A method for regenerating a deactivated Fe-ZSM-5 molecular sieve catalyst
The inactivated Fe-ZSM-5 molecular sieve catalyst is treated by surfactant, persulfate and magnesium sulfate aqueous solution, and the carbon deposit is oxidized and degraded, solving the problem of catalyst deactivation due to carbon deposits, achieving a low-cost and efficient catalyst regeneration effect.
Patent Information
- Application Number
- CN202310932216.0
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2023-07-27
- Publication Date
- 2025-07-18
- Estimated Expiration
- 2043-07-27
AI Technical Summary
In the phenol reaction of benzene oxynitride oxide synthesis, Fe-ZSM-5 molecular sieve catalyst is inactivated due to carbon deposits, and the existing regeneration methods are high in energy consumption, high cost and unsafe, making it difficult to restore catalytic activity.
The aqueous solution of surfactant, persulfate and magnesium sulfate is contacted with the inactivated Fe-ZSM-5 molecular sieve catalyst, combined with air treatment, and carbon deposits are degraded through sulfate radical oxidation to restore catalytic activity.
The catalyst is regenerated and restored to the level of fresh catalyst, which is simple to operate, low cost and safe, and has good catalytic activity recovery.
Abstract
Description
Technical Field
[0001] The present invention belongs to the technical field of catalysts, and relates to a method for regenerating a deactivated Fe-ZSM-5 molecular sieve catalyst, specifically a method for regenerating a deactivated Fe-ZSM-5 molecular sieve catalyst in the reaction of synthesizing phenol by oxidizing benzene with dinitrogen monoxide. Background Art
[0002] In the industrial production process of synthesizing adipic acid by oxidizing cyclohexanol / cyclohexanone with nitric acid, a large amount of dinitrogen monoxide gas is emitted. Although the content of dinitrogen monoxide in the atmosphere is very low, the greenhouse effect it can cause is 300 times that of carbon dioxide, and it has been considered the third largest greenhouse gas after carbon dioxide and methane (Science and Technology Daily, 2013-11-23(002)).
[0003] In addition, dinitrogen monoxide has a long residence time in the atmosphere, can participate in many photochemical reactions in the atmosphere, and can be transported to the stratosphere to destroy the ozone layer. If no measures are taken to limit its emissions, it will become one of the most destructive ozone-depleting substances (Chemistry Bulletin, 2023, 86(02): 244-248).
[0004] Therefore, in the industrial synthesis of adipic acid, the treatment of dinitrogen monoxide has become the key to realizing clean production. There are mainly three traditional methods for treating industrial waste gas of dinitrogen monoxide: The first is to burn dinitrogen monoxide with fuels such as natural gas, that is, the high-temperature decomposition method. This method requires the temperature to be controlled above 1000°C, with high energy consumption and high requirements for equipment. The second is to decompose dinitrogen monoxide with a catalyst, that is, the catalytic decomposition method. This method is further divided into selective catalytic reduction method and direct catalytic decomposition method. Among them, the selective catalytic reduction method requires continuous addition of reducing agents such as CO and CH4, and is prone to produce toxic by-products, while the direct catalytic decomposition method uses noble metals, metal oxides or molecular sieves as catalysts to decompose dinitrogen monoxide into N2 and O2 at about 400°C, with a relatively high conversion rate and relatively low cost. The third is to convert dinitrogen monoxide into nitric oxide or nitrogen dioxide, and then convert it into nitric acid for recycling, that is, the regeneration reduction method. This method has high requirements for equipment and requires the use of expensive noble metal catalysts.
[0005] Researchers such as Panov in Russia developed a green technology route for turning waste into treasure for the treatment of nitrous oxide (Journal of Catalysis 2008, 254 (1), 110 - 120.). Using Fe-ZSM-5 molecular sieve as a catalyst, nitrous oxide is used as an oxidant to react with benzene at 300 - 400 °C to produce phenol. This reaction has high conversion and selectivity, and the obtained phenol has high economic value. It can also be hydrogenated to obtain cyclohexanone, which can be used as a raw material for the production of products such as adipic acid / caprolactam. If this process is successfully developed and widely applied, certain economic benefits can be achieved while solving environmental problems.
