High-efficiency catalyst for aniline production

Abstract

The present application provides an efficient catalyst for aniline production. The efficient catalyst for aniline production comprises a supported cobalt tetraoxide catalyst and a porous carbon catalyst embedded with transition metals, and the preparation raw material of the supported cobalt tetraoxide catalyst comprises a carbon carrier, cobalt nitrate and a first polyethylene glycol. The efficient catalyst for aniline production prepared by using the supported cobalt tetraoxide catalyst and the porous carbon catalyst embedded with transition metals provided by the present application has high nitrobenzene conversion rate and aniline selectivity, and still has high nitrobenzene conversion rate and aniline selectivity at low temperature. The efficient catalyst for aniline production prepared by the present application still has high nitrobenzene conversion rate and aniline selectivity at low temperature after being used for multiple times, and the stability of the efficient catalyst for aniline production prepared by the present application is high.

Description

Technical Field

[0001] This invention belongs to the field of catalyst technology, specifically relating to a high-efficiency catalyst for aniline production. Background Technology

[0002] Aniline, also known as aminobenzene, is an organic compound, a colorless, oily liquid that decomposes upon heating to 370℃. It is slightly soluble in water but readily soluble in organic solvents such as ethanol and ether. Aniline is used not only in the manufacture of dyes, pharmaceuticals, resins, and rubber vulcanization accelerators, but also as a raw material for the preparation of black dyes. Aniline is an important chemical product. With the development of the chemical industry, the demand for aniline is increasing daily.

[0003] Currently, the main industrial methods for producing aniline include: nitrobenzene iron powder reduction, direct phenol ammoniation, and nitrobenzene catalytic hydrogenation. Among these, the nitrobenzene iron powder reduction method is an earlier process for aniline preparation, but it suffers from significant environmental pollution, equipment corrosion, difficulty in continuous production, low efficiency, and difficulty in product separation, and is now rarely used. The direct phenol ammoniation method has advantages such as a simple process flow, continuous and stable operation, less waste, and lower pollution pressure, but it also has disadvantages such as high raw material consumption, low ammonia utilization, and higher overall production costs, thus limiting its use. The nitrobenzene liquid-phase hydrogenation method within the nitrobenzene catalytic hydrogenation process has advantages such as low reaction temperature, fewer side reactions, large equipment production capacity, and low total investment, and is widely used as an energy-saving and environmentally friendly production route.

[0004] The catalyst plays a crucial role in the liquid-phase hydrogenation process of nitrobenzene. Catalysts mainly include noble metal catalysts and non-noble metal catalysts. Among them, noble metal catalysts mainly include Pd-based, Pt-based, Au-based, and Rh-based noble metal catalysts supported on supports such as alumina and activated carbon. Noble metal catalysts have the advantage of high catalytic efficiency, but they also have disadvantages such as high price, which increases the production cost of aniline and limits their use. Non-noble metal catalysts are relatively inexpensive, but they also have problems such as poor stability, poor catalytic efficiency at low temperatures, and significant reduction in catalytic efficiency after repeated use.

[0005] To address the problems existing in existing non-precious metal catalysts, this invention aims to develop a highly efficient catalyst for aniline production that improves the catalytic effect at low temperatures and maintains high catalytic performance even after multiple uses. Summary of the Invention

[0006] The purpose of this invention is to provide a highly efficient catalyst for aniline production, thereby solving the problems of poor stability, poor catalytic efficiency at low temperatures, and significant decrease in catalytic efficiency after repeated use of non-precious metal catalysts mentioned in the background art.

[0007] To achieve the above objectives, the present invention provides the following technical solution: On one hand, the present invention provides a high-efficiency catalyst for aniline production, which comprises a supported cobalt tetroxide catalyst and a porous carbon-type catalyst intercalated with transition metals.

[0008] As a further improvement, the mass ratio of the supported cobalt tetroxide catalyst to the intercalated porous carbon catalyst is 0.2-0.4:1.

[0009] As a further improvement, the porous carbon catalyst with intercalated transition metals is a porous carbon catalyst with intercalated nickel.

