize microporous sodalite crystals; introduces a mesoporous template agent using a hard template method, forming mesopores after calcination; and removes the molding aid and mesoporous template agent by calcination to form macropores, thus obtaining hierarchical interconnected sodalite molecular sieve particles, while avoiding the adverse effects of the molding aid.

Description

Technical Field

[0001] This invention belongs to the field of molecular sieve technology, specifically relating to a multi-level interconnected sodalite molecular sieve particle, its preparation method, and its application. Background Technology

[0002] Sodalite is a microporous molecular sieve with an SOD cage (β-cage) framework structure and a pore size of [missing information]. Because the pore size of sodalite molecular sieves is related to the dynamic diameter of hydrogen molecules... Similarly, sodalite molecular sieves are not only a suitable microporous material for hydrogen storage, but also a promising sulfur-resistant hydrogenation catalyst.

[0003] Currently, sodalite molecular sieves are mainly synthesized using a hydrothermal method, producing crystalline powders typically ranging from a few nanometers to tens of micrometers in size. To avoid problems such as dust accumulation, high pressure drop, operational inconvenience, and even shutdowns in fixed-bed processes, and to meet the demands of sodalite molecular sieves for hydrogen storage and sulfur-resistant hydrogenation catalysis, the powdered crystals must be formed into particles with a certain mechanical strength. During the forming process, forming aids (such as clay and alumina) can clog the pores of the sodalite molecular sieve particles, reducing or even hindering the diffusion of guest molecules within them. Current processes for preparing sodalite molecular sieve particles by mixing powdered crystals with forming aids significantly impact the hydrogen storage performance or sulfur-resistant hydrogenation catalytic activity of the sodalite molecular sieve. This is because sodalite molecular sieves are microporous materials with pore sizes ranging from a few nanometers to tens of micrometers. Only related to the dynamic diameter of hydrogen molecules Similarly, the presence of molding aids can significantly reduce or even hinder the diffusion of hydrogen molecules within sodalite molecular sieve particles. Therefore, how to avoid the adverse effects of molding aids while simultaneously preparing sodalite molecular sieves with interconnected hierarchical pores has become a pressing technical challenge in this field. Summary of the Invention

[0004] The purpose of this invention is to provide a sodalite molecular sieve particle with interconnected hierarchical channels, its preparation method, and its application. The preparation method provided by this invention not only avoids the adverse effects of molding aids but also enables the preparation of sodalite molecular sieve particles with interconnected hierarchical channels.

[0005] To achieve the above-mentioned objectives, the present invention provides the following technical solution:

[0006] This invention provides a method for preparing sodalite molecular sieve particles with interconnected multi-level pores, comprising the following steps:

[0007] (1) Mix aluminum source, alkali source, silicon source, first solvent and mesoporous template agent to obtain a silica-alumina gel solution;

[0008] (2) The silica-alumina adhesive solution obtained in step (1) is aged and dried sequentially to obtain silica-alumina dry adhesive;

[0009] (3) Mix the silicon-aluminum dry adhesive, molding aid and second solvent obtained in step (2) and knead them to form silicon-aluminum adhesive particles.

[0010] (4) The silica-alumina gel particles obtained in step (3) are crystallized and calcined in sequence to obtain sodalite molecular sieve particles with multi-level interconnected channels.

[0011] Preferably, the mesoporous template agent in step (1) is at least one of starch, glucose, polyethylene glycol, carbon nanotubes, carbon nanofibers, nano-carbon molecular sieves, carbon black, and carbon aerogel.

[0012] Preferably, the mass of the mesopore template agent in step (1) is 0.01 to 10% of the total mass of the aluminum source, alkali source and silicon source.

[0013] Preferably, in step (1), the molar ratio of SiO2 to Al2O3 in the aluminosilicate solution is 0.5 to 30, the molar ratio of Na2O to SiO2 in the aluminosilicate solution is 0.5 to 25, and the molar ratio of H2O to SiO2 in the aluminosilicate solution is 20 to 500.

[0014] Preferably, the aging temperature in step (2) is 10 to 100°C, and the aging time is 0.5 to 60 hours.