[0006] However, during the reaction of nitrous oxide oxidizing benzene to produce phenol, due to the relatively high reaction temperature, the catalyst is prone to carbon deposition deactivation. Summary of the Invention
[0007] In view of this, the present invention proposes a new method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst in the reaction of nitrous oxide oxidizing benzene to synthesize phenol. The present invention has the advantages of simple operation, no need for high-temperature calcination, mild conditions, low cost, high safety, etc., and the performance of the catalyst after regeneration can reach the level of fresh catalyst.
[0008] To achieve the above object, the technical solution adopted by the present invention is as follows:
[0009] A method for regenerating a deactivated Fe-ZSM-5 molecular sieve catalyst, and the specific steps of this method are: fully contacting the deactivated Fe-ZSM-5 molecular sieve catalyst with an aqueous solution dissolved with a surfactant, persulfate, and magnesium sulfate, and blowing air for treatment at a temperature of 60 - 100 °C; then filtering, washing, and drying the treated Fe-ZSM-5 molecular sieve catalyst to obtain a regenerated Fe-ZSM-5 molecular sieve catalyst. The catalytic activity of the regenerated Fe-ZSM-5 molecular sieve catalyst obtained by the present invention can be restored to the level of fresh catalyst.
[0010] Furthermore, the surfactant is one or a complex of several of sodium dodecyl sulfonate, nonylphenol polyoxyethylene ether, octadecyl trimethyl ammonium chloride, and dodecyl dimethyl betaine, and preferably nonylphenol polyoxyethylene ether.
[0011] Furthermore, the mass fraction of the surfactant in the aqueous solution is 0.2% - 1%, and preferably 0.5% - 0.8%.
[0012] Furthermore, the persulfate is one or a complex of several of potassium persulfate, sodium persulfate, and ammonium persulfate, and preferably potassium persulfate.
[0013] Further, the mass fraction of persulfate in the aqueous solution is 2% - 6%, preferably 3% - 5%.
[0014] Further, the mass fraction of magnesium sulfate in the aqueous solution is 0.1% - 0.5%, preferably 0.2% - 0.4%.
[0015] Further, the mass ratio of the deactivated Fe-ZSM-5 molecular sieve catalyst to the aqueous solution is 1:5 - 20, preferably 1:8 - 15.
[0016] Further, the time for air injection treatment is 2 - 12 hours. Among them, the temperature is preferably 80 - 90 °C, and the treatment time is preferably 4 - 8 hours.
[0017] Further, the flow rate of the injected air is such that the standard volume of air injected per hour per kilogram of the deactivated Fe-ZSM-5 molecular sieve catalyst is 0.1 - 1 cubic meters, preferably 0.3 - 0.6 cubic meters.
[0018] The chemical reaction principle of the present invention is as follows: Under the synergistic catalysis of iron on the surface of the molecular sieve and magnesium ions in the solution, persulfate generates sulfate radicals (SO4 •- ), which react with the carbon deposits in the Fe-ZSM-5 molecular sieve catalyst, oxidize and degrade the carbon deposits, reduce the adhesion to the Fe-ZSM-5 molecular sieve catalyst. The oxygen in the injected air improves the activation efficiency of persulfate and enhances the removal effect of organic substances. Under the action of the surfactant, the oxidized and degraded carbon deposits are dispersed into the aqueous solution, enabling the catalyst to recover its catalytic activity.
[0019] Compared with the prior art, the beneficial effects of the present invention are as follows:
[0020] The present invention has the advantages of simple operation, no need for high-temperature calcination, mild conditions, low cost, high safety, etc., and the performance of the regenerated catalyst can reach the level of fresh catalyst. Detailed Description of the Specific Embodiment
[0021] The following details the specific embodiments of the technical solution of the present invention, but the present invention is not limited to the following description. The reagents and raw materials used in the embodiments of the present invention are all commercially available.