[0010] The raw materials for preparing the supported cobalt tetroxide catalyst include a carbon support, cobalt nitrate, and polyethylene glycol I.

[0011] Furthermore, the preparation method of the supported cobalt tetroxide catalyst includes the following steps: After ultrasonic treatment of a mixture of carbon support, first polyethylene glycol, and organic alcohol, the mixture was added to a reaction vessel. The temperature of the reaction vessel was controlled at 40-50℃. Then, under magnetic stirring, cobalt nitrate solution and inorganic alkali solution were added dropwise to the reaction vessel. After the addition was completed, the pH of the system was controlled at 9-10. After the reaction was completed, a strong oxide solution was added and stirred evenly. The mixture was then aged, washed, dried, calcined, and cooled to obtain a supported cobalt tetroxide catalyst.

[0012] Furthermore, the first polyethylene glycol includes at least one of polyethylene glycol 10000 and polyethylene glycol 20000.

[0013] Furthermore, the organic alcohols are small molecule organic alcohols.

[0014] Furthermore, organic alcohols include at least one of anhydrous ethanol, anhydrous methanol, ethylene glycol, isopropanol, and n-butanol.

[0015] Furthermore, the strong oxide solution includes at least one of hydrogen peroxide solution and potassium permanganate solution.

[0016] Furthermore, the method for preparing the carbon support includes the following steps: After mixing and stirring the chloride salt, carbon source, and water evenly, continue stirring at 80-90℃ until a viscous liquid is formed. Then, dry and carbonize the liquid. After carbonization, wash and dry to obtain the carbon carrier.

[0017] Furthermore, the carbon source includes, but is not limited to, at least one of glucose, starch, sucrose, and cyclodextrin; furthermore, glucose includes glucose monohydrate.

[0018] Furthermore, the chloride salts include, but are not limited to, at least one of magnesium chloride, sodium chloride, lithium chloride, copper chloride, zinc chloride, calcium chloride, and ferric chloride.

[0019] Furthermore, in the preparation method of the carbon support, the stirring temperature is 85-90℃.

[0020] Furthermore, in the preparation method of the carbon support, the washing process includes acid washing and water washing.

[0021] Furthermore, the pickling is performed using a 0.5 mol / L to 4 mol / L dilute hydrochloric acid solution.

[0022] Furthermore, carbonization is carried out in an inert environment.

[0023] Furthermore, the raw materials for preparing porous carbon-type catalysts embedded with precious metals include nickel-containing solutions and honeycomb ceramics.

[0024] Furthermore, the preparation method of the porous carbon catalyst embedded with transition metals includes the following steps: phenol, aldehyde, nickel-containing solution, and second polyethylene glycol are stirred until dissolved, the pH of the system is adjusted to 8-10, and then polymerized at 60-80℃ for 2-5 hours to obtain an impregnation solution. The honeycomb ceramic is immersed in the above impregnation solution. After full impregnation, the excess resin in the pores is blown away. The impregnated honeycomb ceramic is placed in a mixed atmosphere for full curing, and then calcined, carbonized, reduced, and cooled to obtain the porous carbon catalyst embedded with transition metals.

[0025] Furthermore, the honeycomb ceramics include at least one of silicon carbide honeycomb ceramics, aluminum titanate honeycomb ceramics, and mullite honeycomb ceramics.

[0026] Furthermore, the nickel-containing solution is prepared by mixing nickel nitrate hexahydrate and anhydrous ethanol.

[0027] Furthermore, aldehydes are specifically formaldehyde.

[0028] Furthermore, the second polyethylene glycol includes at least one of polyethylene glycol 1000, polyethylene glycol 4000, polyethylene glycol 6000, and polyethylene glycol 8000.

[0029] Furthermore, the aldehydes are at least one of formaldehyde, terephthalaldehyde, pyromellitic terephthalaldehyde, and 2,5-divinyl-1,4-phenylenedialdehyde.

