High-entropy alloy oxide for catalytic oxidation of toluene as well as preparation method and application of high-entropy alloy oxide

The preparation of CeCoCuFeMn high-entropy alloy oxide catalysts by microwave-assisted coprecipitation method solves the problem of high cost of precious metal catalysts in the prior art, realizes the efficiency and stability of toluene catalytic oxidation, and is suitable for the purification of industrial toluene waste gas.

CN119771437APending Publication Date: 2025-04-08CHONGQING INST OF GREEN & INTELLIGENT TECH CHINESE ACAD OF SCI
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Patent Information

Application Number
CN202510003965.4
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-01-02
Publication Date
2025-04-08

AI Technical Summary

Technical Problem

The prior art relies on precious metal catalysts in toluene pollution control, resulting in high costs; although transition metal oxide catalysts have replacement potential, their catalytic activity and stability still need to be improved.

Method used

The CeCoCuFeMn high-entropy alloy oxide catalyst was prepared by microwave-assisted co-precipitation method. By introducing the mutual coupling of a variety of transition metal elements and rare earth elements, a heterogeneous structure is formed, the surface electronic structure of the catalyst is adjusted, and the catalytic oxidation performance of toluene is improved.

Benefits of technology

It achieves high efficiency and stability of toluene catalytic oxidation, has excellent catalytic activity and carbon dioxide selectivity, and is suitable for thermal catalytic oxidation and purification of industrial toluene waste gas.

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Abstract

The invention belongs to the technical field of atmospheric pollutant treatment, and particularly relates to a high-entropy alloy oxide for toluene catalytic oxidation and a preparation method and application thereof. The high-entropy alloy oxide is CeCoCuFeMn high-entropy alloy oxide, and contains five transition metal elements of Ce, Co, Cu, Fe and Mn and an element O. The CeCoCuFeMn high-entropy alloy oxide catalyst is prepared by adopting microwave irradiation, and the method comprises the following steps: mixing metal precursor salt with a precipitator, then co-precipitating, and carrying out microwave irradiation, aging, washing, filtering and roasting heat treatment on the precipitated mixture to obtain the high-entropy alloy oxide. The CeCoCuFeMn high-entropy alloy oxide has a good catalytic purification effect on toluene waste gas.
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Description

Technical Field

[0001] The invention belongs to the technical field of air pollutant treatment, and specifically relates to a high entropy alloy oxide for catalytic oxidation of toluene and a preparation method and application thereof. Background Art

[0002] The treatment of volatile organic pollutants (VOC) in industrial pollution has become one of the focuses of current environmental protection work. Toluene (C6H5CH3), as an important solvent and raw material in the organic chemical industry, is a typical volatile pollutant with hazardous characteristics such as acute toxicity, biological toxicity and mutagenicity. It is an important source of harm to the air environment and human health. Existing studies have shown that toluene has at least the following hazards:

[0003] 1) Air pollution: Toluene is an important precursor for the formation of ozone and secondary organic aerosol (SOA).

[0004] 2) Harm to human health: Toluene can enter the human body through the respiratory tract. Long-term exposure to a toluene-contaminated environment may cause symptoms such as dizziness, nausea, and vomiting. In severe cases, it may even lead to health problems such as damage to the nervous system and liver disease.

[0005] 3) Harm to the natural environment: Toluene can react with water vapor to form photochemical smog, which reduces air quality and affects plant growth and crop yields.

[0006] 4) Disruption of ecological balance: Toluene can also enter the ecosystem through soil and groundwater, polluting soil microorganisms and groundwater quality, and disrupting the ecological balance.

[0007] Therefore, promoting toluene pollution control is crucial to maintaining the ecological environment and human health.