[0022] The conditions for the reaction of benzene with nitrous oxide to produce phenol using Fe-ZSM-5 molecular sieve as the catalyst and nitrous oxide as the oxidant are as follows:
[0023] The reaction temperature is 320 °C, the pressure is slightly positive pressure, the molar ratio of nitrous oxide:benzene:nitrogen is 1:1:20, and the total gas hourly space velocity is 15000 mL·g -1 催化剂 ·h -1Taking the phenol yield as an index to evaluate the performance of the catalyst, the calculation method is as follows:
[0024] Phenol yield (%) = × 100%
[0025] After the continuous reaction ran for a period of time, the Fe-ZSM-5 molecular sieve catalyst (produced by Henan Shenma Catalysis Technology Co., Ltd.) began to coke and deactivate. The phenol yield decreased from 21.8% in the initial stage to 9.7%. It was necessary to regenerate the deactivated Fe-ZSM-5 molecular sieve catalyst. Example 1
[0026] Take a three-necked flask and successively add 100 g of water, 0.7 g of nonylphenol polyoxyethylene ether, 4 g of potassium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution under sufficient stirring. Heat to a temperature of 90 °C, and under heat preservation and stirring, blow in air at a flow rate of 5 L per hour for 6 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain the regenerated Fe-ZSM-5 molecular sieve catalyst.
[0027] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 in the reaction of catalytically producing phenol from dinitrogen monoxide and benzene, the phenol yield was 21.6%. Example 2
[0028] Take a three-necked flask and successively add 195 g of water, 0.40 g of nonylphenol polyoxyethylene ether, 4 g of potassium persulfate, and 0.2 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution under sufficient stirring. Heat to a temperature of 90 °C, and under heat preservation and stirring, blow in air at a flow rate of 10 L per hour for 8 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain the regenerated Fe-ZSM-5 molecular sieve catalyst.
[0029] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1Under the condition of, for the reaction of catalytically producing phenol from nitrous oxide and benzene, the yield of phenol is 20.5%. Example 3
[0030] Take a three-necked flask, and successively add 50 grams of water, 0.40 grams of nonylphenol polyoxyethylene ether, 3 grams of potassium persulfate, and 0.25 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 grams of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C, and under heat preservation and stirring, introduce air at a flow rate of 5 liters per hour for treatment for 8 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain a regenerated Fe-ZSM-5 molecular sieve catalyst.
[0031] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of nitrous oxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 for the reaction of catalytically producing phenol from nitrous oxide and benzene, the yield of phenol is 20.2%. Example 4
[0032] Take a three-necked flask, and successively add 100 grams of water, 0.7 grams of nonylphenol polyoxyethylene ether, 6 grams of potassium persulfate, and 0.4 grams of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 grams of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 100 °C, and under heat preservation and stirring, introduce air at a flow rate of 5 liters per hour for treatment for 2 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain a regenerated Fe-ZSM-5 molecular sieve catalyst.
[0033] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of nitrous oxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 for the reaction of catalytically producing phenol from nitrous oxide and benzene, the yield of phenol is 21.1%. Example 5
[0034] Take a three-necked flask and successively add 100 g of water, 0.7 g of nonylphenol polyoxyethylene ether, 6 g of potassium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution. Add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst. Under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 60 °C and introduce air at a flow rate of 2 L per hour under heat preservation and stirring for 12 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain the regenerated Fe-ZSM-5 molecular sieve catalyst.
[0035] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide: benzene: nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 it is used for the reaction of catalytically producing phenol from dinitrogen monoxide and benzene, and the yield of phenol is 20.0%. Example 6
[0036] Take a three-necked flask and successively add 100 g of water, 0.8 g of sodium dodecyl sulfate, 5 g of sodium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution. Add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst. Under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C and introduce air at a flow rate of 5 L per hour under heat preservation and stirring for 6 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain the regenerated Fe-ZSM-5 molecular sieve catalyst.
