Rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material and its preparation method and application

Abstract

The present invention provides a method for preparing and applying a nitrogen-containing framework high-strength pyrogallol-based integral CO2 capture material that can be rapidly polymerized, and belongs to the technical field of preparation and application of porous carbon materials. The present invention uses pyrogallol, diglycolamine, and formaldehyde as raw materials, and utilizes the hydroxyl groups and nitrogen-containing groups in the raw materials to increase CO2-affinity active sites. The reaction conditions are mild, the operation is simple, the cost is low, the energy consumption is low, and it can be produced on a large scale and is convenient for application. Rapid polymerization and shaping are achieved, which not only maintains the inherent CO2 capture capacity and excellent comprehensive performance of the integral carbon material, but also gives it higher mechanical strength and recycling performance. It mainly solves the problems of existing carbon materials that are easy to pulverize, need to be re-molded before use, have low mechanical strength, have pores that are too small to be conducive to diffusion, have low activity, and have limited raw material sources, which are not conducive to industrialization. It has broad application prospects in the fields of energy storage, conversion, adsorption, and catalysis.

Description

Technical Field

[0001] The present invention relates to the field of preparation of porous carbon materials, and in particular to a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based integral CO2 capture material, and a preparation method and application thereof. Background Art

[0002] With the increasing use of coal, oil, and other fuels, global carbon dioxide (CO2) emissions have led to serious environmental problems such as global warming, ocean acidification, and extreme weather. Therefore, developing efficient CO2 capture technology has become one of the key pathways to reducing carbon emissions.

[0003] At present, the materials used for CO2 adsorption at home and abroad mainly include porous carbon, zeolite molecular sieves, metal organic frameworks (MOFs), porous polymers, and monolithic carbon. Compared with monolithic carbon materials, other adsorption materials are mostly powdered or blocky, and need to be reshaped during use. They have disadvantages such as easy bending and breaking, large pressure drop, easy loss, and powder shedding. In addition, the molding process is complicated and wasteful. The addition of binders will also clog the pores, resulting in a decrease in porosity and adsorption capacity during the process. In actual applications, there are problems such as separation and collection difficulties. The emergence of monolithic carbon materials just solves the problems of the need to reshape and complex processes during the use of carbon materials. They are widely used in catalysis, adsorption, energy storage, pharmaceutical industries and other fields.

[0004] There are currently reports of monolithic carbons (CN 109734449 B; CN 112264081 B; CN 101723354A). However, while these monolithic carbons possess a rich pore structure and a certain degree of compressive strength, their compressive strength is insufficient, their wear resistance is poor, they experience severe powder shedding, high wear rates, high costs, demanding reaction conditions, long synthesis times, low adsorption capacity, low activity, and limited raw material sources, making them unsuitable for large-scale production and failing to meet industrial requirements. Therefore, it is particularly important to develop a nitrogen-containing framework high-strength monolithic carbon material with a simple preparation method, easily controllable conditions, low cost, short reaction time, a wide range of raw material sources, large-scale production capabilities, and the ability to be directly molded and carbonized in a mold before use, without compromising the overall performance of the carbon material. Summary of the Invention

[0005] To address these issues, the present invention proposes a rapidly polymerizable, nitrogen-containing framework, high-strength pyrogallol-based monolithic CO2 capture material. Using phenol, aldehyde, and amine as raw materials and an environmentally friendly hydroalcoholic solution as solvent, a nitrogen-oxygen-containing amine source is introduced in the presence of bio-based phenol. The resulting material is then polymerized at low temperature to prepare the nitrogen-containing framework, high-strength pyrogallol-based monolithic CO2 capture material. The nitrogen covalently bonds to the carbon, forming one or both of pyrrole and pyridine structures, which are incorporated into the carbon skeleton. The present invention also provides applications for this monolithic CO2 capture material.