[0008] Common treatment methods for toluene mainly include physical adsorption, chemical adsorption, gas phase purification, biological method, low temperature plasma technology, catalytic oxidation, etc. Catalytic oxidation method is widely used in toluene pollution control due to its advantages such as high treatment efficiency and no secondary pollution. However, although the use of precious metal catalysts is efficient, it is limited by the high cost of precious metal extraction, smelting and recovery. Transition metal oxide catalysts have gradually received attention and are considered to be the most likely catalyst to replace precious metals. Among them, high entropy alloy oxides (HEAs) based on a variety of transition metals, each element accounts for 5at% to 35at%, and the total entropy increase is greater than 1.5R. Through the mutual coupling of multiple components at the cation site and the regulation of defective oxygen vacancies, on the basis of giving full play to the comprehensive effects of high entropy oxides (high entropy effect, slow diffusion effect, severe lattice distortion effect, cocktail effect), the spatial disorder and lattice order characteristics of HEAs are regulated to improve the surface electronic structure of the material, so that HEAs show better toluene catalytic oxidation performance than single-component or two-component metal oxide catalysts.

[0009] Some existing technologies have studied high entropy catalysts. For example, CN114950475A patent discloses a low-temperature preparation method and application of a high entropy two-dimensional catalyst. The invention uses polyvinyl pyrrolidone as a template and metal salt as a precursor to form uniform two-dimensional nanosheets through freeze drying technology and air annealing to prepare Ce3CuMnCoLa 0.5 Zr 0.5 O 12.25 A high entropy catalyst, which can be used for the catalytic combustion of toluene. Summary of the invention

[0010] In view of this, the present invention provides a CeCoCuFeMn high entropy alloy oxide and a microwave-assisted preparation method thereof and application in catalytic oxidation of toluene. The metal elements contained in the CeCoCuFeMn high entropy alloy oxide include cerium (Ce), cobalt (Co), copper (Cu), iron (Fe) and manganese (Mn), and have the advantages of good catalytic activity, good thermal stability and low cost. The present invention adopts a microwave-assisted coprecipitation method to prepare the high entropy alloy oxide, and through microwave irradiation, the catalyst grain optimization and strong interaction between metals are achieved, so as to achieve the purpose of improving the catalyst mineralization rate and selectivity, and is suitable for the thermal catalytic oxidation purification of industrial toluene waste gas.

[0011] One of the objects of the present invention is to provide a high entropy alloy oxide for catalytic oxidation of toluene.

[0012] To achieve the above object, the present invention adopts the following technical solutions:

[0013] A high entropy alloy oxide for catalytic oxidation of toluene, the high entropy alloy oxide comprises five transition metal elements, Ce, Co, Cu, Fe and Mn, and an O element; the content of the transition metal elements ranges from 5at% to 35at%.

[0014] Preferably, the content of the transition metal element is in the range of 5 at % to 20 at %.

[0015] Furthermore, the high entropy alloy oxide has a heterogeneous structure.

[0016] A second object of the present invention is to provide a method for preparing the aforementioned high entropy alloy oxide based on microwave-assisted co-precipitation.

[0017] To achieve the above object, the present invention adopts the following technical solutions:

[0018] The method for preparing the aforementioned high entropy alloy oxide based on microwave assisted co-precipitation method comprises the following steps:

[0019] (1) dissolving precursor salts of Ce, Co, Cu, Fe and Mn and fully mixing them with a precipitant to obtain a mixed solution;

[0020] (2) The mixed solution obtained in step (1) is subjected to microwave irradiation heating treatment to remove moisture, and after cooling, it is aged, filtered, washed, and dried to obtain a high entropy alloy oxide precursor;

[0021] (3) The high entropy alloy oxide precursor obtained in step (2) is calcined to obtain CeCoCuFeMn high entropy alloy oxide.

[0022] Preferably, in step (1), the precursor salt is a precursor nitrate of Ce, Co, Cu, Fe, or Mn.

[0023] Most preferably, the precursor salts of Ce, Co, Cu, Fe and Mn include cerium nitrate hexahydrate, cobalt nitrate hexahydrate, copper nitrate trihydrate, iron nitrate nonahydrate and manganese nitrate tetrahydrate.