[0015] Preferably, the molding aid in step (3) is at least one of carboxymethyl cellulose, polyethylene glycol, polyethylene, polypropylene and polyacrylic acid.

[0016] Preferably, the crystallization temperature in step (4) is 100–260°C, and the crystallization time is 1–60 h; the crystallization is carried out in a reaction vessel; during the crystallization, deionized water or a mixture of deionized water and volatile substances is added to the bottom of the reaction vessel; the mass of the deionized water and the mass of the mixture of deionized water and volatile substances are independently 10–10000% of the mass of the silica-alumina gel particles.

[0017] Preferably, the calcination temperature in step (4) is 300-800℃ and the calcination time is 5-25h.

[0018] The present invention also provides sodalite molecular sieve particles with interconnected multi-level pores prepared by the preparation method described above, wherein the pore size includes micropores, mesopores and macropores.

[0019] The present invention also provides the application of the sodalite molecular sieve particles with multi-level interconnected channels described in the above technical solution in hydrogen storage and sulfur-resistant hydrogenation catalysis.

[0020] This invention provides a method for preparing sodalite molecular sieve particles with interconnected hierarchical pores, comprising the following steps: mixing an aluminum source, an alkali source, a silicon source, a first solvent, and a mesoporous template agent to obtain a silica-alumina gel solution; aging and drying the silica-alumina gel solution sequentially to obtain a silica-alumina dry gel; mixing the silica-alumina dry gel, a molding aid, and a second solvent, and kneading to obtain silica-alumina gel particles; and crystallizing and calcining the silica-alumina gel particles sequentially to obtain sodalite molecular sieve particles with interconnected hierarchical pores. This invention uses a dry gel conversion method to synthesize sodalite crystals with micropores; introduces a mesoporous template agent using a hard template method, which forms mesopores after calcination; removes the molding aid and mesoporous template agent by calcination, forming macropores, thereby obtaining sodalite molecular sieve particles with interconnected hierarchical pores, while avoiding the adverse effects of the molding aid. Experimental results show that the sodalite molecular sieve particles with interconnected hierarchical pores provided by this invention have both mesopores and macropores. Attached Figure Description

[0021] Figure 1 X-ray diffraction patterns of the hierarchical channel-connected sodalite molecular sieve particles prepared in Examples 1-3;

[0022] Figure 2 SEM image of the surface of the sodalite molecular sieve particles with interconnected hierarchical pores prepared in Example 1.

[0023] Figure 3 SEM image of a cross section of the sodalite molecular sieve particles with interconnected hierarchical channels prepared in Example 1.

[0024] Figure 4 The attached figures show the BET isothermal adsorption-desorption of the sodalite molecular sieve particles with interconnected hierarchical channels prepared in Examples 1-3.

[0025] Figure 5 The images show the pore size distribution of the multi-level interconnected sodalite molecular sieve particles prepared in Examples 1-3 using mercury intrusion porosimetry. Detailed Implementation

[0026] This invention provides a method for preparing sodalite molecular sieve particles with interconnected multi-level pores, comprising the following steps:

[0027] (1) Mix aluminum source, alkali source, silicon source, first solvent and mesoporous template agent to obtain a silica-alumina gel solution;

[0028] (2) The silica-alumina adhesive solution obtained in step (1) is aged and dried sequentially to obtain silica-alumina dry adhesive;

[0029] (3) Mix the silicon-aluminum dry adhesive, molding aid and second solvent obtained in step (2) and knead them to form silicon-aluminum adhesive particles.

[0030] (4) The silica-alumina gel particles obtained in step (3) are crystallized and calcined in sequence to obtain sodalite molecular sieve particles with multi-level interconnected channels.

[0031] This invention does not impose any special restrictions on the source of the raw materials; commercially available products familiar to those skilled in the art can be used.

[0032] In this invention, the terms "first" and "second" have no special meaning and are only used to distinguish the raw materials.

[0033] This invention mixes an aluminum source, an alkali source, a silicon source, a first solvent, and a mesoporous template agent to obtain a silica-alumina gel solution.