[0037] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide: benzene: nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 it is used for the reaction of catalytically producing phenol from dinitrogen monoxide and benzene, and the yield of phenol is 19.8%. Example 7
[0038] Take a three-necked flask and successively add 100 g of water, 0.6 g of octadecyltrimethylammonium chloride, 5 g of potassium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution. Add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C, and under heat preservation and stirring, introduce air at a flow rate of 5 L per hour for treatment for 6 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain a regenerated Fe-ZSM-5 molecular sieve catalyst.
[0039] For the regenerated catalyst, at a reaction temperature of 320 °C, a slightly positive pressure, a nitrous oxide:benzene:nitrogen molar ratio of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 under the conditions, it is used for the reaction of catalytically producing phenol from nitrous oxide and benzene, and the yield of phenol is 20.4%. Example 8
[0040] Take a three-necked flask and successively add 100 g of water, 0.6 g of dodecyldimethylbetaine, 6 g of ammonium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution. Add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C, and under heat preservation and stirring, introduce air at a flow rate of 5 L per hour for treatment for 6 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain a regenerated Fe-ZSM-5 molecular sieve catalyst.
[0041] For the regenerated catalyst, at a reaction temperature of 320 °C, a slightly positive pressure, a nitrous oxide:benzene:nitrogen molar ratio of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 under the conditions, it is used for the reaction of catalytically producing phenol from nitrous oxide and benzene, and the yield of phenol is 19.7%. Example 9
[0042] Take a three-necked flask and successively add 100 g of water, 0.3 g of sodium dodecyl sulfonate, 0.5 g of nonylphenol polyoxyethylene ether, 4 g of potassium persulfate, 1 g of ammonium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C and introduce air at a flow rate of 5 L per hour under heat preservation and stirring for 6 hours. Filter and wash the obtained molecular sieve, and then dry it at 150 °C for 4 hours to obtain the regenerated Fe-ZSM-5 molecular sieve catalyst.
[0043] For the regenerated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 , it is used in the reaction for catalyzing the formation of phenol from dinitrogen monoxide and benzene, and the yield of phenol is 21.3%. Example 10
[0044] Take a three-necked flask and successively add 100 g of water, 0.7 g of nonylphenol polyoxyethylene ether, 4 g of potassium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C and introduce air at a flow rate of 5 L per hour under heat preservation and stirring for 6 hours. Filter and wash the obtained molecular sieve catalyst, and then dry it at 150 °C for 4 hours.
[0045] For the treated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 , it is used in the reaction for catalyzing the formation of phenol from dinitrogen monoxide and benzene, and the yield of phenol is 21.6%. Comparative Example 1
[0046] Take a three-necked flask and successively add 100 g of water, 4 g of potassium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and under sufficient stirring, make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution. Heat to a temperature of 90 °C and introduce air at a flow rate of 5 L per hour under heat preservation and stirring for 6 hours. Filter and wash the obtained molecular sieve catalyst, and then dry it at 150 °C for 4 hours.
[0047] The processed catalyst was used in the reaction of catalytically producing phenol from nitrous oxide and benzene under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of nitrous oxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 , and the yield of phenol was 12.7%. Comparative Example 2
[0048] Take a three-necked flask, and successively add 100 g of water, 0.7 g of nonylphenol polyoxyethylene ether, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution. Add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution under sufficient stirring. Heat to a temperature of 90 °C, and bubble air at a flow rate of 5 L per hour under heat preservation and stirring for 6 hours. Filter and wash the obtained molecular sieve catalyst, and then dry it at 150 °C for 4 hours.
[0049] The processed catalyst was used in the reaction of catalytically producing phenol from nitrous oxide and benzene under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of nitrous oxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 , and the yield of phenol was 9.4%. Comparative Example 3
[0050] Take a three-necked flask, and successively add 100 g of water, 0.7 g of nonylphenol polyoxyethylene ether, and 4 g of potassium persulfate. Mix the above substances evenly to form an aqueous solution. Add 10 g of the above deactivated Fe-ZSM-5 molecular sieve catalyst, and make the deactivated Fe-ZSM-5 molecular sieve catalyst fully contact with the aqueous solution under sufficient stirring. Heat to a temperature of 90 °C, and bubble air at a flow rate of 5 L per hour under heat preservation and stirring for 6 hours. Filter and wash the obtained molecular sieve catalyst, and then dry it at 150 °C for 4 hours.