[0024] Furthermore, in step (1), the precipitant includes any one or more combinations of sodium hydroxide, urea, ammonium carbonate, ammonia water and ammonium bicarbonate.

[0025] Preferably, the ratio of the concentration of the precipitant anions to the concentration of the metal cations is 1.5-1.0:1, most preferably 1.2:1.

[0026] Preferably, in step (1), the concentration of the metal ion precursor solution is 0.1M to 1M, most preferably 0.1M; the content percentage of each metal cation is controlled to be 5at% to 35at%, preferably 5at% to 20at%.

[0027] Preferably, in step (2), the concentration of the precipitant is 0.5M to 1.5M, most preferably 0.6M.

[0028] Furthermore, the mixed solution obtained in step (1) is placed in a polytetrafluoroethylene tank for microwave irradiation heating treatment.

[0029] Preferably, the internal pressure environment of the polytetrafluoroethylene tank is controlled to be negative pressure.

[0030] Furthermore, in step (2), the microwave irradiation heating treatment conditions include: microwave output power is 0 to 1000 W, the output duty cycle is set to 10% to 100%, the heating treatment temperature is 50 to 100° C., and the heating treatment time is 0 to 20 min; the pressure control range is 0 to 0.1 MPa.

[0031] Preferably, in step (2), the microwave output power is 100-800 W, the output duty cycle is set to 100%, the heating treatment temperature is 100-110° C., the heating treatment time is 20 min; and the pressure control range is 10-20 kPa.

[0032] Preferably, in the microwave irradiation heating treatment, the microwave frequency is 2000-3000 MHz, most preferably 2450 MHz.

[0033] Furthermore, in step (2), the aging treatment is performed for 20 to 30 hours, preferably 24 hours.

[0034] Furthermore, in step (2), the drying temperature is 70 to 120° C. and the drying time is 10 to 15 hours.

[0035] Preferably, in step (2), the drying temperature is 80° C. and the drying time is 12 h.

[0036] Furthermore, in step (3), a calcination treatment is carried out in a tubular furnace.

[0037] Furthermore, in step (3), the calcination treatment atmosphere is oxygen, the calcination temperature is 400°C to 600°C, and the treatment time is 3 to 6 hours; the heating rate of the calcination process is controlled to be 1 to 10°C / min, and the oxygen flow rate is 40 to 200 ml / min.

[0038] Preferably, in step (3), the calcination temperature is 500° C. and the treatment time is 4 h; the temperature rise rate during the calcination process is controlled to be 2° C. / min and the oxygen flow rate is 100 ml / min.

[0039] As a preferred solution, the method specifically comprises the following steps:

[0040] (1) Precursor salts of Ce, Co, Cu, Fe and Mn are weighed according to a set molar ratio and dissolved in pure water, and the mixture is fully stirred to obtain a solution A;

[0041] (2) weighing an appropriate amount of precipitant and dissolving it in pure water to obtain solution B;

[0042] (3) slowly pouring the solution B obtained in step (2) into the stirred solution A, stirring and mixing to form a suspension;

[0043] (4) transferring the mixture obtained in step (3) into a polytetrafluoroethylene (PTFE) tank, placing the polytetrafluoroethylene tank in a microwave oven, and heating the tank under the conditions of set microwave power, output duty cycle, and tank pressure; after the tank temperature drops to room temperature, aging, filtering, washing, and drying are performed to obtain a high entropy alloy oxide precursor;

[0044] (5) The high entropy alloy oxide precursor obtained in step (4) is placed in a ceramic ark and calcined in a tube furnace under an oxygen atmosphere to obtain a CeCoCuFeMn high entropy alloy oxide catalyst.

[0045] The third object of the present invention is to provide an application of the aforementioned high entropy alloy oxide as or in the preparation of a catalyst for catalytic oxidation treatment of toluene pollution.

[0046] A fourth object of the present invention is to provide an application of the aforementioned high entropy alloy oxide in the catalytic oxidation reaction of toluene.

