Amino-functionalized hierarchical pore molecular sieve and preparation method thereof

The preparation of amino functionalized multi-stage pore molecular sieve through specific steps solves the problems of order and drug loading, and achieves uniform dispersion of amino groups and improves drug loading capacity.

CN120440907APending Publication Date: 2025-08-08JILIN UNIVERSITY
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Patent Information

Application Number
CN202510629241.0
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-05-16
Publication Date
2025-08-08

AI Technical Summary

Technical Problem

The existing amino-functionalized molecular sieve has poor order and limited drug loading.

Method used

A mixture of ammonia water, anhydrous ethanol, deionized water, and ethyl orthosilicate and 3-aminopropyltriethoxysilane in a specific proportion was stirred, followed by reaction with sodium hydroxide and sodium metaaluminate, and after crystallization, centrifugation and drying, an amino-functionalized multi-stage pore molecular sieve was prepared.

Benefits of technology

The uniform dispersion of amino groups on the surface and pores of the molecular sieve is achieved, maintaining the order of the molecular sieve, and improving the drug loading capacity.

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Abstract

The invention discloses an amino-functionalized hierarchical pore molecular sieve and a preparation method thereof, and belongs to the technical field of molecular sieves. The technical problems that an existing molecular sieve containing an amino functional group is poor in order degree and limited in drug loading capacity are solved. The preparation method comprises the following steps: sequentially adding ammonia water, absolute ethyl alcohol, deionized water, tetraethoxysilane and 3-aminopropyltriethoxysilane into a reaction container, stirring, reacting, centrifuging, washing with water, drying in air, and calcining to obtain an amino-functionalized silicon source; and sequentially adding sodium hydroxide, sodium metaaluminate and the amino-functionalized silicon source into deionized water, crystallizing, centrifuging and washing after crystallization, and drying in air to obtain the amino-functionalized hierarchical pore molecular sieve. According to the amino-functionalized hierarchical pore molecular sieve, amino groups are uniformly dispersed on the surface and in pore channels of the molecular sieve, the degree of order is high, the molecular sieve has the ability of being stably combined with a biological material, has a microporous-mesoporous space hierarchical pore channel structure, and is beneficial to improving the drug loading capacity of the molecular sieve.
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Description

Technical Field

[0001] The invention belongs to the technical field of molecular sieves, and particularly relates to an amino-functionalized multi-level pore molecular sieve and a preparation method thereof. Background Art

[0002] Molecular sieve is a crystalline aluminosilicate with a regular and uniform pore structure, high porosity and good permeability.

[0003] The surface of molecular sieves is rich in silanol (Si-OH) groups. These active sites can serve as "anchor points" for chemical modification, and amino, epoxy and other functional groups can be grafted through silane coupling agents (such as APTES). Functionally modified molecular sieves can be combined with different material systems through a variety of interfacial interaction mechanisms: in the metal field (such as titanium alloys), based on covalent bond grafting or coordination bond anchoring strategies, molecular sieve coatings with high bonding strength can be prepared on the surface of the substrate material; when compounded with high molecular weight polymers through a blending process, the chemical bond network generated by the functional groups on the molecular sieve surface and the polymer chain segments can significantly improve the stability and interfacial compatibility of the composite material; by constructing heterogeneous structures with organic or inorganic nanomaterials, multifunctional nanocomposites can be formed.

[0004] Among them, the methods used to introduce amino functional groups into the surface or pores of molecular sieves are mainly post-grafting or co-condensation. The post-grafting method is to generate a corresponding covalent bond by causing the organic functional group to undergo a condensation reaction with the silanol (Si-OH) groups on the surface of the molecular sieve. This method does not destroy the pore structure of the molecular sieve, so more organic functional groups can be introduced. However, when using this method, the distribution of organic groups on the surface of the functionalized molecular sieve is often uneven, with the vast majority concentrated on the outer surface of the pores, while the functional groups inside the pores are relatively scarce. The co-condensation method is to directly add a functional organic modifier to a sol composed of a template and a silicon source, so that the modifier and orthosilicate are hydrolyzed and cross-linked with each other. After a certain reaction time, the reaction system is placed in an autoclave for crystallization, and a modified mesoporous material containing organic functional groups is formed by self-assembly. However, the molecular sieve materials prepared by the above methods usually have a poor degree of order, and the degree of order decreases with the increase of the organic group content.