[0006] To achieve the above objectives, the present invention first provides a method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material, comprising the following steps:

[0007] First, pyrogallol and a surfactant are dissolved in an alcohol-water mixed solvent under heating conditions. An amine is added for reaction, followed by the addition of an aldehyde and continued reaction to obtain a benzoxazine-cosol solution. The solution is then placed in a mold, aged, and dried to obtain a monolithic polymer. Finally, the monolithic carbon material is obtained by carbonization and pyrolysis under a nitrogen atmosphere. The amine is selected from one or two of aniline, furfurylamine, diglycolamine, 1,6-hexanediamine, ethylenediamine, and dodecylamine, with a molar ratio of pyrogallol to amine of 275:6.8-27.2. Pyrogallol is a bio-based material containing free phenolic hydroxyl groups extracted from tannins through hydrolysis and decarboxylation.

[0008] Specifically, the surfactant is selected from one or two of the triblock copolymers F127 and P129.

[0009] Preferably, the molar ratio of the phenols to the surfactant is constant at 275:1, and the molar ratio of the phenols to the aldehyde is 1:1 to 1:4.

[0010] Preferably, the carbonization pyrolysis procedure is: under N2 purge, heating to 400°C at 1-3°C / min and holding for 1-2 hours, then heating to 700-900°C at 2-5°C / min and holding for 1-4 hours.

[0011] More preferably, the molar ratio of pyrogallol to amine is 275:27.2, the amine is diglycolamine, and the carbonization pyrolysis procedure is: under N2 purge, heating to 400°C at 1-3°C / min and staying for 1-2h, then heating to 800-900°C at 2-5°C / min and staying for 1-4h.

[0012] More preferably, the molar ratio of pyrogallol to amine is 275:13.6, the amine is diglycolamine, and the carbonization pyrolysis procedure is: under N2 purge, heating to 400°C at 1-3°C / min and staying for 1-2h, then heating to 900°C at 2-5°C / min and staying for 1-4h.

[0013] In order to take into account both the shorter dissolution time and higher reaction rate of pyrogallol and F127, preferably, the mass ratio of anhydrous ethanol to water in the alcohol-water mixed solvent is 1:0.5 to 1:1.

[0014] Preferably, based on 100% total mass of all elements in the carbon material, the nitrogen content is 0.5-15%, the oxygen content is 0.1-10%, and the rest is carbon.

[0015] Preferably, a mold with a certain shape and size is used to adjust the shape and size of the carbon material during the preparation process.

[0016] Preferably, the method for preparing the rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based integral CO2 capture material is characterized in that pyrogallol, a surfactant and an alcohol-water mixed solvent are reacted at 25-35°C for 20-60 minutes to dissolve, amines are added, reacted for 0.5-1 hour, and then an aldehyde solution is added and reacted for 10-30 minutes to obtain a benzoxazine-cosol solution; wherein the alcohol-water mixed solvent is added by directly adding the pyrogallol and the surfactant and then adding the alcohol-water mixed solvent, or adding the alcohol-water mixed solvent together with the pyrogallol and the surfactant, or first adding anhydrous ethanol together with the pyrogallol and the surfactant and then adding the remaining distilled water.

[0017] This invention leverages the flexibility of molecular structure design and the interactions of intramolecular and intermolecular hydrogen bonds. In the presence of bio-based phenol, a nitrogen-containing amine source is introduced, along with a surfactant, into the benzoxazine-cosol. Through a curing, carbonization, and pyrolysis process, a rapidly polymerizable, high-strength, pyrogallol-based monolithic CO2 capture material with a nitrogen-containing framework is prepared in one go. Compared to existing technologies, this invention offers at least the following advantages:

[0018] (1) Using pyrogallol, amines, and formaldehyde as raw materials, an amine source containing nitrogen oxide groups was introduced in the presence of bio-based phenols. A nitrogen-containing porous monolithic carbon material was rapidly synthesized in one step through a sol-gel, curing, and carbonization pyrolysis process. The material was rapidly formed within 15-20 minutes at 90°C and can be scaled up for production.

[0019] (2) The shape, particle size and pore size of the monolithic carbon balls can be controlled by adjusting the amine content, carbonization temperature and the amount of surfactant; the nitrogen content can be adjusted according to different needs.