[0047] A fifth object of the present invention is to provide a production system for preparing the aforementioned high entropy alloy oxide.

[0048] To achieve the above object, the present invention adopts the following technical solutions:

[0049] A production system for preparing the aforementioned high entropy alloy oxide, the production system comprising a microwave irradiation treatment system, the microwave irradiation treatment system comprising a vacuum unit, a pressure control unit, a microwave generating unit, a thermocouple unit, and a polytetrafluoroethylene reaction unit; the polytetrafluoroethylene reaction unit is connected to the pressure control unit and the thermocouple unit, the vacuum unit is connected to the pressure control unit, and the polytetrafluoroethylene reaction unit is placed in the microwave generating unit; a mixed solution of a metal precursor salt and a precipitant is placed in the polytetrafluoroethylene reaction unit for microwave irradiation treatment, and the vacuum unit, pressure control unit, microwave generating unit, and thermocouple unit are used to control vacuum, pressure, microwave and temperature conditions respectively.

[0050] The beneficial effects of the present invention are:

[0051] (1) The present invention introduces the mutual coupling of d-zone transition metal elements (Mn, Fe, Co), ds-zone transition metal elements (Cu), and rare earth element cerium (Ce), and co-precipitates and mixes them through oxidation and roasting to form a heterogeneous high-entropy metal oxide phase. Based on the excellent oxygen storage and release capacity of cerium dioxide and the excellent valence change ability of transition metals, the electronic structure of the catalyst surface is adjusted, the adsorption and conversion capacity of oxygen intermediates is improved, the conversion rate of free oxygen and active oxygen in the catalytic oxidation process of toluene is accelerated, and a better and more stable catalytic oxidation effect of toluene is achieved.

[0052] (2) The present invention uses microwave irradiation to prepare CeCoCuFeMn high entropy alloy oxide nanocatalysts. The obtained high entropy alloy oxide catalyst has a more excellent carbon dioxide selectivity for the catalytic oxidation of toluene. The high entropy alloy oxide catalyst forms a composite state with multiple species as active centers and has good catalytic activity for the catalytic oxidation of toluene.

[0053] (3) The CeCoCuFeMn high entropy alloy oxide nanocatalyst provided by the present invention has a good catalytic purification effect on toluene waste gas with a concentration range of 100ppm to 3000ppm. BRIEF DESCRIPTION OF THE DRAWINGS

[0054] Figure 1 is the X-ray diffraction pattern of CeCoCuFeMn high entropy alloy oxide catalyst;

[0055] Figure 2 This is a diagram for evaluating the catalytic activity of CeCoCuFeMn high entropy alloy oxide catalyst;

[0056] Figure 3 is the mineralization rate diagram of CeCoCuFeMn high entropy alloy oxide catalyst;

[0057] Figure 4 is the selectivity diagram of CeCoCuFeMn high entropy alloy oxide catalyst;

[0058] Figure 5 This is the diagram of the microwave-assisted preparation equipment for CeCoCuFeMn high entropy alloy oxide catalyst. DETAILED DESCRIPTION

[0059] The technical solution of the present invention will be further described clearly and completely in conjunction with specific embodiments below. Obviously, the described embodiments are only part of the embodiments of the present invention, rather than all the embodiments. Therefore, based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative work belong to the protection scope of the present invention.

[0060] The present invention adopts microwave assisted coprecipitation method to prepare CeCoCuFeMn high entropy alloy oxide catalyst, and the microwave assisted preparation equipment used is as follows Figure 5 The microwave irradiation treatment system includes a vacuum pump, a pressure controller, a microwave generator, a thermocouple, a polytetrafluoroethylene sealed tank, connecting pipes and a system control terminal.

[0061] In the examples of the present invention, the cerium nitrate hexahydrate, cobalt nitrate hexahydrate, copper nitrate trihydrate, iron nitrate nonahydrate and manganese nitrate tetrahydrate involved were purchased from Macklin.