[0034] In this invention, the aluminum source is preferably at least one of sodium aluminate, aluminum hydroxide, aluminum isopropoxide, aluminum sulfate, and aluminum powder; the alkali source is preferably at least one of sodium hydroxide, sodium carbonate, and sodium ethoxide; the silicon source is preferably at least one of silica sol, silicic acid, silicon dioxide, ethyl silicate, and sodium silicate; and the mesoporous template agent is preferably at least one of starch, glucose, polyethylene glycol, carbon nanotubes, carbon nanofibers, nano-carbon molecular sieves, carbon black, and carbon aerogel.

[0035] The present invention does not impose any special limitation on the size of the mesoporous template agent; any substance well known to those skilled in the art can be used.

[0036] The present invention does not impose any particular limitation on the molecular weight of the polyethylene glycol, and any polyethylene glycol well known to those skilled in the art can be used.

[0037] In this invention, the mass of the mesoporous template agent is preferably 0.01-10% of the total mass of the aluminum source, alkali source, and silicon source, more preferably 0.1-10%, and even more preferably 0.5-5%. By limiting the mass of the mesoporous template agent within the above range, this invention can further increase the proportion of mesopores in the sodalite molecular sieve particles with interconnected multi-level pores.

[0038] As one implementation, the mass of the mesoporous template agent can be 1%, 1.5%, 2%, 3%, or 4% of the total mass of the aluminum source, alkali source, and silicon source.

[0039] In this invention, the first solvent is preferably an inorganic solvent; the inorganic solvent is preferably deionized water. This invention does not have a specific limitation on the amount of the first solvent used, as long as it completely dissolves the raw materials.

[0040] The present invention does not have any special limitations on the operation of mixing the aluminum source, alkali source, silicon source, first solvent and mesoporous template agent, and any technical solution for preparing the mixture well known to those skilled in the art can be used.

[0041] In this invention, the molar ratio of SiO2 to Al2O3 in the aluminosilicate solution is preferably 0.5 to 30, more preferably 1 to 10; the molar ratio of Na2O to SiO2 in the aluminosilicate solution is preferably 0.5 to 25, more preferably 1 to 20; and the molar ratio of H2O to SiO2 in the aluminosilicate solution is preferably 20 to 500, more preferably 26 to 200.

[0042] In one embodiment, the molar ratio of SiO2 to Al2O3 in the aluminosilicate solution can be 2, 3, 4, 5, 6, 7, 8, or 9; the molar ratio of Na2O to SiO2 in the aluminosilicate solution can be 1.3 to 20, or even 3 to 12; the molar ratio of H2O to SiO2 in the aluminosilicate solution can be 30 to 150, or even 60 to 100.

[0043] In one embodiment, the molar ratio of SiO2, Al2O3, Na2O and H2O in the silica-alumina gel solution can be 2:1:6:120 or 3:1:4:80.

[0044] After obtaining the silica-alumina adhesive solution, the present invention sequentially ages and dries the silica-alumina adhesive solution to obtain silica-alumina dry adhesive.

[0045] In this invention, the aging temperature is preferably 10–100°C, more preferably 20–80°C; the aging time is preferably 0.5–60 h, more preferably 3–48 h. Limiting the aging temperature and time within the above ranges allows for a more uniform pore structure within the aluminum-silicon adhesive, reducing microscopic defects and inhomogeneities.

[0046] In one implementation, the aging temperature can be 30°C, 40°C, 50°C, 60°C or 70°C, or room temperature; the aging time can be 5 to 36 hours, or 10 to 24 hours.

[0047] The present invention does not impose any special limitations on the drying operation; any operation known to those skilled in the art can be used to dry to constant weight.

[0048] After obtaining the silica-alumina dry adhesive, the present invention mixes the silica-alumina dry adhesive, molding aid, and second solvent, and kneads and molds them to obtain silica-alumina adhesive particles.

[0049] In this invention, the molding aid is preferably at least one of carboxymethyl cellulose, polyethylene glycol, polyethylene, polypropylene, and polyacrylic acid; the mass of the molding aid is preferably 0.1-40% of the total mass of the aluminum source, alkali source, and silicon source, more preferably 0.5-30%.