[0020] (3) The present invention has mild reaction conditions, simple operation, low cost, low energy consumption, no need to add binder and re-sinter, and the physical strength of the formed carbon material can be adjusted according to the raw material ratio, avoiding the problem of balancing high strength, high adsorption capacity and high reproducibility of monolithic carbon materials;

[0021] (4) The nitrogen-containing framework pyrogallol-based monolithic carbon prepared by the present invention has a high nitrogen content and CO2-philic groups, has obvious effects in CO2 capture, and has high compressive strength, strong regeneration ability, and can be reused. BRIEF DESCRIPTION OF THE DRAWINGS

[0022] The drawings described herein are used to provide further understanding of the present invention and constitute a part of the present invention. The exemplary embodiments and descriptions of the present invention are used to explain the present invention and do not constitute improper limitations on the present invention.

[0023] Figure 1 The digital photo, SEM image and N2 adsorption-desorption curve of the monolithic carbon prepared in Example 3 are shown;

[0024] Figure 2 is a physical digital photograph of the monolithic polymer (a) and monolithic carbon (b) prepared in Example 3;

[0025] Figure 3 These are SEM images of the monolithic carbon prepared in Example 3 at different magnifications; a is magnified 2000 times, and b is magnified 5000 times;

[0026] Figure 4 Graphs showing nitrogen adsorption-desorption of the monolithic carbons prepared in Examples 1-9;

[0027] Figure 5 This is the CO2 adsorption isotherm of the monolithic carbon prepared in Examples 1-9 at 25°C; for the specific CO2 testing method, please refer to the literature (Journal of the American Chemical Society 133 (2011) 11378-11388.).

[0028] Figure 6 is a physical digital photograph of the polymer and monolithic carbon prepared in the expanded experiment of Example 3;

[0029] Figure 7 This is a SEM image (b) of the monolithic carbon prepared in Example 8 magnified 5000 times and a physical digital photograph (a) of the monolithic carbon prepared in Example 9.

[0030] Figure 8 This is a comparison chart of the compressive strength and CO2 adsorption capacity of the monolithic carbon prepared in Example 3 and existing carbon materials. DETAILED DESCRIPTION

[0031] The present invention is further described below with reference to the examples and drawings so that those skilled in the art can implement the invention with reference to the description. The experimental methods described in the following embodiments are conventional methods unless otherwise specified, and the reagents and materials are commercially available unless otherwise specified.

[0032] Specifically, each embodiment is carried out according to the parameters shown in Table 1.

[0033] Table 1: Experimental conditions, BET parameters and compressive strength corresponding to Examples 1-9 and compressive strength of commercially available carbon materials

[0034]

[0035] Example 1

[0036] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material was prepared by the following molar ratios: the molar ratio of pyrogallol (PG), diglycolamine (DGA) and F127 was constant at 275:6.8:1 (named PG-DGA-1), and the molar ratio of pyrogallol to formaldehyde solution was constant at 1:4.

[0037] First, 1.05 g of pyrogallol, 0.44 g of surfactant F127, and 6 g of a hydroalcoholic solution (anhydrous ethanol:distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes. Subsequently, 0.026 g of diglycolamine was weighed and added to the solution, and stirred for 30 minutes until it turned beige. 1.47 g of formaldehyde solution was quickly injected into the solution, and stirring continued for 10 minutes to obtain a benzoxazine-cosol solution. This solution was then sealed in a cylindrical mold and placed in a 90°C constant-temperature oven. The reaction system polymerized within 15-20 minutes and aged for 4 hours. After aging, the mixture was removed and dried at 50°C for 48 hours to obtain the PG-DGA-1 monolithic polymer. Under a nitrogen purge, the temperature was increased at 2°C / min to 400°C, where it remained for 1 hour. Then, the temperature was increased at 5°C / min to 800°C, where it remained for 2 hours. Finally, the temperature was naturally cooled to obtain the PG-DGA-1 monolithic carbon material.

[0038] Example 2

[0039] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material was prepared by the following molar ratio: the molar ratio of pyrogallol, diglycolamine, and F127 was constant at 275:13.6:1 (named PG-DGA-2), and the molar ratio of pyrogallol to formaldehyde solution was constant at 1:4.