[0062] Example 1. Microwave-assisted preparation method of CeCoCuFeMn high entropy alloy oxide catalyst

[0063] 1) Weigh 0.1 mol of precursor nitrates corresponding to the elements Ce, Co, Cu, Fe, and Mn, i.e., cerium nitrate hexahydrate, cobalt nitrate hexahydrate, copper nitrate trihydrate, iron nitrate nonahydrate, and manganese nitrate tetrahydrate, and dissolve the weighed nitrates in 200 ml of pure water. Stir and ultrasonically treat at room temperature for 1 h to achieve sufficient mixing to prepare a solution A.

[0064] 2) Weigh 0.6 mol of sodium hydroxide and dissolve it in 0.6 L of pure water to prepare a precipitant, which is recorded as solution B.

[0065] 3) The solution B obtained in step 2) is slowly poured into the solution A under stirring, and a precipitate is gradually generated to form a suspension. The ratio of the concentration of the precipitant anion to the concentration of the metal cation is 1.2:1.

[0066] 4) The mixture obtained in step 3) is placed in a polytetrafluoroethylene tank, and the polytetrafluoroethylene tank is placed in a microwave oven, and heated for 20 minutes under the conditions of a microwave power of 100 W, an output duty cycle of 100%, a microwave frequency of 2450 MHz, a tank pressure of 20 kPa, and a maximum temperature of 100° C.

[0067] 5) After the microwave stops, the cooled mixture is placed at room temperature for aging for 24 hours. After the aging is completed, the mixture is filtered to obtain a filter cake, and the filter cake is placed in an oven and dried at 80° C. for 12 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst precursor.

[0068] 6) The catalyst precursor obtained in step 5) is placed in a tube furnace, heated to 500°C at a heating rate of 2°C / min in an oxygen atmosphere (oxygen flow rate of 100 ml / min), and calcined for 4 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst. The phase structure of the obtained catalyst is as follows: Figure 1Calculations show that the content of each element is between 5at% and 20at%.

[0069] Example 2. Microwave-assisted preparation method of CeCoCuFeMn high entropy alloy oxide catalyst

[0070] 1) Weigh 0.2 mol of precursor nitrates corresponding to the elements Ce, Co, Cu, Fe, and Mn, i.e., cerium nitrate hexahydrate, cobalt nitrate hexahydrate, copper nitrate trihydrate, iron nitrate nonahydrate, and manganese nitrate tetrahydrate, and dissolve the weighed nitrates in 200 ml of pure water. Stir and ultrasonically treat at room temperature for 3 h to achieve sufficient mixing to prepare a solution A.

[0071] 2) Weigh 1.2 mol of sodium hydroxide and dissolve it in 1.2 L of pure water to prepare a precipitant, which is referred to as solution B.

[0072] 3) The solution B obtained in step 2) is slowly poured into the solution A under stirring, and a precipitate is gradually generated to form a suspension. The ratio of the concentration of the precipitant anion to the concentration of the metal cation is 1.2:1.

[0073] 4) The mixture obtained in step 3) is placed in a polytetrafluoroethylene tank, and the polytetrafluoroethylene tank is placed in a microwave oven, and heated for 20 minutes under the conditions of a microwave power of 600 W, a microwave frequency of 2450 MHz, an output duty cycle of 100%, a tank pressure of 10 kPa, and a maximum temperature controlled at 100° C.

[0074] 5) After the microwave stops, the cooled mixture is placed at room temperature for aging for 24 hours. After the aging is completed, the mixture is filtered to obtain a filter cake, and the filter cake is placed in an oven and dried at 80° C. for 12 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst precursor.

[0075] 6) The catalyst precursor obtained in step 5) is placed in a tube furnace, heated to 500°C at a heating rate of 2°C / min in an oxygen atmosphere (oxygen flow rate of 100 ml / min), and calcined for 4 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst. The phase structure of the obtained catalyst is as follows: Figure 1 Calculations show that the content of each element is between 5at% and 20at%.