[0030] Compared with the prior art, the beneficial effects of the present invention are as follows: the high-efficiency catalyst for aniline production prepared by using the supported cobalt tetroxide catalyst and the porous carbon catalyst intercalated with transition metal provided by the present invention has high nitrobenzene conversion and aniline selectivity. It still has high nitrobenzene conversion and aniline selectivity at low temperature. Moreover, the high-efficiency catalyst for aniline production prepared by the present invention still has high nitrobenzene conversion and aniline selectivity at low temperature after multiple uses. The high-efficiency catalyst for aniline production prepared by the present invention has high stability. Detailed Implementation

[0031] The present invention will be described below with reference to specific embodiments. It should be noted that the following embodiments are examples of the present invention and are used only to illustrate the invention, not to limit it. Other combinations and various modifications within the scope of the present invention can be made without departing from its spirit or scope.

[0032] In the following examples, except for carbon support A, supported cobalt tetroxide catalyst A, cobalt-containing catalyst A, nickel-embedded porous carbon catalyst A, and nickel-containing catalyst A, all other compound monomers and related reagents used were commercially available. Specifically, polyethylene glycol 20000 and polyethylene glycol 1000 were purchased from Jiangsu Haian Petrochemical Plant; silicon carbide honeycomb ceramics were purchased from Pingxiang Rongjian Environmental Protection Chemical Packing Co., Ltd., with custom-made dimensions (10mm×10mm×20mm); silica sol was purchased from Guangdong Nanolide Nanotechnology Co., Ltd., model HSW-1630; commercially available nickel catalyst was purchased from Shanghai Xunkai New Materials Technology Co., Ltd., model SNCAT-6210P; and commercially available cobalt catalyst was purchased from Shanghai Xunkai New Materials Technology Co., Ltd., model CoCAT-3000Q.

[0033] The preparation method of carbon support A includes the following steps: Mix 60g zinc chloride and 20g glucose monohydrate (molecular formula C6H4) 12 After adding O6·H2O and 60 mL of distilled water to a beaker and mechanically stirring until well mixed, the mixture was added to a reaction vessel. The reaction vessel temperature was controlled at 85℃, and the mixture was magnetically stirred at a constant temperature for 10 hours until a viscous liquid was formed. Then, it was dried in a drying oven (temperature 105℃) for 4 hours. Next, the tube furnace was purged with nitrogen at room temperature for 30 minutes (nitrogen flow rate 50 mL / min). Under a nitrogen atmosphere, the tube furnace was heated to 450℃ at a rate of 3℃ / min, and then carbonized in the tube furnace at 450℃ for 2 hours (nitrogen flow rate 50 mL / min). After carbonization, the material is ground and then acid-washed five times (the acid-washing method is as follows: the carbonized material is mixed with 100 mL of 1 mol / L dilute hydrochloric acid and boiled for 15 min, with stirring during the acid-washing process). Then it is washed with deionized water until neutral and dried in a forced-air drying oven (temperature of forced-air drying oven is 105℃) for 10 h to obtain carbon carrier A. The outlet of the tube furnace is connected to a gas washing bottle containing 200 mL of 1 mol / L sodium hydroxide solution. The number of gas washing bottles can be set according to actual needs.