[0005] Molecular sieves can achieve drug loading by introducing specific ions or molecules into their surfaces and pores, where the exchanged cations bind to the drug. However, as a drug carrier, molecular sieves with only microporous channels can only chelate small amounts of drugs using the cations generated by ion exchange. Drugs with larger particle sizes cannot enter the microporous molecular sieves, resulting in a limited drug loading capacity. Summary of the Invention

[0006] The present invention aims to solve the technical problems in the prior art of poor order and limited drug loading of molecular sieves containing amino functional groups, further improve the bonding ability between the molecular sieve and the substrate material, and provide an amino-functionalized multi-level pore molecular sieve and a preparation method thereof.

[0007] To achieve the above objectives, the present invention adopts the following technical solutions.

[0008] In a first aspect, the present invention provides a method for preparing an amino-functionalized hierarchical pore molecular sieve, comprising the following steps:

[0009] (1) Aqueous ammonia (NH3·H2O), anhydrous ethanol, deionized water, tetraethyl orthosilicate (TEOS), and 3-aminopropyltriethoxysilane (APTES) in a volume ratio of 2.5-4:70-72.5:9.5-11:3:3 are sequentially added into a reaction vessel and stirred evenly, and the mixture is stirred for 10-14 hours, centrifuged, washed with water, dried in air, and calcined to obtain an amino-functionalized silicon source;

[0010] (2) Sodium hydroxide (NaOH), sodium aluminate (NaAlO2), and the amino-functionalized silicon source prepared in step (1) are sequentially added to deionized water in a molar ratio of Al2O3, SiO2, Na2O, and H2O of 1:1-3:2-4:150-250, stirred for 2-3 hours, and then added to a reaction vessel for crystallization for more than 25 hours. After the crystallization is completed, the mixture is centrifuged and washed with water, and then dried in air to obtain an amino-functionalized hierarchical pore molecular sieve.

[0011] Preferably, in step (1), the volume ratio of ammonia water, anhydrous ethanol, deionized water, ethyl orthosilicate and 3-aminopropyltriethoxysilane is 3.14:71.4:10:3:3.

[0012] Preferably, in step (1), the centrifugation temperature is 22-26° C., the centrifugation speed is 9000-11000 rpm, and the centrifugation time is 4-6 min.

[0013] Preferably, in step (1), the drying temperature is 60-100°C, the calcination temperature is 500-600°C, the calcination time is 6-12h, and the heating rate is 1-3°C / min.

[0014] Preferably, in step (2), the molar ratio of Al2O3, SiO2, Na2O and H2O is 1:2:3.2:200.

[0015] Preferably, in step (2), the crystallization temperature is 60-100°C, the crystallization time is 6-48h, and the drying temperature is 60-100°C; more preferably, the crystallization time is 40-48h; and 48h is particularly preferred.

[0016] Preferably, in step (2), the centrifugation temperature is 22-26° C., the centrifugation speed is 9000-11000 rpm, and the centrifugation time is 4-6 min.

[0017] In a second aspect, the present invention also provides an amino-functionalized multi-level pore molecular sieve prepared by the above preparation method.

[0018] Preferably, the amino-functionalized multi-level pore size of the molecular sieve is 0.4-1.9 nm, and the mesopore size is 14-36 nm.

[0019] Preferably, the topological structure of the amino-functionalized multi-level pore molecular sieve includes one of LTA, FAU, SOD, BIK, CHA, MFI, EMT, MOR, and BEA.