[0076] (2) Application of CeCoCuFeMn high entropy alloy oxide catalysts in catalytic oxidation of toluene

[0077] Example 3. Microwave-assisted preparation method of CeCoCuFeMn high entropy alloy oxide catalyst

[0078] 1) Weigh 0.1 mol of precursor nitrates corresponding to the elements Ce, Co, Cu, Fe, and Mn, i.e., cerium nitrate hexahydrate, cobalt nitrate hexahydrate, copper nitrate trihydrate, iron nitrate nonahydrate, and manganese nitrate tetrahydrate, and dissolve the weighed nitrates in 200 ml of pure water. Stir and ultrasonically treat at room temperature for 1 h to achieve sufficient mixing to prepare a solution A.

[0079] 2) Weigh 0.6 mol of sodium hydroxide and dissolve it in 0.6 L of pure water to prepare precipitant solution B.

[0080] 3) The solution B obtained in step 2) is slowly poured into the solution A under stirring, and a precipitate is gradually generated to form a suspension. The ratio of the concentration of the precipitant anion to the concentration of the metal cation is 1.2:1.

[0081] 4) The mixture obtained in step 3) is placed in a polytetrafluoroethylene tank, and the polytetrafluoroethylene tank is placed in a microwave oven. After connecting the pipeline, the mixture is heated for 20 minutes under the conditions of microwave power of 800 W, microwave frequency of 2450 MHz, output duty cycle of 100%, tank pressure of 10 kPa, and maximum temperature of 110° C.

[0082] 5) After the microwave stops, the cooled mixture is placed at room temperature for aging for 24 hours. After the aging is completed, the mixture is filtered to obtain a filter cake, and the filter cake is placed in an oven and dried at 80° C. for 12 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst precursor.

[0083] 6) The catalyst precursor obtained in step 5) is placed in a tube furnace, heated to 500°C at a heating rate of 2°C / min in an oxygen atmosphere (oxygen flow rate of 100 ml / min), and calcined for 4 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst. The phase structure of the obtained catalyst is as follows: Figure 1 Calculations show that the content of each element is between 5at% and 20at%.

[0084] Comparative Example 1

[0085] (1) Conventional preparation method of CeCoCuFeMn high entropy alloy oxide catalyst

[0086] 1) Weigh 0.1 mol of precursor nitrates corresponding to the elements Ce, Co, Cu, Fe, and Mn, i.e., cerium nitrate hexahydrate, cobalt nitrate hexahydrate, copper nitrate trihydrate, iron nitrate nonahydrate, and manganese nitrate tetrahydrate, and dissolve the weighed nitrates in 200 ml of pure water. Stir and ultrasonically treat at room temperature for 1 h to achieve sufficient mixing to prepare a solution A.

[0087] 2) Weigh 0.6 mol of sodium hydroxide and dissolve it in 0.6 L of pure water to prepare precipitant solution B.

[0088] 3) The solution B obtained in step 2) is slowly poured into the solution A under stirring, and a precipitate is gradually generated to form a suspension. The ratio of the concentration of the precipitant anion to the concentration of the metal cation is 1.2:1.

[0089] 4) The mixture obtained in step 3) is aged at room temperature for 24 hours. After aging, the mixture is filtered to obtain a filter cake, and the filter cake is dried in an oven at 80° C. for 12 hours to obtain a CeCoCuFeMn high entropy alloy oxide catalyst precursor.

[0090] 5) The catalyst precursor obtained in step 4) was placed in a tube furnace, heated to 500°C at a heating rate of 2°C / min and calcined for 4 hours in an oxygen atmosphere (oxygen flow rate of 100 ml / min) to obtain a CeCoCuFeMn high entropy alloy oxide catalyst. The phase structure of the obtained catalyst is as follows: Figure 1 Calculations show that the content of each element is between 5at% and 20at%.