[0034] The preparation method of supported cobalt tetroxide catalyst A includes the following steps: A mixture of 10g carbon support A, 5g polyethylene glycol 20000, and 80mL anhydrous ethanol was ultrasonically treated for 20min and then added to a reaction vessel. The temperature of the reaction vessel was controlled at 45℃. Then, under magnetic stirring, cobalt nitrate solution (prepared by mixing 4g cobalt nitrate hexahydrate with 28mL anhydrous ethanol) and inorganic alkali solution (prepared by mixing 2.5g ammonium bicarbonate with 30mL distilled water) were added dropwise to the reaction vessel at a rate of 30 drops / min. After the addition was complete, the pH of the system was controlled to 9 using a 20% ammonia solution. After reacting for 2h, 5mL of 20% hydrogen peroxide solution was slowly added dropwise and stirred evenly. The mixture was then aged at 150℃ for 1.5h, washed four times alternately with distilled water and anhydrous ethanol, and dried in a forced-air drying oven (temperature of forced-air drying oven was 120℃, drying time was 4 hours). The tube furnace was purged with nitrogen for 30 minutes at room temperature (nitrogen flow rate of 50 mL / min). Under nitrogen atmosphere, the tube furnace was heated to 300℃ at a rate of 3℃ / min, and then calcined at 300℃ for 2.5 hours (nitrogen flow rate of 50 mL / min). The tube furnace was then heated to 500℃ at a rate of 3℃ / min, and then calcined at 500℃ for 2.5 hours (mixed atmosphere flow rate of 50 mL / min). Then, nitrogen was introduced at a flow rate of 50 mL / min for 30 minutes, and then the furnace was cooled to room temperature under nitrogen atmosphere (nitrogen flow rate of 50 mL / min) to obtain supported cobalt tetroxide catalyst A. The outlet of the tube furnace was connected to a gas washing bottle containing 200 mL of 1 mol / L sodium hydroxide solution. The number of gas washing bottles can be set according to actual needs.

[0035] The preparation method of cobalt-containing catalyst A includes the following steps: A mixture of 10g glucose monohydrate, 5g polyethylene glycol 20000, and 80mL anhydrous ethanol was ultrasonically treated for 20 minutes and then added to a reaction vessel. The reaction vessel temperature was controlled at 45℃. Under magnetic stirring, a cobalt nitrate solution (prepared by mixing 4g cobalt nitrate hexahydrate with 28mL anhydrous ethanol) and an inorganic alkali solution (prepared by mixing 2.5g ammonium bicarbonate with 30mL distilled water) were added dropwise to the reaction vessel at a rate of 30 drops / min. After the addition was complete, the pH of the system was controlled to 9 using a 20% ammonia solution. After reacting for 2 hours, 5mL of 20% hydrogen peroxide solution was slowly added dropwise and stirred until homogeneous. The mixture was then aged at 150℃ for 1.5 hours, alternating between distilled water and anhydrous ethanol. The sample was washed four times and dried in a forced-air drying oven (temperature 120℃, drying time 4.5h). Then, the tube furnace was purged with nitrogen at room temperature for 30 minutes (nitrogen flow rate 50mL / min). Under nitrogen atmosphere, the tube furnace was heated to 300℃ at a rate of 3℃ / min, and then calcined at 300℃ for 5h (nitrogen flow rate 50mL / min). After purging with nitrogen at a flow rate of 50mL / min for 30 minutes, the temperature was lowered to room temperature under nitrogen atmosphere (nitrogen flow rate 50mL / min) to obtain cobalt-containing catalyst A. The outlet of the tube furnace was connected to a gas washing bottle containing 200mL of 1mol / L sodium hydroxide solution. The number of gas washing bottles can be set according to actual needs.

[0036] A method for preparing a nickel-embedded porous carbon catalyst A includes the following steps: 20g phenol, 25mL formaldehyde, 4g nickel-containing solution (prepared by mixing nickel nitrate hexahydrate and anhydrous ethanol in a mass ratio of 2:8), and 1g polyethylene glycol 1000 were stirred until dissolved. While stirring, a 20% ammonia solution was slowly added to adjust the pH of the system to 8. Polymerization was then carried out at 70℃ for 3 hours to obtain an impregnation solution. Silicon carbide honeycomb ceramics were vacuum-immersed in this impregnation solution at a temperature of 50℃ for 8 hours. After impregnation, excess resin was removed from the pores. The impregnated silicon carbide honeycomb ceramics were then placed in a mixed atmosphere (composed of oxygen and nitrogen in a volume ratio of 1:4, with a flow rate of 50mL / min) for complete curing at 120℃ for 6 hours. After curing, a tube furnace was purged with nitrogen at room temperature for 30 minutes (nitrogen flow rate of 50mL / min). Under a nitrogen atmosphere, the tube furnace was heated to 40℃ at a rate of 2℃ / min. After reaching 0°C, calcination was performed in a tube furnace at 400°C for 1.5 hours. Then, under a nitrogen atmosphere, the temperature was increased to 700°C in the tube furnace at a rate of 2°C / min. Carbonization was then carried out in the tube furnace at 700°C for 5 hours (nitrogen flow rate of 50 mL / min). Afterward, the temperature was lowered to 400°C under nitrogen protection (nitrogen flow rate of 50 mL / min), and a mixed gas (hydrogen and nitrogen in a volume ratio of 1:19) was introduced at a flow rate of 50 mL / min. After purging for 30 minutes, the mixture was reduced in a mixed gas at 400℃ for 3 hours. Then, nitrogen gas was introduced at a flow rate of 50 mL / min to purge for 30 minutes. The mixture was then cooled to room temperature under a nitrogen atmosphere (nitrogen flow rate of 50 mL / min) to obtain a porous carbon catalyst A with embedded nickel. The tube furnace was equipped with a gas washing bottle containing a 500 mL volume of 1 mol / L sodium hydroxide solution to absorb acidic gases. The number of gas washing bottles could be set according to actual needs.