[0040] First, 1.05g of pyrogallol, 0.44g of surfactant F127, and 6g of a hydroalcoholic solution (anhydrous ethanol:distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes. Subsequently, 0.052g of diglycolamine was weighed and added to the solution, and stirred for 30 minutes until it turned beige. 1.47g of formaldehyde solution was quickly injected into the solution and stirred for 10 minutes to obtain a benzoxazine-cosol solution. This solution was then sealed in a cylindrical mold and placed in a 90°C constant temperature oven. The reaction system polymerized within 15-20 minutes and aged for 4 hours. After aging, the system was removed and dried at 50°C for 48 hours to obtain the PG-DGA-2 monolithic polymer. The carbonization process was the same as in Example 1, resulting in the PG-DGA-2 monolithic carbon material.

[0041] Example 3

[0042] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material was prepared by the following molar ratio: the molar ratio of pyrogallol, diglycolamine, and F127 was constant at 275:27.2:1 (named PG-DGA-3), and the molar ratio of pyrogallol to formaldehyde solution was constant at 1:4.

[0043] First, 1.05g of pyrogallol, 0.44g of surfactant F127 and 6g of hydroalcohol solution (anhydrous ethanol: distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20min (turned light yellow). Subsequently, 0.104g of diglycolamine was weighed and added to the above solution, and stirred for 30min until it turned beige. 1.47g of formaldehyde solution was quickly injected into the above solution and continued to stir for 10min to obtain a benzoxazine-cosol solution; after it was placed in a cylindrical mold and sealed, it was transferred to a constant temperature oven at 90°C. The reaction system completed polymerization within 15 to 20min and aged for 4h. The carbonization process is the same as that in Example 1, and the PG-DGA-3 integral carbon material is finally obtained. The actual digital photos of the integral polymer and integral carbon prepared in this embodiment are shown in the figure. Figure 2 As shown in FIG, it can be seen that the monolithic carbon material prepared is intact and resistant to powdering. The scanning electron microscopy of the monolithic carbon prepared in this embodiment is as follows Figure 3 As shown in Figure 2, its morphology is a relatively regular spherical structure with rich mesoporous structure. Its CO2 adsorption capacity is better than many existing carbon materials. Its BET specific surface area is about 316m 2 g -1 ( Figure 4and Table 1). With increasing DGA content, the specific surface area and compressive strength increase. PG-DGA-3 exhibits a compressive strength exceeding 8 MPa, which is 43 times the mechanical strength of monolithic carbon materials prepared using a hard template (0.19 MPa) and 40 times the mechanical strength of monolithic carbon materials prepared using a soft template (0.2 MPa). This monolithic carbon exhibits high CO2 capture capacity precisely due to its high number of CO2-philic groups (N groups) and rich pore structure. The thick spherical structure, cross-linked by chemical bonds, forms a tightly packed network skeleton, resulting in excellent mechanical strength.

[0044] Example 4

[0045] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material is prepared by the following molar ratios: the molar ratio of pyrogallol (PG), diglycolamine (DGA) and F127 is constant at 275:6.8:1, and the molar ratio of pyrogallol to formaldehyde solution is constant at 1:4.

[0046] First, 1.05 g of pyrogallol, 0.44 g of surfactant F127, and 6 g of a hydroalcoholic solution (anhydrous ethanol:distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes. Subsequently, 0.026 g of diglycolamine was weighed and added to the solution, and stirred for 30 minutes until it turned beige. 1.47 g of formaldehyde solution was quickly injected into the solution, and stirring continued for 10 minutes to obtain a benzoxazine-cosol solution. This solution was then sealed in a cylindrical mold and placed in a 90°C constant-temperature oven. The reaction system polymerized within 15-20 minutes and aged for 4 hours. After aging, the reaction mixture was removed and dried at 50°C for 48 hours to obtain the PG-DGA-900-1 monolithic polymer. Under a nitrogen purge, the temperature was increased at 2°C / min to 400°C, where it remained for 2 hours. The temperature was then increased at 5°C / min to 900°C, where it remained for 3 hours. Finally, the PG-DGA-900-1 monolithic carbon material was obtained by natural cooling.

