Lattice oxygen-driven electronegativity enhanced multi-center ozone catalyst for treating wastewater as well as preparation method and application of lattice oxygen-driven electronegativity enhanced multi-center ozone catalyst
By introducing electronegativity enhancer and metal active agent on the alumina framework to form a multi-center structure ozone catalyst, the problems of low efficiency and easy loss of components of the existing catalyst are solved, and efficient reactive oxygen generation and wastewater treatment are achieved.
Patent Information
- Application Number
- CN202510289551.2
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-03-12
- Publication Date
- 2025-04-11
- Estimated Expiration
- 2045-03-12
AI Technical Summary
The existing heterogeneous ozone catalysts have low efficiency in converting ozone to reactive oxygen species and are prone to loss of catalytic components.
Alumina is used as a skeleton, and the introduction of electronegative enhancer, oxygen deletion promoter and metal active agent is used to form a metal-non-metal multi-center structure, and a lattice oxygen-driven electronegative enhancement multi-center ozone catalyst is prepared through multi-stage heating calcination.
It significantly improves the efficiency of converting ozone into reactive oxygen species, enhances the stability and life of the catalyst, and improves the deep treatment capacity of difficult-to-degrade industrial and municipal wastewater.
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Figure CN119793445A_ABST
Abstract
Description
Technical Field
[0001] The invention belongs to the technical field of wastewater treatment, and relates to a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, a preparation method and an application thereof. Background Art
[0002] With the development of technology, new and stubborn organic pollutants continue to appear in industrial enterprises and municipal wastewater, such as persistent organic pollutants, endocrine disruptors, antibiotics, microplastics, chlordane, polychlorinated biphenyls, hexachlorobenzene, hexabromobiphenyl, dioxins, furans, etc. These organic pollutants have the characteristics of environmental persistence, bioaccumulation, and long-range environmental migration potential, which can cause endocrine disruption, reproductive and developmental toxicity, neurotoxicity and immunotoxicity to the human body, or have adverse effects on the ecological environment.
[0003] The above organic pollutants are difficult to remove using conventional water treatment technologies. Catalytic ozone oxidation is a technology developed in recent years for deep treatment of organic pollution in wastewater. It can use catalysts to convert ozone into hydroxyl radicals (•HO), superoxide anion radicals (•O2 - ) and other more active reactive oxygen species (ROS), which convert new and stubborn organic pollutants into small molecular compounds or completely mineralize them into carbon dioxide and water, thus improving the catalytic conversion of ozone into •HO, •O2 - The efficiency of active oxygen is a key issue that needs to be solved urgently.
[0004] The mechanism of ozone catalytic conversion to reactive oxygen species mainly includes: (1) surface hydroxyl groups, (2) generation of reactive oxygen species and (3) catalyst charge balance. Among them, (1) surface hydroxyl groups are: in the solution, due to the introduction of metal and non-metal active sites, water molecules are strongly adsorbed on the surface of the catalyst, and then the Lewis acid sites on the catalyst surface coordinate with the water molecules adsorbed on the surface, resulting in the dissociation of water into surface hydroxyl groups M-OH. (2) The generation of reactive oxygen species mainly includes two pathways: (a) Ozone connects with the hydroxyl groups in the catalyst through electrostatic attraction or hydrogen bonds, and undergoes a series of chain reactions through electron transfer to produce ROS, such as •HO3 (ozone acid radicals), •HO, •O2 - and 1 O2 (singlet oxygen radical), etc. (b) Ozone reacts with the catalytic active sites on the catalyst. The metal ions act as active sites to transfer electrons to the intermediates or act as deoxidizers, weakening the HO and OO bonds, and the intermediates decompose into •O2 - The typical chain reaction of •HO2- and •HO2- will be initiated on the catalyst surface and in the liquid phase, leading to the generation of free radicals and the formation of ROS, such as •HO, •O2 - , HO2 -(superoxide anion free) and 1 O2. (3) Catalyst charge balance means that in order to maintain the charge balance on the catalyst, under the conditions of ozone and pollutant reaction, high-valent metal ions must be converted to low-valent metal ions. Finally, electrons overflow from lattice oxygen to generate oxygen, and high-valent metal ions are reduced to low-valent metal ions, completing M n+ / M n+1 Cycle. Lattice oxygen loses electrons and is oxidized to oxygen, and a hole is formed at the original lattice oxygen position. In an oxygen-rich state, the hole conducts electricity and is quickly reduced to lattice oxygen, thereby ensuring a continuous supply of oxygen and catalytic activity. Therefore, the cyclic transformation process of lattice oxygen and oxygen vacancies is the key step of the entire reaction and also the driving force.