[0037] The preparation method of nickel-containing catalyst A includes the following steps: 4g of a nickel-containing solution (prepared by mixing nickel nitrate hexahydrate and water in a mass ratio of 2:8) and 2g of silica sol were stirred until dissolved. The silicon carbide honeycomb ceramic was then vacuum-immersed in the solution at a temperature of 50°C for 8 hours. After impregnation, the ceramic was dried at 120°C for 6 hours. The dried silicon carbide honeycomb ceramic was then placed in a tube furnace. The furnace was purged with nitrogen at a flow rate of 50 mL / min for 30 minutes at room temperature. The furnace was then heated to 400°C under a nitrogen atmosphere at a heating rate of 2°C / min before calcination. After calcining for 1.5 hours, a mixed gas (hydrogen and nitrogen in a volume ratio of 1:19) is introduced at a flow rate of 50 mL / min and purged for 30 minutes. Then, the mixture is reduced in the mixed gas at a temperature of 400℃ for 3 hours. After that, nitrogen is introduced at a flow rate of 50 mL / min and purged for 30 minutes. Finally, the mixture is cooled to room temperature under a nitrogen atmosphere (nitrogen flow rate of 50 mL / min) to obtain nickel-containing catalyst A. The tube furnace is equipped with a gas washing bottle containing a 1 mol / L sodium hydroxide solution with a volume of 500 mL to absorb acidic gases. The number of gas washing bottles can be set according to actual needs. Example

[0038] A highly efficient catalyst for aniline production comprises a supported cobalt tetroxide catalyst A and a nickel-intercalated porous carbon catalyst A in a mass ratio of 0.3:1. Example

[0039] A highly efficient catalyst for aniline production comprises a supported cobalt tetroxide catalyst A and a nickel-intercalated porous carbon catalyst A in a mass ratio of 0.25:1. Example

[0040] A highly efficient catalyst for aniline production comprises a supported cobalt tetroxide catalyst A and a nickel-intercalated porous carbon catalyst A in a mass ratio of 0.4:1. Example

[0041] A highly efficient catalyst for aniline production comprises a supported cobalt tetroxide catalyst A and a nickel-intercalated porous carbon catalyst A in a mass ratio of 0.1:1. Example

[0042] A highly efficient catalyst for aniline production comprises a supported cobalt tetroxide catalyst A and a nickel-intercalated porous carbon catalyst A in a mass ratio of 1:1. Example

[0043] A highly efficient catalyst for aniline production comprises a cobalt-containing catalyst A and a nickel-intercalated porous carbon catalyst A in a mass ratio of 0.3:1. Example

[0044] A highly efficient catalyst for aniline production comprises a supported cobalt tetroxide catalyst A and a nickel-containing catalyst A in a mass ratio of 0.3:1. Example

[0045] A high-efficiency catalyst for aniline production, comprising a cobalt-containing catalyst A and a nickel-containing catalyst A in a mass ratio of 0.3:1.