[0050] The present invention does not impose any special limitation on the molecular weight of the carboxymethyl cellulose, polyethylene glycol, polyethylene, polypropylene and polyacrylic acid, and molding aids well known to those skilled in the art can be used.

[0051] In one embodiment, the mass of the molding aid can be 1% to 30% of the total mass of the aluminum source, alkali source, and silicon source, or it can be 2%, 3%, 4%, 5%, or 6%.

[0052] In this invention, the second solvent is preferably an inorganic solvent; the inorganic solvent is preferably deionized water. This invention does not have a specific limitation on the amount of the second solvent used; it is sufficient to dissolve the raw material.

[0053] The present invention does not have any special limitations on the operation of mixing the silicon-aluminum dry adhesive, molding aid, and second solvent; any technical solution for preparing the mixture well known to those skilled in the art can be used.

[0054] In this invention, the kneading molding is preferably performed by extrusion molding. This invention does not impose any special limitations on the extrusion molding operation; any operation well-known to those skilled in the art can be used.

[0055] After the kneading and molding process is completed, the present invention preferably dries and cuts the product obtained by kneading and molding in sequence to obtain silica-alumina granules.

[0056] The present invention does not impose any special limitations on the drying operation; drying to a constant weight is sufficient.

[0057] The present invention does not impose any special limitations on the cutting operation; adjustments can be made according to the actual required size.

[0058] In one embodiment, the aluminosilicate particles can be cylindrical aluminosilicate particles with a length of 2cm.

[0059] After obtaining the silica-alumina gel particles, the present invention sequentially crystallizes and calcines the silica-alumina gel particles to obtain sodalite molecular sieve particles with multi-level interconnected channels.

[0060] In this invention, the crystallization temperature is preferably 100–260°C, more preferably 120–200°C; the crystallization time is preferably 1–60 h, more preferably 3–25 h. As one embodiment, the crystallization temperature can be 130–180°C, or even 150–160°C; the crystallization time can be 5–20 h, or even 8 h, 12 h, 15 h, or 16 h. By limiting the crystallization temperature and time within the above ranges, this invention can further obtain sodalite molecular sieve particles with multi-level interconnected pores.

[0061] In this invention, the crystallization is preferably carried out in a reaction vessel. This invention does not specify a particular type of reaction vessel; any instrument or equipment well-known to those skilled in the art can be used.

[0062] In this invention, during crystallization, the silica-alumina gel particles are preferably placed on a support of the reaction vessel; during crystallization, deionized water or a mixed solution of deionized water and volatile substances is preferably added to the bottom of the reaction vessel; the volatile substances include at least one of methanol, ethanol, and acetone. The addition of deionized water or a mixed solution of deionized water and volatile substances to the bottom of the reaction vessel allows for evaporation during crystallization, enabling crystallization to take place in a steam atmosphere, thereby optimizing the crystallization process and improving the structure and properties of the sodalite molecular sieve particles.

[0063] The present invention does not have any special limitations on the operation of placing the silica-alumina gel particles on the support of the reactor; any operation known to those skilled in the art can be used.

[0064] The present invention does not impose any special limitation on the ratio of deionized water to volatile substances, as long as the quality of the mixed solution of deionized water and volatile substances meets the above requirements.

[0065] In this invention, the mass of the deionized water is preferably 10-10000% of the mass of the aluminosilicate particles, more preferably 100-5000%; the mass of the mixed solution of deionized water and volatile substances is preferably 10-10000% of the mass of the aluminosilicate particles, more preferably 100-5000%. By limiting the mass of the deionized water and the mass of the mixed solution of deionized water and volatile substances to the above ranges, this invention can further optimize the crystallization effect.

[0066] In one embodiment, the mass of the deionized water can be 500-1000% of the mass of the aluminosilicate particles, or it can be 600, 800% or 900%; the mass of the mixed solution of the deionized water and the volatile substance can be 500-1000% of the mass of the aluminosilicate particles, or it can be 600, 800% or 900%.

[0067] After crystallization, the present invention preferably washes and dries the crystallized product in sequence.

[0068] The present invention does not impose any special limitations on the washing operation; washing until neutral can be performed using an operation known to those skilled in the art.