[0047] Example 5

[0048] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material is prepared by the following molar ratios: the molar ratio of pyrogallol, diglycolamine, and F127 is constant at 275:13.6:1, and the molar ratio of pyrogallol to formaldehyde solution is constant at 1:4.

[0049] First, 1.05g of pyrogallol, 0.44g of surfactant F127, and 6g of a hydroalcoholic solution (anhydrous ethanol:distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes. Subsequently, 0.052g of diglycolamine was weighed and added to the solution, and stirred for 30 minutes until it turned beige. 1.47g of formaldehyde solution was quickly injected into the solution and stirred for 10 minutes to obtain a benzoxazine-cosol solution. This solution was then sealed in a cylindrical mold and placed in a 90°C constant temperature oven. The reaction system completed polymerization within 15-20 minutes and was aged for 4 hours. The carbonization process was identical to that in Example 4, resulting in the PG-DGA-900-2 monolithic carbon material.

[0050] Example 6

[0051] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material is prepared by the following molar ratios: the molar ratio of pyrogallol, diglycolamine, and F127 is constant at 275:27.2:1, and the molar ratio of pyrogallol to formaldehyde solution is constant at 1:4.

[0052] First, 1.05g of pyrogallol, 0.44g of surfactant F127 and 6g of hydroalcohol solution (anhydrous ethanol: distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes (turning light yellow). Subsequently, 0.104g of diglycolamine was weighed and added to the above solution and stirred for 30 minutes until it turned beige. 1.47g of formaldehyde solution was quickly injected into the above solution and continued to stir for 10 minutes to obtain a benzoxazine-cosol solution; after being placed in a cylindrical mold and sealed, it was transferred to a constant temperature oven at 90°C. The reaction system completed polymerization within 15 to 20 minutes and aged for 4 hours. The carbonization process was the same as in Example 4, and the PG-DGA-900-3 monolithic carbon material was finally obtained. As the carbonization temperature increased, the pore size increased, and the corresponding compressive strength decreased. (Table 1)

[0053] Example 7

[0054] Example 3 was expanded and tested

[0055] First, 3.15g of pyrogallol, 1.32g of surfactant F127 and 18g of hydroalcohol solution (anhydrous ethanol: distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20min (turned light yellow). Subsequently, 0.312g of diglycolamine was weighed and added to the above solution, and stirred for 30min until it turned beige. 4.41g of formaldehyde solution was quickly injected into the above solution and continued to stir for 10min to obtain a benzoxazine-cosol solution; after it was placed in a cylindrical mold and sealed, it was transferred to a constant temperature oven at 90°C. The reaction system completed polymerization within 15 to 20min and aged for 4h. The carbonization process is the same as that in Example 3, and the PG-DGA-3 integral carbon material is finally obtained. The actual digital photos of the integral polymer and integral carbon prepared by the expanded experiment of this embodiment are shown in the figure. Figure 5 As shown, it can be seen that the prepared monolithic carbon material is intact and resistant to powdering.

[0056] Example 8

[0057] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material is prepared by the following molar ratios: the molar ratio of pyrogallol, diglycolamine, 1,6-hexanediamine (DAH) to F127 is constant at 275:13.6:13.6:1, and the molar ratio of pyrogallol to formaldehyde solution is constant at 1:4.

[0058] First, 1.05g of pyrogallol, 0.44g of surfactant F127, and 6g of a hydroalcoholic solution (anhydrous ethanol:distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes. Subsequently, 0.052g of diglycolamine and 0.05g of 1,6-hexanediamine were weighed and added to the solution, and stirred for 30 minutes until it turned beige. 1.47g of formaldehyde solution was quickly injected into the solution, and stirring continued for 10 minutes to obtain a benzoxazine-cosol solution. This solution was then sealed in a cylindrical mold and placed in a 90°C oven. The reaction system completed polymerization within 15-20 minutes and was aged for 4 hours. The carbonization process was identical to that in Example 3, resulting in a PG-DGA-DAH monolithic carbon material. Figure 7 This is the SEM image of the monolithic carbon prepared in this example. Its morphology is a uniform carbon ball network structure, which is the reason for its high compressive strength. By changing the type of amine, higher compressive strength and CO2 adsorption capacity are obtained.