[0046] Comparative Example 1: A highly efficient catalyst for aniline production, specifically a supported cobalt tetroxide catalyst A.

[0047] Comparative Example 2: A highly efficient catalyst for aniline production, wherein the highly efficient catalyst for aniline production is a porous carbon catalyst A with nickel intercalation.

[0048] Comparative Example 3: A highly efficient catalyst for aniline production, wherein the highly efficient catalyst for aniline production is a commercially available nickel catalyst.

[0049] Comparative Example 4: A highly efficient catalyst for aniline production, wherein the highly efficient catalyst for aniline production is a commercially available cobalt catalyst.

[0050] Comparative Example 5: A highly efficient catalyst for aniline production, comprising a commercially available nickel catalyst and a commercially available cobalt catalyst in a mass ratio of 0.3:1.

[0051] The catalysts of Examples 1-8 and Comparative Examples 1-5 were used for the liquid-phase hydrogenation of nitrobenzene to aniline. The reaction process included: placing 100 mL of nitrobenzene, 120 mL of toluene and 0.5 g of a high-efficiency catalyst for aniline production in a reaction vessel, and reacting for 40 min at temperatures of 100 °C and 120 °C and a hydrogen pressure of 2 MPa, respectively. After the reaction was completed, the mixture was cooled to room temperature, and samples were taken for analysis using gas chromatography. The conversion rate of nitrobenzene and the selectivity of aniline are shown in Table 1.

[0052] Table 1

[0053] As can be seen from the comparison of Examples 1 and 4-5 in Table 1, the high-efficiency catalyst for aniline production prepared by using the supported cobalt tetroxide catalyst and the porous carbon catalyst intercalated with transition metals in combination, and when their mass ratio is within a suitable range, has high nitrobenzene conversion and aniline selectivity. Even when the temperature is reduced, it still has high nitrobenzene conversion and aniline selectivity. As can be seen from the comparison of Examples 1 and 6-8 in Table 1, the high-efficiency catalyst for aniline production prepared by using the supported cobalt tetroxide catalyst and the porous carbon catalyst with intercalated transition metals provided by the present invention has high nitrobenzene conversion and aniline selectivity. It still has high nitrobenzene conversion and aniline selectivity at low temperatures. As can be seen from the comparison of Example 1 and Comparative Examples 1-2 in Table 1, compared with using only one of the supported cobalt tetroxide catalyst and the porous carbon catalyst with intercalated transition metal, the high-efficiency catalyst for aniline production prepared by using the combination of the supported cobalt tetroxide catalyst and the porous carbon catalyst with intercalated transition metal has high nitrobenzene conversion and aniline selectivity, and still has high nitrobenzene conversion and aniline selectivity at low temperature; As can be seen from the comparison of Example 1 and Comparative Examples 3-5 in Table 1, the high-efficiency catalyst for aniline production prepared by using the supported cobalt tetroxide catalyst and the porous carbon catalyst intercalated with transition metals provided by the present invention, and the combination of the supported cobalt tetroxide catalyst and the porous carbon catalyst intercalated with transition metals, has high nitrobenzene conversion and aniline selectivity. It still has high nitrobenzene conversion and aniline selectivity at low temperatures. The catalyst from Example 1 was centrifuged and separated. The separated catalyst was then used to catalyze the hydrogenation of nitrobenzene under the same conditions. After being reused 10, 20, and 30 times, the nitrobenzene conversion and aniline selectivity are shown in Table 2.

[0054] Table 2

[0055] As can be seen from the experimental data in Table 2, the high-efficiency catalyst for aniline production prepared by using both the supported cobalt tetroxide catalyst and the porous carbon catalyst with intercalated transition metals provided by the present invention still has a high nitrobenzene conversion rate and aniline selectivity at low temperature after multiple uses. The catalytic effect does not decrease significantly after multiple uses, indicating that the high-efficiency catalyst for aniline production prepared by the present invention has high stability.