[0069] The present invention does not impose any special limitations on the drying operation; drying to a constant weight is sufficient.

[0070] In this invention, the calcination temperature is preferably 300–800°C; the calcination time is preferably 5–25 h. As one embodiment, the calcination temperature can be 350–580°C, or even 400–450°C; the calcination time can be 10–20 h, or even 12, 15, or 18 h. By limiting the calcination temperature and time to the above ranges, this invention can further remove molding aids and mesoporous template agents.

[0071] In this invention, the calcination is preferably carried out in an air or oxygen atmosphere.

[0072] This invention uses a dry gel conversion method to synthesize sodalite crystals with micropores; a hard template method is used to introduce a mesoporous template agent, which forms mesopores after calcination; by calcination, the molding aid and the mesoporous template agent are removed to form macropores, thereby obtaining sodalite molecular sieve particles with multi-level interconnected channels, while avoiding the adverse effects of molding aids.

[0073] This invention prepares sodalite molecular sieve particles with interconnected hierarchical pores by adjusting the amounts of aluminum source, alkali source, silicon source, mesoporous template agent, molding aid, and crystallization conditions in the silica-alumina gel solution. The preparation method provided by this invention not only avoids the adverse effects of molding aids but also constructs molecular sieves with interconnected hierarchical pores, providing a new preparation method for improving the application performance of sodalite molecular sieve particles in hydrogen storage and sulfur-resistant hydrogenation catalysis.

[0074] This invention uses a dry gel conversion method and a hard template method to prepare sodalite molecular sieve particles. Sodalite molecular sieve particles are prepared by directly crystallizing silica-alumina gel particles through the dry gel conversion method. During the crystallization process, a hard template method is used to construct multi-level channels. Finally, the molding aid and mesoporous template agent are removed by calcination to obtain sodalite molecular sieve particles with interconnected multi-level channels.

[0075] The present invention also provides sodalite molecular sieve particles with interconnected multi-level pores prepared by the preparation method described above, wherein the pore size includes micropores, mesopores and macropores.

[0076] The present invention also provides the application of the sodalite molecular sieve particles with multi-level interconnected channels described in the above technical solution in hydrogen storage and sulfur-resistant hydrogenation catalysis.

[0077] The present invention does not impose any special limitations on the operation of the sodalite molecular sieve particles with interconnected multi-level pores in hydrogen storage and sulfur-resistant hydrogenation catalysis; any operation familiar to those skilled in the art can be used.

[0078] The technical solutions of this invention will be clearly and completely described below with reference to the embodiments thereof. Obviously, the described embodiments are only a part of the embodiments of this invention, and not all of them. All other embodiments obtained by those skilled in the art based on the embodiments of this invention without creative effort are within the scope of protection of this invention.

[0079] Example 1

[0080] The preparation method of sodalite molecular sieve particles with interconnected hierarchical channels includes the following steps:

[0081] (1) Sodium aluminate as the aluminum source, sodium hydroxide as the alkali source and silica sol as the silicon source are dissolved in deionized water, and then polyethylene glycol is added at a total mass of 3 wt% of the aluminum source, alkali source and silicon source to obtain a silica-alumina gel solution; wherein, the molar ratio of SiO2, Al2O3, Na2O and H2O in the silica-alumina gel solution is 2:1:6:120; the molecular weight of polyethylene glycol is 1000;

[0082] (2) The silica-alumina adhesive solution obtained in step (1) is aged at room temperature for 24 hours and then dried at 80°C to obtain silica-alumina dry adhesive;

[0083] (3) Weigh 2wt% polyethylene and 30wt% deionized water of the total mass of aluminum source, alkali source and silicon source and add them to the silicon-aluminum dry adhesive obtained in step (2) and mix them. Then, extrude the mixture on an extruder and dry it at 80°C for 12 hours. Then, cut it into cylindrical silicon-aluminum adhesive particles with a length of 2cm. The molecular weight of polyethylene is 1000.