[0005] Based on the above-mentioned mechanism of ozone catalytic conversion into active oxygen, existing ozone catalysts can be divided into homogeneous and heterogeneous according to the method of addition. Heterogeneous ozone catalysts are widely used in the water treatment industry due to their advantages such as easy separation and recovery and no secondary pollution. However, existing heterogeneous ozone catalysts generally have disadvantages such as low efficiency of ozone conversion into active oxygen and easy loss of catalytic components. Summary of the invention
[0006] The purpose of the present invention is to provide a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, a preparation method and an application thereof, so as to solve the problems of low efficiency of ozone conversion into active oxygen and easy loss of catalytic components in existing heterogeneous ozone catalysts.
[0007] To achieve the above object, the present invention adopts the following technical solutions: The present application provides a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater. The catalyst uses aluminum oxide as a skeleton, uses an electronegativity enhancer to regulate the skeleton surface, is immersed in an oxygen vacancy promoter and a metal activator, and is finally prepared by multi-stage temperature-raising calcination.
[0008] Specifically, the preparation method of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater provided in the present application includes: S01: Mix the pretreated alumina skeleton with an electronegativity enhancer solution in a solid-liquid volume ratio of 1:(1-2), shake in a constant temperature shaker at 20°C for 8-10 hours, take out the alumina skeleton and dry it to obtain an electronegativity enhanced alumina skeleton; wherein the electronegativity enhancer solution is prepared from sucrose solution and urea solution.
[0009] The alumina skeleton is washed 3-4 times with deionized water to remove the impurities adsorbed and residual on the surface and in the internal pores of the alumina skeleton. It is placed in a forced air drying oven and dried at 105°C for 2 hours. After the temperature drops to room temperature, it is taken out to obtain a pretreated alumina skeleton. In this application, the alumina skeleton is an alumina particle with a particle size of 3-5 mm.
[0010] A sucrose solution with a concentration of 0.2-0.4 mol / L and a urea solution with a concentration of 0.2-0.4 mol / L were prepared respectively, and the sucrose solution and the urea solution were mixed at a volume ratio of 1:(2-4) to obtain an electronegativity enhancer solution.
[0011] The pretreated alumina skeleton and the electronegativity enhancer solution are mixed in a solid-liquid volume ratio of 1: (1-2) to obtain a solid-liquid mixture. The solid-liquid mixture is placed in a constant temperature shaker at 20°C and a rotation speed of 160rpm for 8-10 hours to allow the electronegativity enhancer solution to adhere to the surface or internal pores of the alumina skeleton through physical adsorption and / or chemical adsorption, and then attach functional groups to the alumina skeleton, so as to achieve the purpose of the electronegativity enhancer solution regulating the electron-acquiring ability of the alumina skeleton. After the shaking treatment, the alumina skeleton is taken out, placed in a forced air drying oven, and dried at 105°C for 2 hours to obtain an electronegativity enhanced alumina skeleton.
[0012] In addition, the introduction of electronegativity enhancers on the alumina skeleton can also increase the degree of bonding between the metal active components and the alumina skeleton, thereby making it difficult for the metal active components to be lost, thereby enhancing the stability of the catalyst and extending the life of the catalyst.
[0013] S02: Mix the electronegativity enhanced alumina framework and the impregnation solution, shake in a constant temperature shaker at 20° C. for 8-10 hours, take out the alumina framework and air dry it naturally to obtain an impregnated alumina framework. The impregnation solution is prepared from an oxygen vacancy promoter and a metal activator.
[0014] An oxygen vacancy promoter solution with a concentration of 0.2-0.4 mol / L and a metal activator solution with a concentration of 0.2-0.4 mol / L are respectively prepared, and the oxygen vacancy promoter solution and the metal activator solution are mixed in a volume ratio of (1.5-2):1 to form an impregnation solution. The oxygen vacancy promoter includes one of cerium nitrate, cobalt nitrate, and nickel nitrate, and the metal activator includes one of manganese nitrate, iron nitrate, and copper nitrate.