[0056] In summary, the highly efficient catalyst for aniline production prepared by simultaneously using the supported cobalt tetroxide catalyst and the porous carbon catalyst intercalated with transition metals provided by this invention exhibits high nitrobenzene conversion and aniline selectivity. It also maintains high nitrobenzene conversion and aniline selectivity at low temperatures. Furthermore, the highly efficient catalyst for aniline production prepared by this invention still maintains high nitrobenzene conversion and aniline selectivity at low temperatures after multiple uses. The highly efficient catalyst for aniline production prepared by this invention has high stability.

[0057] The above embodiments are only for illustrating the technical concept and features of the present invention, and are intended to enable those skilled in the art to understand the content of the present invention and implement it. They should not be used to limit the scope of protection of the present invention. All equivalent changes or modifications made in accordance with the spirit and essence of the present invention should be covered within the scope of protection of the present invention.

Claims

1. A high-efficiency catalyst for aniline production, characterized in that: The high-efficiency catalyst for aniline production comprises a supported cobalt tetroxide catalyst and a porous carbon catalyst intercalated with a transition metal. The raw materials for preparing the supported cobalt tetroxide catalyst include a carbon support, cobalt nitrate, and polyethylene glycol.

2. The high-efficiency catalyst for aniline production according to claim 1, characterized in that: The mass ratio of the supported cobalt tetroxide catalyst to the porous carbon catalyst with intercalated transition metals is 0.2-0.4:

1.

3. The high-efficiency catalyst for aniline production according to claim 1, characterized in that: The porous carbon catalyst with intercalated transition metal is a porous carbon catalyst with intercalated nickel.

4. The high-efficiency catalyst for aniline production according to claim 2, characterized in that: The preparation method of the supported cobalt tetroxide catalyst includes the following steps: After ultrasonic treatment of a mixture of carbon support, first polyethylene glycol, and organic alcohol, the mixture was added to a reaction vessel. The temperature of the reaction vessel was controlled at 40-50℃. Then, under magnetic stirring, cobalt nitrate solution and inorganic alkali solution were added dropwise to the reaction vessel. After the addition was completed, the pH of the system was controlled at 9-10. After the reaction was completed, a strong oxide solution was added and stirred evenly. The mixture was then aged, washed, dried, calcined, and cooled to obtain a supported cobalt tetroxide catalyst.

5. The high-efficiency catalyst for aniline production according to claim 4, characterized in that: The method for preparing the carbon support includes the following steps: After mixing and stirring the chloride salt, carbon source, and water evenly, continue stirring at 80-90℃ until a viscous liquid is formed. Then, dry and carbonize the liquid. After carbonization, wash and dry to obtain the carbon carrier.

6. The high-efficiency catalyst for aniline production according to claim 2, characterized in that: The raw materials for preparing the porous carbon catalyst with embedded noble metals include nickel-containing solutions and honeycomb ceramics.

7. The high-efficiency catalyst for aniline production according to claim 6, characterized in that: The method for preparing the porous carbon catalyst with embedded transition metal includes the following steps: Phenol, aldehydes, nickel-containing solution, and second polyethylene glycol are stirred until dissolved. The pH of the system is adjusted to 8-10, and then polymerized at 60-80℃ for 2-5 hours to obtain an impregnation solution. The honeycomb ceramic is immersed in the above impregnation solution. After full impregnation, the excess resin in the pores is blown away. The impregnated honeycomb ceramic is placed in a mixed atmosphere for full curing, and then calcined, carbonized, reduced, and cooled to obtain a porous carbon catalyst with intercalated transition metals.

8. The high-efficiency catalyst for aniline production according to claim 7, characterized in that: The honeycomb ceramic includes at least one of silicon carbide honeycomb ceramic, aluminum titanate honeycomb ceramic, and mullite honeycomb ceramic.

9. The high-efficiency catalyst for aniline production according to claim 4, characterized in that: The strong oxide solution includes at least one of hydrogen peroxide solution and potassium permanganate solution.

10. The high-efficiency catalyst for aniline production according to claim 5, characterized in that: The carbon source includes at least one of glucose, starch, sucrose, and cyclodextrin.

Images