[0059] Example 9

[0060] A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material is prepared by the following molar ratios: the molar ratio of pyrogallol, dodecylamine (D) and F127 is constant at 275:27.2:1, and the molar ratio of pyrogallol to formaldehyde solution is constant at 1:4.

[0061] First, 1.05g of pyrogallol, 0.44g of surfactant F127, and 6g of a hydroalcoholic solution (anhydrous ethanol:distilled water = 1:1) were placed in a round-bottom flask and stirred at 35°C for 20 minutes. Subsequently, 0.183g of dodecylamine was weighed and added to the solution, and stirred for 30 minutes until it turned beige. 1.47g of formaldehyde solution was quickly injected into the solution and stirred for 10 minutes to obtain a benzoxazine-cosol solution. This solution was then sealed in a cylindrical mold and placed in a 90°C constant temperature oven. The reaction system completed polymerization within 15-20 minutes and was aged for 4 hours. The carbonization process was identical to that in Example 3, resulting in a PG-D monolithic carbon material.

[0062] Although the embodiments of the present invention have been disclosed above, they are not limited to the applications listed in the description and implementation methods. They can be fully applied to various fields suitable for the present invention. For those familiar with the art, additional modifications can be easily implemented. Therefore, without departing from the general concept defined by the claims and the scope of equivalents, the present invention is not limited to the specific details and illustrations shown and described herein.

Claims

1. A method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material, characterized in that: The method comprises the following steps: first, dissolving pyrogallol and a surfactant in an alcohol-water mixed solvent under heating conditions, adding an amine, reacting, adding an aldehyde, and continuing the reaction to obtain a benzoxazine-cosol solution; then, filling the solution into a mold, aging, and drying to obtain a monolithic polymer; and finally, carbonizing and pyrolyzing the solution under a nitrogen atmosphere to obtain a monolithic carbon material; wherein the molar ratio of pyrogallol to the amine is 275:27.2, the amine is diglycolamine, and the carbonization and pyrolysis procedure is as follows: under nitrogen purge, heating to 400°C at a rate of 1-3°C / min, holding for 1-2 hours, then heating to 800°C at a rate of 2-5°C / min, and holding for 1-4 hours; Alternatively, the molar ratio of pyrogallol to amine is 275:13.6, the amine is diglycolamine, and the carbonization pyrolysis procedure is: under N2 purge, heating to 400°C at 1-3°C / min and staying for 1-2 hours, then heating to 900°C at 2-5°C / min and staying for 1-4 hours.

2. The method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 1, characterized in that: The surfactant is selected from one or two of the triblock copolymers F127 and P129.

3. The method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 1, characterized in that: The molar ratio of pyrogallol to surfactant is constant at 275:1, and the molar ratio of pyrogallol to aldehydes is 1:1 to 1:

4.

4. The method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 1, characterized in that: The carbonization pyrolysis procedure is as follows: in a nitrogen atmosphere, the temperature is increased to 400°C at a rate of 1-3°C / min and kept for 1-2 hours, then the temperature is increased to 700-900°C at a rate of 2-5°C / min and kept for 1-4 hours.

5. The method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 1, characterized in that: The alcohol in the alcohol-water mixed solvent is anhydrous ethanol, and the mass ratio of anhydrous ethanol to water is 1:0.5 to 1:

1.

6. The method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 1, characterized in that: The method further comprises the following steps: reacting pyrogallol, a surfactant and an alcohol-water mixed solvent at 25-35° C. for 20-60 minutes to dissolve the pyrogallol, the surfactant and the alcohol-water mixed solvent, adding an amine, reacting the amine for 0.5-1 hour, adding an aldehyde solution, and reacting the aldehyde solution for 10-30 minutes to obtain a benzoxazine-cosol solution.

7. The method for preparing a rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 1, characterized in that: The aldehyde is formaldehyde.

8. A rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material prepared by the method of any one of claims 1 to 7.

9. An application of the rapidly polymerizable nitrogen-containing framework high-strength pyrogallol-based monolithic CO2 capture material according to claim 8, characterized in that: Used for CO2 capture.

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