[0091] Example 4. Application of CeCoCuFeMn high entropy alloy oxide catalyst in catalytic oxidation of toluene

[0092] The toluene catalytic oxidation performance of the CeCoCuFeMn high entropy alloy oxide catalysts prepared in Examples 1 to 3 and Comparative Example 1 was further tested. The test reaction conditions were set as follows: initial toluene concentration of 1000 ppm, O2 concentration of 50%, balance gas N2, and space velocity of 60000 h -1 , the test temperature range is 100-300℃.

[0093] The toluene catalytic oxidation performance, mineralization rate and selectivity test results of each sample are shown as follows: Figure 2 , 3 As shown in Figures 4 and 5. It can be seen that the CeCoCuFeMn high entropy alloy oxides prepared in Examples 1 to 3 have higher mineralization rates and CO2 selectivity than the CeCoCuFeMn high entropy alloy oxides prepared in the comparative example, indicating that the CeCoCuFeMn high entropy alloy oxide catalysts prepared in Examples 1 to 3 can convert more toluene into harmless products.

Claims

1. A high entropy alloy oxide for catalytic oxidation of toluene, characterized in that: The high entropy alloy oxide comprises five transition metal elements, namely Ce, Co, Cu, Fe and Mn, and O element, and the content of the transition metal elements ranges from 5at% to 35at%.

2. A method for preparing the high entropy alloy oxide according to claim 1 based on microwave-assisted coprecipitation, characterized in that: The steps include: (1) dissolving precursor salts of Ce, Co, Cu, Fe and Mn and fully mixing them with a precipitant to obtain a mixed solution; (2) The mixed solution obtained in step (1) is subjected to microwave irradiation heating treatment to remove moisture, and after cooling, it is aged, filtered, washed, and dried to obtain a high entropy alloy oxide precursor; (3) The high entropy alloy oxide precursor obtained in step (2) is calcined to obtain CeCoCuFeMn high entropy alloy oxide.

3. The method according to claim 2, characterized in that In step (1), the precipitant includes any one or more combinations of sodium hydroxide, urea, ammonium carbonate, ammonia water and ammonium bicarbonate.

4. The method according to claim 2, characterized in that: In step (1), the ratio of the concentration of the precipitant anion to the concentration of the metal cation is 1.5 to 1.0:

1.

5. The method according to claim 2, characterized in that: In step (2), the microwave irradiation heating treatment conditions include: microwave output power is 0 to 1000 W, the output duty cycle is set to 10% to 100%, the heating treatment temperature is 50 to 100° C., and the heating treatment time is 0 to 20 min; the pressure control range is 0 to 0.1 MPa.

6. The method according to claim 2, characterized in that In step (2), the aging treatment is for 20 to 30 hours.

7. The method according to claim 2, characterized in that In step (3), the calcination treatment atmosphere is oxygen, the calcination temperature is 400°C to 600°C, and the treatment time is 3 to 6 hours; the heating rate of the calcination process is controlled to be 1 to 10°C / min, and the oxygen flow rate is 40 to 200 ml / min.

8. Use of the high entropy alloy oxide according to claim 1 as or in the preparation of a catalyst for catalytic oxidation treatment of toluene pollution.

9. Use of the high entropy alloy oxide according to claim 1 in the catalytic oxidation reaction of toluene.

10. A production system for preparing the high entropy alloy oxide according to claim 1, characterized in that: The production system comprises a microwave irradiation treatment system, which comprises a vacuum unit, a pressure control unit, a microwave generating unit, a thermocouple unit, and a polytetrafluoroethylene reaction unit; the polytetrafluoroethylene reaction unit is connected to the pressure control unit and the thermocouple unit, the vacuum unit is connected to the pressure control unit, and the polytetrafluoroethylene reaction unit is placed in the microwave generating unit; a mixed liquid of a metal precursor salt and a precipitant is placed in the polytetrafluoroethylene reaction unit for microwave irradiation treatment, and the vacuum unit, the pressure control unit, the microwave generating unit, and the thermocouple unit are used to control vacuum, pressure, microwave and temperature conditions respectively.