[0084] (4) The silica-alumina gel particles obtained in step (3) are loaded onto a support in a stainless steel reactor. 600wt% deionized water of silica-alumina gel particle mass is added to the bottom of the stainless steel reactor. The mixture is crystallized at 160℃ for 12h, then washed until neutral, and dried at 120℃ for 12h. Subsequently, it is calcined in air at 450℃ for 10h to obtain sodalite molecular sieve particles with multi-level interconnected pores.

[0085] Example 2

[0086] The preparation method of sodalite molecular sieve particles with interconnected hierarchical channels includes the following steps:

[0087] (1) Sodium aluminate as aluminum source, sodium hydroxide as alkali source and silica sol as silicon source are dissolved in deionized water, and then starch with a total mass of 3wt% of aluminum source, alkali source and silicon source is added to obtain silica-alumina colloid solution; wherein, the molar ratio of SiO2, Al2O3, Na2O and H2O in silica-alumina colloid solution is 2:1:6:120;

[0088] (2) The silica-alumina adhesive solution obtained in step (1) is aged at room temperature for 24 hours and then dried at 80°C to obtain silica-alumina dry adhesive;

[0089] (3) Weigh 3wt% polyethylene glycol and 20wt% deionized water of the total mass of aluminum source, alkali source and silicon source and add them to the silica-alumina dry adhesive obtained in step (2) and mix them. Then, extrude the mixture on an extruder and dry it at 80°C for 12 hours. Then, cut it into cylindrical silica-alumina adhesive particles with a length of 2cm. The molecular weight of polyethylene glycol is 1000.

[0090] (4) The silica-alumina gel particles obtained in step (3) are loaded onto a support in a stainless steel reactor. 500wt% deionized water of silica-alumina gel particle mass is added to the bottom of the stainless steel reactor. The mixture is crystallized at 130℃ for 16h, then washed until neutral, and dried at 120℃ for 12h. Subsequently, it is calcined in air at 580℃ for 10h to obtain sodalite molecular sieve particles with multi-level interconnected pores.

[0091] Example 3

[0092] The preparation method of sodalite molecular sieve particles with interconnected hierarchical channels includes the following steps:

[0093] (1) Sodium aluminate as the aluminum source, sodium hydroxide as the alkali source and silica sol as the silicon source were dissolved in deionized water, and then carbon nanotubes with a total mass of 1.5 wt% of aluminum source, alkali source and silicon source were added to obtain a silica-alumina gel solution; wherein, the molar ratio of SiO2, Al2O3, Na2O and H2O in the silica-alumina gel solution was 3:1:4:80; the size of carbon nanotubes was 10-20 nm;

[0094] (2) The silica-alumina adhesive solution obtained in step (1) is aged at room temperature for 24 hours and then dried at 80°C to obtain silica-alumina dry adhesive;

[0095] (3) Weigh 3wt% polyethylene glycol and 20wt% deionized water of the total mass of aluminum source, alkali source and silicon source and add them to the silica-alumina dry adhesive obtained in step (2) and mix them. Then, extrude the mixture on an extruder and dry it at 80°C for 12 hours. Then, cut it into cylindrical silica-alumina adhesive particles with a length of 2cm. The molecular weight of polyethylene glycol is 1000.

[0096] (4) The silica-alumina gel particles obtained in step (3) are loaded onto a support in a stainless steel reactor. 800wt% deionized water of silica-alumina gel particles is added to the bottom of the stainless steel reactor. The mixture is crystallized at 160°C for 12 hours, then washed until neutral, and dried at 120°C for 12 hours. Subsequently, it is calcined in air at 580°C for 18 hours to obtain sodalite molecular sieve particles with interconnected multi-level pores.

[0097] Figure 1X-ray diffraction patterns of the sodalite molecular sieve particles with interconnected hierarchical channels prepared in Examples 1-3.

[0098] from Figure 1 It can be seen that the crystals synthesized in Examples 1 to 3 are sodalite molecular sieve particles.

[0099] The sodalite molecular sieve particles prepared in Examples 1-3 are microporous molecular sieves with an SOD cage (β-cage) framework structure, and their pore size is [missing information].

[0100] Figure 2 SEM image of the surface of the sodalite molecular sieve particles with interconnected hierarchical pores prepared in Example 1. Figure 3 This is a SEM image of a cross-section of the sodalite molecular sieve particles with interconnected multi-level pores prepared in Example 1.