[0020] The principle behind this invention is that the amino-functionalized hierarchical pore size molecular sieve has a surface modified with amino groups, and the presence of these groups during the synthesis process does not affect the order of the molecular sieve. The amino groups can form stable bonds with biomaterials. The amino-functionalized hierarchical pore size molecular sieve exhibits superior drug-loading properties due to its microporous-mesoporous structure.

[0021] Compared with the prior art, the present invention has the following beneficial effects:

[0022] The preparation method of the amino-functionalized multi-level pore molecular sieve of the present invention enables the amino groups to be evenly dispersed on the surface and in the pores of the molecular sieve, and the order of the molecular sieve will not be destroyed during the synthesis process.

[0023] The preparation method of the amino-functionalized multi-level pore molecular sieve of the present invention adds 3-aminopropyltriethoxysilane (APTES) during the synthesis of a silicon source to introduce amino groups, synthesize an amino silicon source, and then synthesize an amino-functionalized multi-level pore molecular sieve. This method is beneficial to improving the binding stability of the molecular sieve and biomaterials, and is expected to be combined with material systems in different fields through various interface interaction mechanisms, such as the metal field, the high molecular polymer field, and the organic or inorganic nanomaterial field.

[0024] The amino-functionalized multi-level pore molecular sieve of the present invention has a "micropore-mesopore" spatial multi-level pore structure, which is beneficial to improving the drug loading capacity of the molecular sieve and has important clinical value. BRIEF DESCRIPTION OF THE DRAWINGS

[0025] In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the following briefly introduces the drawings required for use in the description of the embodiments. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without any creative work.

[0026] Figure 1 These are scanning electron microscope (SEM) images of the amino-functionalized multi-level pore molecular sieve prepared in Example 1 of the present invention, wherein a is a low-magnification image of the amino-functionalized multi-level pore molecular sieve, and b is a high-magnification image of the amino-functionalized multi-level pore molecular sieve.

[0027] Figure 2 This is a transmission electron microscope (TEM) image of the amino-functionalized hierarchical pore molecular sieve prepared in Example 1 of the present invention. The arrows indicate the mesoporous structure of the amino-functionalized hierarchical pore molecular sieve.

[0028] Figure 3 This is a scanning electron microscope (SEM) image of sample 1 prepared in comparative example 1 of the present invention, wherein a is a low-magnification image of sample 1, and b is a high-magnification image of sample 1.

[0029] Figure 4 This is a transmission electron microscope (TEM) image of sample 1 prepared in comparative example 1 of the present invention.

[0030] Figure 5 These are scanning electron microscope (SEM) images of sample 2 prepared in comparative example 2 of the present invention, wherein a is a low-magnification image of sample 2, and b is a high-magnification image of sample 2.

[0031] Figure 6 This is a transmission electron microscope (TEM) image of sample 2 prepared in comparative example 2 of the present invention.

[0032] Figure 7 This is an X-ray diffractometer (XRD) image of the amino-functionalized hierarchical pore molecular sieve prepared in Example 1 of the present invention.

[0033] Figure 8 This is a nitrogen adsorption-desorption isotherm graph of the amino-functionalized hierarchical pore molecular sieve prepared in Example 1 of the present invention.

[0034] Figure 9 This is a picture of the pore size distribution of nitrogen adsorption and desorption of the amino-functionalized hierarchical pore molecular sieve prepared in Example 1 of the present invention.

[0035] Figure 10 This is a picture of the mesopore size distribution of nitrogen adsorption and desorption of the amino-functionalized hierarchical pore molecular sieve prepared in Example 1 of the present invention.

[0036] Figure 11 This is a Fourier transform infrared absorption spectrometer (FTIR) image of the amino-functionalized hierarchical pore molecular sieve prepared in Example 1 of the present invention.