[0015] The electronegativity enhanced alumina framework and the impregnation liquid are mixed at a solid-liquid volume ratio of 1: (1-2) so that the electronegativity enhanced alumina framework is impregnated in the mixed liquid formed by the oxygen vacancy promoter and the metal activator. The electronegativity enhanced alumina framework and the impregnation liquid are placed in a constant temperature shaker at 20°C and a speed of 160rpm for 8-10 hours to allow the oxygen vacancy promoter and the metal activator to adhere to the alumina framework to form a metal-non-metal multi-center structure. After the shaking treatment, the alumina framework is taken out, placed in a tray, and naturally air-dried at room temperature for 24 hours to obtain an impregnated alumina framework impregnated with oxygen vacancy promoters and metal activators.
[0016] S03: Under N2 atmosphere, the impregnated alumina skeleton is heated to 200°C at a heating rate of 5°C / min and kept warm for 10 minutes, then heated to 400-500°C and kept warm for 60 minutes, and finally heated to 600-700°C and kept warm for 90 minutes, and calcined to obtain a multi-center ozone catalyst.
[0017] The impregnated alumina skeleton was placed in a N2 atmosphere furnace. Under the N2 atmosphere, the heating rate was set to 5°C / min. The temperature was first raised to 200°C and kept for 10 minutes, then raised to 400-500°C and kept for 60 minutes, and finally raised to 600-700°C and kept for 90 minutes. The lattice oxygen driven electronegativity enhanced multi-center ozone catalyst was calcined to obtain.
[0018] In the present application, a multi-stage temperature-raising calcination method can ensure that multiple metals are effectively decomposed at their respective temperatures. At the same time, after decomposition, they can be effectively combined with the alumina skeleton to prevent loss, and metal oxide catalytic components can also be produced.
[0019] The lattice oxygen driven electronegativity enhanced multi-center ozone catalyst in this application is used for deep treatment of industrial and municipal wastewater.
[0020] The present invention has the following beneficial effects: (1) Using alumina with a strong skeleton and stable chemical properties as the skeleton, introducing an electronegativity enhancer into the alumina skeleton can increase the degree of bonding between the metal active components and the alumina skeleton, thereby making the metal active components less likely to be lost, thereby enhancing the stability of the catalyst and making the catalyst life 1.5 times that of conventional existing catalysts.
[0021] (2) In the present application, after introducing an electronegativity enhancer onto the alumina skeleton, an oxygen vacancy promoter and a metal activator are introduced to form a metal-nonmetal multi-center structure, and the catalytic components are evenly dispersed, having high-efficiency and long-lasting catalytic performance.
[0022] (3) After the electronegativity enhancer is introduced into the alumina skeleton, the electronegativity on the surface of the alumina skeleton is enhanced, and then the acid sites on the alumina skeleton are increased, making the Lewis acid sites on the catalyst surface abundant. The metal-nonmetal multi-center structure formed by the introduction of oxygen vacancy promoters and metal activators allows water molecules to be strongly adsorbed on the surface of the catalyst, and then the Lewis acid sites on the catalyst surface coordinate with the water molecules adsorbed on the surface, achieving efficient surface hydroxyl M-OH, significantly increasing the amount of ozone converted into active free radicals such as hydroxyl radicals, accelerating the removal rate of target pollutants, and significantly improving the treatment efficiency.
[0023] (4) The catalyst is suitable for deep treatment of various difficult-to-degrade industrial and municipal wastewaters. When the inlet COD concentration is 150.0-90.0 mg / L, after 1 hour of reaction purification, the effluent COD reaches 20.0-40.0 mg / L, and the effluent BOD5 / COD value reaches 0.45-0.65, which is 10-20% higher than the removal efficiency of commercial catalysts. BRIEF DESCRIPTION OF THE DRAWINGS
[0024] Figure 1 This is a morphology of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared in Example 1 of the present application; Figure 2 This is a morphology of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared in Example 3 of the present application; Figure 3 This is a morphology of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared in Example 4 of the present application; Figure 4 This is an element distribution spectrum of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared in Example 1 of the present application before use; Figure 5 This is the element distribution spectrum of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared in Example 1 of the present application after use. DETAILED DESCRIPTION
[0025] The technical solution of the present invention is further explained and illustrated by means of specific embodiments below.