[0101] from Figures 2-3 It can be seen that the spherical crystals are sodalite molecular sieves. There are gaps between the spherical sodalite crystals, which are formed by the calcination of mesoporous template agents and forming aids, forming the mesopores and macropores of sodalite molecular sieve particles.

[0102] Figure 4 The attached figures show the BET isothermal adsorption-desorption of the sodalite molecular sieve particles with interconnected hierarchical channels prepared in Examples 1-3. Figure 5 The images show the pore size distribution of the multi-level interconnected sodalite molecular sieve particles prepared in Examples 1-3 using mercury intrusion porosimetry.

[0103] from Figure 4 It can be seen that the BET isotherm exhibits type IV hysteresis, indicating that the sodalite molecular sieve particles with interconnected multilevel channels have a mesoporous structure.

[0104] from Figure 5 It can be seen that the sodalite molecular sieve particles with interconnected multi-level channels contain both mesopores and macropores.

[0105] As can be seen from the above embodiments, the preparation method provided by the present invention can not only avoid the adverse effects of molding aids, but also prepare sodalite molecular sieve particles with multi-level interconnected channels.

[0106] The above description is only a preferred embodiment of the present invention. It should be noted that for those skilled in the art, several improvements and modifications can be made without departing from the principle of the present invention, and these improvements and modifications should also be considered within the scope of protection of the present invention.

Claims

1.A method for preparing a particle of sodalite molecular sieve with multi-level pore penetration, comprising the following steps: (1) mixing an aluminum source, an alkali source, a silicon source, a first solvent, and a mesoporous template to obtain a silica alumina sol solution; (2) sequentially performing aging and drying on the silica alumina sol solution obtained in step (1) to obtain a silica alumina dry gel; (3) mixing the silica alumina dry gel obtained in step (2), a forming aid, and a second solvent, and performing kneading and molding to obtain a silica alumina gel particle; (4) sequentially performing crystallization and calcination on the silica alumina gel particle obtained in step (3) to obtain a particle of sodalite molecular sieve with multi-level pore penetration; the mesoporous template in step (1) is at least one of starch, glucose, polyethylene glycol, carbon nanotube, carbon nanofiber, nano carbon molecular sieve, carbon black, and carbon aerogel; the forming aid in step (3) is at least one of carboxymethyl cellulose, polyethylene glycol, polyethylene, polypropylene, and polyacrylic acid; the calcination in step (4) is performed at a temperature of 300-800℃ for a time of 5-25h in an air or oxygen atmosphere; the mass of the mesoporous template in step (1) is 0.01-10% of the total mass of the aluminum source, the alkali source, and the silicon source; the molar ratio of SiO 2 to Al 2 O 3 in the silica alumina sol solution in step (1) is 0.5-30, the molar ratio of Na 2 O to SiO 2 in the silica alumina sol solution is 0.5-25, and the molar ratio of H 2 O to SiO 2 in the silica alumina sol solution is 20-500; the aging in step (2) is performed at a temperature of 10-100℃ for a time of 0.5-60h; the crystallization in step (4) is performed at a temperature of 100-260℃ for a time of 1-60h in a reaction kettle; deionized water or a mixed solution of deionized water and a volatile substance is added to the bottom of the reaction kettle during the crystallization; the mass of the deionized water and the mass of the mixed solution of deionized water and the volatile substance are independently 10-10000% of the mass of the silica alumina gel particle. 6.The particle of sodalite molecular sieve with multi-level pore penetration prepared by the method of any one of claims 1-5, wherein the pore size includes micropores, mesopores, and macropores. 7.The particle of sodalite molecular sieve with multi-level pore penetration of claim 6, wherein the particle is used in hydrogen storage and sulfur-resistant hydrogenation catalysis. ​ ​ ​ ​ ​ 2. The production method according to claim 1, characterized by, ​ 3. The production method according to claim 1, characterized by, ​ 4. The method of claim 1, wherein, ​ 5. The preparation method according to claim 1, characterized in that, ​ ​ ​

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