[0037] Figure 12These are SEM images of the non-amino functionalized multi-level pore molecular sieve coated porous titanium alloy implant and the amino functionalized multi-level pore molecular sieve coated porous titanium alloy implant before and after ultrasonic treatment in the present invention, wherein a is the SEM image of the non-amino functionalized multi-level pore molecular sieve coated porous titanium alloy implant before ultrasonic treatment, b is the SEM image of the amino functionalized multi-level pore molecular sieve coated porous titanium alloy implant before ultrasonic treatment, c is the SEM image of the non-amino functionalized multi-level pore molecular sieve coated porous titanium alloy implant after ultrasonic treatment, and d is the SEM image of the amino functionalized multi-level pore molecular sieve coated porous titanium alloy implant after ultrasonic treatment.

[0038] Figure 13 These are the coating retention results of the non-amino-functionalized hierarchical pore molecular sieve coated porous titanium alloy implants and the amino-functionalized hierarchical pore molecular sieve coated porous titanium alloy implants before and after ultrasonic treatment in the present invention. In the figure, * indicates that there is a significant difference between the two groups, and a significant difference of *p<0.05 is indicated.

[0039] Figure 14 These are the results of the drug loading capacity of the non-amino-functionalized hierarchical pore molecular sieve coated porous titanium alloy implant and the amino-functionalized hierarchical pore molecular sieve coated porous titanium alloy implant of the present invention. In the figure, *** indicates that there is a significant difference between the two groups, and a significant difference of ***p<0.001 is indicated. DETAILED DESCRIPTION

[0040] In order to enable those skilled in the art to better understand the technical solution of the present invention, the present invention will be further described in detail below with reference to the embodiments.

[0041] In the following examples, various processes and methods not described in detail are conventional methods known in the art. Unless otherwise specified, the materials, reagents, devices, instruments, equipment, etc. used in the following examples can be obtained from commercial sources.

[0042] Example 1

[0043] The preparation method of amino-functionalized hierarchical pore molecular sieve coating comprises the following steps:

[0044] (1) First, 12.56 ml of ammonia water, 285.6 ml of anhydrous ethanol, 40 ml of deionized water, 12 ml of ethyl orthosilicate and 12 ml of 3-aminopropyltriethoxysilane were added to a glass beaker of corresponding volume in sequence and stirred evenly. The stirring was continued for 12 hours. The resulting milky white solution was centrifuged in a centrifuge at a temperature of 24 ° C and a speed of 10000 rpm for 5 minutes and washed three times with deionized water. The resulting precipitate was dried in air at 60-100 ° C. The resulting white powder was calcined in air at 550 ° C for 8 hours at a heating rate of 1-3 ° C / min to obtain an amino-functionalized silicon source with a light yellow color.

[0045] (2) Then, according to the molar ratio of Al2O3, SiO2, Na2O, and H2O being 1:2:3.2:200, 0.445g of sodium hydroxide, 0.691g of sodium aluminate, and 0.4g of the amino-functionalized silicon source prepared in step (1) were added to 10g of deionized water in sequence, stirred for 2-3h, and then added to a 25ml hydrothermal reactor and crystallized at 100°C for 48h. The resulting reactant was centrifuged in a centrifuge at a temperature of 24°C and a speed of 10000rpm for 5min, and washed 3 times with deionized water. The resulting precipitate was dried in air at 60-100°C to obtain an amino-functionalized multi-level pore molecular sieve.

[0046] Comparative Example 1

[0047] (1) First, 12.56 ml of ammonia water, 285.6 ml of anhydrous ethanol, 40 ml of deionized water, 12 ml of ethyl orthosilicate and 12 ml of 3-aminopropyltriethoxysilane were added to a glass beaker of corresponding volume in sequence and stirred evenly. The stirring was continued for 12 hours. The resulting milky white solution was centrifuged in a centrifuge at a temperature of 24 ° C and a speed of 10000 rpm for 5 minutes and washed three times with deionized water. The resulting precipitate was dried in air at 60-100 ° C. The resulting white powder was calcined in air at 550 ° C for 8 hours at a heating rate of 1-3 ° C / min to obtain an amino-functionalized silicon source with a light yellow color.