[0026] Example 1 The present application provides a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, and the preparation method of the catalyst includes: S101: After washing the alumina skeleton with deionized water three times, place it in a blast drying oven and dry it at 105°C for 2 hours. After the temperature drops to room temperature, take it out to obtain a pretreated alumina skeleton. Mix a sucrose solution with a concentration of 0.2 mol / L and a urea solution with a concentration of 0.2 mol / L in a volume ratio of 1:4 to obtain an electronegativity enhancer solution. Mix the pretreated alumina skeleton and the electronegativity enhancer solution in a solid-liquid volume ratio of 1:2, place it in a constant temperature shaker at 20°C and a speed of 160 rpm for 8 hours of shaking treatment. After the shaking treatment, take out the alumina skeleton, place it in a blast drying oven, and dry it at 105°C for 2 hours to obtain an electronegativity enhanced alumina skeleton.
[0027] S102: A 0.2 mol / L cerium nitrate solution and a 0.2 mol / L manganese nitrate solution are mixed at a volume ratio of 2:1 to form an impregnation solution. The electronegativity enhanced alumina framework is mixed with the impregnation solution at a solid-liquid volume ratio of 1:2, and is placed in a constant temperature shaker at 20°C and a rotation speed of 160 rpm for 8 hours of shaking. After the shaking treatment, the alumina framework is taken out, placed in a tray, and naturally air-dried at room temperature for 24 hours to obtain an impregnated alumina framework impregnated with cerium nitrate and manganese nitrate.
[0028] S103: Place the impregnated alumina skeleton into a N2 atmosphere furnace. Under the N2 atmosphere, set the heating rate to 5°C / min, first heat to 200°C and keep warm for 10 minutes, then heat to 500°C and keep warm for 60 minutes, and finally heat to 600°C and keep warm for 90 minutes, and calcine to obtain a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst.
[0029] Example 2 The present application provides a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, and the preparation method of the catalyst includes: S201: After washing the alumina skeleton with deionized water for 4 times, place it in a blast drying oven and dry it at 105°C for 2 hours. After the temperature drops to room temperature, take it out to obtain a pretreated alumina skeleton. Mix a sucrose solution with a concentration of 0.3 mol / L and a urea solution with a concentration of 0.3 mol / L in a volume ratio of 1:3 to obtain an electronegativity enhancer solution. Mix the pretreated alumina skeleton and the electronegativity enhancer solution in a solid-liquid volume ratio of 1:1, place it in a constant temperature shaker at 20°C and a speed of 160 rpm for oscillation treatment for 10 hours. After the oscillation treatment, take out the alumina skeleton, place it in a blast drying oven, and dry it at 105°C for 2 hours to obtain an electronegativity enhanced alumina skeleton.
[0030] S202: A 0.3 mol / L cerium nitrate solution and a 0.3 mol / L manganese nitrate solution are mixed at a volume ratio of 2:1 to form an impregnation solution. The electronegativity enhanced alumina framework is mixed with the impregnation solution at a solid-liquid volume ratio of 1:1, and is placed in a constant temperature shaker at 20°C and a rotation speed of 160 rpm for oscillation treatment for 10 hours. After the oscillation treatment, the alumina framework is taken out, placed in a tray, and naturally air-dried at room temperature for 24 hours to obtain an impregnated alumina framework impregnated with cerium nitrate and manganese nitrate.
[0031] S203: Place the impregnated alumina skeleton into a N2 atmosphere furnace. Under the N2 atmosphere, set the heating rate to 5°C / min, first heat to 200°C and keep warm for 10 minutes, then heat to 400°C and keep warm for 60 minutes, and finally heat to 700°C and keep warm for 90 minutes, and calcine to obtain a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst.
[0032] Example 3 The present application provides a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, and the preparation method of the catalyst includes: S301: After washing the alumina skeleton with deionized water three times, place it in a blast drying oven and dry it at 105°C for 2 hours. After the temperature drops to room temperature, take it out to obtain a pretreated alumina skeleton. Mix a sucrose solution with a concentration of 0.2 mol / L and a urea solution with a concentration of 0.2 mol / L in a volume ratio of 1:4 to obtain an electronegativity enhancer solution. Mix the pretreated alumina skeleton and the electronegativity enhancer solution in a solid-liquid volume ratio of 1:2, place it in a constant temperature shaker at 20°C and a speed of 160 rpm for oscillation treatment for 8 hours. After the oscillation treatment, take out the alumina skeleton, place it in a blast drying oven, and dry it at 105°C for 2 hours to obtain an electronegativity enhanced alumina skeleton.