[0051] The processed catalyst was used in the reaction of catalytically producing phenol from nitrous oxide and benzene under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of nitrous oxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 , and the yield of phenol was 13.2%. Comparative Example 4
[0052] Take a three-necked flask and sequentially add 100 g of water, 0.7 g of nonylphenol polyoxyethylene ether, 4 g of potassium persulfate, and 0.4 g of magnesium sulfate. Mix the above substances evenly to form an aqueous solution, add 10 g of the deactivated Fe-ZSM-5 molecular sieve catalyst, and make the deactivated Fe-ZSM-5 molecular sieve catalyst contact fully with the aqueous solution under sufficient stirring. Heat to a temperature of 90 °C and treat for 6 hours under heat preservation and stirring. After filtering and washing the obtained molecular sieve catalyst, dry it at 150 °C for 4 hours.
[0053] For the treated catalyst, under the conditions of a reaction temperature of 320 °C, a slightly positive pressure, a molar ratio of dinitrogen monoxide:benzene:nitrogen of 1:1:20, and a total gas hourly space velocity of 15000 mL·g -1 催化剂 ·h -1 , it is used in the reaction for catalytically producing phenol from dinitrogen monoxide and benzene, and the yield of phenol is 13.5%.
[0054] It can be known from the comparison between the examples and comparative examples of the present invention that the deactivated Fe-ZSM-5 molecular sieve catalyst in the reaction of oxidizing benzene with dinitrogen monoxide to synthesize phenol is regenerated according to the method described in the present invention, and the activity of the regenerated Fe-ZSM-5 molecular sieve catalyst is restored well and is close to the activity of the fresh Fe-ZSM-5 molecular sieve catalyst.
[0055] Although the embodiments of the present invention have been shown and described, for those of ordinary skill in the art, it can be understood that various changes, modifications, substitutions, and variations can be made to these embodiments without departing from the principles and spirit of the present invention. The scope of the present invention is defined by the appended claims and their equivalents.
Claims
1. A method for regenerating a deactivated Fe-ZSM-5 molecular sieve catalyst, characterized in that, The specific steps of the method are as follows: The deactivated Fe-ZSM-5 molecular sieve catalyst is brought into full contact with an aqueous solution in which a surfactant, persulfate, and magnesium sulfate are dissolved, and air is introduced for treatment at a temperature of 60 - 100 °C; then the treated Fe-ZSM-5 molecular sieve catalyst is filtered, washed, and dried to obtain a regenerated Fe-ZSM-5 molecular sieve catalyst; The surfactant is a complex of one or more of sodium dodecyl sulfonate, nonylphenol polyoxyethylene ether, octadecyl trimethyl ammonium chloride, and dodecyl dimethyl betaine.
2. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, characterized in that, The mass fraction of the surfactant in the aqueous solution is 0.2% - 1%.
3. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, characterized in that, The persulfate is a complex of one or more of potassium persulfate, sodium persulfate, and ammonium persulfate.
4. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, characterized in that, The mass fraction of the persulfate in the aqueous solution is 2% - 6%.
5. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, characterized in that, The mass fraction of magnesium sulfate in the aqueous solution is 0.1% - 0.5%.
6. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, characterized in that, The mass ratio of the deactivated Fe-ZSM-5 molecular sieve catalyst to the aqueous solution is 1:5 - 20.
7. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, wherein The time for air introduction treatment is 2 - 12 hours.
8. The method for regenerating the deactivated Fe-ZSM-5 molecular sieve catalyst according to claim 1, characterized in that, The flow rate of the introduced air is such that the standard volume of air introduced per hour per kilogram of the deactivated Fe-ZSM-5 molecular sieve catalyst is 0.1 - 1 cubic meters.
Citation Information
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