[0048] (2) Then, according to the molar ratio of Al2O3, SiO2, Na2O, and H2O being 1:2:3.2:200, 0.445g of sodium hydroxide, 0.691g of sodium aluminate, and 0.4g of the amino-functionalized silicon source prepared in step (1) were added to 10g of deionized water in sequence, stirred for 2-3h, and then added to a 25ml hydrothermal reactor and crystallized at 100°C for 6h. The resulting reactant was centrifuged in a centrifuge at a temperature of 24°C and a speed of 10000rpm for 5min, and washed three times with deionized water. The resulting precipitate was dried in air at 60-100°C to obtain sample 1.

[0049] Comparative Example 2

[0050] (1) First, 12.56 ml of ammonia water, 285.6 ml of anhydrous ethanol, 40 ml of deionized water, 12 ml of ethyl orthosilicate and 12 ml of 3-aminopropyltriethoxysilane were added to a glass beaker of corresponding volume in sequence and stirred evenly. The stirring was continued for 12 hours. The resulting milky white solution was centrifuged in a centrifuge at a temperature of 24 ° C and a speed of 10000 rpm for 5 minutes and washed three times with deionized water. The resulting precipitate was dried in air at 60-100 ° C. The resulting white powder was calcined in air at 550 ° C for 8 hours at a heating rate of 1-3 ° C / min to obtain an amino-functionalized silicon source with a light yellow color.

[0051] (2) Then, according to the molar ratio of Al2O3, SiO2, Na2O, and H2O being 1:2:3.2:200, 0.445g of sodium hydroxide, 0.691g of sodium aluminate, and 0.4g of the amino-functionalized silicon source prepared in step (1) were added to 10g of deionized water in sequence, stirred for 2-3h, and then added to a 25ml hydrothermal reactor and crystallized at 100°C for 24h. The resulting reactant was centrifuged in a centrifuge at a temperature of 24°C and a speed of 10000rpm for 5min, and washed three times with deionized water. The resulting precipitate was dried in air at 60-100°C to obtain sample 2.

[0052] The amino-functionalized multi-level pore molecular sieve prepared in Example 1 was tested. Figure 1 a and b are SEM images of amino-functionalized hierarchical pore molecular sieves. Figure 1 It can be seen that the classic LTA structure can be formed after 48h crystallization of the molecular sieve, indicating that the crystallization time is sufficient to meet the conditions for synthesizing amino-functionalized hierarchical pore molecular sieves. Figure 2 TEM image of amino-functionalized hierarchical pore molecular sieve. Figure 2 It can be seen that the molecular sieve obtained after 48h crystallization can form a mesoporous structure, indicating that the crystallization time is sufficient to meet the conditions for synthesizing amino-functionalized hierarchical pore molecular sieves.

[0053] Figure 3 and Figure 5 The scanning electron microscope images of sample 1 prepared in comparative example 1 and sample 2 prepared in comparative example 2 are respectively, Figure 4 and Figure 6 The transmission electron microscope images of sample 1 prepared in comparative example 1 and sample 2 prepared in comparative example 2 are shown respectively. Figure 2-6 It can be seen that after crystallization for 6h and 24h, the prepared samples 1 and 2 lack the regular pore arrangement and uniform pore size characteristics typical of molecular sieves, and no ordered crystal framework or periodic pore structure can be observed, which does not meet the structural requirements of molecular sieves.

[0054] Figure 7 This is the XRD pattern of amino-functionalized hierarchical pore molecular sieve. Figure 7 It can be seen that the molecular sieve obtained after 48 hours of crystallization can show the characteristic diffraction peaks of molecular sieves. At the same time, the presence of amino groups does not affect the order of the molecular sieve, and the molecular sieve has good order. Comparison of the XRD pattern with the standard XRD pattern of LTA topology structure shows that the amino-functionalized hierarchical pore molecular sieve has a clear LTA topology structure.