[0033] S302: A 0.2 mol / L cerium nitrate solution and a 0.2 mol / L ferric nitrate solution are mixed at a volume ratio of 1.5:1 to form an impregnation solution. The electronegativity enhanced alumina framework is mixed with the impregnation solution at a solid-liquid volume ratio of 1:2, and is placed in a constant temperature shaker at 20°C and a rotation speed of 160 rpm for 8 hours of shaking. After the shaking treatment, the alumina framework is taken out, placed in a tray, and naturally air-dried at room temperature for 24 hours to obtain an impregnated alumina framework impregnated with cerium nitrate and ferric nitrate.
[0034] S303: Place the impregnated alumina skeleton into a N2 atmosphere furnace. Under the N2 atmosphere, set the heating rate to 5°C / min, first heat to 200°C and keep warm for 10 minutes, then heat to 500°C and keep warm for 60 minutes, and finally heat to 600°C and keep warm for 90 minutes, and calcine to obtain a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst.
[0035] Example 4 The present application provides a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, and the preparation method of the catalyst includes: S401: After washing the alumina skeleton with deionized water for 4 times, place it in a forced air drying oven and dry it at 105°C for 2 hours. After the temperature drops to room temperature, take it out to obtain a pretreated alumina skeleton. Mix a sucrose solution with a concentration of 0.4 mol / L and a urea solution with a concentration of 0.4 mol / L in a volume ratio of 1:2 to obtain an electronegativity enhancer solution. Mix the pretreated alumina skeleton and the electronegativity enhancer solution in a solid-liquid volume ratio of 1:2, place it in a constant temperature shaker at 20°C and a speed of 160 rpm for oscillation treatment for 8 hours. After the oscillation treatment, take out the alumina skeleton, place it in a forced air drying oven, and dry it at 105°C for 2 hours to obtain an electronegativity enhanced alumina skeleton.
[0036] S402: A 0.4 mol / L cerium nitrate solution and a 0.4 mol / L copper nitrate solution are mixed at a volume ratio of 2:1 to form an impregnation solution. The electronegativity enhanced alumina framework is mixed with the impregnation solution at a solid-liquid volume ratio of 1:2, and is placed in a constant temperature shaker at 20°C and a rotation speed of 160 rpm for 8 hours of shaking. After the shaking treatment, the alumina framework is taken out, placed in a tray, and naturally air-dried at room temperature for 24 hours to obtain an impregnated alumina framework impregnated with cerium nitrate and copper nitrate.
[0037] S403: Place the impregnated alumina skeleton into a N2 atmosphere furnace. Under the N2 atmosphere, set the heating rate to 5°C / min, first heat to 200°C and keep warm for 10 minutes, then heat to 500°C and keep warm for 60 minutes, and finally heat to 700°C and keep warm for 90 minutes, and calcine to obtain a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst.
[0038] The present application examples respectively photographed the lattice oxygen driven electronegativity enhanced multi-center ozone catalysts prepared in Examples 1, 3, and 4 to obtain the surface morphologies of the catalysts, as shown in the attached drawings. Figure 1-3 As shown. Figure 1-3 It can be seen that the lattice oxygen driven electronegativity enhanced multi-center ozone catalysts prepared in the examples of the present application are all spherical, and their colors show different colors due to the different selection of oxygen vacancy promoters and metal activators.
[0039] In order to prove that the catalyst prepared in the examples of the present application has good stability, the element distribution of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared in Example 1 was detected before and after use, and the attached Figure 4 , 5 . Figure 4 , 5 It can be seen that before and after use, elements such as Ce, Mn, C, N, and O were detected in the catalyst. The elements were evenly distributed before and after use, and the element distribution remained stable, which shows that the catalyst has good stability during use.