[0055] Figure 8 This is the nitrogen adsorption and desorption isotherm of amino-functionalized hierarchical pore molecular sieve. Figure 8It can be seen that the molecular sieve obtained after 48 hours of crystallization has a type IV isotherm, indicating that the molecular sieve has a multi-level pore structure and that the crystallization time is sufficient to meet the conditions for synthesizing amino-functionalized multi-level pore molecular sieves. Figure 9 This is a picture of the pore size distribution of nitrogen adsorption and desorption of amino-functionalized hierarchical molecular sieves. Figure 10 This is the nitrogen adsorption and desorption mesopore size distribution picture of amino-functionalized hierarchical molecular sieve. Figure 9 and Figure 10 It can be seen that the molecular sieve obtained after 48h crystallization has micropore diameters and mesopore diameters, indicating that the crystallization time is sufficient to meet the conditions for synthesizing amino-functionalized hierarchical pore molecular sieves. Figure 11 This is the FTIR image of amino-functionalized hierarchical pore molecular sieve. Figure 11 It can be seen that the molecular sieve obtained after 48h crystallization has a peak at 3472.13cm -1 There is a characteristic peak at , which corresponds to the stretching vibration of the NH bond, indicating that there are amino groups on the surface of the molecular sieve.

[0056] Titanium alloy implants were used as the base biomaterial to verify the binding stability and drug loading capacity of amino-functionalized hierarchical pore size molecular sieves.

[0057] Verification method: First, a porous titanium alloy implant (diameter: 10 mm, height: 3 mm, prepared according to Hierarchicalzeolite coatings featuring a spatial gradient architecture for sequentially-controlled bisphosphonate release in the modulation of osteogenic–osteoclastic balance, Microporous and Mesoporous Materials, 15, April, 2024) was placed in anhydrous ethanol, acetone and deionized water for ultrasonic cleaning for 15 minutes in sequence. After drying in a 100°C oven for 40 minutes, it was placed in piranha solution (a mixture of 98wt% concentrated sulfuric acid and 30% hydrogen peroxide in a volume ratio of 3:1) and immersed for 15-30 minutes. After rinsing with deionized water, it was blown dry with nitrogen to obtain a pretreated porous titanium alloy implant. The pretreated porous titanium alloy implant was then placed in a 0.3wt% polydiallyldimethylammonium chloride solution for surface modification for 5 minutes, removed and rinsed with deionized water, and dried with nitrogen. The implant was then placed in a 0.3wt% polyacrylic acid solution for surface modification for 5 minutes, removed and rinsed with deionized water, and dried with nitrogen. This process was repeated three times to obtain a porous titanium alloy implant with an organic-inorganic bonding layer. The porous titanium alloy implant with an organic-inorganic bonding layer was first placed in a 0.3wt% polydiallyldimethylammonium chloride solution for surface modification for 5 minutes, removed and rinsed with deionized water, dried with nitrogen, and then immersed in a solution containing 0.3wt% amino-functionalized hierarchical molecular sieve for surface modification for 5 minutes, removed and rinsed with deionized water, and dried with nitrogen. This process was repeated five times, and then calcined at 550°C for 2 hours with a heating rate of 3°C / min to obtain an amino-functionalized hierarchical molecular sieve porous titanium alloy implant.

[0058] Add 4A molecular sieve to deionized water, stir and mix, prepare a 0.3wt% solution of non-amino functionalized multi-level pore molecular sieve, replace the 0.3wt% solution of amino functionalized multi-level pore molecular sieve in the above verification method with a 0.3wt% solution of non-amino functionalized multi-level pore molecular sieve, and obtain a non-amino functionalized multi-level pore molecular sieve porous titanium alloy implant.

[0059] The binding ability of molecular sieve to porous titanium alloy implants was tested in amino-functionalized hierarchical pore molecular sieve porous titanium alloy implants and non-amino-functionalized hierarchical pore molecular sieve coated porous titanium alloy implants. The test process is as follows: the sample is placed in a 15ml centrifuge tube, the centrifuge tube is placed in an ultrasonic oscillator, and it is continuously run at an intensity of 50kHz for 5 minutes. Subsequently, the ultrasonically treated sample is dried at 60°C for 4 hours. The surface morphology and area of the surface coating of the non-ultrasonicated sample and the ultrasonically treated sample are observed using SEM. The results are shown in Figure 2. Figure 12 In AD and Figure 13 As shown. Figure 12 In AD and Figure 13 As shown, the amino-functionalized hierarchical pore molecular sieve coating porous titanium alloy implant has a higher coating retention rate before and after ultrasonic treatment, indicating that the presence of the amino group of the present invention can enhance the physical and chemical bonding ability between the molecular sieve and the titanium alloy implant.

[0060] The drug loading capacity of amino-functionalized hierarchical molecular sieve coated porous titanium alloy implants and non-amino-functionalized hierarchical molecular sieve coated porous titanium alloy implants was tested. Figure 14 As shown, from Figure 14 As shown, the amino-functionalized multi-level pore molecular sieve coated porous titanium alloy implant of the present invention can load more zoledronic acid, which proves that the amino-functionalized multi-level pore molecular sieve of the present invention has a multi-level pore structure and a strong drug loading capacity.

[0061] Obviously, the above embodiments are merely examples for clarity of explanation and are not intended to limit the embodiments. Those skilled in the art will readily appreciate that other variations or modifications based on the above descriptions are possible. It is not necessary and impossible to enumerate all embodiments here. Obvious variations or modifications arising therefrom remain within the scope of protection of the present invention.

Claims

1. A method for preparing an amino-functionalized hierarchical pore molecular sieve, characterized in that: The following steps are involved: (1) Aqueous ammonia, anhydrous ethanol, deionized water, ethyl orthosilicate, and 3-aminopropyltriethoxysilane in a volume ratio of 2.5-4:70-72.5:9.5-11:3:3 are sequentially added to a reaction vessel and stirred evenly, and the mixture is stirred for 10-14 hours, centrifuged, washed with water, dried in air, and calcined to obtain an amino-functionalized silicon source; (2) Sodium hydroxide, sodium aluminate, and the amino-functionalized silicon source prepared in step (1) are sequentially added to deionized water in a molar ratio of Al2O3, SiO2, Na2O, and H2O of 1:1-3:2-4:150-250, stirred for 2-3 hours, and then added to a reaction vessel for crystallization for more than 25 hours. After crystallization, the mixture is centrifuged and washed with water, and then dried in air to obtain an amino-functionalized hierarchical pore molecular sieve.

2. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 1, wherein: In step (1), the volume ratio of ammonia water, anhydrous ethanol, deionized water, ethyl orthosilicate and 3-aminopropyltriethoxysilane is 3.14:71.4:10:3:

3.

3. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 1, wherein: In step (1), the centrifugation temperature is 22-26° C., the centrifugation speed is 9000-11000 rpm, and the centrifugation time is 4-6 min.

4. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 1, wherein: In step (1), the drying temperature is 60-100° C., the calcination temperature is 500-600° C., the calcination time is 6-12 h, and the heating rate is 1-3° C. / min.

5. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 1, wherein: In step (2), the molar ratio of Al2O3, SiO2, Na2O and H2O is 1:2:3.2:

200.

6. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 1, wherein: In step (2), the centrifugation temperature is 22-26° C., the centrifugation speed is 9000-11000 rpm, and the centrifugation time is 4-6 min.

7. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 1, wherein: In step (2), the crystallization temperature is 60-100°C, the crystallization time is 40-48h, and the drying temperature is 60-100°C.

8. An amino-functionalized hierarchical pore molecular sieve prepared according to the preparation method according to any one of claims 1 to 7.

9. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 8, wherein: The amino-functionalized multi-level pore molecular sieve has a micropore diameter of 0.4-1.9 nm and a mesopore diameter of 14-36 nm.

10. The method for preparing an amino-functionalized multi-level pore molecular sieve according to claim 8, characterized in that: The topological structure of the amino-functionalized multi-level pore molecular sieve includes LTA, FAU, SOD, BIK, CHA, MFI, EMT, MOR or BEA.