[0040] In order to prove that the catalyst prepared by the embodiment of the present application can deeply treat industrial and municipal wastewater, the embodiment of the present application takes 500mL of the catalyst prepared by Examples 1-4 respectively, takes the refining biochemical reaction effluent collected from the refinery as the treatment object, takes the commercial catalyst-copper-based ozone catalyst as the comparative example, and adopts continuous reaction to carry out performance evaluation. Among them, the COD of the refining biochemical reaction effluent is 102.60mg / L, the flow rate is 0.6 L / min, and the ozone dosage per minute is 3mg / L. Samples were taken at 0 min, 15 min, 30 min, 45min and 60 min, and the COD value of each group of sampled water was detected. Each embodiment group repeated the experiment 10 times, took the average value, and obtained the results shown in Table 1.
[0041] Table 1: Performance evaluation results of various embodiments As can be seen from Table 1, after 60min catalyst treatment, the COD removal rate of the commercial catalyst is 58.83%, and the effluent COD is 42.24 mg / L. The catalyst provided in the embodiment of the present application has a COD removal effect of more than 50% when treating 15min; and, when treating 60min, the COD removal rates are 75.52%, 68.89%, 70.57% and 75.83%, respectively, which are 16.69%, 10.06%, 11.74% and 17% higher than commercial catalysis, respectively, which shows that the catalyst prepared by the embodiment of the present application can deeply treat industrial wastewater, and the treatment effect is good. In addition, after repeating the experiment 10 times, the removal efficiency of the catalyst of each embodiment is basically not reduced, which shows that the catalyst prepared by the embodiment of the present application is relatively stable.
[0042] The above description is only the preferred embodiment of the present application and is not intended to limit the present application. For those skilled in the art, the present application may have various modifications and variations. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present application shall be included in the protection scope of the present application.
Claims
1. A lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater, characterized in that: The catalyst uses aluminum oxide as a skeleton, uses an electronegativity enhancer to regulate the skeleton surface, is immersed in an oxygen vacancy promoter and a metal activator, and is prepared by calcination.
2. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 1, characterized in that: include: The pretreated alumina framework and the electronegativity enhancer solution are mixed in a solid-liquid volume ratio of 1: (1-2), shaken in a constant temperature shaker at 20° C. for 8-10 hours, and the alumina framework is taken out and dried to obtain an electronegativity enhanced alumina framework; wherein the electronegativity enhancer solution is prepared from a sucrose solution and a urea solution; The electronegativity enhanced alumina skeleton and the impregnation solution are mixed, shaken in a constant temperature shaker at 20° C. for 8-10 hours, and the alumina skeleton is taken out and naturally air-dried to obtain an impregnated alumina skeleton; wherein the impregnation solution is prepared from an oxygen vacancy promoter and a metal activator; Under N2 atmosphere, the impregnated alumina skeleton is heated to 200°C at a heating rate of 5°C / min and kept for 10 min, then heated to 400-500°C and kept for 60 min, and finally heated to 600-700°C and kept for 90 min, and calcined to obtain a lattice oxygen driven electronegativity enhanced multi-center ozone catalyst.
3. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 2, characterized in that: The pretreatment of the alumina skeleton comprises: washing the alumina skeleton with deionized water for 3-4 times, drying at 105° C. for 2 hours, and obtaining a pretreated alumina skeleton after the temperature drops to room temperature.
4. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 2, characterized in that: The electronegativity enhancer solution is prepared by mixing a sucrose solution with a concentration of 0.2-0.4 mol / L and a urea solution with a concentration of 0.2-0.4 mol / L in a volume ratio of 1:(2-4).
5. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 2, characterized in that: The volume ratio of the oxygen vacancy promoter to the metal activator is (1.5-2):
1.
6. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 5, characterized in that: The oxygen vacancy promoter includes one of cerium nitrate, cobalt nitrate and nickel nitrate.
7. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 5, characterized in that: The metal activator includes one of manganese nitrate, iron nitrate and copper nitrate.
8. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 5, characterized in that: The solid-liquid volume ratio of the electronegativity enhanced alumina skeleton to the impregnation liquid is 1:(1-2).
9. The method for preparing the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst for treating wastewater according to claim 2, characterized in that: The rotation speed of the constant temperature shaker is 160 rpm.
10. Use of the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst according to claim 1 or the lattice oxygen driven electronegativity enhanced multi-center ozone catalyst prepared by any one of the methods of claims 2 to 9 in deep treatment of industrial and municipal wastewater.
Citation Information
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